Global NEST Journal, Vol 23, No 4, pp 491-496

Copyright© 2021 Global NEST

Printed in Greece. All rights reserved

Purification of biogas from tofu waste using zeolite and activated

carbon (AC) as adsorbent
Budihardjo M.A.1*, Syafrudin1, Samadikun B.P.1, Wardhana I.W.1, Ramadan B.S.2 and Humaira N.G.2
1Department of Environmental Engineering, Faculty of Engineering, Universitas Diponegoro, Semarang-50275, Indonesia

2Environmental Sustainability Research Group, Department of Environmental Engineering, Faculty of Engineering, Universitas

Diponegoro, Semarang-50275, Indonesia

Received: 12/08/2021, Accepted: 05/11/2021, Available online: 22/11/2021
*to whom all correspondence should be addressed: e-mail: m.budihardjo@ft.undip.ac.id
https://doi.org/10.30955/gnj.003906
Stern and Stern, 2007). The steps to reduce CO2 emissions
Graphical abstract
are very important to reduce the risk of global warming.
Governments from various countries have taken concrete
steps to achieve these goals, including the creation of the
Kyoto Protocol at the 2012 and 2015 COP 21 Conference
in Paris (Ferella et al., 2017; Townsend, 2013). On the
other hand, a lot of research has been done as an effort to
mitigate global warming and safeguard the availability of
fossil fuels, one of which is the use of biogas as an
alternative to fossil fuels (Meyer-Aurich et al., 2012; Shen
et al., 2018; Yousef et al., 2018).
Biogas is a product generated by anaerobic digestion from
a variety of biodegradable materials, such as agricultural
Abstract waste, animal waste, waste in human activities, and
Substitution of fossil fuel into alternative energy sources, industrial waste (Aghbashlo et al., 2019; Zain et al., 2018).
such as biogas, needs to be applied to prevent various One of the industrial wastes that have the potential to
problems in the environment. Biogas purification can be produce biogas is the waste from the tofu industry. The
an alternative technology to improve the quality of tofu industry in Indonesia produces waste in the form of
biogas, which increases the heat value by reducing CO2. solid and liquid waste, which is 1.024 million m3 per year
Purification can be carried out by the adsorption method (solid waste) and 20 million m3 per year (liquid waste)
using solid adsorbents, for example natural zeolite and (Faisal et al., 2016). The number of organic compounds
activated carbon. This study used 12 reactors from PVC, contained in it can produce biogas which can be
with 2 different diameters, 3 different mesh size recovered due to its anaerobic treatment. Biogas that is
(20,50,80) and was given both zeolite (A1-A3; B1-B3) and produced by 1 kg of tofu waste contains (Lay et al., 2013).
activated carbon (A4-A6; B4-B6). Biogas purification with Biogas usually has a CH4 content of 55-65%; CO2 of 35-
the addition of zeolite has an optimal compound content 45%; and a small portion of traces consisting of ammonia
in reactor A3 which has an increase in CH4 (63.63%) and (NH3), nitrogen (N2), oxygen (O2), carbon monoxide (CO),
decrease in CO2 composition (25.07%), which is better and hydrogen sulfide (H2S), with concentrations of less
than other reactors. Meanwhile, the results of than 1% (Abdeshahian et al., 2016; Belaissaoui et al.,
measurements of gas content on the addition of activated 2018; Remy et al., 2014). Biogas can be used as fuel for
carbon showed optimal performance in reactor A6, which vehicles and sources to produce heat and electricity, with
was increased to 76.86% for CH4 levels and CO2 levels the advantage of being a versatile, clean, and inexpensive
dropped to 19.79%. fuel (Aghbashlo et al., 2019; Tabatabaei et al., 2019).
However, the CO2 contained in biogas becomes a
Keywords: Adsorption, activated carbon, biogas contaminant that can reduce the value of heat, is
composition, biogas purification, zeolite. corrosive, and damages the pipeline from biogas (Ahmad
1. Introduction et al., 2017; Duran et al., 2018; Jiang et al., 2018a).
Therefore, removal of these contaminants is needed to
The increase in CO2 gas emissions in 1970-2004 was obtain greater methane content in biogas, where the
recorded at 80%, with the amount of CO2 emitted by heating value of biogas with 60% (v/v) methane content
35.65 million metric tons in 2011 (Boden et al., 2015; reaches 5,000-6,000 kcal/N.m3, while higher methane
Budihardjo M.A., Syafrudin, Samadikun B.P., Wardhana I.W., Ramadan B.S. and Humaira N.G. (2021), Purification of biogas from tofu
waste using zeolite and activated carbon (ac) as adsorbent, Global NEST Journal, 23(4), 491-496.
492 BUDIHARDJO et al.

content (96-97%) can increase the heating value up to Zeolites are three-dimensional crystalline aluminum
8,000 kcal/n.m3 (Ryckebosch et al., 2011). silicates, derived from alkali and alkaline earth cations
Various methods of CO2 removal contained in biogas from (Turan and Ergun, 2009). Zeolites widely used as
different activities are available. Adsorption, absorption, adsorbants because of their removal ability for various
membrane separation, and cryogenic distillation are the chemicals, high thermal and chemical stability, and their
most common method (Petersson and WeLLInGer, 2009; uniqueness in carrying out molecular sifting (Ferella et al.,
Rufford et al., 2012; ; Songolzadeh et al., 2014). 2017; Loureiro and Kartel, 2006; Zhou et al., 2017).
Adsorption is a technology that has advantages in Zeolites can increase removal of CO2 because of their
economic aspects, both cost and energy use, but has high higher selectivity than CH4. However, zeolite's affinity for
efficiency (Duran et al., 2018; Zhou et al., 2017). Zeolites, water is very high, where the water contained in biogas
activated carbons, and metal-organic framework (MOF) reaches 6% of its volume (Bacsik et al., 2016; Ferella et al.,
are microporous materials that are often used in the 2017). Therefore, it is recommended to reduce the water
adsorption process because of their ability to remove CO 2 content that will pass through the adsorban to improve
(Hedin et al., 2013; Li et al., 2013; Möller et al., 2017). the CO2 removal performance.
Table 1 Composition of Biogas (%v/v) CH4 and CO2
CH4 (%v/v) CO2 (%v/v)
Reactor
0 min 30 min 60 min 90 min 120 min 0 min 30 min 60 min 90 min 120 min
A0 0 43.90 43.90 43.90 43.90 0 37.30 43.90 43.90 43.90
B0 0 44.60 136,587 142,977 148,720 0 44.60 136,587 142,977 148,720
Table 2 Adsorbents Properties
Adsorbent (mesh)
Reactor Dimension
Zeolite Activated Carbon
A1 20 -
2 inch
A2 50 -
80 cm
A3 80 -
A4 - 20
2 inch
A5 - 50
80 cm
A6 - 80
B1 20 -
4 inch
B2 50 -
40 cm
B3 80 -
B4 - 20
4 inch
B5 - 50
40 cm
B6 - 80

In addition to zeolite, activated carbon is also widely used production, so this study used two-reactor with different
in CO2 removal due to the high adsorption capacity of surface areas to determine the relationship between
ambient air, low regeneration cost, long-term stability, reactor dimensions and biogas purification performance.
and fast kinetic. The material needed to produce activated
carbon has an economical price and is relatively easy to 2. Materials and methods
obtain because it generally comes from the rest of
2.1. Material characteristics
agriculture and forests. This material is usually found in
the form of wood, starch, coconut shells, or empty fruit Biogas generated from waste treatment of tofu industry
bunch (EFB) (Lee et al., 2013; Li et al., 2018; Vilella et al., was used in this study. The biogas was obtained from
2017). Activation of these materials can be done both waste processing of Wismilak Tofu Industry, Mangkang,
physically and chemically. In contrast to zeolites, activated Semarang City. Before the study began, a preliminary test
carbon has a better tolerance to water because it has low of raw biogas generation was conducted using 2 PVC pipe
affinity and it is a hydrophilic material so that it is able to with 2-inch and 4-inch diameter. The test determined the
maintain its adsorption capacity in high humidity initial composition of methane (CH4) and carbon dioxide
(González et al., 2013). However, activated also has a (CO2) from the raw biogas, which are shown in Table 1.
disadvantage because it has a low CO2 selectivity Biogas purification was carried out by the adsorption
compared to CH4 (Bacsik et al., 2016). method using adsorbents (solids), which are natural
zeolite and activated carbon. Purification process of
The main objective of this study is to determine the trend
biogas from tofu waste using both adsorbents then
of using filters with zeolites and activated carbons to
started to investigate the optimum condition that can
purify biogas, eliminate contaminants in the form of CO2,
improve the biogas quality.
and obtain more CH4 content from the tofu waste
treatment. In addition, according to Ogunwande (2017), In this study, natural zeolite is used because in addition to
the reactor surface area is significantly affected by biogas being easily obtained, the market price is quite cheap, and
PURIFICATION OF BIOGAS FROM TOFU WASTE USING ZEOLITE AND ACTIVATED CARBON (AC) AS ADSORBENT 493

natural zeolite is reactive to CO2. Natural zeolite serves to carried out by inserting it into the biogas purification tube
increase CH4 levels and eliminate CO2 levels in the biogas of tofu waste through the reactor insulator for the
purification process (Jiang et al., 2018b). The use of adsorption process to the outlet. The time spent on each
natural zeolite as an adsorbent requires an activation purification variation was 3 hours each. Samples of biogas
process to enhance the special nature of zeolite and from all reactors were collected every 30 minutes using an
remove impurities. Activation of natural zeolite can be injection (syringe) and stored in a vaculab or vacuum tube.
carried out by chemical and physical methods with the The measurement of CH4 and CO2 contents was
aim of cleaning pore surfaces, removing impurities and conducted using Gas Chromatography Shimadzu-14 A (Liu
rearranging the exchanged atoms. Chemical activation is et al., 2015b), which is able to detect gaseous components
carried out through immersion using a NaOH solution with in the form of methane, carbon dioxide and nitrogen
a concentration of 5% for 24 hours, previously it is based on ASTM D1945-14 (International, 2014), at Pati
necessary to wash zeolite using distilled water (Nikolov et and Research Center Laboratory of Pati Regency.
al., 2017). Afterwards, zeolite is washed with distilled
3. Results
water until it is neutral and then dried. After drying,
natural zeolite is physically activated by heating at 250 oC 3.1. CO2 reduction
for 2 hours in a furnace (Wibowo et al., 2017). CO2 content in the biogas decreases until the end of the
In addition to natural zeolite, activated carbon can also be study. Figure 2a showed the reduction of CO2 in reactor A.
used to carry out biogas purification. Activated carbon is a Reactor A1 had the highest CO2 content of 32.00% in the
material with high porosity that has a large adsorption 30th minute, while A3 had the lowest CO2 content of
capacity and is widely used as an adsorbent for 29.90%. Significant reduction occurred in the A3 reactor
purification (Kim and Pui, 2015). Activated carbon can with final content of 25.07% in the 120th minute. This was
adsorb certain gases and chemical compounds where the lower than the other two reactors, A1 and A2, which are
adsorption properties depend on the size or volume of at 27.08% and 26.37% respectively. Meanwhile, in the
pores and surface area (Sethia and Sayari, 2015). The activated carbon reactor (A4), CO2 content decreased
detailed adsorbent properties is shown in Table 2. gradually from 24.37% to 21.61% in the end of the study.
2.2. Biogas purification reactor Reactor A5 experienced a fall until 120th minute, which
decreased from 23.91% to 20,38%. Reactor A6 also
There were 12 reactors that were made from PVC pipes decreased significantly starting from 60 minutes with
with 2 variations in size, which were 2-inch tubes with 80 19.79% in the final composition, which also showed that it
cm height (A1-A6) and 4-inch tubes with 40 cm height (B1- has the lowest CO2 composition in the end of the study.
B6). All of these reactors were planned to have the same
volume with a different diameter that determined from CO2 composition in reactor B (Figure 2b) shows the same
the results of preliminary study. Figure 1 illustrates the pattern with those in reactor A. Reactor B1 had the
series of measurement tools and test positional schemes highest CO2 content of zeolite reactor in the 120th minute
in this study. Both zeolite and activated carbon will be with 29.75% while reactor B3 had the lowest CO2 value of
inserted in the reactor with 3 different mesh (20, 50, and 27.69%. In reactor B4, CO2 was eliminated from 28.96% in
80), with the weight of 300 grams. The mesh size was the first 30 minutes into 24.64% in the final content of
specified to obtain the most suitable dimension of biogas. On the other hand, Reactor B6 showed the most
adsorbent during the biogas purification process. The decrease compared to other activated carbon reactors,
higher the mesh size the smaller the screen opening and which fell from 26.67% to 22.19%. These results showed
the smaller the particle that will pass through. that activated carbon could decrease carbon dioxide
composition of biogas more than zeolite in both reactor A
and B. All of reactors that added with adsorbent had
significant improvement of CO2 composition, which was
reduced until less than 30% v/v.

Figure 1. Scheme of biogas purification.

2.3. Measurement test

Figure 2. (a) Changes of carbon dioxide in reactor a, (b) changes
On biogas purification test, the collected gas flowed from of carbon dioxide in reactor B.
the source into the reactor using a hose and tap with flow
3.2. CH4 generation
meter installed to control the biogas flow rate. The flow
rate was maintained in 10 liter/min, which adjusted from In this biogas purification test, it is known that the
the flow of gas generation at tofu waste treatment. The composition of CH4 gases subsequently increased until it
addition of adsorbent, zeolite and activated carbon, was reached the highest content in the 120th minute. Figure 3a
494 BUDIHARDJO et al.

and 3b shows the level of CH4 in reactor A and B during framework of carbon determine the adsorption of CO 2
the study. The final composition of CH4 in A1 – A3 was takes place, which is between single or multilayer of
ranged between 61% – 64%. The early CH4 value in A1 activated carbon. Moreover, the adsorption of CO2
reactor is the lowest, which was 55.70% in the 30th performed differently based on the level of interaction
minute, while the CH4 content in A3 reactor is the highest between quadrupole of CO2, which is higher than CH4, and
value (58.90%). Reactor A3 produced the highest methane gradient of electric field. This interaction is determined by
after 2 hours generation, which was 63.63% and the the ratio of Si/Al in the adsorbent (Jiang et al., 2018a; Li et
lowest was reactor A1 with CH4 content of 61.30%. al., 2013).
On the other hand, CH4 in reactor A4 – A6 was ranged Fernández (Juárez et al., 2018) has conducted research
from 71% to 77%. Reactor A6 increased significantly about purification of biogas using biomass ash. The
compared to A4 and A5, which reached 76.86% methane purified methane gas increased significantly more than
content in the 120th minutes, which was also higher than crude CH4. It also applied on purified CO 2 and crude CO2.
A3. Meanwhile, A4 had the lowest methane content with The reaction of CO2 occurred rapidly because of high
73.86% methane in the end of the study. alkalinity and the ash humidity. CO2 broke through the
Reactor B3 had the highest CH4 level in the 30th minute of filter in several hours after most of alkaline mineral and
57.61% while the reactor B1 is the lowest with a value of reactive hydroxides were consumed. Durán et al. (Duran
54.51%. The CH4 level in the 120th minute on the reactor et al., 2018), who used activated carbon from pine
B3 became the highest with a value of 61.96% and B1 is sawdust, stated that CH4 broke faster than CO2 but CH4
the lowest with a value of 59.72%. Reactor B using will be replaced later because of roll-up effect. The gas
activated carbon had higher CH4 content compared to mixture affected the adsorptive performance of the
zeolite. Reactor B6 experienced greater increment than activated carbon due to the decrease of partial pressure
the other activated carbon reactor with the final methane when mixing components.
content of 71.27% while B4 had about 5% less methane Besides the type of adsorbent, the mesh size also affects
content, which is the least amount in the other two. the performance of the biogas purification process. It can
be seen that the reactor with the size of 80 mesh has the
lowest CO2 content compared to other mesh sizes. This is
because the smallest adsorbent size is at 80 mesh size,
which causes a larger contact area and increases the
adsorption rate. The finer adsorbent can absorb more CO2
than the coarser one because of the smaller fraction size,
thus increasing the adsorption process. (Jafari et al., 2017;
Mastalerz et al., 2017). Furthermore, gas adsorption
capacity is strongly related to the specific surface area and
Figure 3. (a) Changes of Methane gas in reactor A, (b) changes of micropore volume (Lee and Park, 2011). Usually, gas
methane gas in reactor B. molecules in the gas-solid interaction (adsorption)
potential are driven by strong van der Waals forces. In
4. Discussion particular, the gas adsorption potential is highest in the
Compared to the preliminary study results, both zeolite sub-nanometer pores as they begin to overlap with
and activated carbon reactor had better biogas decreasing pore size, leading to much higher binding
composition. This means the addition of both adsorbents energy come from the creation of deep potential wells
increases CH4 and reduces CO2 content. Although zeolite (Romanos et al., 2011). Therefore, it is crucial to
has higher CO2-CH4 selectivity, activated carbon improved maximizing the number of sub-nanometer pores by
the biogas composition better than zeolite, which was increasing the specific surface area.
shown in higher methane and lower carbon dioxide. In this study, reactors A and B have the same volume but
CH4 is an inert material towards the adsorption on have different results. The composition of biogas in
activated carbon (Liu et al., 2015a). Inactosite methane reactor A showed a better improvement than reactor B.
molecules are completely neutral (neither acidic nor Reactor A produced less CO2 and more CH4 content than
basic). Methane has a regular tetrahedral structure, which reactor B. It happens because the diameter/surface area
favors incompletely non-polar structure. In contrary, CO2 in reactor A is wider than in reactor B. According to
is acidic and polar, which makes chemical reactions in Ogunwande (2017) study, the reactor surface area is
basic interaction with activated carbon. Based on Mamun significantly affected by biogas production. Biogas yield
(Al Mamun et al., 2016), activated carbon, which has high increases when the surface area increases. Furthermore,
porosity, is able to adsorb carbon dioxide and separate it specific surface area, porosity, surface roughness, pore
from a certain gas mixture. The use of activated carbon is size, and orientation of the packing material were found
more beneficial because it can in generation while zeolite to play an important role in anaerobic reactor
does. (Hauchhum and Mahanta, 2014). CO2 can form a performance (Singh and Prerna, 2009).
permanent polarity because there are transformations of
5. Conclusion
CO2 molecules that perform stretching motion of
asymmetric bond at normal pressure and temperature. This study discusses the effect of adding size variations of
The van der Waals force in CO2 molecule and the adsorbents-zeolite and activated carbon-on biogas
PURIFICATION OF BIOGAS FROM TOFU WASTE USING ZEOLITE AND ACTIVATED CARBON (AC) AS ADSORBENT 495

purification. Both of these materials have a variety of González A., Plaza M., Rubiera F. and Pevida C.J.C.e.j. (2013).
advantages, such as high adsorption that can increase CH 4 Sustainable biomass-based carbon adsorbents for post-
levels and eliminate CO2 levels in the biogas purification combustion CO2 capture. 230, 456–465.
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is more appropriate than zeolite. This is due to activated
Adsorbents for the post-combustion capture of CO2 using
carbon could eliminate the most CO2 contaminants and
rapid temperature swing or vacuum swing adsorption. 104,
obtain the most CH4 content. Furthermore, using the
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for Analysis of Natural Gas by Gas Chromatography. ASTM
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mixture of two ingredients can be alternative research in simultaneous removal of dyes: Multivariate optimization.
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Jiang Y., Ling J., Xiao P., He Y., Zhao Q., Chu Z., Liu Y., Li Z. and
Acknowledgment
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This research was funded by Kemenristekdikti through DRPM CO2 capture by vacuum swing adsorption using zeolite
under Grant Number 101-49/UN7.P4.3/PP/2019. NaUSY. Chemical Engineering Journal, 334, 2593–2602.
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