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Uncertainties in a "Screening Limit" for

the Rate of Gas Generation from an


Intermediate-level Waste Package

To: Radioactive Waste Management Ltd.

Date: 14 March 2017

From: Amec Foster Wheeler

Your Reference: NPO002317

Our Reference: AMEC/000795/001 Issue 3


Document Issue Record
Title Uncertainties in a "Screening Limit" for the Rate of Gas Generation
from an Intermediate- level Waste Package

Prepared for Radioactive Waste Management Ltd.

Your reference NPO002317

Our reference AMEC/000795/001 Issue 3

Date 14 March 2017

Confidentiality, copyright & This report is submitted by Energy, Safety and Risk Consultants
reproduction (UK) Limited (hereafter referred to as Amec Foster Wheeler) in
connection with a contract to supply goods and/or services.

Contact Details Amec Foster Wheeler

Building 150

Thomson Avenue

Harwell Campus

DIDCOT

Oxfordshire OX11 0QB

United Kingdom

Tel +44 (0) 1635 280415

Fax +44 (0) 1635 280301

amecfw.com

Name Signature Date

Author(s) Andrew Hoch, Phil Bamforth † 14 March 2017

Reviewed
David Lever 14 March 2017
by

Approved
David Lever 14 March 2017
by

† Phil Bamforth Consultant


To minimise our impact on the environment, Amec Foster Wheeler uses paper from sustainable sources.

AMEC/000795/001 Issue 3 Page ii


Preface
This report has been prepared by Amec Foster Wheeler under contract to Radioactive Waste
Management Limited (RWM). The report has been reviewed by RWM, but the views expressed
and conclusions drawn are those of the authors and do not necessarily represent those of RWM.

CONDITIONS OF PUBLICATION

This report is made available under the RWM Transparency Policy. In line with this policy, RWM is
seeking to make information on its activities readily available, and to enable interested parties to
have access to and influence on its future programmes. The report may be freely used for
non-commercial purposes. RWM is a wholly owned subsidiary of the Nuclear Decommissioning
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permission from the NDA. All copyright, database rights and other intellectual property rights
reside with the NDA.

Applications for permission to use the report commercially should be made to the NDA Information
Manager.

Although great care has been taken to ensure the accuracy and completeness of the information
contained in this publication, the NDA cannot assume any responsibility for consequences that may
arise from its use by other parties.

© Nuclear Decommissioning Authority 2017 – all rights reserved.

BIBLIOGRAPHY

If you would like to see other reports available from RWM and the NDA, a complete listing can be
viewed at our website www.nda.gov.uk, or please write to us at the address below.

FEEDBACK

Readers are invited to provide feedback on this report and on the means of improving the range of
reports published. Feedback should be addressed to:

RWM Feedback
Radioactive Waste Management Limited
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Curie Avenue
Harwell Oxford
Didcot
OX11 0RH

Email: rwmfeedback@nda.gov.uk

AMEC/000795/001 Issue 3 Page iii


Foreword
The report describes modelling work undertaken during 2009, with an initial draft of this report
being produced in January 2013. Therefore, it reflects the state of knowledge, and references
reports that were available, at the time when the work was performed. The work follows that
described in A. Hoch, “Screening Limit” on the rate of Gas Generation from Individual Intermediate-
level Waste Packages, Amec Foster Wheeler Report SA/ENV-0888 Issue 3, 2017.

The objective of the work described in this report is to identify uncertainties in deriving a “screening
limit”, taking into account the process of backfilling, as well as the changing characteristics of the
backfill during setting and hardening. The modelling shows that the limit of the rate of gas
generation that could disrupt the Nirex Reference Vault Backfill during emplacement and early set
could be lower than that for a hardened backfill. However, there remained many uncertainties in the
modelling.

Subsequent to the work described in this report, RWM has undertaken an experimental study of
gas migration through the NRVB as it flows across a drum vent and cures. The results of that study
are described in: N. Bowmer, Potential Effects of Gas Release from Vented Waste Packages
during Backfill Emplacement on Properties of the Backfill, Nuclear Technologies Report R1492,
3 -1
NNL Report NNL(17)13807 Issue 5, 2017. That work showed that a gas flow of 7 dm h (the
lowest rate used in the study) was sufficient to form a single gas channel through fluid NRVB as it
cured.

Abstract
Previous work has attempted to establish a “screening limit” on the rate of gas generation from
individual vented intermediate-level waste packages below which gas should not pose a risk to the
integrity of a hardened cementitious backfill (NRVB). The work was not concerned with modelling
the gas generation processes in a waste package; rather, a constant gas generation rate was
assumed, and then an upper bound for that rate was determined, below which it was considered
unlikely that the backfill would crack. However, a caveat was added that:

“… the formation of the gas pathway is likely to be rapid, occurring


during the period when the backfill is curing and has low strength,
and could be associated with a very significant increase in gas
pressure inside the container. The model developed for the flow of
gas through the NRVB has limited validity while the properties of the
backfill material (e.g. porosity, permeability, and strength) are
evolving.”

The objective of this work is to identify uncertainties in deriving a “screening limit”, taking into
account the process of backfilling, as well as the changing characteristics of the backfill during
setting and hardening.

AMEC/000795/001 Issue 3 Page iv


Executive Summary
Radioactive Waste Management Limited (RWM) has prepared a “generic” Disposal System Safety
Case (DSSC) that considers: the safety of radioactive waste transport to a Geological Disposal
Facility (GDF); the safety of the construction and operation of a GDF; and the safety of the facility
in the very long term. The DSSC assumes that the GDF will have a disposal area for packages of
intermediate-level waste (ILW) and some low-level waste (LLW) separate from that for packages of
high-level waste (HLW) and spent fuel. In the case of either a higher strength host rock or a lower
strength sedimentary host rock, the illustrative disposal concept anticipates that ILW will be
disposed of in vaults, which will be backfilled with a cementitious material. The backfill serves a
number of purposes, including: providing mechanical stability; establishing alkaline conditions
(which would reduce both the corrosion rate of the steel waste containers and also the solubility of
some key radionuclides); and providing sorption sites for radionuclides. The candidate backfill for
the disposal of ILW in a higher strength host rock is the NRVB (Nirex Reference Vault Backfill).

The formation of gases by processes (e.g. corrosion of metal wastes, microbial degradation of
organic wastes, and radiolysis of porewater) that will occur in many of the waste packages is
unavoidable, and therefore gases may be generated during transport, in the course of operation
and after closure of a GDF. Many ILW and LLW containers will be vented to allow the gas to
escape and to avoid the build-up of pressure within the containers. If the gas from a waste
container emplaced in a vault backfilled with cementitious material were generated quickly and
could not flow sufficiently easily through the backfill, then the pressure within the container could
rise. If sufficient, the pressure rise could ultimately lead to fracturing of the hardened backfill.

Previous work attempted to establish a “screening limit” on the rate of gas generation from
individual waste packages, below which the gas should not affect the integrity of the backfill. The
work was not concerned with modelling the gas generation processes in a waste container; rather,
a constant gas generation rate was assumed, and then an upper bound for that rate was
3 -1
determined (10 m yr ), below which it was considered unlikely that hardened backfill material
would crack. However, a caveat to this conclusion was:

“… the formation of the gas pathway is likely to be rapid, occurring


during the period when the backfill is curing and has low strength,
and could be associated with a very significant increase in gas
pressure inside the container. The model developed for the flow of
gas through the NRVB has limited validity while the properties of the
backfill material (e.g. porosity, permeability, and strength) are
evolving.”

The objective of this work is to identify uncertainties in a “screening limit”, taking into account the
process of backfilling, as well as the changing characteristics of a backfill during setting and
hardening for the case of the NRVB.

The performance of the NRVB while it is in its fluid state, and whether gas generation from a waste
package could disrupt the backfill during this stage, has been assessed. It is estimated that during
3 -1
the backfilling process, rates of gas generation as low as about 0.3 m yr may cause disruption of
the fluid NRVB, particularly in locations adjacent to the waste package vents. Such disruption may
also lead to continuous leak paths through the grout.

The properties of the NRVB change most rapidly during the first few days after placing, and are
dependent on the temperature rise resulting from the heat of hydration. Estimates have been
made of the development of compressive strength and permeability (to both water and gas) from
initial set up to 100 days, beyond which time it is assumed that there will be only insignificant
changes.

AMEC/000795/001 Issue 3 Page v


Migration of gas through the NRVB while it is hardening has been modelled. If the NRVB has
3 -1 1
hardened and the gas generation rate is below about 10 m yr at STP , then at steady-state the
gas will be able to flow through the NRVB without a detrimental increase in gas pressure inside the
container. This is consistent with previous studies. However, during the first few hours from initial
3 -1
set, it has been estimated that rates of gas generation below 1 m yr at STP may cause disruption
of the NRVB, particularly in locations adjacent to the waste package vents.

The changing characteristics of the backfill material during placing, setting and hardening may thus
be important in attempting to define a “screening limit” on the rate of gas generation from individual
waste packages, below which the gas should not affect the integrity of the backfill. Although this
work has explored this particular issue through numerical modelling, there are many uncertainties
about how the backfill will mature, and how it will interact with the gas phase as it does so.
Additionally, it is unclear how much disruption of the backfill material in the immediate vicinity of
waste package vents might be tolerable. A programme of experimental work may be required to
reduce these uncertainties.

1
STP indicates conditions of Standard Temperature (To = 273.15 K) and Pressure
5
(Po = 10 Pa).

AMEC/000795/001 Issue 3 Page vi


Contents
1 Introduction 1
1.1 Objective 2
1.2 Gas Migration through a Backfill during Placement and Curing 2
1.3 Structure of Report 3

2 Assumptions 4
2.1 Waste Packages 4
2.2 Vaults 5
2.3 Backfill 5
2.4 Backfilling Strategy 6

3 Gas Migration across NRVB while Fluid 9


3.1 Increase in Gas Pressure and Resistance by the NRVB 9
3.2 Example Calculation 11
3.3 Discussion 12

4 Properties of NRVB at Early Age 17


4.1 Build-up of Gas Pressure and Failure of the NRVB 17
4.2 Strength 18
4.3 Water Permeability 24
4.4 Gas Permeability 26
4.5 Porosity and Degree of Saturation 28
4.6 Two-phase Flow Properties 31
4.7 Variation of Properties within a Vault during Backfilling 33

5 Gas Migration across NRVB at Early Age 35


5.1 Background 35
5.2 Atmospheric Pressure Initial Condition 37
5.3 Instantaneous Setting and Hardening 42
5.4 Instantaneous Setting and Hardening – New Boundary 45
5.5 Gradual Setting and Hardening 48

6 Conclusions 51
6.1 Gas Migration across NRVB while Fluid 51
6.2 Properties of NRVB at Early Age 51
6.3 Gas Migration across NRVB at Early Age 52
6.4 Information Required to Support a “Screening Limit” 52

7 References 54

AMEC/000795/001 Issue 3 Page vii


AMEC/000795/001 Issue 3 Page viii
1 Introduction
Radioactive Waste Management Limited (RWM) has prepared a “generic” Disposal System Safety
Case (DSSC) [1] that considers: the safety of radioactive waste transport to a Geological Disposal
Facility (GDF); the safety of the construction and operation of a GDF; and the safety of the facility
in the very long term.

Currently, the DSSC is at an early stage of development, because as yet neither a site nor a design
for the GDF has been chosen. It is termed “generic” because it must cover a range of possible
geological environments and facility designs. Specifically, the DSSC considers three generic host
rocks as the basis for discussion: a higher strength rock; a lower strength sedimentary rock; and an
evaporite.

The DSSC assumes that the GDF will have a disposal area for packages of intermediate-level
waste (ILW) and some low-level waste (LLW) that is separate from that for high-level waste and
spent fuel packages. In the case of either a higher strength rock or a lower strength sedimentary
rock, the illustrative disposal concept anticipates that ILW and LLW will be disposed of in vaults,
which will be backfilled with a cementitious material (see Figure 1.1). The backfill serves a number
of purposes, including: providing mechanical stability; establishing alkaline conditions (which would
reduce both the corrosion rate of steel waste containers and also the solubility of some key
radionuclides); and providing sorption sites for radionuclides.

Figure 1.1 UK illustrative disposal concept for ILW and LLW in a higher strength rock

AMEC/000795/001 Issue 3 Page 1


The formation of gases by processes (e.g. corrosion of metal wastes, microbial degradation of
organic wastes, and radiolysis of porewater) that will occur in many of the waste packages is
unavoidable, and therefore gases may be generated during transport, in the course of operation
and after closure of a GDF. It is necessary to understand the rates of generation of these gases
during all phases of a GDF, their potential effect on the engineered barrier system, and their
migration from the facility after closure, in order to demonstrate safety [2].

Many ILW and LLW containers will be vented to allow the gas to escape and to avoid the build-up
of pressure within the containers. If the gas from a waste container emplaced in a vault backfilled
with cementitious material was generated quickly and could not flow sufficiently easily through the
backfill, then the pressure within the container could rise. The pressure rise could ultimately lead to
fracturing of the backfill material in the vaults, which may be undesirable. The candidate backfill for
the disposal of ILW in a higher strength host rock is the NRVB (Nirex Reference Vault Backfill).

Previous work [3] attempted to establish a “screening limit” on the rate of gas generation from
individual vented ILW packages below which the gas should not pose a risk to the integrity of the
backfill. The work was not concerned with modelling the gas generation processes in a waste
container; rather, a constant gas generation rate was assumed, and then an upper bound for that
3 -1
rate of 10 m yr , was determined, below which it was considered unlikely that the backfill material
would crack. However, a caveat to this conclusion was:

“… the formation of the gas pathway is likely to be rapid, occurring


during the period when the backfill is curing and has low strength,
and could be associated with a very significant increase in gas
pressure inside the container. The model developed for the flow of
gas through the NRVB has limited validity while the properties of the
backfill material (e.g. porosity, permeability, and strength) are
evolving.”

1.1 Objective
The formation of gases by many ILW and LLW waste packages will be a continuous process. Most
ILW packages will be vented to allow gas to escape and avoid a build-up of pressure within the
package. The previous analysis [3] recognised that there were uncertainties in deriving a limit
because the two-phase flow model used to calculate the build-up of pressure within the container
was inappropriate during the period when the backfill would be hardening. Therefore, the objective
of this work is to identify uncertainties in deriving a “screening limit” for vented ILW packages in a
disposal concept using NRVB as a backfill, taking into account the process of backfilling, as well as
the changing characteristics of the backfill during setting and hardening.

1.2 Gas Migration through a Backfill during Placement and


Curing
This report considers how a cementitious backfill (the NRVB) will evolve from its fluid to its
hardened state, and how the strength and flow properties of the backfill may develop during its
early life. In particular, three aspects relating to the behaviour of the NRVB are considered:
1. The performance of the backfill while in its fluid state, and whether gas generation from a
waste package could disrupt the backfill during this stage.
2. The development of strength in the backfill during hardening, and how that compares to the
build-up of pressure within a container due to gas generation.
3. The change in flow properties (e.g. permeability, pore structure and moisture content) of the
backfill during hardening, and how that alters the pressure within a container.

AMEC/000795/001 Issue 3 Page 2


In each case, it is not only the properties of the backfill that are significant. The geometry of both
the container vent and the adjacent backfill will also influence whether or not the integrity of the
backfill is affected.

1.3 Structure of Report


The structure of this report is as follows:
§ Section 2 lists some parameters and assumptions (about the waste packages, the vault, the
NRVB, and the process of backfilling) that are used later in the report.
§ Section 3 considers the performance of the NRVB while it is in its fluid state, and whether gas
generation from a waste package could disrupt the backfill during this stage.
§ Section 4 describes both the development of strength and the change in flow properties of the
NRVB during hardening.
§ Section 5 presents a calculation of the build-up of pressure within a container during the period
when the NRVB is hardening, and compares that pressure against the changing strength of
the backfill.
§ Finally, Section 6 gives the conclusions of this work.

AMEC/000795/001 Issue 3 Page 3


2 Assumptions
This section discusses parameters and assumptions that are used later in the report, when we
assess whether or not gas generation from a waste package could affect the integrity of the
backfill. The assumptions concern:
§ the waste packages (see Section 2.1);
§ the vaults (see Section 2.2);
§ the backfill (see Section 2.3); and
§ the process of backfilling (see Section 2.4).

They are the same parameters and assumptions as those used in a previous study to investigate
cracking of the backfill [4]. Note that:
§ Assumptions about the waste package design and emplacement arrangements, the vault
dimensions and operating environment, and the backfilling strategy, determine:
- the rate at which backfill will flow into a vault; and
- how the backfill will fill the spaces between the waste packages.
§ Assumptions about the backfill specification determine:
- how the properties of the backfill will change during and after the filling process.

As in the previous work [3], we do not model the gas generation processes inside a waste
package; rather, a constant gas generation rate is assumed, and then an upper bound for that rate
is determined, below which it is considered unlikely that the hardened backfill would crack. The
vault operating environment (e.g. temperature) and the properties of the backfill (e.g. heat of
hydration) will influence the rate of gas generation.

2.1 Waste Packages


The assumptions about waste package design and emplacement arrangements are summarised in
Table 2.1.

Table 2.1 Summary of Waste Package Design and Emplacement Arrangements [5]

Item Assumption Comment

500L drum 0.8m diameter × 1.2m high; Stillage:


Four drums per stillage 1.665m × 1.665m × 1.245m high
3
3 m box 1.72m × 1.72m × 1.225m high
3
3 m drum 1.72m diameter × 1.225m high

Stacking Each column will comprise a single type of


3 3
package. The 3 m box and 3 m drum have
identical lifting and stacking features, and so
are capable of being mix-stacked.

Spacing 0.23m between stillages Backfill capping layer:


3
0.35m between 3 m boxes and drums 0.5m thick
0.29m between stillages and boxes
0.5m between packages and side wall

AMEC/000795/001 Issue 3 Page 4


2.2 Vaults
The assumptions about vault dimensions and operating environment are summarised in Table 2.2.
Table 2.2 Summary of Vault Dimensions and Operating Environment [6, 7, 8]

Item Assumption Comment

Cross section Reference Case: 16m x 16m Higher Strength Rock

Maximum: 20m x 20m Higher Strength Rock

Minimum: 5m x 5m Lower Strength Sedimentary Rock



Length 300m

Temperature Variable: 25 – 35°C To be considered in relation to the


rate of stiffening of the fluid
Relative Humidity Variable: 70 – 85% backfill, and the subsequent
Air speed Variable: Up to 10 km hr
-1 development of properties.

300m is the length of ILW/LLW vaults in the illustrative design for a higher strength host rock.
Vaults are shorter in the illustrative design for a lower strength sedimentary host rock [8], and
this would have implications for the backfilling strategy (see Section 2.4).

2.3 Backfill
The candidate backfill for the disposal of ILW in a higher strength host rock is the NRVB, and its
properties, as summarised in Table 2.3, have been used in this work.
Table 2.3 Summary of NRVB Properties [9]

Item Assumption Comment


-3
Mix CEM 1 450 kg m Water/Cement Mass Ratio 1.37
-3
Limestone Flour 495 kg m Water/Solids Mass Ratio 0.55
-3
Lime 170 kg m
-3
Water 615 kg m
-3 -3
Density 1730 kg m (wet) 1095 kg m (oven dried)

Settlement 1.7%

Setting time 4 hours Will increase at lower temperatures


(at 40°C)

Heat of hydration 46°C rise Actual temperature rise will depend


(under adiabatic conditions) on rate of placing, and heat loss to
waste packages and air

Compressive After 07 days 4.95 MPa Cured at 40°C


strength After 28 days 5.95 MPa
After 90 days 6.26 MPa
-16 2
Water permeability 1 x 10 m
-15 2
Gas permeability 2 x 10 m (dry) It is assumed that flow in the
-17 2
5 x 10 m (saturated) saturated state is determined by the
water permeability.

AMEC/000795/001 Issue 3 Page 5


2.4 Backfilling Strategy
Although there has been previous work on vault backfilling [10], at the time of this study RWM had
not determined in detail either the backfilling strategy or the filling procedure. To provide a basis
for this study, we have made a number of assumptions about vault backfilling. For consistency
with earlier work, the assumptions are the same as those used in a previous study, which
investigated cracking of the backfill [4]. (More details are available in Reference [4].)

For the reference case, backfilling is assumed to be in layers. This will involve placing backfill over
the full width of the vault, and to a predetermined length and thickness achievable in 24 hours. The
ratio of backfill to waste package volume is assumed to be 1:1. Therefore, at a proposed
3 -1
production rate of 20 m hr , the relationship between the selected length of a 24 hour pour and the
layer height is shown in Figure 2.1 for four different vault cross-sections. The relationship between
-1
length and rate of filling (in mm hr ) is shown in Figure 2.2.

3
5x5
Layer height (m)

10 x 10
2
16 x 16

1
20 x 20

0
0 50 100 150 200 250 300
Length (m)

Figure 2.1 The relationship between the selected length of a 24 hour pour and the layer
height for a number of vault cross-sections [4].

200
5x5
Rate of filling (mm/h)

150
10 x 10

100 16 x 16

50

20 x 20
0
0 50 100 150 200 250 300
Length (m)

Figure 2.2 The relationship between the selected length of a 24 hour pour and the rate of
-1
filling (in mm hr ) for a number of vault cross-sections [4].

AMEC/000795/001 Issue 3 Page 6


When investigating the effect of gas generation on the integrity of the NRVB, the rate of filling is a
particularly important parameter because it determines the head of fluid NRVB (which will resist the
pressure of the gas) at various stages during the backfilling process.

In selecting a backfilling strategy [4], the following factors were considered:


§ Preventing a fluid head that generates too much bleed (i.e. migration of water upwards to the
top surface), which would imply excessive settlement (i.e. settlement of solids suspended in
the water) and associated cracking.
§ Maintaining a fluid head that generates sufficient bleed to avoid plastic shrinkage cracking.
§ Limiting the thickness of each layer to control the early-age temperature rise.

An assessment of three examples (see reference [4] for the details) is given in Table 2.4 for bay
lengths of 50m, 100m and 150m with layer thicknesses of 1200mm, 600mm and 400mm
respectively.

Table 2.4 Three Examples of Different Pour Sizes


3 -1
(assumes 300m long vault, 20 m hr production rate, 2 hr transportation from
mixing to placing in the vault, and 25°C)

Example 1 Example 2 Example 3 Comments

Length (m) 50 100 150


-1
Rate of filling (mm hr ) 50 25 16.7

Fluid head (mm) 364 182 122

Potential settlement (mm) 8.74 5.3 3.5 Only the top 300mm is
influential in determining
settlement and bleed
-2 -1
Rate of bleed (kg m hr ) 1.46 0.73 0.49 At T = 25°C, RH = 75% and
-1
wind speed = 10 km hr , the
-2 -1
rate of bleed is 0.21 kg m hr

Depth of layer (mm) 1200 600 400

Period between layers (hr) 120 48 24

Temperature rise in 39 30 25 Upper layers are cast onto


single layer (°C) warm backfill and lose less
heat downwards. This has
Temperature rise after 39 30 32 less effect for the thicker pour,
multiple layers (°C) which also has 5 days cooling
before the next layer is placed.

Casting in thinner, large area pours has the benefits of less settlement and a lower temperature
rise, whereas casting in thicker pours generates more bleed and therefore less risk of plastic
shrinkage cracking.

In practice, plastic shrinkage cracking is unlikely to be a major concern. It affects only the top
surface, and as each layer is covered progressively, so any cracks will become filled. In view of
this, and if practicable, the final layer could be cast as thicker pours to increase the amount of
bleed and decrease the risk of plastic shrinkage cracking.

Based on this assessment [4], a potential backfilling strategy is to cast thin, large area layers up to
the penultimate layer, with the final layer cast as thick, smaller area pours.

AMEC/000795/001 Issue 3 Page 7


In other studies [10], the backfill strategy was assumed to involve 160m long sections cast at a rate
3 -1
of 20 m hr , and this is similar to Example 3 shown in Table 2.4. Therefore Example 3 is used as
our reference case.

AMEC/000795/001 Issue 3 Page 8


3 Gas Migration across NRVB while Fluid
This section considers the performance of the NRVB while it is in its fluid state, and whether gas
generation from a waste package could disrupt the backfill during this stage.

3.1 Increase in Gas Pressure and Resistance by the NRVB


Gas generation may occur in the waste packages prior to backfilling. A vent provides a means for
the gas to escape. As there is no resistance to the gas flow, the pressure within the package will
be atmospheric.

At some stage in the backfilling process the NRVB will flow over the vent, offering resistance to the
escape of the gas (see Figure 3.1).

NRVB Vent

Ullage space
Gas

Gas

Gas

Gas

Figure 3.1 Condition when the vent of a waste package initially is covered with NRVB.

As the NRVB will be fluid at this stage and may remain so, albeit with increasing viscosity, for
several hours, the gas will attempt to escape by bubbling through, or simply displacing the NRVB.
Whether or not this can occur will be determined by the potential increase in pressure and the
resistance offered by the NRVB. The potential pressure build-up will be determined by the rate of
gas generation and the size of the void space within the package.

Previous work [3], attempting to derive a “screening limit” on the rate of gas generation within a
3 -1 1
waste package, calculated rates of up to 10 m yr at STP would be unlikely to affect the integrity
-1
of hardened NRVB. This is about 1.142 L hr at STP. If the vent were blocked, the rate of
pressure build-up would be determined not only by the rate of gas generation, but also by the
2
volume of the ullage space . In a 500L drum which has a diameter of 800mm, the potential rate of

1
STP indicates conditions of Standard Temperature (To = 273.15 K) and Pressure
5
(Po = 10 Pa).
2
This supposes that the volume of the ullage space will be the largest contributor to the
effective void space within the package.

AMEC/000795/001 Issue 3 Page 9


pressure increase (assuming the vent is blocked) has been estimated for different depths of ullage
space (using the ideal gas law, and with the starting pressure at atmospheric pressure). The
results are shown in Figure 3.2.

3 -1
Figure 3.2 Assuming gas generation at a rate of 10 m yr and a blocked vent, the
estimated increase in pressure (above atmospheric pressure) is shown as a
function of the depth of the ullage space.

The gas pressure will be resisted by the fluid NRVB. In order to establish the magnitude of the
resistance, the NRVB is considered as a viscous fluid. In its fluid state, cementitious grout acts as
a solid suspension (i.e. solid particles in a liquid phase) [11]. The fluid behaviour of such materials
may be defined by the general equation:

t = t 0 + a g& n (3.1)

where:
t is the shear stress (Pa);
t0 is the stress required to induce strain (Pa)
(i.e. the intercept on the shear stress axis of the stress strain relationship);
g& -1
is the rate of shear strain (Pa s ); and
a and n are constants.

Most cement paste, mortar and concrete may be represented by the simplest form of
Equation (3.1), in which:
t0 is equal to the yield stress, tY (Pa);
a is equal to the plastic viscosity, m (Pa s); and
n is equal to 1.

This is the Bingham model:

t = t Y + m g& (3.2)

The yield stress is the value below which the rate of shear strain is zero. Thus this may be
considered as the limiting stress that fluid NRVB could sustain before the gas pressure causes
disruption. Consider the (very) simplified model shown in Figure 3.3.

AMEC/000795/001 Issue 3 Page 10


d

Yield stress, τy h

Gas pressure, P

Figure 3.3 Conceptual model for determining the gas pressure that will cause disruption
to the NRVB.

The gas pressure P acts over the area of the vent, assumed to be circular, with diameter d. The
force generated by the gas is resisted by the shear stress around the circumference of a plug of
NRVB of thickness h and diameter d, together with the self-weight of the plug. Thus the force
generated by the gas is:

p d2
F= P (3.3)
4

and the resistance to this force is:

πd2
R = π d ht Y + ρgh (3.4)
4

where the second term is the self-weight of the plug (r is the density of saturated NRVB, and g is
the acceleration due to gravity). To avoid disruption of the NRVB, we require that F ≤ R. Thus:

πd2 πd2
P £ π d ht Y + ρgh
4 4
or:

æ t ö
P £ ç 4 Y + ρ g ÷h (3.5)
è d ø

3.2 Example Calculation


As an example, we assume that:
§ the effective void space within the package corresponds to an ullage space that is 100 mm
deep;
§ the diameter of the package vent (d) is 100 mm; and
§ the thickness of the layer of NRVB above the package vent (h) is 50 mm.

The density of saturated NRVB (r) is 1730 kg m .


-3

Cementitious grout has a reported yield stress [11] in the range from 10 Pa to 100 Pa. A value of
16.8 Pa was derived for the NRVB [9], although from a mix that did not comply with the 28 day
strength requirement. Failure to achieve the 28 day strength suggested that the water content was

AMEC/000795/001 Issue 3 Page 11


too high, and this would lead to a lower plastic viscosity than a compliant mix with less water and
fluidity. In addition, the age of the NRVB when placed in the vault will be greater than that of the
test sample (the yield stress of the test sample was measured immediately after mixing).

Taking the value of 100 Pa, at the higher end of the reported range for grouts in general, the
resistance estimated using Equation (3.4) is 8.2N, while the gas pressure generated in one hour
3 -1
(assuming 10 m yr ) is more than double this, being of the order of 18N. In this example, the gas
pressure will exceed the resistance within about 28 minutes of the NRVB covering the vent.

Using the reported yield stress for the (non-compliant) NRVB of 16.8 Pa, the resistance reduces to
6.9N and the pressure will exceed the resistance in 23 minutes. The relatively small reduction in
relation to the change in yield stress (from 100 Pa to 16.8 Pa) is due to the self-weight of the plug
offering most of the resistance at these low levels of yield stress.

The limiting gas flow rate to avoid disruption of the NRVB during emplacement has been estimated.
The relationship between the times when the pressure will have built up to a level sufficient to
overcome the resistance of the NRVB and the gas generation rate is shown in Figure 3.4. It is
assumed that the NRVB flows over the vent and immediately forms a layer either 25 mm or 50 mm
thick.

900

800 50mm
Time to breach NRVB (mins)

700
600
0.68
500
0.34
400 25mm
Initial setting time
300
200

100
0
0.1 1 10
3
Gas generation (m /yr)

Figure 3.4 Estimated times to breach the layer of NRVB above a vent in a 500L drum.

With a start of setting time of 340 minutes [9], to avoid disruption of the NRVB the gas generation
3 -1 3 -1
rates would be required to be less than 0.34 m yr and 0.68 m yr for 25 mm and 50 mm thick
layers of NRVB respectively.

3.3 Discussion
In reality the NRVB is unlikely to form an immediate and uniform layer above the vent, but will flow
across the vent as indicated in Figure 3.1. This process is very difficult to model. As the NRVB
covers part of the vent, the gas will continue to escape through the unblocked area. At some stage
the vent will be covered completely, and the pressure within the ullage space will begin to increase
until it reaches a level sufficient to breach the NRVB. At this point the pressure in the ullage space
will be relieved, which may allow the NRVB to flow back across the vent. In an extreme case, the
NRVB may be breached in minutes rather than hours, and this mechanism could occur many times

AMEC/000795/001 Issue 3 Page 12


before the NRVB stiffens to the extent that either it is not breached again while in its fluid state or it
fails to flow back over the vent. This process is illustrated schematically in Figure 3.5.

Figure 3.5 The development of gas pressure in relation to the increase in the yield stress
of the NRVB.

The pattern of flow across the top surface of a 500L drum is shown in Figure 3.6. In this case it is
assumed that the NRVB will flow from one side to the other. A possible outcome at a high rate of
gas generation is the creation of a gas leakage path from the vent to the leading edge of the NRVB
flow.

AMEC/000795/001 Issue 3 Page 13


PLAN ON 500L DRUM CONDITION

NRVB flows from one side of a drum until it


reaches the vent. Until the vent is fully covered
by the NRVB, the gas may escape and there is
little or no pressure build-up in the ullage space.
When the vent is covered, the pressure will
Vent increase until the NRVB is breached. This is
most likely to occur at the front edge of the
NRVB FLOW
NRVB where the layer is thinnest.
Top View
of Drum

NRVB

As the NRVB continues to flow across the


surface of the drum, the resistance to gas flow
will increase behind the direction of flow and
any escape of gas is most likely to occur from
the leading edge, this being the point of least
resistance.
NRVB FLOW GAS FLOW

This will continue until the NRVB has flowed


across the surface of the drum, resulting in a
leakage path from the vent to the leading edge
of the NRVB flow.

NRVB FLOW GAS FLOW

Figure 3.6 The possible development of a leakage path (at a high rate of gas generation)
as the NRVB flows across the top of a 500L drum.

AMEC/000795/001 Issue 3 Page 14


When the NRVB has covered the drum, the gas will continue to escape along the leakage path
providing least resistance. As backfilling proceeds, the NRVB at the location of the leakage path
will rise to the level of the base of the next drum, thus attempting to block the leakage path, as
shown in Figure 3.7. However, with sufficient gas generation a gap will open and the leakage path
may propagate upwards along the edge of the next drum.

Development of the leakage path at the


periphery of the drum.

NRVB Vent

Propagation of the leakage path through the


subsequent layer along the edge of the drum.

Joint Joint

NRVB Vent

Figure 3.7 Possible propagation of a leakage path.

When flow across the top of a drum ceases as the gap is filled, the NRVB in the space between the
drums will bleed and settle, forming an additional leakage path below the base of an upper drum or
stillage.

In the unlikely event that the NRVB flows uniformly over the surface of a drum from all directions,
this would continue until there is a balance between the head of NRVB and the pressure within the
enclosed space. At this point, as the pressure continues to develop, the gas would find the path of
least resistance to escape. For this scenario to arise, the rate of filling would have to be much
-1
greater than the 16.7 mm hr likely to occur based on current assumptions about backfill
emplacement. Thus, even if flow into the space were approximately uniform around the edge of
the drum, in practice a similar situation to that shown in Figure 3.7 would develop, with the leakage
path forming at the final point of closure around the periphery of the drum.

To estimate a rate of gas generation below which the NRVB will not be compromised during
backfilling, it is necessary to quantify the rate at which the yield stress will develop as the NRVB
goes through its stiffening and setting process. In relation to this approach, there are a number of
additional uncertainties, as follows:
1. The rate at which the NRVB will flow over the vent (i.e. how quickly the head of NRVB will
build-up).

AMEC/000795/001 Issue 3 Page 15


2. The mechanism by which the gas pressure will breach the NRVB. (The mechanism assumed
in Section 3.1 is very simplistic.)
3. The extent to which the NRVB will recover from an escape of gas (i.e. whether the NRVB will
flow back to cover the vent).
4. Will the gas bubble through the NRVB (i.e. will bubbles form on the lower surface and rise up
through the NRVB)?

As it will be impossible to predict precisely how the NRVB will flow over the large area of the vault,
many of these questions may be answered only by testing the local behaviour of the NRVB at full
scale.

AMEC/000795/001 Issue 3 Page 16


4 Properties of NRVB at Early Age
This section describes both the development of strength and the change in flow properties of the
backfill during hardening.

4.1 Build-up of Gas Pressure and Failure of the NRVB


At some point, several hours after emplacement, the NRVB will stiffen and set. Beyond this stage
the failure mechanism will change in two principal respects:
§ a much higher pressure will be needed to cause disruption; and
§ any damage that does occur (mainly in the form of cracking) will be permanent.

While the tensile strength of the NRVB is low, the strength immediately after setting will still be
considerably higher than the yield stress in the fluid state. If it is assumed that the tensile strength
3
of the NRVB is about 0.6 MPa at 28 days, and that the tensile strength immediately after setting is
only 1% of the value at 28 days, then the estimated tensile strength is 6000 Pa, compared with the
fluid yield stress of only 100 Pa. Thus, the time to achieve a pressure in excess of the tensile
strength could be of the order of 3 hours (see Figure 3.2). But after 3 hours the tensile strength will
have increased further, thus requiring more pressure to cause failure. This is illustrated
schematically in Figure 4.1. As long as the NRVB resistance develops faster than the force
generated by the gas pressure, no damage will occur. However, while gas generation will continue
into the long term, the rate of development of strength of the NRVB will reduce; the strength of the
backfill will reach a value close to its ultimate strength within the initial 28 days or so, with little gain
thereafter. Thus over a long enough period, with no flow of gas through the NRVB, the resistance
may be overcome, resulting in disruption of the NRVB.

Figure 4.1 The development of gas pressure in the medium term, while the NRVB is
developing strength.

3
The tensile strength of the NRVB is assumed to be about 10% of its compressive strength,
which is about 6 MPa at 28 days (see Table 4.1).

AMEC/000795/001 Issue 3 Page 17


When the NRVB has set, hydration will result in a change in pore structure and free moisture
content. As hydration proceeds, so the porosity of the solid phase of the NRVB will reduce, but at
the same time the free water content will reduce, decreasing the degree of saturation. As the
porosity and degree of saturation change, gas may permeate through the NRVB, resulting in the
increment of force associated with gas generation also reducing. If the gas flow is of sufficient
magnitude the NRVB resistance may not be exceeded, as shown in Figure 4.2.

Figure 4.2 The development of gas pressure in the medium term, while the NRVB is
developing strength – accounting for gas flow through the NRVB.

The rate of development of strength, as well as changes in permeability and degree of saturation,
are dealt with in the remainder of this section.

4.2 Strength
The hydration of cement is an exothermic reaction, in which heat is liberated during the reaction of
the cementitious materials with water.

Maturity methods have been used extensively in recent years to predict the strength of
concrete [12]. These methods assume that concrete strength is related directly to the quantity of
heat developed from the hydrating cement. The theoretical benefit is the ability to predict concrete
strength over a wide range of conditions based on the thermal history of the modelled concrete.

The Arrhenius method is commonly used for deriving the rate at which the properties of concrete
develop [12], and therefore has been selected for this project. The method provides an equivalent
age function, which converts the chronologic age t of a concrete cured at a temperature T to an
equivalent age te for a specimen cured at a reference temperature Tr according to the expression:

t
é Eæ 1 1 öù
t e = ò exp ê- çç - ÷÷ú dt ¢ (4.1)
0 ë R è 273.15 + T 273.15 + Tr øû

where:
te is the equivalent age at the reference curing temperature;

AMEC/000795/001 Issue 3 Page 18


t is the chronologic age;
-1
E is the activation energy (J mol ), which is a function of the curing temperature T, and
therefore of the chronologic age t;
-1 -1
R is the molar gas constant, 8.314 J mol K ;
T is the curing temperature (°C), which is a function of the chronologic age t; and
Tr is the reference curing temperature (°C).

This model assumes that the ultimate hydration, and therefore the ultimate strength, is independent
of the curing temperature. However, it has been recognised for many years that while the early
age strength is increased at a higher curing temperature, the long term strength may be adversely
affected [13, 14]. In a recent study by Abdel-Jawad [15], this effect has been quantified and used
to predict more reliably the strength gain of concrete from early age through to late life.

The modification involves firstly deriving a value of the activation energy E, as affected by the
curing temperature T and the water/cement ratio w/c using the expression:

1- w / c
38000 æ Tr - T0 ö
E= çç ÷÷ (4.2)
1.10 - 0.004 T è T - T0 ø

where:
E is the activation energy (J mol-1);
T is the curing temperature (°C);
Tr is the reference curing temperature (°C);
T0 is the datum temperature below which it is assumed that hydration ceases (-10°C); and
w/c is the mass ratio of water to cement.

Then, to estimate the compressive strength fc (T, t) of a concrete cured at temperature T for time t
the following empirical expression is applied:

f c (T , t ) = f c (Tr , t e ) {1 - 0.01 (1 - exp[- 0.05 t e ]) (T - Tr )} (4.3)

where fc (Tr, te) is the compressive strength after curing at a reference temperature Tr for an
equivalent age te.

Strength data were obtained for the NRVB as part of its development programme [9]. The results
were obtained for cubes cured at T = 40°C, and are given in Table 4.1. Also listed in Table 4.1 are
estimates of the equivalent age (calculated using Equations (4.1) and (4.2); note that the activation
-1
energy is 48.8 kJ mol ) and the adjusted strength (calculated using Equation (4.3)) for curing at
20°C.

Table 4.1 Measured Compressive Strength at 40°C [9], and Estimated Compressive
Strength at 20°C
° °
Measured at 40 C Estimated for 20 C

Age Strength Equivalent Age Adjusted Strength


(days) (MPa) (days) (MPa)

7 4.95 25.2 5.78

28 5.95 100.7 7.43

90 6.26 323.6 7.82

AMEC/000795/001 Issue 3 Page 19


A lower curing temperature leads to a longer equivalent age compared with the test results, which
were obtained at 40°C. Therefore it is necessary to extrapolate the data to estimate the strength at
early age of a concrete cured at 20°C. This extrapolation was achieved using the function b(t),
defined in EN1992-1-1 [16], which applies to concrete cured at 20°C:

f c (T = 20, t ) = b (t ) f c (T = 20, t = 28) (4.4)

and is of the form:

é æ 28 öù
b (t ) = exp ê s çç1 - ÷ú (4.5)
êë è t ÷øúû

where:
t is the time (days);
s is a coefficient which depends on the type of cement:
= 0.38 for slow hardening cement (class S)
= 0.25 for normal hardening cement (class N)
= 0.20 for rapid hardening cement (class R)

The cement combination used in NRVB is CEM 1 (Portland cement) plus lime, which will also
contribute to the hydration process. Strength development curves for each of the three basic
cement types are shown in Figure 4.3, and compared with the strengths estimated for the NRVB
cured at 20°C (from Table 4.1; these data are shown as open blue circles).

Figure 4.3 Compressive strength development curves derived using the age relationship
of EN1992-1-1 for slow, normal and rapid hardening cement.

The curve for the slow hardening cement provides a reasonably close fit to the strengths estimated
for the NRVB cured at 20°C, while the curves for normal and rapid hardening cement both
underestimate the strength gain in the long term. Therefore Equation (4.5) with s = 0.38 has been
used to provide a reference curve for strength development at 20°C.

AMEC/000795/001 Issue 3 Page 20


Having established the reference curve for strength development at a curing temperature of 20°C,
the Arrhenius method with the modification by Abdel-Jawad [15] has been used to derive curves at
different curing temperatures. These are shown in Figure 4.4.

Figure 4.4 Compressive strength development curves for NRVB estimated at different
curing temperatures.

Having established a model for estimating the rate of strength development for the NRVB under
conditions of constant curing temperature, this may be developed into a model for estimating the
rate of strength development under conditions of varying temperature.

The empirical Equation (4.3) deals with a constant curing temperature, but may be used in a
numerical analysis for a temperature cycle. To do this, the term (T – Tr) must be modified to
reflect the peak temperature that has been achieved during the temperature cycle. That is
because in studies on concrete, the peak hydration temperature has been shown to be a primary
factor in determining the long term strength gain [13, 14].

In a previous study of cracking in the NRVB [4], a numerical model was used to estimate the
temperature rise at various locations within the vault. Here this has been extended to allow the
strength development to be estimated as well.

Over the plan area of a vault, the NRVB will vary in thickness depending upon the way in which the
waste packages have been stacked. Therefore the local rise in temperature will also vary, causing
differences in both the rate of strength development and the ultimate strength. Two situations have
been investigated, representing the space between four 500L drums within a stillage and the space
3
between four 3m drums. (These provided the upper and lower limits on the peak temperature
estimated as part of the study on NRVB cracking [4].) Estimates of temperature rise (measured
from the in situ temperature, which is assumed to be 25°C) and strength development for the two
situations are shown in Figure 4.5.

Within each time increment, the term (T – Tr) is replaced by the term K (Tmax – Tr). Tmax is the
maximum temperature that has occurred prior to the current time. K is a coefficient to take account

AMEC/000795/001 Issue 3 Page 21


of the fact that the peak temperature is of relatively short duration, and does not occur immediately.
The coefficient K has been estimated to be 0.65, by comparing the predicted strength development
under varying temperature curing conditions with the strength development at a constant
temperature that is equal to the peak temperature within the temperature cycle. With K = 0.65, the
strength at 28 days is similar for both the varying temperature (i.e. the blue curve, labelled as “Heat
cycled”) and the constant temperature (i.e. the grey curve, labelled as “Constant temp”) curing
conditions as shown in Figure 4.5.

AMEC/000795/001 Issue 3 Page 22


Situation 1: Situation 2:
3
space between 500L drums within a stillage space between 3m drums
effective NRVB thickness = 146mm effective NRVB thickness = 726mm

3m3 3m3
drum drum

3m3 3m3
drum drum

estimated maximum temperature rise = 18°C estimated maximum temperature rise = 35°C
estimated peak temperature = 43°C estimated peak temperature = 60°C

60 60

50 50
Temperature (°C)

Temperature (°C)
40 40

30 30

20 20

10 10

0 0
0.1 1.0 10.0 100.0 0.1 1.0 10.0 100.0
Tim e (Days) Tim e (Days)

estimated strength development estimated strength development

9 9
Ref at 20°C Ref at 20°C
8 8
Heat cycled Heat cycled
7 7
Constant temp Constant temp
Strength (MPa)

Strength (MPa)

6 6
5 5
4 4
3 3
2 2
1 1
0 0
0.1 1.0 10.0 100.0 0.1 1.0 10.0 100.0

Tim e (days) Tim e (days)

Figure 4.5 Estimated temperature rise and compressive strength development at different
locations within the NRVB.

AMEC/000795/001 Issue 3 Page 23


4.3 Water Permeability
Permeability, like strength, is related to the porosity of the concrete, although in the latter case the
continuity of pores has a much greater impact. The reported value for the water permeability of the
-16 2 -17 2
NRVB is 1 10 m , while the gas permeability is 5 10 m when saturated. In the case of gas
flowing through saturated NRVB, it may be assumed that it was the water permeability that was
measured rather than the gas permeability, as water would have been entirely blocking the pores,
and so the rate of gas flow would have been limited by the rate of liquid flow. The water
permeability and the gas permeability of saturated NRVB differ by a factor of only 2. Considering
that the permeability coefficients for concrete may vary by several orders of magnitude, as shown
in Figure 4.6, the difference between these two values is considered insignificant.

Figure 4.6 shows relationships between the water permeability and the water/cement ratio for a
variety of concretes [17]. The NRVB has a water/Portland cement ratio of 1.37, but if the lime is
included as part of the cementitious component of the mix, then the water/cement ratio reduces to
0.99. As shown, the performance of the NRVB is broadly within the range for concrete with the
same water/cement ratio.

Figure 4.6 Plot of water permeability against water/cement ratio [17].

As both the permeability and the strength are related to porosity, it may be reasonable to relate the
change in the permeability to the development of compressive strength. In studies on
concrete [18], these properties have been related as shown in Figure 4.7. It can be seen that the
period of curing is a significant factor. In practice the NRVB is not cured externally, but has very
high water content, with more water than necessary to achieve full hydration. This is reflected in
the reported values for the permeability, which are consistent with concrete cured for a period in
excess of 28 days.

AMEC/000795/001 Issue 3 Page 24


Figure 4.7 Plot of water permeability at 28 days against compressive strength as affected
by the period of curing [18].

No information has been identified showing the way in which the permeability develops in concrete
over the initial days and weeks after casting. Generally measurements are reported at an age of
28 days or later [17]. Therefore a relationship between permeability and strength has been used to
estimate the change in permeability based on the development of strength.

Based on the results for concrete shown in Figure 4.7, it may be assumed that with little strength
-15 2
immediately after setting the water permeability is 1 10 m and that this reduces to a value of
-17 2 2
5 10 m after 28 days on a log-linear basis. Thus the water permeability kw (m ) may be
estimated by the expression:

k w = 10 -15-0.218 f c (4.6)

Using this expression and the predicted strength development, the change in water permeability
has also been determined. The results are shown in Figure 4.8 for the two extreme situations
introduced in Figure 4.5.

AMEC/000795/001 Issue 3 Page 25


Situation 1: Situation 2:
3
space between 500L drums within a stillage space between 3m drums
effective NRVB thickness = 146mm effective NRVB thickness = 726mm

3m3 3m3
drum drum

3m3 3m3
drum drum

estimated changes in water and gas permeability estimated changes in water and gas permeability

1.E-14 1.E-14
Gas Gas
Water Water
Permeability (m 2)

Permeability (m 2)
1.E-15 1.E-15

1.E-16 1.E-16

1.E-17 1.E-17
0.1 1 10 100 0.1 1 10 100
Time (days) Time (days)

Figure 4.8 Estimated changes in water and gas permeability at different locations within
the NRVB.

4.4 Gas Permeability


Bamforth [19] has shown that the theory of gas slippage proposed by Klinkenberg [20] can be used
4
to explain differences between the permeabilities for concrete obtained using water and gas .
Klinkenberg suggested the following equation, relating the gas permeability kg to the water
permeability kw and the mean pressure p g at which the gas is flowing:

æ B ö÷
k g = k w ç1 + (4.7)
ç p g ÷ø
è

4
Normally, the intrinsic permeability that is measured for a porous medium is approximately
independent of the fluid. However, if the pores are small, then gas slippage at the pore walls
increases the gas permeability compared with the water permeability. The Klinkenberg
correction is used to account for this difference.

AMEC/000795/001 Issue 3 Page 26


where:
kg is the gas permeability (m2);
kw is the water permeability (m2);
B is the Klinkenberg parameter (Pa), which is a constant for a given porous material and a
given gas; and
pg is the mean pressure of the gas (Pa).

Bamforth [19] derived the following empirical relationship between the Klinkenberg parameter B
and the water permeability kw:

B = 0.001657 k w-0.5227 (4.8)

Using this expression, values of the gas permeability have been estimated (assuming that
p g = 105 Pa), and are given in Table 4.2.
Table 4.2 Estimated Gas Permeability of the NRVB

Gas Permeability
2
Measurement B (m )
2
(m ) (Pa)
Estimated Measured

Water permeability from a


-16 † 5 -16
direct measurement 1 10 3.82 10 4.82 10
-15
2 10
Water permeability inferred from a
-17 † 5 -16
measurement of the gas permeability of 5 10 5.49 10 3.25 10
saturated NRVB

These experimental data were summarised in Table 2.3.
A comparison between the water permeability and the gas permeability is also shown in Figure 4.9.
The difference between the water permeability and the gas permeability is larger than predicted.
This may be due, at least in part, to the fact that the water permeability of concrete reduces during
an experimental test until a steady state is reached. This is due to a combination of continued
hydration of the cement and the silting of pores. For structural concrete, the reduction in water
permeability during a test may exceed a factor of 10 and approach a factor of 100 [17], with the
change tending to be greatest in concretes with lower water/cement ratio and higher strength. As
the gas permeability of the NRVB was derived using a dried specimen, similar changes would not
be expected during the measurement of gas permeability.

AMEC/000795/001 Issue 3 Page 27


1.E-13 Water permeability Water Water permeability
assumed to be gas permeability consistent w ith gas
permeability for measured permeability using the
saturated NRVB directly Klinkenberg conversion
1.E-14
Gas permeability (m 2)

Measured gas permeability


10,000Pa
1.E-15
30,000Pa Estimated gas permeability
at Pm = 100000Pa
100,000Pa
1.E-16
300,000Pa
LINE OF EQUALITY

1.E-17
1.E-17 1.E-16 1.E-15
Water permeability (m 2)

Figure 4.9 Plot of gas permeability against water permeability.


-15 2
To achieve a gas permeability of 2 10 m using the Klinkenberg conversion as modified by
-16 2
Bamforth, the water permeability of the NRVB would have to be 9.05 10 m , i.e. about ten times
the measured value. Hence, assuming that the Klinkenberg adjustment for gas slippage applies to
the NRVB, the results would be consistent with a change in permeability during the test of a similar
order to that observed for concrete with a high water/cement ratio.

Using Equation (4.7) to compute the gas permeability from the water permeability, the estimated
change in the gas permeability of the NRVB over the first 100 days is shown in Figure 4.8 for the
two extreme situations introduced in Figure 4.5.

4.5 Porosity and Degree of Saturation


The porosity of the NRVB is determined initially by the free (evaporable) water content of the grout,
and subsequently by the degree of hydration and the associated volume change.
-3
The free water content of the NRVB is 615 L m , and therefore the maximum porosity is 0.615.

During hydration, water and cement become chemically combined, thus reducing the free water
content. Furthermore, the hydration of Portland cement leads to a reduction in volume, i.e. the
volume of the hydration products (calcium silicate hydrates, or CSH) is less than the volume of the
water and cement used in the reaction. The volume reduction is of the order of 8% [21], and full
hydration may occur at a water/cement ratio (by mass) of about >0.42 [21]. The NRVB has a
-3 -3
water/cement ratio of 1.37 (i.e. 615 kg m of water and 450 kg m cement). Therefore for full
-3 -3
hydration to occur only 0.42 x 450 kg m = 189 kg m of water is required. The remaining water
-3
(615 - 189 = 426 kg m ) will remain as capillary water, not having been consumed in the hydration
process. Thus the porosity after full hydration will be the sum of the residual free water and the
volume reduction due to hydration.

AMEC/000795/001 Issue 3 Page 28


Estimated volumes before and after full hydration are shown in Figure 4.10. After full hydration of
the Portland cement, the overall volume reduction is estimated to be only 2.6% and the residual
5
degree of saturation is 94% .

Figure 4.10 Estimated volume proportions before and after hydration of the NRVB.

Therefore even with no excess water there will be sufficient internal moisture to ensure that full
hydration occurs, and the NRVB may be expected to perform as a concrete with prolonged external
curing provided that significant drying does not occur. Moreover significant drying is unlikely
because the duration of placing the NRVB is relatively short, and each layer is covered, within a
relatively short period, by another wet layer.

The way in which the porosity will change during the initial period of curing has been estimated by
assuming that the porosity and compressive strength are related by the expression [22]:

fc = f I X n (4.9)

where:
fc is the compressive strength;
fI is the intrinsic strength of the cement;
X is the gel-space ratio (i.e. the ratio of the volume of the hydrated cement to the sum of the
volumes of the hydrated cement and the capillary voids); and
n is a coefficient with a value typically in the range from 2.6 to 3.0.

The gel-space ratio may be determined using the expression [22]:

0.68a
X = (4.10)
0.32a + w / c

where:
a is the degree of hydration; and

5
If it is assumed that the lime also contributes to the reaction, effectively increasing the cement
-3 -3
content from 450 kg m to 450 + 170 = 620 kg m , then the volume reduction increases to
about 3.6% and the degree of saturation reduces to about 91%.

AMEC/000795/001 Issue 3 Page 29


w/c is the mass ratio of water to cement.

Combining Equations (4.9) and (4.10) allows the degree of hydration to be estimated from the
strength as follows:

1
æ fc ö n
çç f ÷÷
a= è Iø w/c (4.11)
1
æf ön
0.68 - 0.32 çç c ÷÷
è fI ø

Assuming a value for n of 3, the intrinsic strength has been adjusted so that the degree of
hydration does not exceed 1. This is achieved at a value of fI = 115 MPa, this being consistent
with reported values for the intrinsic strength of cement of 99 MPa and 129 MPa [22]. Therefore
the degree of hydration a can be estimated from the measured strength of the NRVB fc using the
expression:

1
æ fc ö 3
ç ÷
a= è 115 ø w/c (4.12)
1
æ fc ö 3
0.68 - 0.32 ç ÷
è 115 ø

Having estimated the degree of hydration, the porosity j can be estimated based on the volume
changes that occur as hydration proceeds. For the NRVB volume proportions [9], this leads to the
expression:

j = 0.615 - 0.163 a (4.13)

Finally, the degree of saturation Sw is the ratio of the specific volume of free water Vw to the
porosity j. The free water is that which remains after hydration, and is estimated using the
expression:

Vw = S w j = 0.615 - 0.189 a (4.14)

Estimated values for the degree of hydration, the porosity and the degree of saturation are shown
in Figure 4.11.

AMEC/000795/001 Issue 3 Page 30


Situation 1: Situation 2:
3
space between 500L drums within a stillage space between 3m drums
effective NRVB thickness = 146mm effective NRVB thickness = 726mm

3m3 3m3
drum drum

3m3 3m3
drum drum

estimated changes in degree of hydration, estimated changes in degree of hydration,


porosity and degree of saturation porosity and degree of saturation

Figure 4.11 Estimated changes in the degree of hydration, the porosity and the degree of
saturation.

4.6 Two-phase Flow Properties


The flow of gas through the NRVB will be coupled with the flow of porewater, and the coupling will
influence both the permeability to gas and the gas pressure. Therefore this is a two-phase flow
problem.

In the conventional approach to modelling two-phase flow:


§ There is a difference in pressure across the interfaces between liquid and gas phases within
the pores of the porous medium. This difference in pressure is called the “capillary pressure”,
and it causes gas to access larger-sized pores before smaller-sized pores. When the capillary
pressure increases, the smaller-sized pores start to fill with gas and the volume fraction of the
porosity occupied by gas increases.
§ Darcy’s law is used to calculate the flux of each phase, but the permeability of the porous
medium is replaced by the phase permeability. In our case, the phase permeability is equal to
the permeability of the NRVB multiplied by a “relative permeability” function for the phase.

The capillary pressure and relative permeability functions, which jointly are called saturation
functions, have important consequences for gas migration.

Our previous work [3] performed a review of the literature on saturation functions that had been
measured for cementitious materials. The review noted that there was considerable uncertainty

AMEC/000795/001 Issue 3 Page 31


about which parameterisation of the saturation functions to select for the NRVB, and then went on
to recommend using van Genuchten forms [23] for both the capillary pressure and relative
permeability functions, as given by the following expressions:

1- m
Pc = Pa æç S ew m - 1ö÷
-1
(4.15)
è ø

and:

2
é mù
= S ew ê1 - æç1 - S ewm ö÷ ú
1
k rw (4.16)
êë è ø úû

2m
é ù
k rg = S eg ê1 - çæ1 - S egm ÷öú
1
(4.17)
ë è øû

where:

Sb - Sb r
S eb = β = w (water) or g (gas)
(
1 - S w r + S gr ) (4.18)

and:
Pc is the capillary pressure (Pa).
Pa is the “apparent” gas entry pressure, which is a constant (Pa).
Pa was set to 3.2 105 Pa [3].
m is an adjustable parameter (related to the pore size distribution of a porous
medium) that controls the shape of the capillary pressure function (–).
m was set to 0.5 [3].
krβ is the relative permeability to phase β = w (water) or g (gas) (–).
Sb is the saturation of phase b (i.e. the fraction of the porosity occupied by
phase b).
Sβr is the residual saturation of the fluid phase β (–).
Swr was set to 0.25 [3], and Sgr was set to 0 [3].

These capillary pressure and relative permeability functions are plotted in Figure 4.12.

AMEC/000795/001 Issue 3 Page 32


1 3

0.9

0.8

0.7
2

Capillary pressure (MPa)


Relative permeability

0.6

0.5

0.4

1
0.3

0.2

0.1

0 0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
Scaled liquid saturation S ew

Relative gas permeability Relative water permeability Capillary pressure

Figure 4.12 The saturation functions which were selected for hardened NRVB [3].

No data were identified which show how these saturation functions might develop over the initial
days and weeks after casting. In the absence of any data:
§ Following Leverett [24], we assume that the capillary pressure function will scale with the
inverse square root of the water permeability kw as the NRVB hardens. That is:

k w¥
Pa (k w ) »
kw
´ Pa k w¥( )
(4.19)
5 ´ 10 -17 m 2
= ´ 3.2 ´ 10 5 Pa
kw

where:
Pa is the “apparent” gas entry pressure; and
k w¥ is the water permeability of the NRVB in the long term.

§ We assume that the relative permeability functions will not change.

These (admittedly crude) assumptions are sufficient for us to develop a model illustrating how gas
might flow from within a waste package through the backfill during hardening.

4.7 Variation of Properties within a Vault during Backfilling


The backfilling of each bay of the vault to full height is expected to take about one month. Thus,
when the final layer of NRVB is cast the age variation between the bottom and the top of the vault
will be about one month as well. The properties also will vary during this early period, with the
deeper, older grout having the higher strength and the lower permeability, as shown in Figure 4.13.
This variation could be taken into account in a global vault analysis, based on the age of the NRVB
in each layer and the temperature history.

AMEC/000795/001 Issue 3 Page 33


In addition, the variation in the NRVB geometry, and the resulting variations in temperature rise, will
lead to differences in the strength and the permeability over the area of the vault, although to a
lesser extent than over the height. This is too complex to model in practice, and recognising the
limitations of the predictive model for gas generation within a waste package and its migration
through the NRVB (see Section 5), it would be more appropriate in global modelling to assume
mean values at each level.

3m3 3m3

Increasing permeability
box MBGWS drum
box
Reducing strength

3m3 3m3
box MBGWS drum
3m3 box 3m3
box drum
MBGWS
3m3 box 3m3
box drum
MBGWS
3m3 box 3m3
box drum
MBGWS
3m3 3m3
box
box drum
3m3 MBGWS 3m3
box box drum

Figure 4.13 Variation in properties over the height of a vault during the first month
following placing the backfill.

AMEC/000795/001 Issue 3 Page 34


5 Gas Migration across NRVB at Early Age
This section presents a calculation of the build-up of gas pressure within a waste container during
the period when the backfill is hardening, and compares that pressure against the changing
strength of the backfill.

5.1 Background
In a first study [25] of the problem (i.e. the ease with which gas could escape from the vents in
waste containers and flow through the backfill of a vault), it was assumed that the waste containers
were cylindrical and stacked vertically. The movement of gas from a circular vent in the centre of
the top of a 500L drum and through the backfilled horizontal gap between the drum and the one
above was considered. The presence of porewater in the backfill material was neglected, and only
the flow of gas was modelled.

Therefore, the equations to be solved were the steady-state continuity equation:

(
Ñ × rgqg = 0 ) (5.1)

together with the ideal gas law:

M
rg = pg (5.2)
RT
and Darcy’s law:

k
qg = - Ñp g (5.3)
mg

where:
ρg is the density of the gas phase (kg m );
-3

-1
qg is the Darcy velocity of the gas phase (m s );
-1
M is the molecular weight of the gas (kg mol );
-1 -1
R is the ideal gas constant 8.314 J mol K ;
T is the temperature of the gas phase (K);
pg is the pressure of the gas phase (Pa);
2
k is the gas permeability tensor of the backfill (m ); and
μg is the viscosity of the gas phase (Pa s).

These equations were solved subject to the boundary conditions that pg = Pin at the vent, and
pg = Pout on the outer cylindrical surface of the backfilled gap. It was noted that if the vertical
separation of the containers is small compared with the container radius, then:

Q gv =
To 1 k
Po T m g
ph
æbö
(P 2
in - Pout
2
) (5.4)
logç ÷
èaø

AMEC/000795/001 Issue 3 Page 35


where:
Q gv 3 -1
is the volumetric flow rate of gas through the backfill (m s ) at STP ;
6

To is Standard Temperature, 273.15 K;


5
Po is Standard Pressure, 10 Pa;
2
k is the magnitude of the (isotropic) permeability tensor of the backfill (m );
h is the vertical separation of the containers (m);
b is the container radius (m); and
a is the vent radius (m).

The conclusions of this first study were that for gas generation rates then considered to be at the
3 -1 7
upper end of expectations (i.e. 2 m yr at STP for a 500L drum ):

… the excess pressure [i.e. Pin – Pout] is insignificant compared to


the hydrostatic pressure … for backfill permeabilities [to gas] greater
-19 2 -18 2
than about 10 m for the 10 cm diameter vent and about 10 m
for the 1 cm diameter vent.

… gas is likely to be able to escape from vented canisters and


through backfill without serious pressure rises.

A second study [26] presented a similar calculation, but this time for a spherical geometry (which
was simpler to analyse) rather than a cylindrical geometry, and arrived at the same conclusions. It
extended the first study by presenting experimental data on the permeability of the NRVB to gas,
and comparing the gas pressure with the tensile strength of NRVB to determine whether the
backfill material would crack. It was argued that the tensile strength of NRVB would be about
5
6 10 Pa.

Finally, the previous work was reviewed as part of a third study [3], which identified some
limitations. In particular:
§ The previous analyses were steady-state, and did not consider the formation of the gas
pathway. The formation of a gas pathway is likely to be accompanied by larger gas pressures
than those pertaining at steady-state.
§ The gas generation rate used was based on an average gas generation rate for a GDF rather
than gas generation rates for specific waste streams. Therefore, the gas generation rate could
be an underestimate for some waste packages, for example those containing reactive metals
(i.e. Magnox, aluminium and uranium).

The third study went on to develop a two-phase flow model of the build-up of gas pressure within a
waste container, and the migration of gas from a vent in the container through hardened NRVB.
This model coupled together the flow of gas in the backfill and the flow of porewater.

6
STP indicates conditions of Standard Temperature (To = 273.15 K) and Pressure
5
(Po = 10 Pa).
7
To put this number into context, we note that an “average” 500L drum from waste stream
2D38/C will contain about 150 kg of encapsulated Magnox cladding, which will be present in
the approximate form of metal plates with a thickness of 2 mm. Current calculations suggest
that this 500L drum would generate hydrogen at a rate that depends on the temperature of the
3 -1 3 -1
waste package: ~0.03 m yr at standard pressure and 25°C, and ~0.35 m yr at standard
pressure and 45°C.
3
A larger waste package, a 3 m box, could contain up to 1,000 kg of Magnox fuel element
3 -1
debris, and would generate hydrogen at a rate of ~2.33 m yr at standard pressure and 45°C.

AMEC/000795/001 Issue 3 Page 36


3
The model was applied to both a 500L drum and a 3 m box to attempt to define a “screening limit”,
3 -1
and it was shown that if the maximum gas generation rate is less than 10 m yr at STP, then the
gas will be able to flow through hardened NRVB without a potential increase in gas pressure that
could affect the integrity of the NRVB. This value for a “screening limit” on a tolerable rate of gas
generation from an individual waste package was consistent with the previous studies. It is less
than the limits derived from the requirement to be able to transport the waste packages
safely [1, 5]. However, a caveat was noted:

“… the formation of the gas pathway is likely to be rapid, occurring


during the period when the backfill is curing and has low strength,
and could be associated with a very significant increase in gas
pressure inside the container. The model developed for the flow of
gas through the backfill has limited validity while the properties of
the backfill material (e.g. porosity, permeability, and strength) are
evolving.”

The caveat motivated this study, which has the objective of developing an understanding of
uncertainties in deriving a “screening limit”, taking into account the process of backfilling as well as
the changing characteristics of the backfill during setting and hardening.

In the following subsections, therefore, we present a sequence of calculations using


TOUGHv2.0 [27], starting from a calculation similar to one presented in Reference [3], and then
gradually including more and more “realism”, until the last calculation takes due account of our
understanding of the changes in the permeability, the porosity, the degree of saturation, and the
strength of the NRVB during setting and hardening (see Section 4).

5.2 Atmospheric Pressure Initial Condition


Our first calculation is based on one of the variant calculations in Reference [3], and assumes that
when gas generation in the waste container begins the surrounding NRVB is partially saturated and
is at an ambient pressure equal to atmospheric pressure.

5.2.1 Numerical Grid

The model includes a representation of:


§ the ullage space at the top of a waste package, which is assumed to be a 500L drum;
§ the vent in the top surface of the waste package; and
§ the NRVB between the waste package and an overlying container. The thickness of the layer
of NRVB is assumed to be 75 mm [3].

The geometry of the model domain is indicated in Figure 5.1, and the discretisation of the model
domain by a numerical grid is shown in Figure 5.2.

AMEC/000795/001 Issue 3 Page 37


(a) (b)
Figure 5.1 The geometry of the model domain: (a) shows detail around the vent; and
(b) shows detail at the outlet boundary. The ullage space is coloured pink, the
vent is green, the NRVB is blue, and the outlet boundary is yellow.

Figure 5.2 The numerical grid used in the simulation.

5.2.2 Properties of the NRVB

The NRVB is assumed to harden instantaneously, and to have the properties listed in Table 5.1.

Table 5.1 Properties of the NRVB

Property Value Value in Reference [3]


-16 2 -16 2
Permeability 10 m 10 m
5
Klinkenberg parameter 3.82 10 Pa 0 Pa

Porosity 0.5 0.5

Saturation functions van Genuchten form van Genuchten form


(see Section 4.6) (see Section 4.6)

Tortuosity 0.25 0
5 5
Tensile strength 6 10 Pa 6 10 Pa

AMEC/000795/001 Issue 3 Page 38


These properties are mainly consistent with those used in Reference [3], but there are a couple of
differences:
§ Although the previous work [3] recognised that the gas permeability of the NRVB would be
larger than the water permeability because of gas slippage, the calculations did not include the
Klinkenberg parameter.
§ In addition, the previous work [3] did not consider the process of diffusion, and therefore set
the tortuosity of the NRVB to zero.

5.2.3 Initial Condition

In the model, when gas generation in the waste container starts the NRVB is partially saturated
Sw = 0.75 [28] and is at an ambient pressure equal to atmospheric pressure Pout = 1.01325 105 Pa.

As discussed in Section 4.5, the saturation of water in the NRVB is expected to reduce from 1.0,
when the backfill is poured, to 0.94, when the backfill is fully hydrated. The following subsections
present a sequence of calculations, of increasing realism, that take into account this variation of the
properties of the NRVB. However, before considering these other calculations, it is convenient to
show the results for this variant, with Sw = 0.75 initially, because:
§ The variant is consistent with an earlier calculation [3], and therefore the results obtained can
be used to verify our current implementation of the problem.
§ The variant has a high initial value of gas saturation. This should make it easier for a gas
pathway away from the vent of the waste container to form, and therefore this should lead to
an upper bound on the rate of hydrogen generation that would be compatible with not cracking
the NRVB.

5.2.4 Boundary Condition

The boundary condition on the outlet surface of the NRVB is chosen to be air at atmospheric
5
pressure Pout = 1.01325 10 Pa. The other surfaces of the model domain are no flow boundaries.

Hydrogen is injected into the ullage space, which initially is an air-filled void space, at a constant
3 -1
rate. The hydrogen injection rates considered are Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP.
(These are the same hydrogen injection rates as considered previously [3]; the values are chosen
3 -1
to form a geometric series spanning rates from 1 to 100 m a at STP, where the upper limit is
based on estimates of the maximum rate of hydrogen generation from a package containing
reactive metals, i.e. Magnox, aluminium or uranium.)

5.2.5 Results

The simulation shows the following behaviour:


§ Water, under the influence of gravity, starts to infiltrate the backfilled horizontal gap between
waste containers. The gas saturation of the NRVB decreases.
§ As hydrogen is injected into the ullage space of the waste container, the gas pressure there
increases.
§ When the gas pressure in the ullage space has increased sufficiently, the hydrogen is able to
flow into the NRVB.
§ Initially the hydrogen flows radially away from the vent in the top of the waste container
through the NRVB, and subsequently flows horizontally through the backfilled gap between the
500L drum and the one above. During this stage, when a gas pathway is forming, the gas
pressure in the ullage space continues to increase.

AMEC/000795/001 Issue 3 Page 39


§ Eventually the hydrogen propagates to the boundary (i.e. the gas pathway “breaks through”).
Depending on how the rate of formation of the gas pathway compares to the rate of injection of
hydrogen in the ullage space, breakthrough of the gas pathway may be associated with a peak
in the gas pressure in the ullage space (see Figure 5.3). The time to breakthrough typically is
less than a day.
§ After breakthrough, the variables characterising the gas pathway (e.g. the gas pressure, gas
saturation and relative gas permeability) continue to evolve towards a steady-state. The
steady-state is achieved within a few days.

Figure 5.3 shows how the excess gas pressure (i.e. the pressure above the ambient pressure) in
the ullage space of a 500L drum is predicted to evolve at different hydrogen injection rates.

2.5E+06

2.0E+06
Excess Gas Pressure (Pa)

1.5E+06

1.0E+06

5.0E+05

0.0E+00
0 10 20 30
Time (days)

Tensile strength Q=1 Q=2 Q=4 Q=8 Q = 16 Q = 32 Q = 64 Q = 128

Figure 5.3 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

At the highest hydrogen injection rates, there is a peak in the excess gas pressure that occurs just
before the gas pathway breaks through. If the hydrogen injection rate is higher than about
3 -1
32 m yr at STP, the peak in the excess gas pressure is greater than the tensile strength of the
concrete and therefore could crack it.

Figure 5.4 shows the steady-state excess gas pressure in the ullage space of a 500L drum at
different hydrogen injection rates. Note that the presentation is in terms of steady-state pressure
rather than peak pressure, because:

1. That is consistent with previous studies (see Subsection 5.1);

2. The peak pressure is more dependent on modelling assumptions (e.g. about the saturation
functions of the NRVB, and the initial condition) than the steady-state pressure; and

3. The steady-state pressure is similar to the peak pressure at the low gas injection rates that are
of most interest (see Figure 5.3).

AMEC/000795/001 Issue 3 Page 40


1.4E+06

1.2E+06

1.0E+06
Excess Gas Pressure (Pa)

8.0E+05

6.0E+05

4.0E+05

2.0E+05

0.0E+00
1 10 100 1000
Gas Injection Rate (m 3yr-1 at STP)

Tensile strength Steady-state pressure

Figure 5.4 Steady-state excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

For a 500L drum, the limit on the maximum rate of gas generation during transport of the drum is
3 -1
about 26 m yr at STP [1, 5]. This calculation suggests that the NRVB could accommodate this
rate of gas flow without any threat to its structural integrity.

5.2.6 Verification

The pressures shown in Figure 5.3 and Figure 5.4 are about seventy-five percent of the pressures
determined previously for this variant calculation [3]. That is because there are a number of
differences between the current implementation of the calculation and the previous calculation.
This subsection addresses the question: “Can the differences explain the change in pressures?”

The differences between the current calculation and the previous calculation can be summarised
as follows:
§ Both hydrogen and air are modelled in the current implementation of the calculation.
Therefore we could assume that the NRVB initially is partially saturated with air, and the
hydrogen, which is injected into the ullage space, migrates as a distinct component through
the NRVB. Previously, only hydrogen was modelled, and so we assumed that the NRVB
initially was partially saturated with hydrogen. This difference will affect the predicted
formation of the gas pathway through the NRVB.
§ We have improved the numerical representation of the ullage space in the current
implementation of the calculation. The appropriate spatial weighting scheme for averaging
flow properties is an important issue in petroleum reservoir and groundwater flow
simulation [29, 30]. It is usual to employ fully upstream weighting of the relative permeability
functions when discretising Darcy’s law for multiphase flow [31]. However, it has been argued
that a “physically-based upwind weighting” of the relative permeability functions is preferable in

AMEC/000795/001 Issue 3 Page 41


some circumstances [32]. We have used a physically-based upwind weighting scheme to
determine the flows between the ullage space and the NRVB.
§ We have included some additional processes in the current implementation of the calculation.
In particular, we have accounted for:
- the process of gas slippage, using the theory proposed by Klinkenberg [20]; and
- the process of molecular diffusion.

It was straightforward to modify the current calculation to eliminate some of these differences. If
only one gas component (i.e. hydrogen) is modelled, and if the processes of gas slippage and
molecular diffusion are neglected, then Figure 5.5 shows how the excess gas pressure in the
ullage space of a 500L drum is predicted to evolve for two different hydrogen injection rates.

2.5E+06

2.0E+06
Excess Gas Pressure (Pa)

1.5E+06

1.0E+06

5.0E+05

0.0E+00
0 10 20 30
Time (days)

Q = 1 (previous) Q=1 Q = 128 (previous) Q = 128

Figure 5.5 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1 and 128 m yr at STP) are compared with previous results [3].

The pressures have increased and are more than ninety percent of the pressures determined
previously for this variant calculation [3]. This is considered sufficiently close to verify the current
implementation of the calculation.

5.3 Instantaneous Setting and Hardening


The properties of the NRVB (see Section 5.2.2) and its initial state (see Section 5.2.3) were chosen
above to be consistent with a previous implementation of the calculation [3], but some of these
properties are slightly inconsistent with the analyses presented in Section 4. This second
calculation updates the properties of the NRVB to be consistent with Section 4, and then repeats
the simulations of Section 5.2.

5.3.1 Numerical Grid

The model domain and numerical grid are unchanged from Section 5.2.

AMEC/000795/001 Issue 3 Page 42


5.3.2 Properties of the NRVB

The NRVB is assumed to harden instantaneously, and to have the properties listed in Table 5.2.

Table 5.2 Properties of the NRVB

Property Value
-17 2
Permeability 5 10 m
5
Klinkenberg parameter 5.49 10 Pa

Porosity 0.452

Saturation functions van Genuchten form


(see Section 4.6)

Tortuosity 0.25
5
Tensile strength 6.63 10 Pa

These properties are slightly different to those used in Section 5.2.

5.3.3 Initial Condition

When gas generation in the waste container starts, the NRVB is partially saturated Sw = 0.94 and is
5
at an ambient pressure equal to atmospheric pressure Pout = 1.01325 10 Pa.

5.3.4 Boundary Condition

The boundary conditions are unchanged from Section 5.2.

5.3.5 Results

The results for this variant are shown in Figure 5.6 and Figure 5.7.

The decrease in the permeability of the NRVB and the increase in the initial degree of saturation
both contribute to a lower permeability to gas. As a consequence, the maximum and the
steady-state excess gas pressures in the ullage space increase. The increase is about a factor
of 2, which corresponds to the decrease in the permeability of the NRVB.
3 -1
The results suggest that if the gas generation rate is below about 10 m yr at STP, then at
steady-state the gas will be able to flow through the (hardened) NRVB without a detrimental
increase in gas pressure inside the container. This is consistent with previous studies [3].

AMEC/000795/001 Issue 3 Page 43


2.5E+06

2.0E+06
Excess Gas Pressure (Pa)

1.5E+06

1.0E+06

5.0E+05

0.0E+00
0 10 20 30
Time (days)

Tensile strength Q=1 Q=2 Q=4 Q=8 Q = 16 Q = 32 Q = 64 Q = 128

Figure 5.6 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

1.4E+06

1.2E+06

1.0E+06
Excess Gas Pressure (Pa)

8.0E+05

6.0E+05

4.0E+05

2.0E+05

0.0E+00
1 10 100 1000
Gas Injection Rate (m 3yr-1 at STP)

Tensile strength Steady-state pressure

Figure 5.7 Steady-state excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

AMEC/000795/001 Issue 3 Page 44


5.4 Instantaneous Setting and Hardening – New Boundary
The discussion of backfilling strategy in Section 2.4 makes it apparent that the backfill could be
cast in layers. The layers could be 400 mm thick, and there could be a period of 24 hours between
successive pours.

Our third calculation modifies the model domain and the boundary conditions to represent this
backfilling procedure, and then repeats the simulations of Section 5.3.

5.4.1 Numerical Grid

The model includes a representation of:


§ the ullage space at the top of a waste package, which is assumed to be a 500L drum;
§ the vent in the top surface of the waste package; and
§ the NRVB between the waste package and an overlying container.

Assuming that the backfill is cast in layers that are 400 mm thick, then the layer that covers the
vent will fill the void space above the waste package to a height of 200 mm on average. Therefore,
the model domain was extended to include an extra quantity of backfill between adjacent waste
packages. (We note that the thickness of backfill above the waste package will increase as
subsequent layers are cast, but this particular effect was not considered in our model.)

The geometry of the model domain is indicated in Figure 5.8, and the discretisation of the model
domain by a numerical grid is shown in Figure 5.9.

(a) (b)
Figure 5.8 The geometry of the model domain: (a) shows detail around the vent; and
(b) shows detail at the outlet boundary. The ullage space is coloured pink, the
vent is green, the NRVB is blue, and the outlet boundary is yellow.

AMEC/000795/001 Issue 3 Page 45


Figure 5.9 The numerical grid used in the simulation.

5.4.2 Properties of the NRVB

The properties of the NRVB are unchanged from Section 5.3.

5.4.3 Initial Condition

The initial condition of the NRVB is unchanged from Section 5.3.

5.4.4 Boundary Condition

The boundary condition on the outlet surface of the NRVB is chosen to be:
5
§ air at atmospheric pressure Pout = 1.01325 10 Pa for a period of 24 hours after the layer has
been poured; and thereafter
5
§ water at atmospheric pressure Pout = 1.01325 10 Pa.

The other surfaces of the model domain are no flow boundaries.

Hydrogen is injected into the ullage space, which initially is an air-filled void space, at a constant
3 -1
rate. The hydrogen injection rates considered are Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP.

5.4.5 Results

The results for this variant are shown in Figure 5.10 and Figure 5.11.

The increase in the size of the model domain and the change to the boundary condition on the
outlet surface of the NRVB have a modest effect on the maximum and the steady-state excess gas
pressures in the ullage space.

AMEC/000795/001 Issue 3 Page 46


2.5E+06

2.0E+06
Excess Gas Pressure (Pa)

1.5E+06

1.0E+06

5.0E+05

0.0E+00
0 10 20 30
Time (days)

Tensile strength Q=1 Q=2 Q=4 Q=8 Q = 16 Q = 32 Q = 64 Q = 128

Figure 5.10 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

1.4E+06

1.2E+06

1.0E+06
Excess Gas Pressure (Pa)

8.0E+05

6.0E+05

4.0E+05

2.0E+05

0.0E+00
1 10 100 1000
Gas Injection Rate (m 3yr-1 at STP)

Tensile strength Steady-state pressure

Figure 5.11 Steady-state excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6 10 Pa).

AMEC/000795/001 Issue 3 Page 47


5.5 Gradual Setting and Hardening
The fourth (and final) calculation takes into account our understanding of the changes in the
permeability, the porosity, the degree of saturation, and the strength of the NRVB during setting
and hardening (see Section 4). The calculation modifies the computer code to represent the
evolving properties, and then repeats the simulations of Section 5.4.

5.5.1 Numerical Grid

The model domain and numerical grid are unchanged from Section 5.4.

5.5.2 Properties of the NRVB

The NRVB is assumed to harden gradually, and to have the evolving properties listed in Table 5.3.

Table 5.3 Evolving properties of the NRVB

Property Value

Permeability See Figure 4.8


5
Klinkenberg parameter 5.49 10 Pa

Porosity See Figure 4.11

Saturation functions van Genuchten form


(see Section 4.6)

Tortuosity 0.25

Tensile strength Estimated as one-tenth of


the compressive strength

Compressive strength See Figure 4.5

5.5.3 Initial Condition

When gas generation in the waste container starts, the NRVB is saturated Sw = 1.0 and is at an
5
ambient pressure equal to atmospheric pressure Pout = 1.01325 10 Pa.

5.5.4 Boundary Condition

The boundary conditions are unchanged from Section 5.4.

5.5.5 Results

The results for this variant are shown in Figure 5.12 and Figure 5.13.

The maximum excess gas pressures in the ullage space are much reduced, probably because the
gas pathway forms during the period when the NRVB is still reasonably permeable.

In the longer term, both the steady-state excess gas pressures and the tensile strength of the
NRVB appear to be approaching the values obtained when it is assumed that the NRVB hardens
instantaneously. This suggests that if the NRVB has hardened and the gas generation rate is
3 -1
below about 10 m yr at STP, then at steady-state the gas will be able to flow through the NRVB
without a detrimental increase in gas pressure inside the container.

AMEC/000795/001 Issue 3 Page 48


2.5E+06

2.0E+06
Excess Gas Pressure (Pa)

1.5E+06

1.0E+06

5.0E+05

0.0E+00
0 10 20 30
Time (days)

Tensile strength Q=1 Q=2 Q=4 Q=8 Q = 16 Q = 32 Q = 64 Q = 128

Figure 5.12 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
tensile strength of the NRVB.

1.0E+06

8.0E+05
Excess Gas Pressure (Pa)

6.0E+05

4.0E+05

2.0E+05

0.0E+00
1 10 100 1000
Gas Injection Rate (m 3yr-1 at STP)

Tensile strength Steady-state pressure

Figure 5.13 Steady-state excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
5
tensile strength of the NRVB (i.e. 6.63 10 Pa).

AMEC/000795/001 Issue 3 Page 49


Although the peaks in the excess gas pressures in the ullage space are much reduced, the peaks
occur while the NRVB is hardening and has low strength (see Figure 5.14; this is the same as
Figure 5.12, but with an expanded time axis that shows only the first six hours). During the first few
3 -1
hours from initial set, rates of gas generation below 1.0 m yr could cause disruption of the NRVB,
particularly in locations adjacent to the waste package vents. Therefore this calculation suggests
3 -1
that a gas generation rate significantly less than 10 m yr at STP could damage the backfill
material.

1.0E+05

9.0E+04

8.0E+04

7.0E+04
Excess Gas Pressure (Pa)

6.0E+04

5.0E+04

4.0E+04

3.0E+04

2.0E+04

1.0E+04

0.0E+00
0 1 2 3 4 5 6
Time (hours)

Tensile strength Q=1 Q=2 Q=4 Q=8 Q = 16 Q = 32 Q = 64 Q = 128

Figure 5.14 Evolution of excess gas pressure (i.e. pressure above ambient) in the ullage
space of a waste container – results at different hydrogen injection rates
3 -1
(i.e. Q = 1, 2, 4, 8, 16, 32, 64 and 128 m yr at STP) are compared with the
tensile strength of the NRVB.

AMEC/000795/001 Issue 3 Page 50


6 Conclusions
The objective of this work was to identify some uncertainties in the “screening limit”, taking into
account the process of backfilling as well as the changing characteristics of the backfill during
setting and hardening.

Three topics relating to the performance of the backfill during placement and curing have been
considered:
1. The performance of the backfill while in its fluid state, and whether gas generation from a
waste package could disrupt the backfill during this stage.
2. The development of strength in the backfill during hardening, and how that compares to the
build-up of pressure within a container due to gas generation.
3. The change in flow properties (e.g. permeability, pore structure and moisture content) of the
backfill during hardening, and how that alters the pressure within a container.

The conclusions of this report as regards these three topics are presented below.

6.1 Gas Migration across NRVB while Fluid


The performance of the NRVB while it is in its fluid state, and whether gas generation from a waste
package could disrupt the backfill during this stage, has been assessed. Prediction of the
behaviour of the NRVB is complicated by:
§ the inability to predict precisely how the fluid grout will flow during the backfilling process; and
§ the interaction of the NRVB and the gas flows.
3 -1
It is estimated that during the backfilling process, rates of gas generation as low as about 0.3 m yr
may cause disruption of the fluid NRVB, particularly in locations adjacent to the waste package
vents. Such disruption may also lead to continuous leak paths through the grout.

In view of the difficulties in predicting the behaviour of the NRVB during the backfilling process,
experiments would be required to determine, more reliably, the effects of gas generation. Such
tests would have to be at full scale, reproducing the rate of filling expected in a vault. Important
factors include:
§ The effective void space within the waste package, as it affects the rate of pressure build-up.
§ The rate of filling, as it affects the head of fluid grout covering the vent.
§ The age of the NRVB when it flows over the vent, as it affects the yield stress of the grout.
§ The flow pattern of the NRVB.

6.2 Properties of NRVB at Early Age


The properties of the NRVB change most rapidly during the first few days after placing, and are
dependent on the temperature rise resulting from the heat of hydration.

Estimates have been made of the development of compressive strength and permeability (to both
water and gas) from initial set up to 100 days, beyond which time it is assumed that there will be
only insignificant changes. Calculations of the temperature rise, strength development, the
permeability, the porosity and the degree of saturation have been made using a modified version of
the Arrhenius method that accounts for the consequences of a higher curing temperature, including
acceleration in early age development and a detrimental effect on the ultimate strength.

AMEC/000795/001 Issue 3 Page 51


Over the plan area of a vault, the NRVB will vary in thickness depending upon the way in which the
waste packages have been stacked. Therefore the local rise in temperature also will vary, causing
differences in the rate of strength development, the ultimate strength and the permeability. (A
thicker layer of NRVB will achieve a higher temperature rise, a lower ultimate strength and a higher
permeability.) This is probably too complex to model in practice, and therefore it is recommended
that within each horizontal layer mean values should be assumed.

During the backfilling process, properties will also vary significantly through the height of a vault.
The deeper, older grout will have higher strength and lower permeability. This variation could be
taken into account in a global vault analysis, based on the age of the NRVB in each layer and the
temperature history.

It is estimated that the porosity will reduce from about 0.62 to about 0.45 after full hydration. The
degree of saturation will remain high (>90%), because only a relatively small proportion (i.e. about
a third) of the water is required to complete the hydration process.

6.3 Gas Migration across NRVB at Early Age


3 -1
If the NRVB has hardened and the gas generation rate is below about 10 m yr at STP, then at
steady-state the gas will be able to flow through the NRVB without an increase in gas pressure that
could affect the integrity of the NRVB. This is consistent with previous studies.

Migration of gas through the NRVB while it is hardening has been modelled. Prediction of the
behaviour of the NRVB is complicated by a lack of detailed knowledge about how the properties of
the NRVB will evolve during curing. However, during the first few hours from initial set, it has been
3 -1
estimated that rates of gas generation below 1 m yr at STP may cause disruption of the NRVB,
particularly in locations adjacent to the waste package vents.

6.4 Information Required to Support a “Screening Limit”


It seems that the changing characteristics of the backfill material during placement, setting and
hardening may be important for deriving a “screening limit” on the rate of gas generation from
individual waste packages, below which the gas should not pose any risk to the integrity of the
backfill material.

Although this work has explored this particular issue through numerical modelling, there are many
uncertainties about how the properties of the backfill will change as it cures, and how it will interact
with the gas phase. However, it is also unclear how much changes in the physical integrity of the
backfill in the immediate vicinity of waste package vents might be tolerable, from the perspective of
a post-closure safety case. A programme of experimental work may be required to address these
uncertainties.

Based on the processes described in Sections 3, 4 and 5, the following information would be
required to derive a “screening limit” on the rate of gas generation from individual waste packages.

6.4.1 Waste Packages


1. The effective void space within the waste package.
2. The size of the horizontal gap between adjacent packages.

AMEC/000795/001 Issue 3 Page 52


6.4.2 Backfill
8
3. The characteristics of the fluid NRVB, and how they change with time.
4. The stiffening time, when the NRVB ceases to exhibit fluid behaviour.
5. The setting time, when hydration commences to form a rigid pore structure.
6. The rate of development of the pore structure, and how this affects permeability.
7. The rate at which the moisture content, or degree of saturation, of the NRVB changes.
8. The effect of temperature on all of the above.

6.4.3 Backfilling Strategy


9. The rate at which the head of fluid NRVB is established at the vent locations.
10. The rate at which the horizontal gap between adjacent packages is filled.
11. The rate at which the head of fluid NRVB is established in the gap between adjacent
packages.
12. The period over which the vault is backfilled.

8
These could be in the form of yield stress and plastic viscosity, which would characterise the
NRVB as a Bingham plastic material.

AMEC/000795/001 Issue 3 Page 53


7 References
1. Nuclear Decommissioning Authority, Geological Disposal: An Overview of the Generic
Disposal System Safety Case, NDA Report NDA/RWMD/010, 2010.
2. Nuclear Decommissioning Authority, Geological Disposal: Gas Status Report, NDA
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3. A.R. Hoch, “Screening Limit” on the Rate of Gas Generation from Individual Intermediate-level
Waste Packages, Serco Report SA/ENV-0888, Issue 3, 2017.
4. B.T. Swift, P.B. Bamforth, A.R. Hoch, C.P. Jackson, D.A. Roberts and G.M.N. Baston,
Cracking, Flow and Chemistry in NRVB, Serco Report SERCO/TAS/000505/001,
Issue 3, 2010.
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Designs in Clays and Evaporites, Wardell Armstrong Report NL05847J01v2, 2007.
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NDA Report NDA/RWMD/048, 2010.
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Report on Current Status in 1994, Nirex Science Report S/97/014, 1997.
10. S.R. Newson, Backfilling, Sealing and Closure – Logistics Study, Wardell Armstrong Report,
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Using Liquid and Gas, Magazine of Concrete Research, 39, Nos. 138, pp. 3-11, 1987.

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Microstructure, Journal of the American Ceramic Society, 80, Nos. 1, pp. 3-21, 1997.
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for the Two-phase Flow of Immiscible Fluids in the Subsurface, Water Resources
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into a Repository Vault, Nirex Report NSS/R201, 1989.
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