Applied Energy 242 (2019) 1064–1073

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Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

An overall perspective for the energetic valorization of household food T

waste using microbial fuel cell technology of its extract, coupled with
anaerobic digestion of the solid residue
⁎
G. Antonopouloua,b, , I. Ntaikoua,b, C. Pastorec, L. di Bitontoc, S. Bebelisd, G. Lyberatosa,b
a
School of Chemical Engineering, National Technical University of Athens, Zografou Campus, GR 15780 Athens, Greece
b
Institute of Chemical Engineering Sciences, Foundation for Research and Technology, GR 26504 Patras, Greece
c
Istituto di Ricerca Sulle Acque, Consiglio Nazionale delle Ricerche, Viale De Blasio 5, 70132 Bari, Italy
d
Department of Chemical Engineering, University of Patras, Caratheodory 1, University Campus, GR 26504 Patras, Greece

H I GH L IG H T S G R A P H I C A L A B S T R A C T

• Production of electricity and methane

from predried and shredded house-
hold food waste (HFW).
• 11.8 3
W/m was obtained at an HRT of
18 h, using glucose.
• kg 3
For dried HFW, 7.7 W/m or 0.31 MJ/
TS was obtained.
• Energy recovery of 12.32 MJ/kg TS
DHFW from both processes.

A R T I C LE I N FO A B S T R A C T

Keywords: The valorization of typical household food waste (HFW) produced at municipality level was studied for the
Microbial fuel cell production of electricity in a microbial fuel cell (MFC) from its extract, and methane, through anaerobic di-
MFC gestion of the solid extraction residue. HFW, after heat drying and shredding, was subjected to extraction using
Household food waste warm water, which resulted in a liquid fraction (extract) and a solid residue. The rich in soluble chemical oxygen
Energetic valorization
demand extract was used for electricity production in a four air– cathodes single chamber MFC, operating under
Anaerobic digestion
different organic loading rates, while the solid residue from the extraction process was used as substrate for
Biochemical methane potential
methane production in biochemical methane potential experiments. On the basis of the energy outputs estimated
for the optimum operational conditions of both aforementioned processes, it can be concluded that the ex-
ploitation of dried HFW is quite appealing as it leads to promising energy recovery.

1. Introduction such a transition would greatly contribute to a boost in the economic

development of the European Union (EU) and improve its competi-
In December 2015 the European Commission proposed a package tiveness and resource efficiency. In this framework, emphasis was given
on circular economy, in which a framework enabling the transition to the minimization of wastes, through a “waste directive proposal” [2]
from a linear to a circular economy was presented [1]. It was noted that which sets clear targets for municipal solid waste (MSW) reduction and

⁎
Corresponding author at: Institute of Chemical Engineering Sciences, Foundation for Research and Technology, GR 26504 Patras, Greece.
E-mail address: geogant@chemeng.upatras.gr (G. Antonopoulou).

https://doi.org/10.1016/j.apenergy.2019.03.082
Received 6 December 2018; Received in revised form 11 February 2019; Accepted 8 March 2019
Available online 22 March 2019
0306-2619/ © 2019 Elsevier Ltd. All rights reserved.
G. Antonopoulou, et al.
management in the EU by 2030.
The generation of MSW varies significantly across the EU Member
States, with an average annual of 482 kg per capita in 2016 [3]. This
amount was slightly lower than that generated in Greece (497 kg per
capita in 2016). Food waste (FW) represents the major fraction of MSW,
with a production of 88 million tons in 2012 [4], 55% of which being
generated in households.
Due to its composition, household food waste (HFW) are susceptible
to fermentation and bacterial attack, becoming a possible source of
infection associated with health and safety issues [5,6]. For countries
like Greece, where landfilling is still the main MSW management
method [7], the exploitation of different approaches either for reducing
FW generation or for identifying ways for its valorization, upon sepa-
rate collection at the source, seems to be the only alternative solution
[8].
Utilization of HFW as a raw material presents a great challenge, due
to its heterogeneity, which depends on the season and place of collec-
tion and also due to the inherent difficulty for its preservation attrib-
uted to its high moisture content and biodegradability [9]. Thus, fer-
mentable HFW separate collection at source and its dehydration in a
large scale dryer/shredder at municipality level [10] is an alternative
MSW management strategy, resulting to a homogeneous biomass pro-
duct (dried HFW (DHFW)) with low water content, and different uti-
lization possibilities [10–12]. For instance, Ntaikou et al. [10] in-
vestigated the possibility of using DHFW for ethanol production using
mono- and co-cultures of the yeasts Saccharomyces cerevisiae and Pichia
stipitis, while di Bitondo et al. [12] used the same substrate for pro-
duction of ethyl levulinate through a combined Lewis-Brønsted acid
ethanolysis process. In addition, in the study of Papadopoulou et al.
[11] alternative schemes for the valorization of DHFW are presented,
including production of pellets, biogas, animal feed, activated carbon,
compost and the exploitation of this biowaste as an alternative energy
source for the cement industry. In this respect, the exploitation of
DHFW in a Microbial Fuel Cell (MFC) for electricity generation seems
very promising, due to its high content in readily fermentable carbo-
hydrates, which can be ideal substrates for biological processes, which
take place in such a system.
MFCs are bio-electrochemical systems in which electricity is directly
produced, through the microbial catalytic activity, providing new op-
portunities for energy production and simultaneous wastewater/waste
treatment [8,13]. A typical MFC consists of a biological anode and an
abiotic cathode, where exoelectrogenic microbes attached to the bio-
anode produce electrons and protons, catalyzing the electrochemical
reactions through interaction with the anode electrode [14]. The elec-
trons which are produced through the anaerobic respiration of electron
donors are transferred through the external circuit to the cathode where
reduction of an oxidant takes place with participation of protons,
transported from the anode compartment through a membrane
[15–17].
Recent investigations have shown that the current density produced
by MFCs has been increased significantly in the last 10 years [18].
Despite their potential applications, the maximum power generation of
MFCs is still limited, impeding their commercial development, pri-
marily because of their high internal resistances, mainly associated with
anode overpotential and ohmic losses [19,20]. Improvements of power
production depend significantly on the electrode materials and the
design/configuration of MFCs, as well as on the exo-electrogenic cap-
abilities of the implicated microorganisms [21]. In this respect, dif-
ferent reactor configurations have been proposed [22–24]. The concept
of air-cathode single-chamber MFC is considered promising, as the
absence of aeration and polymeric membrane offer the possibility of
enhanced power generation and reduced capital costs.
In the present study, the novel concept of valorization of a typical
DHFW as a fuel for the production of electricity in an MFC was assessed.
DHFW was initially subjected to extraction using warm water resulting
to a liquid fraction (extract) and a solid residue. This strategy has also
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Applied Energy 242 (2019) 1064–1073
been presented in other studies, in which the rich in soluble- com-
pounds water extract that was produced from DHFW was used for
biofuels production in batch reactors [25] or in continuous systems
[26]. Water extraction has also been applied to other types of wastes,
such as food industry waste, the diluted soluble fraction of which was
assessed as substrate in an anaerobic continuous up-flow column bior-
eactor (AUFCR) [27], and sweet sorghum biomass the extract of which
was used for hydrogen and methane production in continuous bior-
eactors [28].
The rich in soluble chemical oxygen demand (s-COD) extract of
DHFW was used for the first time, for electricity production, via a four-
air cathode single-chamber MFC with MnO2 as cathode catalyst and a
packed bed of graphite granules as anode, initially developed by
Tremouli et al. [29]. The MFC performance was assessed under dif-
ferent organic loading rates, aiming at DHFW valorization, using the
highest possible initial organic loading, To our knowledge, it is the first
time that HFW has been used for direct electricity production in a
single-chamber MFC system. Before using HFW extract, preliminary
experiments with synthetic glucose based medium were conducted, in
order to assess the optimum operational conditions (optimum hydraulic
retention time (HRT)) and to establish a long term stable continuous
operation of the MFC. Apart from the main biochemical and physico-
chemical characteristics determination, the electrochemical character-
ization of the MFC was assessed by conducting Electrochemical Im-
pedance Spectroscopy (EIS) experiments under open circuit conditions,
using glucose and DHFW extract as substrates. The possibility of using
anaerobic digestion (AD) for the valorization of the solid residue from
the extraction process was also investigated, via biochemical methane
potential (BMP) experiments, aiming thus to achieve maximum energy
recovery from the whole DHFW biomass. The experimental results
obtained are promising indicating that the entire biomass of DHFW
could be valorized through the novel proposed scheme of processes.
2. Materials and methods
2.1. Raw material
2.1.1. Characteristics
HFW were collected at municipality level twice a week from 240
houses of the Municipality of Halandri, Greece. It was source-separated,
and included fermentable wastes solely, such as kitchen food waste,
fruit, vegetables, used tissue paper (cellulose), free of bones and fluids.
Upon collection, the waste was subjected to simultaneous heat-drying
at 95–98 °C (treatment for 9 h) and shredding in a pilot-scale dryer/
shredder, resulting in a homogeneous organic product (DHFW). The
characteristics of DHFW used are presented in Table 1.
2.1.2. The extraction process
The extraction process was optimized in terms of maximum COD
recovery (% gCOD/gTS) and maximum concentration of COD in the
extract, by varying the extraction duration and the temperature. Thus,
Table 1
The main characteristics of DHFW used in the present study.
Characteristic Value
TS (%) 91.3 ± 0.8
VS (g/100 gTS) 92.3 ± 0.7
Total carbohydrates (g/100 gTS) 43.0 ± 3.0
Recoverable dissolved sugars (g/100 gTS) 21.0 ± 2.0
Cellulose (g/100 gTS) 11.0 ± 1.0
Hemicellulose (g/100 gTS) 3.0 ± 0.0
Lignin (g/100 gTS) 5.0 ± 0.0
Starch (g/100 gTS) 16.0 ± 2.0
Proteins (g/100 gTS) 11.0 ± 1.0
Extractives (g/100 gTS) 32.1 ± 2.1
Ash (g/100 g TS) 8.0 ± 0.1
G. Antonopoulou, et al.
different solids loadings, namely 5, 10, 15 and 20% (gTS DHFW/
100 mLwater), were mixed for 30 or 60 min at room temperature
(25 °C) or upon heating at 30 °C and the liquid fraction (extract) was
characterized in terms of COD concentration.
2.2. Valorization processes
2.2.1. Electricity production in MFC
2.2.1.1. MFC construction. The experiments were performed using the
single-chamber four air–cathode MFC presented in Tremouli et al. [29].
Briefly, the MFC consisted of a single cylindrical chamber and four
tubes, homogenously drilled with holes (total geometrical surface area
of 164 cm2), placed in the chamber. The empty bed volume of the MFC
was filled with graphite granules with a density of 0.904 ± 0.0303 g/
mL, serving as the anodic biofilm support, connected to the circuit using
a graphite rod. The graphite granules were subjected to treatment with
HCl, as described in Zhuang el al. [30,31] through which their specific
surface area increased by 27% (from 0.9443 ± 0.0074 to
1.2032 ± 0.0091 m2/g, according to Brunauer–Emmett–Teller (BET)
analysis). The cathode was made of GORE-TEX ® cloth
(7.5 cm × 7.5 cm) wrapped on the four plexiglas tubes and coated
with MnO2 at a loading of 213.3 mg/cm2, as described in Zhuang et al.
[30]. A closed electrical circuit was formed with a 100 Ω external
resistor connecting, via copper wires, the anode graphite rod and the
cathode. The temperature of the MFC during the experiments was
maintained at almost 28 °C, by setting it in a constant temperature
chamber.
2.2.1.2. Acclimation period. Inoculum from the anaerobic digester of
the wastewater treatment plant located in Metamorphosis, Attica,
Greece, was used with the following characteristics:
pH = 7.00 ± 0.10, s-COD = 0.28 ± 0.1 g/L, total suspended solids
(TSS) = 39.54 ± 2.12 g/L and volatile suspended solids
(VSS) = 16.71 ± 0.75 g/L. In each cycle, glucose at initial
concentration of 0.8 g COD/L, also supplemented by a buffer solution
of Na2HPO4·2H2O: 3.4472 g/L and NaH2PO4: 3.668 g/L, NaHCO3: 5 g/
L, KCl: 0.16 g/L and a solution of 10 mL/L with trace metals [32] was
added as substrate, along with methanogenic sludge in 10% ratio.
Glucose addition along with inoculum was performed for four
successive cycles, at a batch mode, in order for the establishment of
an electrogenic microbial consortium in the anode.
2.2.1.3. Operation of the MFC using synthetic substrate. When the
acclimation phase was completed, the operational mode of the MFC
was switched to continuous for overall period of 75 days. A glucose-
based synthetic medium was used as substrate, with initial
concentration of 0.79 ± 0.04 g COD/L. The medium was also
supplemented with buffer solution, NaHCO3, KCl, and trace metals
solution, as described above. The feed of the MFC was maintained at
∼4 °C, and it was supplied continuously, using a peristaltic pump and
adjusting the flow rate appropriately to achieve the different HRTs. As
such, the MFC operated at a HRT of 38 h (days 1–11), 30 h (days
11–26), 24 h (days 26–33), 18 h (days 33–57), 14 h (days 57–63), 9 h
(days 63–66) and, then, again at a HRT of 18 h (days 66–78), ensuring
the achievement of steady state in each case, i.e. for < 10% variation of
the monitored parameters.
2.2.1.4. Operation of the MFC using DHFW extract. Following the
continuous reactor operation using glucose based synthetic medium,
the extract of the DHFW was used as energy source, at an HRT of 18 h
and for different initial concentrations, so as to achieve maximum
exploitation of the substrate. The extract of DHFW was also
supplemented with the buffer solution, NaHCO3 and KCl, as described
above. The reactor was initially operated at a concentration of
0.64 ± 0.03 g COD/L (days 78–101); then the concentration of the
feed was increased to 1.23 ± 0.05 g COD/L (days 101–110) and finally
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Applied Energy 242 (2019) 1064–1073
to 2.13 ± 0.07 g COD/L (days 110–121), ensuring that a steady state
was reached in each case.
2.2.2. Methane production
2.2.2.1. Seed culture. Inoculum from the anaerobic digester of
Metamorphosis, Athens wastewater treatment plant, using sewage
sludge as substrate and operating at steady state at an HRT of 15 d,
was used. The sludge characteristics were: pH = 7.41 ± 0.15,
TSS = 39.53 ± 0.12 g/L and VSS = 18.62 ± 0.52 g/L. For ensuring
anaerobic conditions, the sludge was gassed with an inert gas (N2/
CO2:80/20) before use.
2.2.2.2. Biochemical methane potential (BMP) tests. BMP tests were
performed on the solid fraction obtained after the optimized
extraction process (organic loading 20%, 25 °C, 30 min). The
experiments were carried out in duplicate at 35 °C according to the
protocol described in Alexandropoulou et al. [25].
2.3. Analytical methods
2.3.1. Analysis of chemical composition and characterization
TS, VS, TSS, VSS and COD were determined according to Standard
Methods [33]. For the quantification of total and soluble carbohydrates
the protocol of DuBois et al. [34] was applied, whereas the quantifi-
cation of starch was made via a total starch assay kit (Megazyme).
Extractives, cellulose, hemicellulose and lignin content were analysed
following the National Renewable Energy Laboratory (NREL) standard
laboratory analytical procedures (LAP) for determination of extractives
and structural carbohydrates in biomass [35,36]. Τotal Kjeldahl Νi-
trogen (TKN) was determined according to Standard Methods [33]
while the protein content was calculated by multiplying TKN by a factor
of 6.25 [37].
2.3.2. Methods and calculations for MFC experiments
Recording of the MFC potential (Ucell) was performed every 50 s
using a data acquisition system (ADAM-4017). In order to obtain the
polarization curves the external resistance of the circuit was altered
(0.1–1000 kΩ) recording the potential and current values. The cou-
lombic efficiency, CE (%), defined as the ratio of total charge actually
transferred to the anode from the substrate to the maximum theoretical
charge that would result if all the substrate removal produced current,
was determined according to Eq. (1):
M∗I
CE =
F ∗ b ∗ q ∗ ΔCOD (1)
where I is the current (A), M = 32 is the molecular weight of oxygen
(g / mol), F is Faraday’s constant (96,485 C/mol-e), b = 4 is the number
of electrons exchanged per mol of oxygen, q is the volumetric rate (L/s)
and Δ(COD) is the change in s-COD (g/L).
Electrochemical characterization of the fuel cell was performed
under open circuit conditions as described in Antonopoulou et al. [14].
Briefly, an Autolab PGSTAT302 potentiostat - galvanostat equipped
with a frequency response module (FRA32) and controlled by the
NOVA software package was used for the electrochemical impedance
spectroscopy (EIS) measurements. The frequency range of
100 kHz–1 mHz, using a stimulus of 10 mV amplitude, was used.
Equivalent circuit fitting to the impedance data was performed using
the ZSimpWin software (Princeton Applied Research).
Specific surface area (SBET) of the graphite granule samples before
and after HCl treatment were determined by nitrogen adsorption at
−196 °C using a Quantachrome Autosorb-1 instrument. For the de-
termination of the specific surface area (SBET) of the samples (pre-
viously out gassed at 200 °C for 2 h under vacuum) the BET method was
used at six relative pressures of nitrogen (0.05–0.3).
SEM images were captured using a Zeiss SUPRA 35VP scanning
electron microscope, after coating the samples with a homogeneous Au
G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

(a) (a)
100 0.7
25oC, 30min 35 oC, 30 min
25 oC, 60 min 35 oC, 60min 0.6
80
0.5
COD (g/L)

60

Ucell (V)
0.4

40 0.3

0.2
20
0.1

0 0.0
5 10 15 20 0 100 200 300 400 500
Solids loading, % Time (h)
(b) (b)
60
25oC, 30min 35 oC, 30 min
700
COD recovery (% w/w TS)

50 25 oC, 60 min 35 oC, 60min

600
40 500

COD (mg/L)
30 400

20 300

200
10
100
0
5 10 15 20 0
Solids loading (%) 0 100 200 300 400 500
Time (h)
Fig. 1. COD concentration (a) and recovery (b) for different extraction condi-
tions. Fig. 2. MFC potential (a) and COD (b) versus time during the acclimation
period, at batch mode. External resistance: R = 100 Ω.
layer via ion sputtering.
The concentration of the volatile fatty acids (VFAs) (acetic, pro- 32.1 ± 2.1 g/100 g TS with a COD content of 1.33 g COD/g extractive.
pionic, iso-butyric, butyric, iso-valeric, valeric, hexanoic acids) was Taking into account that a small amount of extractives is probably in-
determined via gas chromatography under the conditions described in organic and the ash content of DHFW is 8 g/100 gTS, supports the
Antonopoulou et al. [28]. above arguments, since the estimated s-COD balance is almost com-
plete. For this reason, the conditions which were selected as optimum
2.3.3. Analytical methods for BMP experiments for the extraction process were 20% solids loading, 25 °C and 30 min.
The composition in methane of the produced gas was quantified The resulting extract had 78.05 ± 1.20 g COD/L, with
with a gas chromatograph (SRI 8610c MG#1), equipped with a thermal 43.27 ± 1.95 g/L sugars. After proper dilution, the rich in COD extract
conductivity detector and a packed column. The carrier gas was helium. was used for electricity production in the four air– cathodes single
The injector, column and detector temperatures were set at 90 °C, 35 °C chamber MFC, while the solid residue was used as substrate in BMP
and 100 °C, respectively. experiments.

3. Results and discussion 3.2. Valorization of DHFW for electricity and methane production

3.1. Optimization of the extraction method 3.2.1. MFC operation

In order to obtain maximum recovery of soluble compounds from
the DHFW via extraction, different approaches were followed in terms
of solids loading, water temperature and time of extraction process. In
Fig. 1, the COD concentration and COD recovery at different extraction
conditions are presented. It is obvious from the Figure that the ex-
traction time and temperature did not influence COD, for the same
solids loading. The mean yield of COD recovery was estimated to be
40 ± 1%, indicating that the maximum amount of soluble COD con-
tained in the DHFW can be recovered even using the lowest tempera-
ture and extraction time and the highest solids loading, which is more
favourable for the process economy. The assumption that the yield of
COD recovery presented in Fig. 1 corresponds to the maximum re-
coverable s-COD of DHFW is further justified by the amount of ex-
tractives contained in DHFW (presented in Table 1), which is
3.2.1.1. Acclimation phase. The air cathode MFC was initially operated
in batch mode using anaerobic sludge and a synthetic nutrient solution
based on glucose, where acclimation of the mixed anaerobic microbial
culture was conducted. In Fig. 2, the MFC potential and COD
consumption during this operation phase are presented. The use of
glucose as feed-substrate during the acclimation phase was conducted
in order to establish a microbial consortium consisting of different types
of microorganisms, among which the presence of electrogenic ones
would be expected, since glucose can be assimilated from almost all
types of heterotrophic bacterial strains [38]. Park et al. [39] also found
that the pre-acclimation strategy affected the microbial community
structure, as they observed a great variation of the bacterial community
in an air cathode MFC due to the use of different substrates during
acclimation.
During the first cycle of the MFC operation, a COD removal of 83%

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G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

was observed. However only a small ratio of electrons produced from (a)
the anaerobic respiration of glucose led to electricity generation, as it 0.6
HRT: 38h HRT: 24h
can be assumed by the low CE (it was estimated at 10.8%). The time HRT: 30h HRT: 18h HRT: 18h

that was required for the complete consumption of glucose (Fig. 2b) 0.5
was almost 150 h, after which a rapid drop of the cell voltage to zero,
HRT: 14h
occurred. Thereafter, draining of the anolyte and addition of fresh 0.4
glucose based medium together with inoculum of anaerobic sludge, was

Ucell (V)
HRT: 9h
performed. At this point a rapid increase of the cell potential to 0.31 V 0.3
was observed. The duration of this cycle was shorter, i.e. 125 h, the CE
0.2
slightly increased to 16.5%, and the COD removal efficiency remained
stable at 84%. During the third cycle of the acclimation phase, a further
0.1
increase of the potential and the CE was noted, reaching 0.62 V and
22%, respectively. Such an increase indicated the firm establishment of 0.0
desirable microorganisms with exo-electrogenic activity on the anode, 0 10 20 30 40 50 60 70
which is in accordance with other studies reporting that anaerobic
(b) Time (d)
sludge is a suitable inoculum for MFCs [14].
Finally, in the fourth cycle, the voltage and the CE were approxi-
mately the same with those of the third cycle (0.63 V and 22.5% re- HRT: 24h
800 HRT: 38h HRT: 18h
spectively), confirming the reproducibility of the MFC operation. After HRT: 30h HRT: 18h
HRT: 9h
acclimation for four cycles, noticeable biofilm growth was observed on
the surface of graphite granules, which is crucial for the production of 600

COD (mg/L)
HRT: 14h
electricity [20]. The biofilm formed could be used as catalyst for con-
ducting the experiments in continuous mode. It is worth mentioning 400
that the COD removal efficiency was at high levels (> 83%) in all ac-
climation cycles.
200
3.2.1.2. Operation with synthetic substrates. Following the acclimation
phase, the operational mode of the MFC was switched to continuous 0
using as feed glucose-based synthetic medium at a concentration of 0 10 20 30 40 50 60 70
0.78 ± 0.04 g COD/L and the effect of HRT was investigated. The MFC Time (d)
potential (Ucell) and the COD of the effluent, as well as the main
characteristics of the MFC, at steady state at each HRT (38, 30, 24, 18, Fig. 3. MFC potential (a) and COD (b) versus time at different HRTs with
14, 9 h and then again to 18 h) are presented in Fig. 3 and Table 2, glucose as substrate. External resistance: R = 100 Ω.
respectively. It should be noted that the HRT was increased eventually
back to 18 h in preparation for the MFC operation with real wastewater- Table 2
DHFW extract, since this HRT was found to be the optimum one. The main characteristics of the MFC at each HRT, using glucose as energy
In the first days of MFC operation in continuous mode the cell source.
voltage decreased from 0.63 (in batch mode) to 0.51 V (at steady state HRT (h) Ucell (V)* COD removal CE** (%) Pmax (W/ Energy yield
in continuous mode, with HRT = 38 h). This small decrease in MFC efficiency (%) m3)*** (MJ/kg
voltage when the operation switched from batch to continuous mode CODin)****
has also been reported in the literature, for the same substrate [15,29].
38 0.501 76.0 19.1 8.6 1.50
Reducing the HRT, the voltage further decreased to 0.456 and 0.468 V 30 0.487 67.5 16.3 8.4 1.15
at the HRT = 14 and 18 h, respectively. These are typical operational 24 0.478 71.1 12.1 10.3 1.13
values of voltage for single chamber MFCs, which generally produce an 18 0.472 68.7 12.4 11.8 0.97
open-circuit voltage of approximately 0.8 V with a resultant working 14 0.456 52.6 11.7 10.2 0.65
9 0.470 55.7 7.6 8.2 0.34
voltage of 0.5 V [18], under similar conditions (R = 100 Ω).
18 0.468 77.6 10.9 8.7 0.72
Apart from the voltage, reduction of the HRT also led to a CE re-
duction, from 19.1% at the HRT of 36 h to 7.6% at the HRT of 9 h * R = 100 Ω.
(Fig. 3a). Similar CEs (11.7–12.4%) were observed for the HRTs of ** Columbic efficiency.
14–24 h, which were gradually decreased upon decrease of the HRT to *** Maximum power density.
9 h. When the HRT increased from 9 to 18 h, in order to study the **** Soluble COD of the influent.
system flexibility and the experimental results reproducibility, the CE
increased from 7.6 to 10.9%, which is slightly lower than the CE ob- oxygen at the anode, due to the permeability of the separator between
tained for MFC operation at the HRT of 18 h for the first time (12.4%). anode and cathode (typically, the membranes in conventional two-
These results are in agreement with those of other studies, in which chamber MFCs). Increased oxygen concentration is expected to lead to
higher CEs were observed at lower organic loading rates (higher HRTs) the partial oxidation of the substrate, a process which is competitive to
[40,41]. The observed effect of HRT on CE could be associated either the electrogenic reactions for energy generation. Similar to the ion or
with mass transfer limitations within the biofilm or with the existence proton exchange membranes in which oxygen permeability from
of non-exoelectrogenic microbial species, which prevail at low HRTs cathode to the anode is reported [14,42], the open pore structure of
and get involved in competitive reactions without producing electricity. GORE-TEX® cloth, used in the current study, might be favorable for
The CEs obtained in the present study, even at the higher HRTs are oxygen diffusion, thus leading to low CEs [31,43].
below 20%. Similar CEs were obtained in a previous study conducted in Oxygen permeability and partial substrate oxidation are also cor-
the same MFC system under different HRTs, using glucose as substrate roborated by the relative high values of the COD removal efficiency
[29]. In that study, CEs in the range of 3–8.4% were observed at short obtained in this study (Table 2 and Fig. 3b), as well as confirmed by the
HRTs (1.76–5 h) and 10–18% at relatively longer ones (7.5–15 h). It is low VFAs concentration (Fig. 4) observed in the anolyte effluent. It is
well known that reduced CEs could be associated with the increase of worth mentioning that there was no production of methane throughout

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G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

160 (a)
Metabolic products (mg/L) acetic acid 0.6
propionic acid
butyric acid
120 0.5

0.4

-Ucell (V)
80
38 h
0.3 30 h
24 h
40 0.2 18 h
14 h
9h
0.1 18 h *
0
38 30 24 18 14 9 18 0.0
HRT (h) 0 10 20 30 40 50
Current density (A/m3 )
Fig. 4. The mean values of the effluent concentrations of the main metabolic
products (VFAs) at steady state at different HRTs, with glucose as substrate. (b)
18
38 h
15 30 h

Power density (W/m3 )

the operation period, which means that no methanogenic - activity
occurred. Thus, the observed relative high COD removal efficiency with
a relatively low CE (i.e., at the HRT of 18 h the COD removal efficiency
was 77.6% with only a 10.9% of the electrons produced by oxidation of
the substrate converted to electricity) implies that part of the organic
substrate was probably oxidized by non-electrogenic bacteria forming
carbon dioxide, thus reducing the efficiency of the MFC. In addition,
part of the organic substrate could be converted to biomass, especially
in the solid biofilm phase, which is also not accounted in the effluent
COD concentration. It is worth mentioning that the formation of biofilm
on the graphite granules was evident, even visually. The sum of VFAs
concentration at steady state at each HRT (Fig. 4) was consistent with
the measured COD concentration, closing the carbon mass balances of
the substrate.
In Fig. 5, the polarization curves, at each HRT are presented. The
maximum power density, Pmax, (normalized to the working volume of
the MFC-anode), obtained in the present study at the conditions tested,
using glucose as substrate was 11.8 W/m3 at HRT = 18 h, with a cur-
rent density of 32.2 A/m3 and a MFC potential of 0.2 V (external load
10 Ω). It should be noted that for the HRTs of 24–9 h, the maximum
power density is expected to be higher than that reported in Table 2,
since the calculation of table values was based on the variation of the
external load from the value 0.1 to 1000 kΩ, and the power density was
maximum at even lower external loading values (R < 0.1 kΩ), as also
confirmed by Fig. 5b.
The HRT change did not considerably affect Pmax. Thus, a Pmax of
8.6 W/m3 (at 8.9 A/m3, 0.30 V and external load 20 Ω) were obtained at
the HRT of 36 h whereas the respective values were 8.2 W/m3, 34.9 A/
m3 and 0.24 V (external load 10 Ω) when the HRT decreased to 9 h. The
Pmax produced by this MFC is comparative to the values reported in
other studies in which air-cathode MFCs were used. According to the
study of You et al. [44] a Pmax of 50.2 W m3 was achieved from a
tubular membrane-less air cathode MFC with graphite-granules as
supporting media for biofilm formation. In addition, Tremouli et al.
[29] reported a Pmax of 13.6 W/m3 for a MFC same as the one used in
the present study, fed with synthetic wastewater, while Zhuang et al.
[30] reported a Pmax of 2.8 W/m3 when using a tubular air–chamber
MFC, packed with graphite granules as the anode and conductive paint
and MnO2 catalyst as a cloth cathode assembly.
It is evident from the polarization experiments that the internal
resistance of the tested MFC is very low (20 Ω at the HRTs of 38 and
30 h and R < 10 Ω for lower HRTs), as also confirmed by a previous
study on the same MFC system [29]. In that study, the internal re-
sistance of the MFC was calculated from polarization experiments to be
40 Ω, corresponding to a power density of 13.6 W m3. Internal re-
sistance of a MFC is associated with the anodic and cathodic reactions
which take place in the MFC as well as with mass transport and ohmic
limitations, thus with the materials used and the MFC geometry and
24 h
18 h
12
14 h
9h
9 18 h *
6
3
0
0 10 20 30 40 50
Current density (A/m3 )
Fig. 5. MFC voltage (a) and power density (b) versus current density, for glu-
cose as substrate at different HRTs, at 0.78 ± 0.04 g COD/L.
architecture [18,23,24]. By using GORE-TEX® as cathode material a
high proton transfer rate is possible, facilitating the cathodic reduction
of oxygen to water and resulting in a reduced internal resistance of the
MFC [45]. This was reported by Zhuang et al. [31] who found that the
diffusion rate of proton through GORE-TEX® cloth was approximately
65 times higher than that through anion and cation exchange mem-
branes (AEC and CEM, respectively). The anode reaction in which the
protons are produced is also important and associated with the internal
resistance of the MFC.
Τhe energy yield (expressed in MJ/kg CODin) corresponding to Pmax
at each HRT was also calculated. From the energy yield values listed in
Table 2, it is concluded that the energy recovery from the operation of
the MFC with glucose at HRTs in the range 9–38 h varied from 0.34 to
1.5 MJ/kg COD, with the maximum yield obtained at the higher HRT of
38 h.
3.2.1.3. Operation with DHFW extract. Following the continuous reactor
operation using glucose-based synthetic wastewater, diluted extract of
the DHFW was used as energy source at HRT of 18 h and for different
substrate concentrations in the feed (0.64 ± 0.03, 1.23 ± 0.05 and
2.13 ± 0.07 g COD/L). The MFC voltage (Ucell), for R = 100 Ω, and the
COD of the influent and effluent, as well as the main characteristics of
the MFC at steady state at each organic loading using diluted DHFW
extract are presented in Fig. 6 and Table 3, respectively.
As shown in Fig. 6a, the MFC voltage varied from 0.40 to 0.48 V, i.e.
it was lower compared to the voltage obtained using glucose as sub-
strate. This could be attributed to the fact that glucose and diluted
DHFW extract had a different composition and concentration, since
sugars represent almost 55% of the COD of diluted DHFW extract, with
the rest 45% being other soluble compounds. Comparing glucose
(HRT:18 h, 0.78 ± 0.04 g COD/L) and DHFW extract as MFC

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G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

(a) HRT 18h (a)

0.6
HFW HFW HFW 0.6
0.64 g/L 1.23 g/L 2.13 g/L
0.5 0.64 g/L
0.5 1.23 g/L
2.13 g/L
0.4 0.4
Ucell (V)

0.3

-Ucell (V)
0.3

0.2 0.2

0.1 0.1

0.0 0.0
80 85 90 95 100 105 110 115 120 0 10 20 30 40
Time (d) Current density (A/m3 )
(b) (b)
14
2500
0.64 g/L
12
COD reactor 1.23 g/L

Power density (W/m3 )

2000 COD feed
10 2.13 g/L

8
COD (mg/L)

1500
6
1000 4

500
0 0
80 85 90 95 100 105 110 115 120
Time (d)
Fig. 6. MFC voltage (a) and COD (b) vs. time when using diluted DHFW extract
as energy source, at different organic loadings. HRT = 18 h. External load:
R = 100 Ω.
substrates at similar conditions (HRT:18 h, 0.64 ± 0.03 g COD/L), it is
clear that the COD removal efficiency was quite high (over 70%) in
both cases (Tables 2 and 3), which indicates that DHFW extract also
composed of biodegradable compounds. The fact that the maximum
power density and the CE at the lowest DHFW extract organic loading
(0.64 ± 0.03 g COD/L) were similar to those obtained using glucose
(Tables 2 and 3, HRT = 18 h) also corroborates this argument.
Increasing the DHFW extract organic loading, the COD removal
efficiency decreased, since at the lowest concentration the COD re-
moval efficiency was 74% and decreased to 55.7% when the con-
centration increased to 2.13 ± 0.07 g COD/L (Table 3). At this organic
loading, the reactor was probably kinetically limited. This was not the
case for organic loading 1.23 ± 0.05 g COD/L for which the COD re-
moval efficiency was also high. The CE also gradually decreased from
12.3% to 4.79%, by increasing the feed concentration from 0.64 g COD/
L to 2.13 g COD/L (Table 3). The CE of 12.3% was similar to that ob-
tained when glucose was used as substrate (12.4%) at similar conditions
(HRT of 18 h and feed concentration of 0.64 g COD/L.
2
0
10 20 30 40
Current density (A/m3 )
Fig. 7. MFC voltage (a) and power density (b) versus current density, for di-
luted DHFW extract at different organic loadings, when HRT = 18 h.
In Fig. 7 the polarization curves at all tested organic loadings of the
DHFW extract are presented. As shown in Fig. 7a and Table 3, Pmax
(normalized to the working volume of the MFC anode) obtained using
diluted DHFW extract as substrate was 8.1 W/m3 (at 35.11 A/m3,
0.23 V, external load: 10 Ω). As previously mentioned for the case of
glucose, the maximum power density would be higher than that re-
ported in Table 3, since, as it is obvious from Fig. 7b, the maximum of
the power density curve would be observed at lower external loading
values than the respective applied in the present study (R < 10 Ω).
The substrate concentration did not seem to affect considerably the
values of Pmax. Specifically, a Pmax of 7.7 W/m3 (27.6 A/m3, 0.28 V,
external load: 10 Ω) was obtained for feed concentration of
0.64 ± 0.03 g COD/L, while the same power density value was ob-
tained for a feed concentration of 2.13 ± 0.07 g COD/L, corresponding
to 35.3 A/m3 and 0.22 V (external load: 10 Ω). It is noted that the Pmax
values obtained using DHFW extract as substrate is within the range of
the power densities using glucose as energy source. Thus, taking into
account the enormous quantities and the availability of HFW, the use of
this kind of biomass as substrate for bioelectricity generation is very
promising. The successful use of FW as a source for electricity

Table 3
The main characteristics of the MFC at each organic loading, using DHFW extract as energy source, for HRT equal to 18 h.
COD (g/L) Ucell (V)* COD removal efficiency (%) CE** (%) Pmax*** (W/m3) Energy yield (MJ/kg CODin)****

0.64 ± 0.03 0.41 74.0 12.3 7.7 0.78

1.23 ± 0.05 0.48 71.3 7.76 8.1 0.43
2.13 ± 0.07 0.40 55.7 4.79 7.7 0.23

* R = 100 Ω.
** Columbic efficiency.
*** Maximum power density.
**** Soluble COD of the influent.

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G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

production directly in MFCs has also been confirmed by other studies, 4

Open Circuit Potential (0.52V)
the majority of them referring to the use of FW kitchen leachate as
Food waste
energy source [46–50]. Among the priorities of these studies was the Glucose
optimization of the efficiency of the two-chambered MFCs used, by 3 0.01Hz
studying the effect of parameters such as the organic loading [50], the

-Zim (ȍ)
pH and the ionic strength [48], the recirculation [46] and the use of
alternative microbial inoculum [47]. Specifically, Moharir and Temb- 2
hurkar [46] observed a maximum power density of 0.98 W/m3
(29.32 mW/m2) when using FW leachate at initial COD concentration 0.1 Hz
of 1.25 g/L, in a two-chamber MFC operated in fed-batch mode, under 1 100Hz

recirculation conditions. Even higher power densities values (15.14 W/

m3) were reported by Rikame et al. [49] for a much higher COD con-
0
centration of 5 g/L and by using Ultrex (Membrane International Inc. 0 1 2 3 4 5 6 7
USA) as proton exchange membrane (PEM).
Zre (ȍ)
From the energy yield values, corresponding to Pmax at each organic
loading (Table 3), it can seen that lower concentration of COD in the Fig. 9. Nyquist plots for glucose and DHFW extract as energy sources, under
feed resulted also to a higher yield of energy (0.78 MJ/kg COD), which open circuit conditions (HRT = 18 h).
was similar to that for glucose (for the same organic loading and HRT).
The energy yield decreased to 0.23 MJ/kg COD when the COD con-
nature of some physical property of the system) which is connected in
centration in the feed was increased to 2.13 ± 0.07 g/L (Table 3), since
parallel with a series combination of a Warburg element, with im-
at this high concentration the HRT (18 h) was not adequate for the
pedance ZW = Υ0,W−1 (jω)−1/2 (associated with semi-infinite mass
biofilm to degrade the DHFW extract and to produce electricity (kinetic
transfer resistance) and a charge transfer (faradaic) resistance, RF. This
limitation). On the contrary, fermentation towards acetate and pro-
parallel circuit is connected in series with an ohmic resistance (RΩ).
pionate probably occurred, as confirmed by parallel VFAs measure-
ments (Fig. 8). These reactions were probably carried out by anaerobic
acidogenic bacteria which were present in the biofilm, not contributing
to the electricity generation.
Similarly to the case of synthetic substrate, it was concluded from
the polarization experiments that the internal resistance of the MFC was
very low (R < 10 Ω for all conditions).
(EC(1))
Impedance parameters obtained via fitting and associated with
3.2.1.4. Electrochemical impedance spectroscopy characterization of the
charge transfer (RF) and mass transfer (Yo,W) processes are listed in
MFC. In order to complete the electrochemical characterization of the
Table 4. The listed values correspond to the entire cell, under open
MFC, its impedance characteristics were investigated by conducting EIS
circuit conditions, for glucose and DHFW extract as substrate. However,
experiments under open circuit conditions, using glucose and DHFW
as the cathode was the same for both substrates, their comparison can
extract as substrates. The data are presented in the form of Nyquist
convey useful information as it concerns the effect of substrate on MFC
plots, i.e. as -imaginary vs. real part of the impedance plots (Fig. 9). For
characteristics. Specifically, this comparison denotes that mass transfer
both substrates, mass transfer limitations are evident. The straight line
limitations are less pronounced for the MFC operating with DHFW ex-
below ca. 10 Hz inclined at ca. 45° to the real axis implies the existence
tract compared to that operating with glucose, while the opposite holds
of a Warburg impedance element, associated with semi-infinite linear
for the charge transfer resistance. However, it has to be noted that these
diffusion of the bio-electroactive species to or from the electrochemical
data correspond to open circuit conditions and conclusions cannot be
reaction site.
directly projected to MFC operation under current.
The impedance data were successfully fitted to the equivalent cir-
The fact that the mass transfer limitations were significant in the
cuit (EC(1)) presented below, where Q denotes a constant phase ele-
MFC system could be attributed to the intense biofilm formation, all
ment with impedance ZQ = Y0,Q−1 (jω)−n (associated in most cases
around the graphite granules. The fact that biofilm formation continued
with a non-ideal capacitance, but, in general, with the distributed
with the progression of time can partly explain why mass transfer
500 limitations appear to be more pronounced during the operation of the
acetic acid MFC with DHFW as energy source, since experiments with DHFW fol-
propionic acid lowed glucose-based experiments. SEM images of biofilms grown on
Metabolic products (mg/L)

400 butyric acid graphite granules located at different MFC chamber heights (obtained
at the end of the experiments, after DHFW addition of 2.13 ± 0.7 g
300 COD/L) showed that the biofilm characteristics were different at the
different heights, since the biofilm formation was more intense at the
bottom of the chamber (where the feed entered the MFC) compared
200
with other positions (Fig. 10).

100

Table 4
0 Impedance parameters for the MFC under open circuit conditions (Figs. 9 and
0.64 1.23 2.13 10), for glucose and DHFW extract as substrate.
COD (g/ L)
Glucose DHFW
Fig. 8. The mean values of the concentrations of the main metabolic products
Y0,W for W (Ω−1 s0.5) 0.982 ( ± 1.6%) 1.575 ( ± 2.1%)
(VFAs), at steady state for different organic loadings in the feed, when using
RF (Ω) 1.613 ( ± 3.7%) 2.372 ( ± 1.4%)
diluted DHFW extract as substrate. HRT = 18 h.

1071
G. Antonopoulou, et al.
Fig. 10. SEM images of the biofilm on graphite granules prior to use (a) and after the experiments with DHFW for graphite granules obtained from the bottom of the
MFC chamber (b) and from the top of the MFC chamber (c).
3.2.2. Methane production
BMP experiments were performed in order to assess the methane
potential produced from the solid residue obtained after the optimized
extraction process (25% organic loading), and as such to access the
energy recovery from the full exploitation of DHFW (extract and re-
sidue).
In Fig. 11 the cumulative methane production during the experi-
ments is presented.
The calculated yield in methane from the solid fraction of the
DHFW, after subtracting the methane produced from blank experi-
ments, was almost 434 ± 1 mL CH4/g TS of solid fraction, or
330 ± 1 L CH4/kg TS DHFW, indicating its high biodegradability. In
order to calculate the stored energy in the form of methane, its energy
density was used (36.4 kJ/L). As such, the recoverable energy from the
solid residue in the form of methane was 12.01 MJ/kg TS DHFW.
3.2.3. Energy input and energy recovery from DHFW
Beyond the scientific aspect, the present study concerns the im-
portant issue of MSW management, which is one of the main problems
of urban societies. Especially for countries like Greece, where land-
filling is still the main MSW management method, the exploitation of
different approaches for its valorization, following separate collection
at the source, seems to be a most promising solution. It should be
emphasized that the HFW used was collected at municipality level from
240 residences, through the active participation of the citizens. Thus, by
this study an alternative approach of fermentable HFW management is
proposed, which is expected to enhance the quality of citizen's life with
health benefits, whereas preventing environmental degradation and
disruption of the ecosystems.
Regarding the whole process economy, it should be taken into ac-
count that MSW management is primarily a public sector responsibility.
Given though the current economic circumstances in many EU Member
150
125
Cumulative methane
production (mL)
100
75
50
25
0
0 10 20 30 40
ȉime (d)
Fig. 11. Cumulative methane production of the solid fraction obtained after the
optimized DHFW extraction process.
1072
Applied Energy 242 (2019) 1064–1073
States, the establishment of a cost-effective management scheme could
be the only solution to achieve relevant policy goals and save money.
Key components of MSW management are waste collection, transpor-
tation, processing (treatment) and residues disposal. MSW collection
and transportation is the most fuel-intensive step in waste management,
accounting for 40–60% of the total MSW management budget, being
also an environmental concern due to CO2 emissions from diesel com-
bustion [51].
Regarding processing, the present study describes a pilot-scale col-
lection of HFW which is subjected to proper pre-processing (drying and
shredding) where DHFW is produced. Based on Papanikola et al. [52],
the total energy consumption for drying HFW and producing DHFW is
8 MJ/kg DHFW. In the sequel, DHFW water extraction takes place,
where 20 g DHFW are mixed with 100 mL water, meaning that for each
tone of DHFW, 5 m3 of water are needed. At a large scale, this could be
accomplished by the use of a low cost decanter or a leaching bed
bioreactor, packed with low cost materials, where mixing and homo-
genization of DHFW with tap water could be performed. In order to
reduce the quantity of water and process cost, either the use of a higher
DHFW solids loading, producing a more concentrated extract or the
recirculation of part of the water used, could be accomplished.
Comparing the energy recovery from DHFW using the processes
tested in this study, it is concluded that 0.31 MJ/kg TS in the form of
electricity could be obtained from the extract (at 0.64 g COD/L organic
loading, taking into account that the COD recovery yield during ex-
traction was 40%) and 12.01 MJ/kg TS from the solid residue in the
form of biogas (12.32 MJ/kg TS DHFW in total). Through a crude es-
timation, and not taking into consideration the purchase cost (FOB cost)
of the equipment, cost of utilities and the operating labor cost, the
energy recovery of the process is higher than the energy required for
the production of DHFW. In addition, taking into account that the net
calorific value (NCV) of DHFW is 18.09–18.38 MJ/kg [52], which is the
maximum theoretical energy yield of combustion, as well as the en-
vironmental benefits of biochemical processes compared to the ther-
mochemical ones, the proposed scheme of processes could be con-
sidered as a promising alternative for DHFW valorization.
4. Conclusions
The production of electricity and methane from preserved predried
and shredded household food waste (HFW) is a promising strategy for
its valorization. Experiments concerning the production of electricity in
a four-air cathode single chamber microbial fuel cell (MFC) operating
with a synthetic nutrient solution at different hydraulic retention times
(HRTs) showed that the maximum power density was obtained at an
HRT of 18 h (11.8 W/m3). At this HRT, testing of the MFC operation
with diluted dried HFW (DHFW) extract as feed, at different organic
loadings, showed that at the lowest tested substrate concentration
(0.7 g COD/L) the best MFC performance was achieved (power density:
7.7 W/m3) with an energy yield of 0.78 MJ/kg CODin or 0.31 MJ/kg TS.
G. Antonopoulou, et al. Applied Energy 242 (2019) 1064–1073

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