International Journal of Greenhouse Gas Control 4 (2010) 638–646

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International Journal of Greenhouse Gas Control

journal homepage: www.elsevier.com/locate/ijggc

Techno-economic evaluation of biogas upgrading process using CO2 facilitated

transport membrane
Liyuan Deng, May-Britt Hägg *
Department of Chemical Engineering, Faculty of Natural Sciences and Technology, Norwegian University of Science and Technology (NTNU), Sem Saelandsvei 4, NO-7491 Trondheim,
Norway

A R T I C L E I N F O A B S T R A C T

Article history: The biogas upgrading by membrane separation process using a highly efficient CO2-selective
Received 30 July 2009 polyvinylamine/polyvinylalcohol (PVAm/PVA) blend membrane was investigated by experimental
Received in revised form 29 November 2009 study and simulation with respect to process design, operation optimization and economic evaluation.
Accepted 29 December 2009
This blend membrane takes advantages of the unique CO2 facilitated transport from PVAm and the
Available online 25 January 2010
robust mechanical properties from PVA, exhibits both high CO2/CH4 separation efficiency and very good
stability. CO2 transports through the water swollen membrane matrix in the form of bicarbonate. CO2/
Keywords:
CH4 selectivity up to 40 and CO2 permeance up to 0.55 m3(STP)/m2 h bar at 2 bar were documented in
Biogas upgrading
lab with synthesized biogas (35% CO2 and 65% CH4). Membrane performances at varying feed pressures
CO2 separation
Membrane process were recorded and used as the simulation basis in this work. The process simulation of an on-farm scale
Process optimization biogas upgrading plant (1000 Nm3/h) was conducted. Processes with four different membrane module
Biomethane configurations with or without recycle were evaluated technically and economically, and the 2-stage in
cascade with recycle configuration was proven optimal among the four processes. The sensitivity of the
process to various operation parameters was analyzed and the operation conditions were optimized.
ß 2010 Elsevier Ltd. All rights reserved.

1. Introduction lowest, 47%, in the landfill gas, while biogas from a typical farm
biogas plant contains 55–58% methane and 37–38% CO2. The
To secure a sustainable long-term energy supply, our exploita- amount of hydrogen sulfide in the farm biogas varied from 32 to
tion of the earth’s finite resource such as fossil fuel, must be 169 ppm (Rasi et al., 2007; Maltesson, 1997).
reduced, while renewable energy must be developed as alter- Raw biogas of above-listed composition exhibits a significantly
natives. The proportion of energy generated from renewable lower Wobbe index (heating value) compared to natural gas. The
resources is expected to increase to >20% by 2020. During the conventional way to directly burn biogas for heating is apparently
same period, the greenhouse gas should decrease by 14% in 2020 low energy efficient. The removal of carbon dioxide (CO2) from
compared with 2005 (Anon, 2008). The use of upgraded biogas is biogas to a level of methane (CH4) >90%, termed ‘‘upgrading’’, can
considered as one of the most efficient means of utilizing the not only effectively increase the Wobbe index, but also reduce
renewable energy and reducing greenhouse gas emission. corrosion caused by acid gas and therefore extend the biogas
Biogas is a mixture of gases generated from anaerobic microbial utilization as a renewable energy resource. Upgraded biogas
digestion from organic wastes such as manure, landfill or sewage. containing 98% of CH4 may be compressed and liquefied for vehicle
The composition of biogas varies depending on the source. fuel or injected into a public natural gas grid. In addition, by
Typically biogas contains 60–65% CH4, 35–40% CO2, small amounts preventing the unnecessary emissions of carbon dioxide and
of hydrogen sulfide (H2S), water vapour and traces of other gases. methane gas, upgrading of biogas also helps towards both Kyoto
Depending on the source, nitrogen (N2) may be present in a larger and EU greenhouse gas abatement commitments: CO2 is well
amount. The content of methane, carbon dioxide, oxygen, nitrogen known as greenhouse gas, while CH4 is approximately 21 times
and hydrogen sulfide in three biogas sources and the variation more harmful as a greenhouse gas than CO2 (NESDIS, 2009). Today
within them are listed in Table 1. The highest methane content, more and more attentions were paid on the exploitation and
65%, was detected in the gas from the sewage digester and the upgrading of biogas.
Water washing, membrane separation, chemical absorption
and pressure swing adsorption (PSA) are the four techniques which
* Corresponding author. Tel.: +47 73594033; fax: +47 73594080.
may be used for biogas upgrading. Membrane separation method
E-mail addresses: [email protected], [email protected] exhibits many advantages, including low operation cost, easy to
(M.-B. Hägg). maintain with high process flexibility and no pollution. According

1750-5836/$ – see front matter ß 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijggc.2009.12.013
 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646 639

Table 1
Composition of biogas from different sources (Rasi et al., 2007; Maltesson, 1997).

Component Farm biogas plant Sewage digester Landfill

CH4 55–58 61–65 47–57

CO2 37–38 34–38 37–41
N2 Trace Trace 1–17
O2 Trace Trace 0-2
H2S <1 <1 <1
H2O 4–7 4–7 4–7
Aromatic hydrocarbon Trace Trace Trace

to the ‘Biogas from manure and waste products - Swedish case

studies’ published by the Swedish Gas Association in May 2008
(Anon, 2008), however, 25 out of 34 biogas upgrading plants in
Fig. 2. Schematic illustration of the PVAm/PVA blend network (Deng et al., 2009).
Sweden were using the water washing process based on physical
absorption, which produced a big amount of waste water, required
high capital investment and energy consumption while showed if product purity requirements are not extremely stringent. An on-
very low CO2 capture efficient—it was difficult to reach the farm biogas upgrading is usually a small-scale process according to
methane concentration for the direct usage of biogas as a natural this definition and therefore is technically preferable to use
gas substitute. Other plants were using chemical absorption or PSA membrane separation. Membranes with both high selectivity and
in order to increase CO2 capture efficiency although they obviously CO2 permeance are desired for this process to minimize the CH4
brought in more pollution problems and consumed more energy— loss and achieve high CH4 purity. The membranes are also required
none upgrading plant employed membrane technology as yet to operate at high pressure with the presence of water vapour.
might be due to the low separation efficiency of the currently The aim of this work has been to design and optimize a highly
commercially available membranes: the CH4 recovery of the efficient biogas upgrading membrane process by using a CO2
membrane separation units was the lowest among the listed four facilitated transport PVAm/PVA blend membrane with both high
techniques. Moreover, the pre-treatment is normally required for a CO2 permeance and selectivity. The schematic illustration of the
membrane process to remove the water vapour and hydrogen PVAm/PVA blend polymer matrix is given in Fig. 2. Benefited from
sulfide, which considerably increases the process cost. the reversible reaction between CO2 and the amino groups
Today commercial membranes for CO2/CH4 separation are in (carriers) fixed in the membrane polymer matrix, CO2 could
general conventional polymeric dense membranes based on the transport through this membrane by carrier-mediated diffusion
solution-diffusion mechanism, which are subject to a trade-off (facilitated transport) and in the form of HCO3, hence water
between the CO2 separation selectivity and the flux, as illustrated vapour in raw biogas favours the CO2 separation. The PVAm/PVA
in Robeson plot in Fig. 1 (Robeson, 1991, 2008). A membrane with blend membrane exhibited excellent intrinsic CO2/CH4 separation
high CO2 selectivity is inevitably suffering a poor permeance of CO2 properties that could overcome the Robeson upper bound. In
and vice versa. For example, limited by the solution-diffusion addition, robust mechanical properties of the blended hydrogel
mechanism, the cellulose acetate (CA) membrane, the most polymers make it capable of withstanding relatively high-pressure
commonly used commercial CO2 separation membrane, exhibits biogas feed as well as being tolerant to water vapour. The
a CO2/CH4 selectivity of only about 12–15 under operating membrane works in water swollen condition, and hence no pre-
conditions, which is too low to compete with the amine absorption treatment is required to remove water vapour, which simplified
process according to simulations by Baker (2002). Baker also stated the process. The transport mechanism of the PVAm/PVA blend
that membrane technology is advantageous in small (less than membrane is illustrated in Fig. 3 (Deng et al., 2009). More
6000 Nm3/h) and medium scale (6000–50,000 Nm3/h) separations discussion about the facilitated transport mechanism and effects of
operating conditions can be found in (Deng et al., 2009; Hägg and
Quinn, 2006; Kim et al., 2004).
In the current study, CO2/CH4 selectivity up to 40 and CO2
permeance of 0.55 m3(STP)/(m2 h bar) at 2 bar, and selectivity up
to 32 and CO2 permeance of 0.18 m3(STP)/(m2 h bar) at 20 bar
were obtained in simulated separation conditions with water
saturated biogas (35% CO2 and 65% CH4). Experiments showed that
the relative humidity and feed pressure strongly affected the
separation performances, and operation with or without sweep gas

Fig. 1. Robeson upper bounds for the CO2/CH4 membrane separation (Robeson,
1991, 2008). Fig. 3. Gas transport through PVAm/PVA blend FSC membrane.
640 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646

at permeate side did not exhibit significant difference on the CO2 could be reached at the given pressure. The CO2 purity in the
separation performance at high pressures (>10 bar). The CO2 permeate was measured directly by GC except for experiments at
separation using this membrane was therefore possible to operate 2 bar and 3 bar, which were carried out with sweep gas on the
with no sweep gas flow, which may significantly simplify the permeate side, hence CO2 in permeate gas was diluted. However,
process. The simulation of an on-farm scale biogas upgrading plant since biogas is carbon neutral (i.e. part of the natural carbon cycle)
(1000 Nm3/h) was conducted. Processes with four different and therefore the purity of CO2 may be of less concern; it will most
membrane configurations with or without recycle were evaluated. likely not be sequestrated. Sweep gas on the membrane permeate
The sensitivity of the optimal process using 2-stage cascade side may thus be used in biogas upgrading process.
configuration with recycle was analyzed and the operating
conditions were optimized technically and economically. The 3. Simulation basis
simulation result with CH4 recovery of 99% at a low cost of 0.17 $/
Nm3 was achieved by using the FSC membrane and the 2-stage ChemBrane was employed for the simulations of this biogas
recycled process. upgrading process. This is an in-house simulation membrane
module (Grainger, 2007; Grainger and Hagg, 2008) interfaced to
2. Experimental results Aspen HYSYS1 and hence has the strong capacity of HYSYS. The
Peng–Robinson property package in ChemBrane was used. Cross-
The defect-free homogenous PVAm/PVA blend membrane with flow, co-current and counter-current flow with or without sweep
a thin selective layer (0.3–2.5 mm) on a polysulfone (PSf) gas on the permeate side are considered in this program. Users can
ultrafiltration membrane was developed and tested with synthetic choose a spiral-wound module or hollow fiber module with or
biogas (35 vol.% CO2 in CO2/CH4 gas mixture, AGA AS). Most without a sweep gas. Cross-flow is typical for a spiral-wound
experiments were carried out without supplying sweep gas on module, while counter current is typically used for hollow fibers.
permeate side. The permeate gas composition were analyzed on Here the membrane module was assumed as hollow fiber module
line with a micro-GC equipped with auto-sampling. Details of the with the counter-current flow. Hollow fiber membrane module is
preparation and characterization techniques of this membrane had well known to be the most efficient and practical membrane
been reported elsewhere (Deng et al., 2009). CO2 permeance ðP CO2 Þ module design with the highest packing density (up to 30,000 m2/
in the unit of m3(STP)/(m2 h bar) and CO2/CH4 selectivity (a) are m3) while countercurrent flow exhibits the best separation and
the two key indices for the evaluation of membrane separation requires the lowest membrane area in hollow fiber modules
performance and can be calculated by Eqs. (1) and (2). (Grainger and Hagg, 2008; Lie et al., 2007; Hägg and Lindbrathen,
2005). A hollow fiber membrane module is illustrated in Fig. 4. The
Ji qi separation performance of the hollow fiber membrane module
Pi ¼ ¼ (1)
D pi A  D pi was simulated based on the data obtained from flat sheet
membrane experiments.
P CO2
a¼ (2) 3.1. Process description
PCH4

where Ji is the flux of component i (m3(STP)/m2 h) and qi is its The schematic diagram in Fig. 5 gives a concept of an on-farm
standard volume flow rate (m3(STP)/h). biogas generating system integrated with membrane separation
Effects of operation parameters were investigated in a lab scale unit for biogas upgrading. Raw biogas from the bioreactor
membrane unit with the synthetic biogas. Due to the unique containing CH4 and CO2 was saturated with water vapour. As
hydrogel feature and CO2 facilitated transport mechanism in the indicated with the desulfurization agent FeCl2 in Fig. 5, the
PVAm/PVA blend membrane, CO2 separation performance of this desulfurization process was integrated within the bioreactor, and
membrane is strongly dependent on the relative humidity of the most part of hydrogen sulfide could be removed as precipitates.
separation environment. Feed pressure also significantly influ- According to the durability test on the PVAm/PVA blend membrane
enced the CO2 transport and consequently the separation already performed in-house, H2S did not seem to affect the
performance of the membrane. Room temperature was found membrane performance, hence the effect of H2S was not
the optimal temperature for CO2-selective separation of this considered in this study. In this process, raw biogas was firstly
membrane, so all experimental results for this study were taken at compressed to 20 bar and then filtered at room temperature to
room temperature. Details about the effects of operating condi- capture liquid impurities before biogas was feed into the
tions on separation performance of the PVAm/PVA membrane can membrane separation unit. The upgraded biogas – the retentate
be found in (Deng et al., 2009). A selectivity of CO2/CH4 up to 40 and gas from the membrane unit – was delivered into a natural gas
CO2 permeance up to 0.55 m3(STP)/(m2 h bar) have been docu- network after being compressed to 40 bar. The CO2 enriched
mented at 2 bar and 25 8C with a relative humidity of 92%. Table 2 permeate gas (CO2 >80%) was recompressed to 10 bar from
lists the separation performance of the PVAm/PVA membrane at atmospheric pressure and then sent to a 2nd stage membrane
different feed pressures with maximum relative humidity that module to recover CH4. The operating pressures at the 1st and 2nd

Table 2
Experimental results at various operation conditions*.

Pressure (bar) CO2 permeance CO2/CH4 selectivity

(m3(STP)/m2 h bar)

2 0.55 40
3 0.48 38
5 0.3 35
10 0.2 30
15 0.18 31
20 0.18 32
*
Feed gas: CO2 35%, CH4 65% and saturated with water vapour. Fig. 4. Schematic drawing of a hollow fiber membrane module.
 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646 641

Fig. 5. Conceptual schematic diagram of an on-farm biogas upgrading system providing fuel gas to natural gas network. 1: Bioreactor; 2: thickener; 3: filter; 4: 1st stage
membrane module; 5: 2nd stage membrane module.

Fig. 6. Proposed membrane module configurations for biogas upgrading process.

stages were chosen based on the process optimization by Hao et al., 2008, 2002; Rautenbach and Dahm, 1987). In all four
simulation results. cases, the retentate stream will be the upgraded biogas (CH4)
The simulation of an on-farm scale biogas upgrading plant and the permeate will be the CO2-rich stream.
using PVAm/PVA blend membrane was performed with respect to
required membrane area, capital and operation cost, energy 3.3. Base-case conditions and general assumptions
demands for compression and the purity and recovery of CH4.
The base-case conditions for the four biogas upgrading
3.2. Process configurations processes are summarized in Table 3. The input membrane gas
permeation data were based on the experimental results listed
Processes with 2-stage configurations are the most commonly in Table 2, obtained at 25 8C and pressures in a 2–20 bar range.
used multi-stage processes; 3-stage configurations may result in The capacity of the simulated plant was approximately
better separation (Kaldis et al., 2004), but the complexity of the 1000 Nm3/h raw biogas containing 35 vol.% CO2 and 65 vol.%
process variable control and the extra costs limited its applications, CH4-impurities and minor components present were neglected
thus it will not be discussed in this study. in the simulations. The raw biogas pressure from bioreactor was
Fig. 6 illustrates the flow sheets of four simulated module set as 1.2 bar.
arrangements using the PVAm/PVA blend membrane for biogas
upgrading, including a single stage configuration (a) and a 2- Table 3
stage configuration (b) without recycle as well as two 2-stage Base-case conditions for the biogas upgrading process.
configurations with recycle: symmetric cascade (c) and asym- Parameters Case
metric cascade (d). In configuration (b), the CO2 concentration in
a b c d
the retentate streams from the 1st and 2nd stages was fixed at
3
the same value, and the required membrane area for each stage Feed raw biogas (Nm /h) 1000 1000 1000 1000
Feed pressure (bar) 1.2 1.2 1.2 1.2
thus found by simulation. In the symmetric 2-stage cascade
Feed CO2 concentration (vol.%) 35 35 35 35
configuration (c), the permeate stream of the 1st stage is the Permeate T and P at 1st stage (8C, bar) 25, 1 25, 1 25, 1 25, 1
feed of the 2nd stage, and the retentate of the 2nd stage is Permeate T and P at 2nd stage (8C, bar) – 25, 1 25, 1 25, 1
recycled. While in case (d) the feed of the 2nd stage is the CH4 purity (%) 98 98 98 98
CH4 recovery (%) – 98 98 –
retentate of the 1st stage, and the permeate flow of the 2nd
Upgraded biogas delivery pressure (bar) 40 40 40 40
stage is recycled (Stern et al., 1998; Bhide and Stern, 1993a,b;
642 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646

Fig. 7. Flow sheet of the simulated process of case (c) in Aspen HYSYS1.

Following assumptions were made to simplify the simulation: and Baker (2002), was used to estimate the total capital cost of the
plant. The capital cost calculated with CAPCOST includes the direct
- Outlet temperature in the compressors was maximum 150 8C. and indirect project expenses by multiplying a bare module factor
Accordingly, the compression ratio over each compressor stage is with the equipment cost. The bare module factor associated with
limited to 3.5. the installation of equipment includes the material and labor for
- Compressors were assigned an adiabatic efficiency of 75%. installation, the freight, insurance and taxes, construction over-
- The pressure drop through exchangers and membrane feed to head, contractor engineering expenses. The contingency and fee
retentate were assumed to be 0.5 bar. are included in calculating the total module cost, and the auxiliary
- The compression duty includes the compression to 40 bar. facilities are included in the total grass roots cost of plant. The
scaling-up factor has been taken into account by CAPCOST with a
As an example of the simulation using Aspen HYSYS1 with six-tenth rule in calculating equipment cost. In this case, the major
ChemBrane interfaced, a flow sheet is shown in Fig. 7 for process equipment items were the membrane modules and the compres-
configuration (c). sors. The compressors were assumed to be constructed mainly
from carbon steel. The bare module factor was 3.5 for the
3.4. Economic evaluation compressors and 3 for the membrane modules in calculating
equipment costs. Since the membrane life is set as 5 years, the total
In principle, the optimization of a process is based on the membrane area is hence four times of the process required
economic considerations, including reducing the capital cost and membrane area for a project designed as 20-year lifetime.
operating cost of the process. A rough economic evaluation was Since the CAPCOST results are given in 1996 US$, the inflation
performed to find the best membrane configuration based on the factor is considered using the Chemical Engineering Plant Cost
operating cost and the capital cost of the main equipments, e.g. Index (CEPCI). The total capital cost including inflation can be
membrane modules and compressors in this process. The mem- calculated from Eq. (3).
brane was not a standard equipment item (Turton et al., 2003), thus
 
an assumption was made to be 20 $/m2 for the cost of the I2
C2 ¼ C1 (3)
membranes module fabrication according to an estimation given by I1
Lie et al. (2007) and Koros (2003). Some other assumptions were
made to simplify the evaluation, including the life time of the where C2 is the current total capital cost including the inflation
membrane as 5 years, the compressors material as stainless steel, factor, C1 is the total cost calculated by CAPCOST software, I2 is the
the interest rate of 6%, the operating cost as 1.1% of capital latest CEPCI value (575.4 for 2008 in this case) (Chemical
investment, maintenance as 2.3% of capital investment, insurance of Engineering, 2009) and I1 for 1996 (382 in the software). A sample
2% capital investment and 5% discount rate of the capital for the calculation is given in Table 4.
investment. The total cost per tonne of upgraded biogas could be
calculated from the annualized yearly capital cost, the yearly 4. Simulation results and discussion
operating costs and the number of tonnes of upgraded biogas
produced. Since biogas from farms is usually used locally for heat 4.1. Optimization of membrane process configurations
and power production, the cost of the raw biogas was estimated as
0.087 $/Nm3, calculated from the low heat value (LHV) of 65% CH4 4.1.1. Parameter study in a basic membrane process
(36 MJ/Nm3 CH4) with fuel cost as 2.4 $/GJLHV. The electricity price In a biogas upgrading process, CH4 purity and recovery are the
is set as the average of 0.05 $/kWh (Grainger and Hagg, 2008). most important technical factors in determining an optimal
CAPCOST, a capital cost estimation software based on the module arrangement in order to ensure a low CH4 loss and meet
equipment module approach and developed by Turton et al. (2003) the gas product specifications, while the required membrane area

Table 4
A sample for the capital cost calculation with CAPCOST (CEPCI = 382, CEPCI2008 = 575.4).

Equipment list Amount Key design parameters Bare module factor Equipment cost Bare module cost

Axial compressor 6 200 kw carbon steel 3.5 $288,904 $1,011,164

Membrane module (m2) 1297  4 Hollow fiber 5-year lifetime 3.0 $103,760 $311,280
Total bare module cost $1,322,000
Total module cost $1,560,000
Total grass roots cost of plant (C1) $2,030,000
Total capital cost in 2008 (C2) $3,060,000
 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646 643

Fig. 8. Effect of operating pressure on CH4 recovery and required membrane area in single stage process.

and compression energy are critical economic factors. In this study, in this case must include the compression of the upgraded biogas
the influence of operating pressure was simulated to optimize the to 40 bar (the injection pressure for the natural gas network), the
operating condition with respect to the separation performance membrane separation at higher pressure does not necessarily lead
and economics in a basic single stage membrane process. CH4 to higher energy consumption. The pressure of 20 bar without
purity was set as 98% to meet the product specification, and the gas sweep gas exhibits the best performance and lowest cost, thus has
permeation data at different pressures were input from the been defined as the optimal condition of the membrane process for
experimental data listed in Table 2. The process was simulated in further simulation.
the conditions of with sweep gas and without sweep gas,
respectively. The simulated CH4 recovery and required membrane 4.1.2. Comparison of configurations
are plotted as a function of operating pressure in Fig. 8. In the In principle, any CH4 purity can be achieved for binary mixtures
process without sweep gas, the increase of the operating pressure of CO2 and CH4, but in a single stage membrane process, it has to be
reduces considerably the required membrane area while increases at the expense of the recovery rate, exhibiting a trade-off between
the CH4 recovery. The required membrane area of the operation at CH4 purity and recovery, as can be seen from the trend of plot (a) in
3 bar is >10 times more than that at 20 bar, and the CH4 recovery is Fig. 9. By using the 2nd stage, however, process can achieve both
much lower. The use of sweep gas on the permeate side high CH4 purity and recovery, since the 2nd stage can recover CH4
remarkably improved the separation, especially to the low- from the permeate side of the 1st stage. The separation
pressure operations. However, even though the membrane has a performances of the processes with the four configurations have
higher CO2 permeance at 3 bar (0.48 m3/(m2 h bar)) than 20 bar been simulated and are presented in Fig. 9. The simulations of
(0.18 m3/(m2 h bar)), the simulated CH4 recovers are still higher these processes are at the optimal operating pressures of 20 bar.
and the required membrane area still lower for high-pressure The plots of CH4 recovery as a function of CH4 purity exhibits
operations, in both processes with or without sweep gas. Table 5 apparently different trends for the processes without recycle (a
lists the simulation results of the processes at 3 bar and 20 bar with and b) and with recycle (c and d), while the plot for the single stage
and without sweep gas. The feed raw biogas flow is set as configuration (a) exhibits much lower recovery than a 2-stage
1000 Nm3/h. Since it needs one more compressor stage to operate process (b).
at 5 bar, while process at 2 bar has too low energy efficiency, the Since the capital cost in a membrane separation process is
operating pressure of 3 bar was chosen to represent low-pressure roughly determined by the required membrane area while the
process as a comparison with 20 bar (representing high pressure). operating cost depends to a large extent on the compression
The table shows that the operation at 20 bar without sweep gas has
the lower cost for per cubic meter product, and the process is
simpler and its footprint is smaller than the operation at low
pressure or/and with sweep gas. Since the total compression duty

Table 5
Simulation results of single stage process.

Parameters 3 bar 20 bar

No sweep Sweep No sweep Sweep

Upgraded biogas 378 588 566 593

flow rate (Nm3/h)
CH4 purity (vol.%) 98.0 98.0 98.0 98.0
CO2 purity (vol.%) 55 82 78 83
CH4 recovery (vol.%) 57 88.8 85.5 89.5
Required membrane 12,780 2344 956 685
area (m2)
Compression duty (kw) 99 127 157 158
Capital cost (M$) 8.39 2.78 1.86 1.86
Running cost 0.419 0.089 0.062 0.059
($/Nm3 biogas
Fig. 9. Comparison of the simulated separation performance of the processes with
upgraded)
the four configurations, at 20 bar.
644 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646

Fig. 10. Comparison of required membrane area (a) and compression duty (b) of the processes with the four configurations.

expense, these two factors are crucial to evaluate the process. The 4.2. Sensitivity analysis
extra process cost for the recycle and the 2nd stage is concerned in
the process evaluation for the four configurations. The simulation The operating pressure, the raw biogas feed flow rate (plant
of the required membrane area and compression duty of the four capacity) and composition are the most critical parameters that
configurations is presented in Fig. 10, showing that a larger affect the upgraded biogas quality and CH4 recovery in the biogas
membrane area is required to obtain a higher CH4 purity, and upgrading process. A sensitivity analysis of the variations of these
consequently larger compression due to a higher recycle ratio. parameters was made to evaluate the effects of these factors to
Table 6 summarizes the simulation results of the biogas specify the limits of operation parameters. The variable ranges for
upgrading processes using the four configurations with the CH4 the sensitivity study are given in Table 7.
purity in upgraded biogas set as 98% to meet the product
specifications. The single stage configuration (a) shows the lowest 4.2.1. Effect of the 2nd stage pressure
capital costs, but the CH4 recovery in this process is the lowest. The The simulation of the influence of the 2nd stage pressure was
approx. 15% CH4 lost is the main disadvantage for this process. In made with the 1st stage pressure fixed at 20 bar. The required total
addition, since the upgraded biogas of the single stage process is membrane area and compression duty are plotted as a function of
low due to the low CH4 recovery, the total running cost per unit the 2nd stage pressure in Fig. 11. The plot shows that the higher
product for the single stage process is the highest, especially when operating pressure in the 2nd stage results in a lower required total
considering the raw biogas value. For the three 2-stage processes, membrane area as expected. According to the simulation,
the main criteria to evaluate these processes are the CH4 recovery operation at a pressure less than 10 bar requires a dramatic
and the total running cost per unit product, and the process of the increase in membrane area, and the minimal compression duty
2-stage cascade configuration (c) with recycle shows to be optimal will be at around 10 bar, since a larger recycle flow must be given at
for the biogas upgrading process according to the separation low pressures to ensure a sufficient CH4 recovery, hence the higher
performance and the cost of the four processes listed. compression energy consumption is required. The increasing of the
2nd stage pressure to more than 10 bar might also result in extra
Table 6 energy consumption and must have one more compressor stage,
Simulation results of the four cases presented in Fig. 6. which would largely increase the capital costs. The optimal 2nd
Parameters Case
stage pressure was therefore chosen as 10 bar in this study.

a b c d
4.2.2. Effect of feed flow rate
Feed raw biogas flow rate (Nm3/h) 1000 1000 1000 1000 Effect of feed flow rate on separation performance was
Feed pressure at 1st and 2nd stages (bar) 20, – 20, 20 20, 20 20, 19.5 simulated with the optimal membrane area fixed as 1080 m2 in
Upgraded biogas flow rate (Nm3/h) 566 745 769 638
CH4 purity (vol.%) 98.0 98.0 98.0 98.0
CO2 purity (vol.%) 78.0 92.2 98.1 92.5
CH4 recovery (vol.%) 85.5 97.3 99.7 95.7
Recycle ratio – – 0.24 0.26
Total membrane area (m2) 956 1167 1297 1226
Compression duty (kw) 157 220 220 203
Capital cost (M$) 1.86 2.99 3.06 2.34
Energy cost ($/Nm3 biogas upgraded) 0.013 0.013 0.013 0.012
Running cost ($/Nm3 biogas upgraded) 0.062 0.089 0.088 0.084
Total cost including raw 0.228 0.206 0.201 0.220
biogas value ($/Nm3 biogas upgraded)

Table 7
Variable ranges for the sensitivity study.

Parameters Range

2nd stage pressure (bar) 5–20

Feed flow rate (Nm3/h) 250–1500
Fig. 11. Influence of 2nd stage pressure on required membrane area and
CO2 concentration in feed (vol.%) 25–50
compression duty, CH4 and CO2 purity 98%, 1st stage at 20 bar, in configuration (c).
 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646 645

Fig. 12. Influence of feed flow rate on separation performance and total membrane
area 1440 m2.

Fig. 13. Effect of plant capacity on economics factors.

the 1st stage and 360 m2 in the 2nd stage. As shown in Fig. 12,
when the feed flow rate decreases under the design capacity of
1000 Nm3/h, CH4 purity would increase, so the upgraded biogas Fig. 14(a), CH4 purity monotonously decreases with the increasing
quality could still meet the product specifications. However, CH4 CO2 concentration in feed while CH4 recovery slightly increases,
recovery would decease due to the loss of CH4 through the extra since the CH4 recovery is mainly determined by the loss of CH4 in
membrane area. When the feed flow increases over the design the 2nd stage, which increases with the increasing of the CO2
capacity, the membrane area is no longer sufficient for the purity. It suggests that if the CO2 concentration in the feed were
separation. As a consequence, the increase of the feed flow rate higher than designed (>35%), it would result in a lower CH4 purity
would result in the decrease of the CH4 purity and hence the than the product specification (<98%), and should be avoided.
product quality could not meet the specifications. An increase of When CO2 concentration decreases to be lower than the design
the 1st stage feed pressure could partly solve the problem in this value, the CH4 purity would be higher than the product
situation, but the new operation parameters must be given specification, but CO2 purity would decrease and hence the CH4
accordingly to meet the capacity change. recovery decreases. Fig. 14(b) shows the simulation on the
The capital cost and the total running cost per normal cubic compression duty and recycle flow with respect to the influence
meter upgraded biogas are plotted in Fig. 13 as the function of the of the feed CO2 concentration. The recycle flow increases with the
plant capacity in a practical range from 200 Nm3/h to 1500 Nm3/h increasing CO2 concentration in feed. When CO2 concentration is
for on-farm biogas plants to investigate the influences of the plant over 40%, the recycle flow dramatically increases, resulted in a
capacity on economic factors. As shown in Fig. 13, the running quick increase of the compression duty. The simulation suggested
costs per normal cubic meter upgraded biogas for the plants over that a variation of CO2 concentration in the range of 30–40% might
500 Nm3/h show a nearly linear decrease with the capacity lose separation efficiency but not cause serious problems. When
increasing. However, the running cost plot for smaller plant the CO2 concentration in feed was out of this range, however, the
(<500 Nm3/h) shows a quick increase with the decrease of the membrane process must be redesigned to ensure a sufficient
plant capacity, which suggests that for smaller plants it will be separation.
more expensive to produce the same quality of upgraded biogas to
the natural gas network. 4.3. Simulation results for optimal process

4.2.3. Effect of CO2 concentration in feed From the comparison of the processes with four configurations
The effect of CO2 concentration in the feed gas varying from 25% and the optimization of the operating pressures, it can be
to 50% was simulated in a designed process with a fixed membrane concluded that the most efficient membrane process for biogas
area of 1440 m2 and 35% CO2 in feed raw biogas. As shown in upgrading using the PVAm/PVA membrane was the process with a

Fig. 14. Influence of feed composition on separation performance (a), the required compression duty and recycle flow rate (b), total membrane area 1440 m2.
646 L. Deng, M.-B. Hägg / International Journal of Greenhouse Gas Control 4 (2010) 638–646

Table 8 of the membrane in a gas stream containing H2S and heavy

Simulation results of the optimal process.
hydrocarbon are ongoing.
Parameters Simulation results

Total membrane area (m ) 2

1440
Acknowledgements
Feed pressure at 1st stage and 2nd stage (bar) 20, 10
Temperature and Pressure at permeate (8C, bar) 25, 1.0 The authors want to thank Arne Lindbråthen and David
Upgraded biogas flow rate (Nm3/h) 761 Grainger for the help with Hysys ChemBrane simulation module
CH4 purity (vol.%) 98.0
and to the Gas Technology Centre NTNU-SINTEF for the financial
CO2 purity (vol.%) 98.0
CH4 recovery (vol.%) 99.0 support for this work.
Compression duty (kw) 234
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