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2001 International Ash Utilization Symposium, Center for Applied Energy Research, University of Kentucky, Paper #97.

Copyright is held by the Authors.

http://www.flyash.info

Field Leaching of Bricks and Concrete


Containing Coal Fly Ash

Ruud Meij , Esther Kokmeijer, Leendert Tamboer and Henk te Winkel

KEMA Power Generation & Sustainables, P.O. Box 9035, NL 6800 ET Arnhem, the
Netherlands, telephone +31-26-3562225, fax +31-26-4453659, e-mail: r.meij@kema.nl

KEYWORDS: leaching, field tests, laboratory tests, diffusion test, availability test, bricks,
concrete, hydrology, coal fly ash

SUMMARY

In the Netherlands building materials must comply with leaching limits as laid down in the
Buildings Materials Decree. The leaching behaviour of the building materials has to be
determined by standardised tests at the laboratory. The results of these tests are used as
input in formulas that calculate the cumulative emissions over 100 years. The question
arises whether this approach is a good prediction of what will happen in the field. At
KEMA a major research item is to investigate leaching behaviour under field conditions.
This paper presents the results of field leaching of two types of bricks for five and a half
years and of concrete for two years. For these three types of building material two forms
are tested, one ordinary form and one in which 20% coal fly ash (CFA) is used. The
results are compared between the different types of clay, between materials with and
without CFA and between prolonged field tests and brief laboratory leaching tests.

The use of CFA as a raw material in bricks and concrete increases the leaching of As, Mo
and sulphate. Vanadium also shows this increase of leaching in bricks, but not in
concrete. The effect of using CFA in one type of brick is that the Cr leaching increases,
while in another type of brick and in concrete it decreases. In all cases and for all
elements the leaching stays well below the limits as laid down in the Building Materials
Decree, so CFA can well be used in building materials without contaminating the soil or
surface water.

Compared to the 5½ years field test, the extrapolation of the diffusion test to 5½ years
gives a reasonable prediction of the leaching of molybdenum and vanadium; however,
the diffusion test overestimates the leaching of arsenic and barium and it underestimates
the leaching of chromium and sulphate.
Field leaching behaviour of
building materials

Dr. Ruud Meij, Dr. Esther Kokmeijer,


Leendert Tamboer B.Sc. and Henk te Winkel B.Sc

KEMA the Netherlands

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 1


Content

ý Introduction

ý Building Materials Decree and leaching


test
ý Leaching in lab versus field

ý Conclusions

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KEMA
Power Generations
&
Sustainables

Arnhem

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 3


Dolmen or megalithic grave in the Netherlands
Buildings Materials Decree
In order to prevent soil, groundwater and surface water
pollution limits are set for immissions into the soil for use
of primary, secondary and waste materials.
Ä two limits one for building materials in
contact with rain, surface water and
/or ground water and one for buildings
materials isolated from water

Ä two type of limits one for moulded


products and one for unmoulded products

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Buildings Materials Decree
Gives maximum immission levels for the soil
the next step is
translation of emission levels, to be determined via
column test for unmoulded materials, into immission
levels according to the formula below:
IbN = 1550 * (Emean (L / S = 10 ) − a) * h * fext − N

t •Ni
−k •
1 −e 1550•h
fext −N =
1 − e −k •10
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Characteristics of the various leaching
tests for unmoulded materials
type of leaching Dutch column Dutch cascade EPA test 1) Dutch availability
test test test test

L/S ratio 10 5x20=100 20 2 x 50

time scale in 5-50 50-100/ 100-500 extreme long


years pe riod
short/medium longterm
worst case

demineralized initial pH=4 initial pH=4 constant pH=5 constant pH=7


water at pH: 1) alkaline and pH=4
e quilibrium- alkaline
pH equilibrium pH

process upward flow shake test 5x shake test shake test 2x


<2 cm•h -1 refreshment re freshment

time 3 weeks 5x23 hours 24 hours 2x3 hours


1)
the pH is adjusted by adding HNO3; for the EPA test this is a deviation from the prescribed
acetic acid; for some ashes the equilibrium pH is acid, but those ashes are not taken into
consideration in these experiments, because they are hardly produced any more.

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For moulded materials one
have to perform a tank leaching
test during 64 days and
calculate the diffusion
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Translation from laboratory test into emission

E(64d) = db·Ebes·√ (De/π)·√ t


E(64d) = emission as determined by the diffusion test for 64 days

db = density of the material (kg.m-3 )

Ebes = emission as determined by the availability test (mg.kg -1 )

De = effective diffusion coefficient

t = contact time (s).

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Translation from emission into immissions

Ical.(Y) = Edif(64d)·fext,v(h,x%,De)·ftem
Ical.(Y) = calculated immissions after Y years in mg.m-2

Edif(64d) = calculated diffusion after 64 days in mg.m-2

fext,v(h,x%,De) = extrapolation factor of 64 days to Y years taking into con-

sideration the size (high) of the building (h), wet periods

(x%) and the possible change in De (see equation (1))

ftem = correction factor for the temperature difference of the labo-

ratory and field conditions

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The composition of the building materials
code type mass composition PFA
(kg)
sand lime bricks 0-60% SDA
A half-bricks 182 bronze fired clay
B half-bricks 178 bronze fired clay 20%
C half-bricks 185 red fired clay
D half-bricks 178 red fired clay 20%
E reference 178 trespa (plastic)
F hollow wall 2*178 bronze fired clay 20%

G concrete Portland cement CEM I 32,5

H concrete Portland cement CEM I 32,5 20% + o.v. cement


320 kg/m3
I concrete Portland cement CEM I 32,5, 20% recycled 20% + o.v. cement
concrete granules as artificial gravel 320 kg/m3
J concrete Portlandcement CEM I 32,5, 100% recycled 20% + o.v. cement
concrete granules as artificial gravel 320 kg/m3

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 11


Availability test of clay bricks
Availability test of clay bricks

18

bronze fired
16
bronze fired + PFA
14
red fired
mg/kg (g/kg SO4)

12 red fired + PFA

10

As Ba Cr M o V SO4

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The calculated diffusion coefficient
De (10–12 m.s –1)
for the various types of bricks

code composition As Ba Cr Mo V SO42-


A bronze-fired clay 2.3 0.1 8.8 6.5 9.1 2.0
B idem + 20% CFA 1.5 6.8 40.8 22.0 4.3 3.9
C red-fired clay 0.4 0.2 9.2 8.4 5.2 3.0
D idem + 20% CFA 1.0 0.2 58.7 17.9 22.6 1.0

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Diffusion test of clay bricks
diffusion test of clay bricks
80 bronze fired
bronze fired + PFA
70
mg/m2 (g/m2 SO4)

red fired
red fired + PFA
60
mortal
50

40

30

20

10

As Ba Cr Mo V SO4

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 14


mg.m-2
time 64 days
BMD1) test2) Limits
according
wall U1a U2,1b A B, F C D mortal
As 41 140 20.1 18.6 8.2 14.8 <0.9
Ba 600 2000 6.5 32.3 5.2 6.6 50 to the
Buildings
Cd 1.1 3.8 0.1 <0.05 0.12 <0.05 <0.05
Co 29 95 <1.1 <1.1 <1.1 <1.1 <1.1
Cr 140 480 3 3.2 4.3 3 1.9 Materials
Cu 51 170 3 1.2 <1.1 <1.1 <1.1
Hg 0,4 1.4 <0.06 <0.06 <0.06 - <0.06
Decree
and lab.
Mo 14 48 4.7 14.3 3.3 10.3 <2.3
Ni 50 170 <1.7 <1.7 <1.7 <1.7 <1.7
Pb
Sb
120
3.7
400
12
15.6
<1.7
6.9
<1.7 <1.7
9 3.8
<1.7
<2.3
<1.7
test
Se 1,4 4.8 <1.1 <1.1 <1.1 <1.1 <1.1 results in
Sn
V
29
230 760
95 <1.1
51.4
<1.1
73.6
<1.1
59.9
<1.1
66.2
<1.1
4.8
mg.m-2
Zn 200 670 3.1 <2.9 8 <2.9 <2.9
SO42- 27000 80000 5096 3184 2322 1603 793

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Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 17
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Hydrology of the walls

type of wall amount of amount of


leachate evaporation
reference (plastic) 100% 0%
concrete 77% 23%
half-bricks 17% 83%
hollow wall 1.3% 90-94%

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 19


Cumulative Field leaching of bricks
10 in 5½ years under field conditions
A bronze
As
8
diffusion in mg/m2

B bronze+CFA

5
C red

3
D red+CFA

0
0 50 100 150 200 250 300 F red hollow
weeks

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 20


10
mg.m-2 30

As Mo
diffusion in mg/m2 8

diffusion in mg/m2
Cumulative
20

10

Field
3

leaching of
0 0

1 100

Ba

bricks
V
A bronze
1 75

diffusion in mg/m2
diffusion in mg/m2

B bronze+CFA

in 5½
1 C red 50

D red+CFA

years
0 25

F red hollow

under field
0 0

30 30

Cr S O 4 2-

conditions
25
diffusion in mg/m2

diffusion in g/m2

20 20

15

10 10

0 0
0 50 100 150 200 250 300 weeks 0 50 100 150 200 250 300

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 21


Cumulative Field leaching of bricks
in 5½ years under field conditions
30 A
bronze
Cr
diffusion in mg/m2

B
20 bronze
+CFA
C red

10
D
red+CF
A
0 F red
0 50 100 150 200 250 300 hollow
weeks

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 22


Cumulative Field leaching of bricks
in 5½ years under field conditions
1,5%

As
field leaching in %
of availability test

1,0%

0,5%

0,0%
0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70

L/S in l/kg

A bronze B bronze+CFA C red D red+CFA F hollow+CFA

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mg.m-2
1.5
1,5%

As
25 25%

Mo
field leaching in % of 20%

field leaching in % of
Cumulative
availability test

availability test
1,0%
15%

10%
0,5%

Field
5%

0,0% 0%

leaching of
0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70 0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70

0.2 0,2%

Ba A bronze
15
15%

bricks
field leaching in % of

0,2% B bronze+CFA

field leaching in % of
availability test

availability test
C red 10%

0,1%
D red+CFA

in 5½
F hollow+CFA 5%
0,1%

years
0,0%
0%
0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70
0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70

120
under field
120% 100%

Cr 100 SO4
2-
field leaching in % of

field leaching in % of

75%
availability test

availability test

conditions
80%

50%

40%
25%

0% 0%
0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70 0,00 0,10 0,20 0,30 0,40 0,50 0,60 0,70
L/S in l/kg L/S in l/kg

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 24


Cumulative Field leaching of concrete in 2
years under field conditions
0,3

Mo
cumulative diffusion in mg/m2

0,2

0,1 G concrete
H concrete+CFA

0,0
0 20 40 60 80 100 120
weeks

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 25


mg.m-2
0,3 5,0

As V
cumulative diffusion in mg/m2

cumulative diffusion in mg/m2


Cumulative
3,8
0,2

2,5

Field
0,1
G Concrete
G concrete
H concrete+CFA 1,3
H concrete+CFA

leaching of
0,0 0,0

6,0 2,0

S O 4-2
concrete

cumulative diffusion in g/m2


cumulative diffusion in mg/m2

Cr
1,5
4,0

in 2 years
G concrete
1,0
H concrete+CFA
`

2,0 G concrete
0,5 H concrete+CFA

0,0

0,3
0,0
0 20 40
w e6e0k s 80 100 120 under field
cumulative diffusion in mg/m2

conditions
Mo

0,2

G concrete
0,1
H concrete+CFA

0,0
0 20 40 w e6e0k s 80 100 120

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 26


Limits according to the Buildings Materials
Decree and field test results in mg.m-2
time 100y 5.5 years3) 2y
BMD test field test field field test field test field field field
wall A A B B F C C D D G H
As 435 24.9 3.4 23.1 7.8 0.6 10.2 1.2 18.4 5 0.12
Ba 6300 8.1 0.6 40 0.7 0.2 11.6 0.6 14.8 0.7
Cd 12
Co 300
Cr 1500 3.7 11 4 17.1 6.9 5.3 26.9 3.7 15.7 1.2 0.8
Cu 540
Hg 4.5
Mo 150 5.8 5.7 17.7 22.2 2.7 4.1 7.6 12.8 17.6 0.1 0.2
Ni 525
Pb
Sb
1275
39 mg.m-2
Se 15
Sn 300
V 2400 63.8 58.6 91.3 95.5 21.6 74.3 36.2 82.1 68.2 4.2 3.7
Zn 2100
SO 42- 100000 6320 17000 3950 25300 6000 2880 23700 1990 23900 1200 1600

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 27


Field leaching in % of diffusion test (5,5 years)

1400%

1200%

1000% As
800% Ba
Cr
600%
Mo
400% V
200% SO4

0% V
A Cr
B + F+
As
C
D+

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 28


Field leaching in % of diffusion test (5,5 years)

200%
180%
160%
140% As
120% Ba
100% Cr
80% Mo
60%
V
40%
SO4
20%
0% V
A Cr
B + F+
As
C
D+

Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 29


Conclusions
ý CFA (20%) in bricks and concrete can meet the strict Dutch
leaching limits

ý the leaching of As, Mo and sulphate increases. V also


shows this increase of leaching in bricks, but not in concrete.
The leaching of Cr is however rather complicated; in one clay it
shows an increase in leaching after adding CFA and in another
clay and in concrete it shows a decrease.

ý the results of the diffusion test extrapolated to the observed


5½ years give a reasonable pre-diction of the leaching of Mo and
V; however, it overestimates the leaching of As and Ba and it
underestimates the leaching of Cr and sulphate, with respect to
the half-brick wall.

Thank you for your attention


Lexington, Kentucky * October 22-24 2001 International Ash Utilisation Symposium 30