Application field of biotrickling filters for biogas H2S removal: optimization of

its operating conditions and long-term operation

N. de Arespacochaga*, C. Mesa*, A. Hornero*, L. Bouchy*, E. Larrotcha**, C. Peregrina***
* CETaqua, Water Technology Centre, , Carretera dEsplugues 75, 08940 Cornell de Llobregat, Barcelona, Spain,
narespacochaga@cetaqua.com)
** Agbar, Avinguda Diagonal 211, 08018 Barcelona, Spain
***CIRSEE, 38 Rue du President Wilson, 78230 Le Pecq - France

Short Abstract
The most harmful biogas contaminant for energy conversion equipment is hydrogen sulphide,
thus efficient and cost-effective treatment systems for this compound should be designed and
developed. A pilot-scale biotrickling filter was constructed in a WWTP in Spain in order to
evaluate the effect of three key important process parameters (temperature, retention time and
pH) on its operational performance. Short-term tests showed that H2S removal efficiencies
greater than 90% and outlet concentrations of about 300 ppm can be obtained at temperatures of
30C, retention times of 80 seconds and pH of 1,5. However, long-term experimentation at these
conditions showed much lower performance (a removal efficiency of 80% and an availability of
86%) as a result of progressive filter clogging due to elemental sulphur and gypsum
accumulation. Therefore, today bio-trickling filters are not a reliable alternative for biogas
desulphurisation.
Keywords: biogas, biotrickling filter treatment, removal efficiency, availability, fuel cells

Introduction
Within the framework of sustainable
development, and ever-increasing energy
costs, sewage biogas utilisation is the main
approach today for wastewater treatment
operators for on-site energy production.
Biogas contains contaminants like sulphur
compounds, siloxanes, hydrocarbons and
halogenated organic compounds. The most
harmful for energy conversion equipment is
hydrogen sulphide (Monteleone et al, 2011),
thus in most cases, costly and energy
consuming H2S removal technologies must
be installed upstream in order to meet the
inlet requirements (300-500ppmv for internal
combustion engines; 1ppmv for fuel cells or
grid injection, Deublein and Steinhauser,
2008). Therefore, it is necessary to develop
efficient and cost-effective technologies for
biogas desulphurization; and biological
treatments show very promising prospects
(Abatzoglu and Boivin, 2009).

In biological gas treatment systems

contaminants are transferred into a liquid
phase (absorption or adsorption on a media)
to be degraded by micro-organisms, usually
under aerobic conditions (Mudliar et al,
2010). The products of this degradation are
either released in the gas phase (eg CO2), or
remain within the liquid phase either
suspended or on the media (eg NO2-, SO42-).
Two important biological technologies are
available
for
biogas
applications:
bioscrubbers and biotrickling filters.
Bioscrubbers consist of two reactor vessels:
an absorption tower followed by a biological
reactor. H2S is removed from biogas at the
first stage by chemical absorption with
caustic soda, which is the most conventional
scrubbing agent in these systems. The
washing solution is biologically regenerated
in the second stage and then recycled to the
scrubber, where it can absorb again

Page 1 of 7

hydrogen
sulphide.
This
2-reactor
configuration allows these systems to have
all the advantages of chemical systems (high
reliability and up to 99% H2S removal
efficiency) and to achieve a reduction of
around 75 80% in NaOH consumption
(Boonstra et al, 1999).

accumulation
strongly
affects
the
biotrickling
filter
operation
and
performance, since the available cross
section area of packing material is
dramatically decreased, thus reducing the
contact time between biogas and SOB and
affecting then H2S removal efficiency.

On the other hand, in biotrickling filters

(BTF), the overall process takes place in
only one reactor. Sulphur oxidizing bacteria
(SOB), which form a biofilm on an inorganic
packing material inside the reactor,
metabolize hydrogen sulphide into elemental
sulphur and sulphuric acid (depending on the
oxygen availability; reactions below):

In
biotrickling
filters
for
biogas
desulphurization, this is mainly the result of
bacterial growth and elemental sulphur
formation (S0) due to partial oxidation. In
addition, make-up water hardness also plays
an important role in the clogging rate of the
column because of gypsum (CaSO4)
production by combination of calcium
cations from water and sulphate anions from
H2S full oxidation.

H 2 S ( g ) + 2O2( g ) H 2 SO4( aq )

2 H 2 S ( g ) + O2( g ) 2S (0s ) + 2 H 2 O( aq )
2S (0s ) + 3O2( g ) + 2 H 2 O( aq ) 2 H 2 SO4( aq )
Differently from bioscrubbers, no reagent
addition is necessary to operate these
systems; effluent water from wastewater
treatment plants (WWTP) is used as a source
of nutrients for biological activity, thus low
operating costs are expected. However, these
systems face several technical challenges in
order to achieve comparable removal
efficiency and operational reliability with
bioscrubbers. The most important ones are
listed below:
1. Oxygen supply to SOB
2. Ability to cope with concentration
peaks
3. Long-system start-up
4. Filter clogging
The latter has often been described as the
most important drawback (Fortuny et al,
2008). Filter clogging occurs due to
accumulation of biomass, and other
compounds, in the contact surface where the
biological degradation takes place. This

As a result, many design and operation

conditions still require optimisation and the
limits of the systems are still to determine.
The aim of this paper is to evaluate the effect
of three key important process parameters
(temperature, retention time and pH) on the
short and long term performance of
biotrickling
filters
for
biogas
desulphurisation and assess its applicability
as upstream system for several biogas energy
conversion systems (internal combustion
engines, fuel cells and injection into the gas
grid).

Methods
The pilot-scale biotrickling filter showed in
Figure 1 was constructed in a WWTP in
Matar (Spain). This unit is part of a bigger
biogas valorisation plant, which consists of,
apart from the BTF, a polishing stage
(adsorption on iron oxides and activated
carbon) and a Solid Oxide Fuel Cell (SOFC).
The available range for the most important
BTF design parameters and packing material
characteristics are set forth in Table 1.

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Several definitions should be taken into

account when assessing BTF performance:

Residence time ( ): Actual time that

the gas remains in the filter bed.

Vvoid Vbed
=
Q
Q
Loading rate (LR): quantity of H2S
introduced per unit of reactors
volume (g H2S/(m3h).

Q Cin
V
Elimination capacity (EC): quantity
of H2S removed per unit of volume
(g H2S/(m3h).

LR =

Figure 1. Pilot-scale BTF in Matar WWTP

Operating
parameter

Inlet biogas
flow

Range

6 11
Nm3/h

Temperature 5 35C
Circulation
water

800
1.100 L/h

pH

1,5 7

EC =

Needle valve and

mass flow meter
(FCI ST75)
Heater and
thermostat
Ball valve and
rotameter (Stbbe
DFM 165)
Make-up water
dosage

Table 1. Operating parameters range

Parameter
Material
Packing

Block size
Packing height
Packing volume
Surface area
Bulk density
Void fraction ()

Control/Operation

Unit

Value
Polypropylene
Structured blocks model
HD Q-PAC
mm
305 x 305 x 305
m
1,8
3
m
0.16
m2 m-3
433
-3
Kg m
112
%
87,8

(Qin Cin QOUT C out )

V
Removal efficiency (RE): fraction of
the pollutant removed (%).
EC
100
LR
Availability: number of running
hours
Running hours
Availability =
100
Total hours
RE =

Biogas analysis
An extractive on-line biogas analyser was
installed at the inlet and outlet of the BTF,
according to the information in Table 3.
Furthermore, grab gas samples were also
analysed with Drger tubes (ref. CH 29 101
and ref. CH 28 101).

Sensor Measure
CH4
CO2
O2
H2S

Table 2. Features packing material

5 min
5 min
5 min
30 min

Measurement Accuracy
principle
Infrared
2%
Infrared
2%
Paramagnetic
2%
Electrochemical
3%

Table 3. Biogas analysis sensors

Page 3 of 7

Filter clogging
Two methods were identified to determine
the clogging status of the column.
1. Quantitative method: mass balance
of the different sulphur compounds
that may play a role in the clogging
process (Figure 2) which lead to a
very precise estimation of the
clogging rate inside the packing
material of the column. However,
this method necessarily involves offline and time-consuming analysis of
sulphates, elemental sulphur and
water hardness, thus being somewhat
useless
for
online
clogging
monitoring.

significantly polluted with H2S and a broad

variation is also observed depending on the
season. These two factors pose a challenge
to the BTF efficiency.

Compound Unit Average Max Min

CH4
%
63,8
70,5 57,7
CO2
%
32,0
36,1 26,2
O2
%
0,7
1,3
0,2
H 2S
ppm 2.600 4.300 1.200
Table 4. Raw biogas composition (2010)

Short-term
experiments:
operating conditions

optimized

The system was started up (inoculated with

secondary sludge from the WWTP) and was
operated to the steady-state. Afterwards, 3day experiments were carried out by
changing the studied process parameter and
keeping constant the rest.
Temperature is expected to be a key
parameter for bacterial growth, thus for H2S
removal efficiency. Results at 10, 15, 20, 25,
30 and 35C are presented in Table 5 (biogas
flow rate 9 10 Nm3/h and pH 1,5):

Figure 2. Mass balance of compounds involved in

the clogging processes

2. Qualitative method: determine the

degree of clogging by tracking the
pressure drop within the column.
Although it is not as accurate as the
previous one, it allows for a costeffective and rapid method for
monitoring filter clogging.

Results
Table 4 depicts a one-year average raw
biogas composition. As it is shown, biogas is

T (C)

H2S in
(ppm)

H2S out
(ppm)

RE (%)

10
15
20
25
30
35

2.910
2.780
2.823
3.039
3.420
3.210

1.342
1.179
921
821
790
732

49,3
53,3
64,1
70,3
74,6
74,9

Table 5. Temperature effect on RE (9-10 Nm3/h,

pH = 1,5)

As it is shown, bacteria show its highest

performance at around 30C and become
inactive below 15C. Greater temperatures
could not be tested because the packing
material could melt, but no significant effect

Page 4 of 7

is expected by comparing performance from

30 and 35C. Maximum removal efficiency
was only 75% and outlet H2S concentrations
did not go below 700 ppm, which is too high
even for cogeneration applications.
Residence time: In order to increase the
removal efficiency of the BTF, the residence
time was increased by lowering the biogas
flow rate. As it is overviewed in Figure 3
(temperature 30C and pH 1,5), 90%
efficiency can be achieved at residence times
greater than 80 seconds, which corresponds
to a biogas flow rate of around 7 Nm3/h.
Within these experiments, H2S outlet
concentrations of 310 ppm were observed,
meaning that the gas could have been used in
an internal combustion engine.

into NO3- (Deshusses et al, 1998). Because

of this, recommended values for pH are
between 1 and 2, as nitrifying bacteria die at
extremely acidic conditions.

Long-term operation
operating conditions

at

optimized

A 4-month experiment was conducted at

optimized operating conditions (temperature
30C, biogas flow rate 7,5 Nm3/h and pH
1,5) in order to assess filter clogging and
long-term performance.
Filter clogging: Pressure drop over the BTF
is displayed in Figure 4.

Figure 4. Pressure drop over a 1 month period

Figure 3. Residence time effect on RE (T = 30C,
pH = 1,5)

pH is also considered an important

parameter as H2S solubility into the liquid
phase is enhanced at alkali conditions,
favouring pollutants mass transfer to the
biofilm and thus increasing removal
efficiency. However, Deshusses and Gabriel
(2003) observed that the more the pH
decreases, the greater the efficiency. The
reason roots on the fact that at greater pH,
SOB will have to compete with nitrifying
bacteria, which also can use oxygen to
oxidise NH4+ (contained in sewage effluent)

The BTF was stopped when pressure drop

values reached 20 25 mbar. This limitation
was because inlet biogas pressure is around
25 28 mbar and the system can not be
operated under negative outlet pressures,
which would be the case at those pressure
drop levels. A 24 48 hours batch NaOH
cleaning was performed in order to reduce
the pressure drop again to acceptable levels
(i.e.: 2 3 mbar). As it is observed in Figure
4, this procedure was performed at least once
per month. All clogging cycles follow the
same profile: constant pressure drop for the
first two/three weeks, while exponentially
increasing at the end of the cycle.

Page 5 of 7

BTF performance is presented in Table 6.

The system showed low availability, 86%,
because of NaOH cleanings. Furthermore,
low removal efficiency was also observed,
80% (10% lower compared to short-term
experiments at the same conditions) because
bacterial activity was drastically influenced
by the number of start/stop. Finally, it must
be noted that H2S outlet concentration was
around 600 ppm, which is too high for most
energy conversion systems.
Period
(month)

H2S in
(ppm)

H2S out
(ppm)

Availability
(%)

RE
(%)

2.900

612

82

76,8

3.181

571

91

80,3

3.752

516

87

84,9

4
3.631
671
84
79,7
Average
3.366
593
86
80,4
Table 6. Long-term performance of the BTF
(average results 4-months)

Discussion and Conclusions

Short-term experiments showed that H2S
removal efficiencies greater than 90% and
outlet concentrations of about 300 ppm can
only be obtained at temperatures of 30C and
retention times of 80 seconds. However, a
lower operating performance was observed
during long-term experimentation at these
conditions as a result of progressive filter
clogging.
According to the high outlet H2S
concentration observed on a 4-month period,
only micro-turbines and internal combustion
engines may be considered as a possible
downstream alternative for BTF. Fuel cells
and gas grid injection are not recommended
(even with a polishing system installed
afterwards) because the reduced availability
of the BTF could not is not compatible with
the limited number of starts and stops of those
systems (Trgisch et al, 2005). Instead,

bioscrubbers, although having a higher

operating cost due to NaOH consumption, can
fully overcome these drawbacks, thus should
be the preferred alternative for these systems.
To conclude, today BTF show unreliable and
not efficient performance for biogas
desulphurisation. If they want to be a future
feasible option to replace conventional
chemical scrubbers or bioscrubbers, their
long-term performance must be significantly
improved.

References
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Acknowledgments
Authors would like to thank LIFE+
programme for the financial support to carry
out this study (BIOCELL project LIFE07
ENV / E / 000847, www.life-biocell.eu) and
the project stakeholders (Agncia Catalana
de lAigua, Entitat Metropiltana de
Mediambient, Consell Comarcal del
Maresme, Entidad de Saneamiento de la
regin
de
Murcia
and
Aquagest
Medioambiente). Special thanks are given to
Eva Torrecillas, WWTP operator at Matar
(Agbar).
Disclosures
Authors have nothing to disclose.

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