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Article history: Treatment of food waste by anaerobic digestion can lead to an energy production coupled to a reduction
Received 20 March 2014 of the volume and greenhouse gas emissions from this waste type. According to EU Regulation EC1774/
Received in revised form 2002, food waste should be pasteurized/sterilized before or after anaerobic digestion. With respect to
26 June 2014
this regulation and also considering the slow kinetics of the anaerobic digestion process, thermal and
Accepted 30 July 2014
chemical pretreatments of food waste prior to mesophilic anaerobic digestion were studied. A series of
Available online
batch experiments to determine the biomethane potential of untreated as well as pretreated food waste
was carried out. All tested conditions of both thermal and ozonation pretreatments resulted in an
Keywords:
Anaerobic digestion
enhanced biomethane production. The kinetics of the anaerobic digestion process were, however,
Thermal pretreatment accelerated by thermal pretreatment at lower temperatures (<120 C) only. The best result of
Ozonation pretreatment 647.5 10.6 mlCH4/gVS, which is approximately 52% higher as compared to the specic biomethane
Organic solid waste production of untreated food waste, was obtained with thermal pretreatment at 80 C for 1.5 h. On the
Energy requirement basis of net energy calculations, the enhanced biomethane production could cover the energy require-
ment of the thermal pretreatment. In contrast, the enhanced biomethane production with ozonation
pretreatment is insufcient to supply the required energy for the ozonator.
2014 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jenvman.2014.07.042
0301-4797/ 2014 Elsevier Ltd. All rights reserved.
J. Ariunbaatar et al. / Journal of Environmental Management 146 (2014) 142e149 143
Various mechanical, biological, chemical, thermal pretreatment % Wet weight Average from Distribution of Final concentration
methods or a combination of them can be applied for FW. The ef- fraction literature miscellaneous applied in the BMP
fects of various pretreatment methods are highly different review (%)a fraction over test (%)
the knowna
depending on the characteristics of the substrates and the pre- fraction (%)
treatment type (Ariunbaatar et al., 2014). Although according to EU
Fruits and vegetables 58.4 20.2 78.6e79.0
regulation EC1774/2002, FW is categorized as a catering waste, and
Pasta/rice/our/cereals 3.6 1.3 4.9e5.0
it should be pasteurized or sterilized prior to or after AD (Kirchmayr Bread and bakery 4.7 1.7 6.4e6.0
et al., 2003). Taking this regulation into account, a thermal or a Meat and sh 6.1 2.1 8.2e8.0
chemical pretreatment of FW could be more effective. These pre- Dairy products 1.4 0.5 1.9e2.0
Miscellaneous 25.8 e 0
treatments could cause the degradation of complex molecules as
well as the solubilization of recalcitrant particles, making the
Total 100 25.8 100
substrate more available for the anaerobes.
a
Thermal pretreatment is one of the easiest and most studied MTT Agrifood Research Finland (2010).
Methanomicrobium, Methanobacterium, and Methanosarcina on the outdoor temperature, various scenarios of ambient air
(Daquiado et al., 2014). temperature (10 to 20 C) were considered.
Biomethane was measured once a day by a volumetric method The total energy required for ozonation depends on the ozonation
as described by Esposito et al. (2012c) (Browne and Murphy, 2013). method and the characteristics of the ozonator. Ozone generation
Each BMP test bottle was connected to an inverted 1 L glass bottle from air with the lowest energy efciency of 2e3% requires 40 kWh/
containing an alkaline solution (120 gNaOH/L) to absorb the carbon kgO3 energy, whereas a high-energy efciency of 30% requires
dioxide. The cumulative biomethane production (CBP) was 2.5 kWh/kgO3 energy (Fridman, 2008). The average (21.3 kWh/kgO3)
normalized to standard temperature and pressure (STP). of reported values was used to estimate the required energy for
ozonation pretreatment. The calculation of the net energy produc-
tion could not be compared with any other research, as so far no
2.4. Analytical methods
literature was found specically referring to FW.
Total Solids (TS), Volatile Solids (VS) and Total Kjeldahl Nitrogen
3. Results
(TKN) of both the synthetic FW and the inoculum were analysed
according to the APHA standard methods (APHA). Total proteins
3.1. Characteristics of substrate and inoculum
were calculated based on TKN, using a correction coefcient of 6.25
(Codex Guidelines on Nutrition Labelling CAC/GL 2-1985 (Rev.1 e,
The results of the chemical and physical characterization of both
1993). Total carbohydrates were determined with the phenol-
the synthetic FW and the inoculum are shown in Table 2. The
sulphuric method and measured spectrophotometrically (TUV
synthetic FW contains a high percentage (76.5 0.7% VS) of car-
SR03210002) using glucose as standard solution (Codex Guidelines
bohydrates, making it a suitable substrate for the AD process (Neves
on Nutrition Labelling CAC/GL 2-1985 (Rev.1e, 1993)). Total lipids
et al., 2008). Values shown in Table 2 are the averages of the three
were extracted with a mixture of chloroform and methanol (1:2 by v/
sets of experiments and standard deviations are calculated based
v), dried and weighted (Phillips et al., 1997).
on the values of triplicate experiments of each set. The inoculum
contains a higher amount of protein and lipids than carbohydrates.
2.5. Net energy production This suggests that the TS are mainly contained in the microbial
biomass and very little FW substrate is available in the inoculum.
The net energy production was calculated based on the extra
energy produced (E Produced) and the required energy for operating 3.2. Cumulative biomethane production
the pretreatments. The extra energy from the enhanced bio-
methane production can be calculated as follows (Ma et al., 2011): 3.2.1. Thermal pretreatment: effect of pretreatment temperature
The rst set of experiments was conducted to investigate the
EProduced EBiomethane *VBiomethane *h (1) effect of temperature (70e140 C) to pretreat FW for an hour.
Biomethane production of FW reached its maximum amount after
where:
154 days, though the experiment was kept running for another
EBiomethane energy content of biomethane (6.5 kWh/m3);
2 months to make sure the maximum was attained. The CBP curves
VBiomethane extra biomethane produced due to pretreatment
are shown in Fig. 1A.
(m3);
FW pretreated with the thermal method produced more bio-
h conversion factor (0.85 for thermal energy); methane than the untreated FW (Fig. 1). The CBP of pretreated FW
The total required energy for the thermal pretreatment is the
was enhanced by 22.2 1.3, 18.9 4.1, 9.9 0.6, 7.5 0.9, 3.8 1.2%
sum of the required energy (EThermal) to obtain the desired pre-
at pretreatment temperatures of 80, 100, 70, 120 and 140 C,
treatment temperature and the energy of the pretreatment
respectively.
chamber (EChamber) to maintain the heat (Ma et al., 2011):
The next set of BMP tests was carried out with FW pretreated at
140e150 C for 30 min (Fig. 1B). FW pretreated at higher temper-
EThermal CFW *MFW * DT CWater *MWater *DT (2)
atures produced less methane than the untreated FW during the
where: initial 16e18 days. At the end of the experiment, the CBP of pre-
CFW heat capacity of dry food waste (1.92 kJ kg1 C1); treated substrates were nevertheless increased by 6.9 0.3 and
MFW dry mass of food waste and/or TS (kg/ton FW); 4.5 0.8% at 140 and 150 C, respectively. After the thermal pre-
CWater heat capacity of water (4.18 kJ kg1 C1); treatment at 120, 140 and 150 C for both 1 h and for 30 min at 140
MWater mass of water in FW (kg/ton FW); and 150 C, the substrate turned brown.
DT temperature increase from room temperature to desired The effect of the thermal pretreatment on the AD process is
temperature ( C) particularly clear when comparing the specic biomethane pro-
duction (SBP) of the initial 20 days of biomethanation (Fig. 2). Most of
and EChamber DT*A*k=s*t (3) the organic matter (80e85%) is converted into biomethane in the
initial 20 days. Fig. 2 shows that all the thermally pretreated FW
where: substrates have a higher SBP than the untreated FW
A total surface area of the pretreatment chamber (m2); (426.0 8.5 mlCH4/gVS). The highest SBP of 539.8 8.7 mlCH4/gVS
s thickness of the pretreatment chamber wall (m); k heat was achieved with a pretreatment at 80 C, followed by 516.1 7.1 at
conductivity of material used of pretreatment chamber (W/m, C); 100 C, 492.1 16.3 at 120 C and 479.3 7.9 at 70 C. The energy
t pretreatment time (hours). requirement for a thermal pretreatment higher than 100 C is mostly
The density of FW ranges between 0.3 and 1 ton/m3 depending utilized for evaporating the water, thus high temperatures (>100 C)
on its characteristics and compaction (Tchobanoglous et al., 1993). were not suitable for the pretreatment of FW due to a higher energy
For simplicity, 1 ton/m3 was considered for this research. Hence, a requirement and lower enhancement of the SBP. The BMP tests on
small pretreatment chamber with 1.1 m-height and 0.55 m-radius the effect of treatment time were carried out with temperatures at
width, made of polyurethane (k 0.022 W/m, C) was considered 70 and 80 C. Although for comparison reason, the net energy pro-
for the thermal pretreatment of 1 ton FW. Since EChamber depends duction was estimated for 120 C.
J. Ariunbaatar et al. / Journal of Environmental Management 146 (2014) 142e149 145
Table 2
Characterization of FW and inoculum used in this experiment.
TS (%) VS (%) VS/TS (%) TKN (mg/L) Protein (%VS) Lipid (%VS) Carbohydrates (% VS)
FW 22.2 0.2 21.1 0.2 89.9 1.9 4.7 0.6 14.3 1.8 9.2 1.1 76.5 0.7
Inoculum 2.7 0.2 1.5 0.1 57.0 1.8 0.8 0.1 59.3 5.2 38.7 5.3 2.1 0.1
4. Discussion
The CBP curves (Figs. 1A, 1B, 3A, 3B, 5A) of the untreated FW
Fig. 2. Effect of thermal pretreatment on the specic biomethane production during suggest a typical AD of a substrate rich in carbohydrates (Neves
the initial 20 days of the BMP test. et al., 2008; Appels et al., 2010), which agrees with the chemical
146 J. Ariunbaatar et al. / Journal of Environmental Management 146 (2014) 142e149
Fig. 4. Effect of (A) 70 C; and (B) 80 C thermal treatment time on the biomethane
production during the initial 20 days of the BMP test.
Fig. 3. CBP curves of FW pretreated at (A) 70 C; and (B) 80 C for various treatment research (Mata-Alvarez et al., 2000; Ariunbaatar et al., 2014; Neves
times. et al., 2008; Eskicioglu et al., 2006). These results indicate that the
thermal pretreatment caused a deocculation of macromolecules
analyses of the FW (Table 2). AD of lipids and proteins are relatively (Eskicioglu et al., 2006; Protot et al., 2011), which increases the
slow as compared to carbohydrates (Vavillin et al., 2008), and surface area of the substrates as proposed by previous research.
Breure et al. (1986) suggested that a complete degradation of Esposito et al. (2011b) conrmed that the increased surface area
proteins cannot be achieved in the presence of high carbohydrate results in a better contact between the substrate and the microbial
concentrations (Breure et al., 1986). Hence, the entire potential population, thus more organic matter is converted into biomethane
biomethane source cannot be recovered from a normal unstimu- (Esposito et al., 2011b).
lated biomethanation of complex substrates (such as FW), which In addition to the well-known enhancement of the CBP, this
contains both easily biodegradable (carbohydrates) and recalcitrant study showed the various effects of pretreatment temperature and
organic matter (lipids and proteins). This study, however, showed time that was not very well explained specically for FW by pre-
that pretreatment of FW with thermal and ozonation methods vious research. The effects of temperature and treatment time on
prior to AD can enhance the CBP (Fig. 1A, B, 3A, B, 5 A). The results the CBP and SBP were not linear, but parabolic (Figs. 2 and 4). This
suggest that the recalcitrant organic matter was degraded to less suggests that the thermal pretreatment also caused the degrada-
complex substrates that are easily available for the anaerobic mi- tion of complex substances and/or increased the soluble organic
crobes. In this regard, focussing only on the favourable C/N ratio, matter (Valo et al., 2004), resulting in the Maillard reaction, i.e. a
which is reported to be in the range of 14.7e36.4 (Zhang et al., reaction between amino acids and sugars. The product from the
2007; Esposito et al., 2011a) for the AD of FW is not suitable, as Maillard reaction, melanoidins, is difcult to degrade anaerobically
FW contains considerable amounts of recalcitrant complex sub- (Carrere et al., 2010; Vavillin et al., 2008). Depending on the type of
stances. Moreover, thermal and ozonation pretreatments disinfect carbohydrates and proteins in the substrates, the temperature
the substrates, which contribute to a hospitable environment for range to cause Maillard reaction differs, though the colour devel-
the methanogenic consortia in the anaerobic digesters. Conse- opment is an important indication of the reaction (Ma et al., 2011;
quently, the more specialised microbial community could convert Appels et al., 2010). The FW pretreated at higher (>120 C) tem-
more organic matter to biomethane. Nevertheless, the effects of peratures indeed turned brownish. Liu et al. (2012) obtained a
pretreament methods were different depending on the conditions similar conclusion with a study on the thermal pre-treatment of FW
applied. and fruit and vegetable waste at 175 C, which resulted in a 7.9% and
11.7% decrease of the CBP, respectively, due to the formation of
4.1.1. Effect of thermal pretreatment melanoidins (Liu et al., 2012). Moreover, the FW pretreated at lower
Thermal pretreatment resulted in an enhanced CBP at all the (70 and 80 C) temperatures for longer times (4 and 8 h) turned
tested conditions (Figs. 2, 3 and 5), which agrees with the previous light brownish, suggesting an incomplete or mild Maillard reaction
J. Ariunbaatar et al. / Journal of Environmental Management 146 (2014) 142e149 147
Table 3
Cost benet analysis of ozonation pretreatment.
had occurred. Bougrier et al. (2008) proposed that the thermal 4.1.2. Effect of ozonation pretreatment
pretreatment could also cause a reaction between the soluble car- Ozonation pretreatment yielded 22e46% enhancement of CBP
bohydrates and soluble proteins, forming amadori like compounds (Fig. 5A), which is comparable with the previous results by Cesaro
(Protot et al., 2011). These amadori compounds are the by-products and Belgiorno (2013), who reported a 37% increase of CMP from
of melanoidins (Appels et al., 2010; Vavillin et al., 2008; Breure ozonated source-separated OFMSW. Even though the CBP
et al., 1986; Eskicioglu et al., 2006; Protot et al., 2011); and the enhancement is comparable, the ozone dose for such enhancement
formation of such compounds might have also yielded a lower is much lower (0.068 gO3/gTS as compared to 0.16 gO3/gTS) in this
enhancement of the SBP at these pretreatment conditions. research, and the CBP curves illustrate different trends. Fig. 6 shows
Further to the Maillard reaction, which is a conrmation of that all the ozonated FW produced less biomethane as compared to
increased degradation of proteins and carbohydrates, degradation untreated FW during the initial 18 days.
of lipid compounds was also induced by the thermal pretreatment. Ozone is a strong oxidant, which decomposes itself into radicals
that react with organic substrates in two ways: directly and indi-
rectly (Carballa et al., 2007). The direct reaction based on the rad-
icals of ozone can destroy the easily fermentable sugar, thus
resulting in a loss of biomethane production. This effect is com-
parable with the more extreme thermal pretreatment conditions,
e.g. higher temperatures and longer treatment times (Section 4.1.1).
The indirect reaction of ozone, which depends on the hydroxyl ion,
causes the degradation of complex organic compounds such as
lipids and proteins in FW, thus yielding a sudden increase in the
biomethane production (Fig. 4A). However, a previous study on the
AD of ozonated SS-OFMSW produced a higher biomethane yield
from the beginning of the AD process (Cesaro and Belgiorno, 2013),
probably the SS-OFMSW used for their experiment contained a
higher level of lipids and proteins. Unfortunately, the authors did
not analyse the chemical content of the substrate. Based on the
results obtained in this study (Table 3), ozonation was found to be
an inefcient method to enhance the AD of FW. Even though
ozonation resulted in a higher CBP at all concentrations, consid-
Fig. 6. Effect of ambient air temperature on the net energy production from thermal ering the initial 20 days of the AD process a high ozone dose of
pretreatment at 80 C for 1.5 h. 0.202 gO3/gTS found to be an inhibitory condition. It can be
148 J. Ariunbaatar et al. / Journal of Environmental Management 146 (2014) 142e149
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reach the desired temperature, but also the energy to maintain the energy system for the urban environment. Renew. Energy 41, 200e209.
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matter of waste activated sludge before and after thermal pretreatment. Water
Res. 40, 3725e3736.
This research investigated the thermal and ozonation pretreat- Esposito, G., Frunzo, L., Panico, A., Pirozzi, F., 2011a. Model calibration and validation
ment methods to enhance the biomethanation of a synthetic FW, for OFMSW and sewage sludge co-digestion reactors. Waste Manag. 31,
which was prepared mimicking a typical FW in selected European 2527e2535.
Esposito, G., Frunzo, L., Panico, A., Pirozzi, F., 2011b. Modelling the effect of the OLR
countries. Based on a series of batch experiments, a thermal pre-
and OFMSW particle size on the performances of an anaerobic co-digestion
treatment at 80 C for 1.5 h yielded the highest enhancement (52%), reactor. Process Biochem. 46, 557e565.
amounting to 647.5 10.6 mlCH4/gVS. The enhanced biomethane Esposito, G., Frunzo, L., Panico, A., Pirozzi, F., 2012a. Enhanced bio-methane pro-
duction by co-digestion of different organic wastes. Environ. Technol. 33,
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(0.034e0.202 gO3/gTS) resulted in a loss of fermentable sugars. digestion of complex organic substrates. Open. Environ. Eng. J. 5, 1e8.
Therefore, such aggressive pretreatment methods found out to be FAO, 2011. Swedish Institute for Food and Biotechnology, Global Food Losses and
Food Waste e Study Conducted for the International Congress.
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This research was nancially supported by Erasmus Mundus Landll Gas in Cooperation with Bioexell e Biomethane Center of Excellence.
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authors would like to thank Prof. Andreozzi, Robert and the
Neves, L., Goncalo, E., Oliveira, R., Alves, M.M., 2008. Inuence of composition on
Department of Chemical Engineering, University of Naples, Feder- the biomethanation potential of restaurant waste at mesophilic temperatures.
ico II for their help in conducting the ozonation pretreatment. Waste Manag. 28, 965e972.
Phillips, K.M., Tarrago -Trani, M.T., Grove, T.M., Grn, I., Lugogo, R., Harris, R.F.,
Stewart, K.K., 1997. Simplied gravimetric determination of total fat in food com-
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