ARTICLE IN PRESS

Energy 32 (2007) 1375–1380

www.elsevier.com/locate/energy

Trace compounds of biogas from different biogas production plants

S. Rasi, A. Veijanen, J. Rintala
Department of Biological and Environmental Science, University of Jyväskylä, P.O. Box 35, FI-40014 Jyväskylä, Finland
Received 24 February 2006

Abstract

Biogas composition and variation in three different biogas production plants were studied to provide information pertaining to its
potential use as biofuel. Methane, carbon dioxide, oxygen, nitrogen, volatile organic compounds (VOCs) and sulphur compounds were
measured in samples of biogases from a landfill, sewage treatment plant sludge digester and farm biogas plant. Methane content ranged
from 48% to 65%, carbon dioxide from 36% to 41% and nitrogen from o1% to 17%. Oxygen content in all three gases was o1%. The
highest methane content occurred in the gas from the sewage digester while the lowest methane and highest nitrogen contents were found
in the landfill gas during winter. The amount of total volatile organic compounds (TVOCs) varied from 5 to 268 mg m 3, and was lowest
in the biogas from the farm biogas plant. Hydrogen sulphide and other sulphur compounds occurred in landfill gas and farm biogas and
in smaller amounts in the sewage digester gas. Organic silicon compounds were also found in the landfill and sewage digester gases. To
conclude, the biogases in the different production plants varied, especially in trace compound content. This should be taken into account
when planning uses for biogas.
r 2006 Elsevier Ltd. All rights reserved.

Keywords: Landfill; Sewage treatment plant; Biogas plant; Methane; Volatile organic compounds

1. Introduction o1% nitrogen, biogas from organic waste digesters usually

Biogas is produced in different environments, e.g., in
landfills, sewage sludge and biowaste digesters during
anaerobic degradation of organic material. Methane,
which is the main component of biogas, is a valuable
renewable energy source, but also a harmful greenhouse
gas if emitted into the atmosphere. Methane, upgraded
from biogas, can be used for heat and electricity produc-
tion or as biofuel for vehicles to reduce environmental
emissions and the use of fossil fuels. Biogas is considered a
carbon dioxide-neutral biofuel and if used as vehicle fuel,
emits lower amounts of nitrogen oxide, hydrocarbon and
carbon monoxide emissions than petrol or diesel engines
[1]. Upgrading of biogas for use as vehicle fuel is feasible in
large-scale sewage and biowaste digesters (e.g.) [1], and
pioneering work has recently also been done on farm-scale
biogas concepts in this field [2].
Biogas from sewage digesters usually contains from 55%
to 65% methane, from 35% to 45% carbon dioxide and
Corresponding author. Tel.: +358 14 2602340; fax: +358 14 2602321.
E-mail address: saija.rasi@bytl.jyu.fi (S. Rasi).
contains from 60% to 70% methane, from 30% to 40%
carbon dioxide and o1% nitrogen while in landfills methane
content is usually from 45% to 55%, carbon dioxide from
30% to 40% and nitrogen from 5% to 15% [3]. Typically
biogas also contains hydrogen sulphide and other sulphur
compounds, compounds such as siloxanes and aromatic and
halogenated compounds. Although amounts of trace com-
pounds are low compared to methane, they can have
environmental impacts such as stratospheric ozone depletion,
the greenhouse effect and/or reduce the quality of local air.
Many volatile organic compounds (VOCs) harmful to the
environment or to humans can occur in biogases as they
have high vapour pressure and low solubility. Aromatics,
heterocyclic compounds, ketones, aliphatics, terpenes, alco-
hols and halogenated aliphatics are found, especially in
landfill gas [4–8]. Many toxic VOCs are emitted from or
formed in household waste which includes cleaning com-
pounds, pesticides, pharmaceuticals, plastics, synthetic tex-
tiles and coatings [9]. Aromatic and chlorinated
hydrocarbons are widely used in industry as solvents and
fluorinated hydrocarbons have been used as refrigerating
aggregates, foaming agents, solvents and propellants [10].

0360-5442/$ - see front matter r 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.energy.2006.10.018
 ARTICLE IN PRESS
1376 S. Rasi et al. / Energy 32 (2007) 1375–1380
If biogas is used for energy production, compounds
containing organosulphur or organochloride contribute to
corrosion in vehicle or combustion engines [4]. Biogas
containing organic silicon compounds is harmful to engines
because the silicon compounds are oxidised to silicon
oxides during combustion, causing scuffing to engine parts
[1]. Biogas from sewage treatment and biogas plants is
commonly used for heat and electricity production but also
increasingly for vehicle fuel production. Landfill gas is used
for heat and electricity production in many countries, but
its use for vehicle fuel production is considered in many
cases to be too complicated and thus expensive because it
contains trace compounds, such as sulphur, chloride and
silicon compounds [7].
The objective of the present study was to determine the
major and trace organic compounds in biogas and the
variation in biogas composition in three different types of
biogas producing plants, a municipal landfill, a sewage
treatment plant and a farm biogas plant in order to assess
the need for upgrading the biogas in each case. More
specifically, the aim was to determine methane, carbon
dioxide, oxygen and nitrogen content and to identify VOCs
that have potential corrosive or toxic effects. Biogas
samples from the landfill and sewage digester were taken
at different seasons to determine variations in gas content
under different climatic conditions while biogas samples
from the farm were taken only in summertime, as climate
was not considered a significant factor in farm-scale biogas
production.
2. Materials and methods
2.1. Biogas sources
The biogas samples were taken from a municipal landfill
and a mesophilic municipal sewage treatment plant sludge
digester both in Jyväskylä, Finland and from a farm
mesophilic biogas plant in Laukaa, Finland. In the landfill
studied, gas is collected from a 12-extraction well system
over an area of 16 ha. The extraction well system was built
in 2001 and the gas was flared until December 2003, since
when most of the gas has been used for district heating.
The landfill gas samples were taken from a collector pipe
[11]. The sewage treatment plant treats sewage from
Jyväskylä and three other surrounding towns and indus-
trial wastewater from two factories. Biogas is produced in
two 2750 m3 digester tanks where the primary and
secondary sludge of the plant is stabilised. Most of the
biogas is used to produce heat and mechanical energy for
the plant and rest of the gas is flared [12]. The biogas from
the farm, produced by digesting cow manure and confec-
tionary by-products, is used for combined heat and power
generation and also to produce vehicle fuel. All of the gas
produced is used for energy production. In the year 2003,
1.9 Mm3 of biogas was collected from the landfill, 1.5 Mm3
from the sewage treatment plant and about 0.06 Mm3 from
the farm biogas plant [13].
2.2. Biogas sampling and gas analyses
The gas samples from the landfill and sewage treatment
plant were collected during 2004–2006 and from the farm
in summer 2005. Samples for methane, carbon dioxide,
oxygen, nitrogen and sulphur compound measurements
were collected in TECOBAG (PETP/AL/PE 12/12/75)
aluminium gas bags (volume 10 l).
Samples for VOC measurements were collected in
Nalophan NAr bags. The samples were drawn from the
bags into sampling tubes at a rate of 90 ml/min using a
Gillian Personal Air Sampler (LFS-113DC). The adsorp-
tion material in the sampling tubes was Tenax GR. The
tubes were capped and stored at 18 1C until analysed. The
adsorbed VOC samples were analysed using thermal
desorption gas chromatograph–mass spectrometry (Tek-
mar Purge & Trap Concentrator 3000/Agilent 6890+/5973
N MSD).
Methane, carbon dioxide and oxygen were measured
with an infra-red gas analyser (GA 94) and nitrogen with
Perkin-Elmer Autosystem XL gas chromatograph. Ammo-
nia was analysed using Rae Systems gas detection tubes
(range 1–30 ppm). Methylmercaptan, dimethylsulphide
(DMS) and dimethyldisulphide (DMDS) were measured
with a portable gas chromatograph (Photovac GC/PID).
Hydrogen sulphide was measured with an infra-red gas
analyser (GA 94) equipped with electro-chemical cell,
Dräger and Rae Systems gas detection tubes (range 0.2–6
and 2.5–60 ppm) and portable gas chromatograph (Photo-
vac GC/PID).
3. Results
The content of methane, carbon dioxide, oxygen,
nitrogen and hydrogen sulphide in the three biogases and
the variation within them were determined. The highest
methane content, 65%, was detected in the gas from the
sewage digester and the lowest, 47%, in the landfill gas
(Table 1 and Fig. 1). The methane content of the biogas
from the sewage digester and the farm varied by less than
4% and carbon dioxide, oxygen and nitrogen by less than
2%, while in the landfill gas differences in methane and
nitrogen content were from 10% to 15%. The amount of
hydrogen sulphide in the landfill gas varied from 36 to
115 ppm and in the farm biogas from 32 to 169 ppm, while
hydrogen sulphide was not detected in the gas from the
sewage digester. Other reduced sulphur compounds were
found in all biogas samples (Fig. 3).
The occurrence of VOCs in landfill, sewage digester and
farm biogases was studied. The farm biogas contained lower
amounts of total volatile organic compounds (TVOCs)
(from 5 to 8 mg m 3) than the other gases (Fig. 2) and
variation between samples was small. In the landfill and
sewage digester, the amounts of TVOCs varied from 46 to
173 mg m 3 and from 13 to 268 mg m 3, respectively.
Chromatograms from the different gas samples were
compared and differences in VOC qualities evaluated.
 ARTICLE IN PRESS
S. Rasi et al. / Energy 32 (2007) 1375–1380 1377

Table 1
Methane, carbon dioxide, oxygen, nitrogen, hydrogen sulphide, benzene and toluene contents in biogas from different biogas producing plants

Biogas CH4 (%) CO2 (%) O2 (%) N2 (%) H2S (ppm) Benzene (mg m 3) Toluene (mg m 3) Ref.

Landfill 47–57 37–41 o1 o1–17 36–115 0.6–2.3 1.7–5.1 a

Sewage digester 61–65 36–38 o1 o2 b.d. 0.1–0.3 2.8–11.8 a

Farm biogas plant 55–58 37–38 o1 o1–2 32–169 0.7–1.3 0.2–0.7 a

Landfill 59.4–67.9 29.9–38.6 n.a. n.a. 15.1–427.5 21.7–35.6 83.3–171.6 [7]

Landfill 37–62 24–29 o1 n.a. n.a. o0.1–7 10–287 [4]
Landfill 55.6 37.14 0.99 n.a. n.a. 3.0 55.7 [6]
Landfill 44 40.1 2.6 13.2 250 n.a. 65.9 [8]
Sewage digester 57.8 38.6 0 3.7 62.9 n.a. n.a. [21]
Sewage digester 62.6 37.4 n.a. n.a. n.a. n.a. n.a. [22]
Sewage digester 58 33.9 0 8.1 24.1 n.a. n.a. [23]

b.d.—Below detection limit 0.1 ppm. n.a.—not analysed.

a
This study.

Nitrogen Carbon dioxide Methane Toluene and benzene were detected in all the gas samples
100 % (Table 1) while halogenated compounds were found in the
90 % landfill and sewage digester gases, 0.3–1.3 and
80 %
70 % o0.1 mg m 3, respectively. The landfill gas contained more
60 % benzene than either the sewage digester gas or farm biogas
50 % while toluene content was higher in the sewage digester gas.
40 % Benzene concentration in the farm biogas was higher that
30 %
20 %
in the sewage digester gas. The amounts of organic silicon
10 % compounds found in the landfill gas were from 0.7 to
0% 4 mg m 3, in the sewage digester gas from 1.5 to
10.6 mg m 3 and in the farm biogas less than 0.4 mg m 3.
Ju 4
Ap -04

Ap 4

Ju 04

Ju 04

Ju 4

Au 5

O 5

N 5

D 5

Ja 5
06
-0
-0

-0

-0

0
-0

-0

-0
-

g-

n-
ch

ril

ril

ne

ne

ly

ov

ec
ly

ct
ar
M

Fig. 1. Methane, carbon dioxide and nitrogen contents of landfill gas at
different seasons.
Differences in the amounts and quality of VOCs are given
in Fig. 3, which shows example chromatograms of biogas
samples from the landfill, sewage treatment plant and farm,
with a list of the major trace components. Gas samples
from different plants are on the same scale and thus
comparable with each other. In the landfill gas molecular
weights of most of the compounds varied from 62 to 140 g/
mol and in the sewage digester gas from 92 to 198 g/mol, as
the retention times in the chromatograms show. In farm
biogas, molecular weights of the compounds varied more
widely but concentrations of compounds were lower. Most
of the VOCs, especially in the landfill and sewage digester
gas samples, were aliphatic and aromatic hydrocarbons
although organic silicon, halogenated and reduced sulphur
compounds were also detected. The landfill gas contained
more aromatic and halogenated hydrocarbons than the
biogas from either the sewage digester or farm. Most of the
VOCs from sewage digester were aliphatic but there were
also some aromatic compounds. The biogas from the farm
mostly contained reduced sulphur compounds and only
small amounts of aromatic and aliphatic hydrocarbons.
Benzene, toluene, halogenated and organic silicon
compounds were determined from the VOC samples.
4. Discussion
The present results showed some differences in biogas
contents—both in major components as well as in trace
components—in the studied biogas production plants
producing biogas from different and varying substrates
under different conditions. Differences in biogas composi-
tion should be taken into account when biogas utilisation is
planned because certain compounds, such as VOC and
sulphur compounds also found in all the biogases in the
present study, can cause health problems to humans,
environmental impacts, as emissions, and be harmful to
engines when used as a source of energy [7].
The amount of methane and carbon dioxide in different
biogases in this study were on the same level as found in
previous studies in similar plants (Table 1). The low
variation in methane and carbon dioxide content observed
in the sewage digester and farm biogases in this study
makes the gas utilisation easier and apparently less
expensive. The amount of nitrogen and oxygen in biogases
from sewage digester and farm biogas plant are usually
low, as found also in this study, because the biogas is
produced in sealed tanks, avoiding contact with air. The
presence of nitrogen and oxygen in the landfill gas is due to
air flow in the gas collection pipes. In landfills the
recovered gas flow (and gas composition) is controlled by
the vacuum pressure in the gas collection system. With a
small vacuum, landfill gas flows from landfill body into
 ARTICLE IN PRESS
1378 S. Rasi et al. / Energy 32 (2007) 1375–1380

extracting wells and air flows from surface of the landfill
into collection systems are small, but gas also can pass the
gas recovery system. On the other hand, if air flows into the
collection system because the vacuum is too high, it can
also reduce anaerobic degradation and reduce the energy
value of the landfill gas by increasing nitrogen and oxygen
content [14]. High amounts of air in landfill gas can be
harmful because the higher concentrations of oxygen
increase the risk of explosion, although the levels of
oxygen in the landfill gas studied were less than 1%. In the
present study the observed lower methane and higher
nitrogen content in the landfill gas in the winter was either
due to adjustments in gas recovery system or due to
differences in landfill gas production. In landfills gas
production is dependant, on the degradation status of the
waste material as well as moisture and temperature, all of
which may vary greatly in different parts of the landfill
body.

300
250
mg/m3

200
150
100
50
0
Ap -04

ar 4
Ju -04
Ju -04

Ju -04

Ju -04
Ju -04
Ju -04

Ju -05
Ap -04
Ju l-04

Ju 04
Au 05
O 05

Ju 05
5
5

M -0

-0
-0

-0
-0
-
-
g-

-
ch

ch
ch
ne

ne
ne
ne
ne

ne
ril

ly
ly

ly
ly
ct
ri
ne

Fe
ar

ar

Ju
M

M
Landfill Sewage plant Biogas farm

Fig. 2. TVOC content of landfill gas, sewage digester gas and farm biogas.

13* *
8000000
11* * Landfill gas
7000000 *
6000000
Abundance

3-8 16
5000000 *
4000000
12 * * *
3000000 14
2000000 9 15 ** 17
2 10 * 19 22
1000000 ** 20 23
1 18 * 21 24-26 27
2.00 4.00 6.00 8.00 10.00 12.00 14.00 16.00 18.00 20.00 22.00 24.00 26.00
Time→

Sewage gas
8000000 13*
7000000
6000000
Abundance

5000000 16 20
4000000
3000000 3,4,
11*
2000000 6-9,
28 29
1000000 15
12 30

2.00 4.00 6.00 8.00 10.00 12.00 14.00 16.00 18.00 20.00 22.00 24.00 26.00
Time→

Farm biogas
8000000
7000000
6000000 11*
Abundance

5000000
4000000 3,4,6,
3000000 7,32 13*
2000000 27 24 20,38, *
30 17,18, 16,17, 27, 23, 25,26,
12 39
1000000 15 34,35 21,22 36,37 40,41
33 31 42,43

2.00 4.00 6.00 8.00 10.00 12.00 14.00 16.00 18.00 20.00 22.00 24.00 26.00
Time→
 ARTICLE IN PRESS
S. Rasi et al. / Energy 32 (2007) 1375–1380 1379

The hydrogen sulphide content in the biogas of the
studied sewage digester was lower than in the other
biogases and previously reported digester biogases
(Table 1). In the studied sewage treatment plant, ferro
sulphate (FeSO4) which is used to precipitate phosphorus
from sewage, also precipitates hydrogen sulphide under
anaerobic condition of sludge digestion. In the present
study the biogas from the farm contained greater amounts
of different reduced sulphur compounds than either the
landfill or sewage digester gas (Fig. 3). In biogas hydrogen
sulphide and other sulphide compounds originate in
anaerobic conditions along several different pathways
[15]. For example, methanethiol and DMS are formed
from the degradation of sulphur-containing amino acids
(present e.g. in manure) and from the anaerobic methyla-
tion of sulphide. DMS is reduced to form methane and
methanethiol following to methanogenic conversion.
Methanethiol later forms methane, carbon dioxide and
hydrogen sulphide [16]. In the present farm biogas plant
hydrogen sulphide is upgraded by aeration, so the variation
in hydrogen sulphide content indicates some variation in
aeration.
The fact that TVOC content and variation was lower in
the studied farm biogas than in the landfill and sewage
digester gases was probably due to more homogenous
material (manure and confectionery by-products) in the
farm biogas plant. Although much waste material is
recycled, wastes in landfills still contain wide range of
different kind of materials and probably even some
hazardous waste from time when it was not separately
collected. In the sewage treatment plant biogas production
takes place in a stable environment but the source of the
treated material is both industrial and household. The
presence and variation in biogas VOC contents in landfills
has also been reported by other researchers [4,7].
Although the concentration of TVOCs in this study
varied across the different samples and different biogas
producing plants, the trace components were similar from
sample to sample for a given location. In case of landfill
gases this has also been reported by other researchers [6,7].
The higher amounts of aromatic compounds in landfill
compared to sewage digester or farm biogases (Fig. 3) are
probably associated with older waste [4] even though high
concentrations of aromatic compounds have also been
measured in urban waste disposal bins [17]. Aromatic
compounds are produced during anaerobic process via
breakdown of abundant lignins [15]. Levels of alkanes and
aromatic compounds as well as halogenated and oxyge-
nated compounds are dependant on stage of decomposi-
tion and composition of waste [4]. In the studies on
halocarbons in landfill gases, Allen et al. [4] and Jaffrin et
al. [8], respectively, detected from 118 to 735 and
169 mg m 3 of total chloride and from 63 to 256 and
25.9 mg m 3 of total fluorine. In the present study the total
amount of halogenated compounds was even lower
(0.3–1.3 mg m 3) than either of those alone.
Benzene content in the landfill gas was higher than in the
sewage digester and farm biogas probably for the reason
that benzene is a natural component of crude oil and is
widely used in industry, wastes from which enter the
landfill. The toluene concentrations in this study were also
higher in the landfill and sewage digester gas than farm

Fig. 3. Total ion current chromatograms (TIC) of VOCs from landfill gas (above), sewage digester gas (middle) and farm biogas (below)

1. 1-Chloro-1-fluoroethane (1.71), Ethyl chloride (1.80)

2. Dichlorofluoromethane
3. Methylene chloride
4. Carbon disulphide
5. 1-Chloropropane
6, 8. Thiols
7. Trimethylsilanol
9. 1,2-Dichloroethene
10. 1,1,1-Trichloroethane
11. Benzene
12. Hexamethyldisiloxane
13. Toluene
14. Tetrachloroethylene
15. Hexamethylcyclotrisiloxane
16. Octamethylcyclotetrasiloxane
20. 2,4-bis(trimethylsiloxy) benzaldehyde
26. Decamethyltetrasiloxane
28. 1-Propanethiol
29. Thiophene
30, 31. Methylthiophenes
32. DMS
33. DMDS
34, 35. Ethylthiophenes
17, 18, 19, 21, 22, 24, 27, 36, 37, 38, 39, 40, 41, 42, 43. Alkyl disulphides (C3–C10)
23, 25. Alkyl trisulphides (C6)
*Aromatic hydrocarbons
 ARTICLE IN PRESS
1380 S. Rasi et al. / Energy 32 (2007) 1375–1380
biogas, probably because toluene is compound commonly
used in industry as a solvent, carrier, or thinner in the
paint, rubber, printing, cosmetic, adhesives and resin
industries [18] hence material containing toluene can be
found in landfills and sewage. Organic silicon compounds,
found from landfill and sewage digester biogases, are
widely used, e.g., in shampoos, skin creams, tooth paste
and food production, hence the presence of volatile silicon
compounds in refuse [19]. The farm biogas plant mainly
handles manure and confectionery by-products with the
result that the content of toluene and organic silicon
compounds is lower. The highest variation in toluene
content occurred in the sewage digester gas but TVOC
content also showed wide variation. Benzene and toluene
concentrations in landfill gas found in this study were lower
than in previously reported landfill gases (Table 1)
probably due to differences in sizes and waste fractions
and different climatic conditions in different studies. For
example, the highest benzene concentrations were detected
in the largest waste treatment site in Korea [7] and in the
three landfills in the Midlands, UK [4].
The results of this study indicate that if biogas is to be
considered as a vehicle fuel, it would appear to be simpler
to produce it from manure or sewage sludge as the lower
content of nitrogen and halogenated and silicon com-
pounds make these biogases easier to upgrade. Upgrading
landfill gas may be more demanding because of the
presence of trace compounds and nitrogen. On the other
hand still today on the global level, most landfill gas is not
collected and thus biogas, together with all its compounds,
is being emitted into the atmosphere creating environ-
mental and health issues. Techniques for upgrading biogas
are not new as raw natural gas has been upgraded for years
using the same methods. For example, in North America
the methane content of raw natural gas can vary from 45%
to 97%, carbon dioxide from 0% to 54% and nitrogen
from 0.2% to 21%, depending on the location of the
source. Raw natural gas also contains hydrogen sulphide
and other sulphur compounds, and hydrocarbons like
propane, butane and pentane. Many upgrading technolo-
gies exist especially for the removal of carbon dioxide and
hydrogen sulphide from natural gas, however, knowledge
about upgrading landfill gas remains limited. Also it should
be remembered that gasoline production from crude oil is a
complicated process [20].
Acknowledgments
This work was funded by the Maj and Tor Nessling
Foundation, National Technology Agency of Finland,
Grenovia Ltd. and Tampere Regional Solid Waste Manage-
ment Ltd. Thanks goes to Mustankorkea landfill, Jyväskylä
Waste Water Treatment Plant and Erkki Kalmari for
providing the opportunity to take biogas samples.
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