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Journal of Energy Chemistry

http://www.journals.elsevier.com/
journal-of-energy-chemistry/
journal homepage: www.elsevier.com/locate/jechem

Fuel cell performance assessment for closed-loop renewable energy

systems
Q1 Fabio V. Matera, Irene Gatto∗, Assunta Patti, Enza Passalacqua
CNR-ITAE, Institute for Advanced Energy Technologies “N. Giordano”, Via Salita S. Lucia sopra Contesse, 5-98126 Messina, Italy

a r t i c l e i n f o a b s t r a c t

Article history: Fuel cells and electrolysis are promising candidates for future energy production from renewable energy
Received 23 July 2015 sources. Usually, polymer electrolyte fuel cell systems run on hydrogen and air, while the most of elec-
Revised 28 September 2015
trolysis systems vent out oxygen as unused by-product. Replacing air with pure oxygen, fuel cell elec-
Accepted 19 November 2015
trochemical performance, durability and system efficiency can be significantly increased with a further
Available online xxx
overall system simplification and increased reliability. This work, which represents the initial step for
Keywords: pure H2 /O2 polymer electrolyte fuel cell operation in closed-loop systems, focuses on performance vali-
Polymer electrolyte fuel cell (PEFC) dation of a single cell operating with pure H2 /O2 under different relative humidity (RH) levels, reactants
H2 /O2 fuel cell stoichiometry conditions and temperature. As a result of this study, the most convenient and appropri-
Closed-loop fuel cell system ate operative conditions for a polymer electrolyte fuel cell stack integrated in a closed loop system were
selected.
© 2016 Science Press and Dalian Institute of Chemical Physics. All rights reserved.

1 1. Introduction fuel cells, is temporarily stored in the phase-separation tanks (one 25

tank for each gas) and periodically purged to another tank. When 26
2 A typical polymer electrolyte fuel cell (PEFC) combines hydro- the fuel cell is not operative, the water stored in this latter tank 27
3 gen from a tank and oxygen from the air to produce electricity, is then used by an electrolyzer to produce hydrogen and oxygen, 28
4 with water and heat like its byproducts [1]. A regenerative fuel which are stored back in the pressurized vessels to feed again the 29
5 cell also operates the reverse cycle, using the excess electric power fuel cell. Hence, these systems use the stored oxygen, produced 30
6 to split water into hydrogen and oxygen, which are stored and fed from electrolysis process and they are totally hermetic to the 31
7 back to the fuel cell to produce peak power when it needs [2]. In environment, without any mass exchange with the environment. 32
8 the case of electrolysis, the decision to store oxygen or vent it into This aspect can be decisive for the applications whereas there is 33
9 the atmosphere strongly depends on the application. Closed-loop the need to separate the environment from the system (such as 34
10 systems are designed to recirculate the reactants within the fuel submarines, space applications and harsh environments) [3]. The 35
11 cell, without an external purge. This means that the excess hydro- main space agencies are investigating the potential of the fuel cell 36
12 gen at the exit of the anode (or oxygen at the cathode) is fed back technology in different scenarios, mainly for space exploration. 37
13 to the anode (or cathode) inlet, after the removal of liquid phase It seems that fuel cell can be suitable [4], in the medium-term, 38
14 water within a tank. The line pressure, after the reactants have for advanced robotic exploration missions and, in the longer term 39
15 been partially consumed by the reaction, is restored by means of (>2030), for possible human explorations of the Moon and Mars. 40
16 a pressure regulator supplying hydrogen (at the anode) or oxygen Fuel cell technology was already used before [5–11] as power sup- 41
17 (at the cathode). A small twin-head reciprocating compressor ply system for space vehicles; this technology can be also used in 42
18 (one head for each gas) is dedicated to the recirculation of the the life support systems and in-situ resource utilizations systems. 43
19 reactants, the supply of reactants to the fuel cell inlet and water However, the operation conditions of a closed-loop system are 44
20 removal from exhausts. Being the compressor placed at the fuel generally very far from the standard conditions of a PEFC [12,13]. 45
21 cell outlet, the volume to be recirculated at the anode is usually Pure oxygen fuel cell operation results in a higher cell voltage 46
22 within the 10–20% of the stoichiometric flow for the anode, or compared to air operation [1,2]. The gain, due to a higher partial 47
23 within 50–100% at the cathode, respectively. The by-product of pressure of oxygen, is usually higher than that solely predicted by 48
24 the reaction, which is only pure water for hydrogen–oxygen fed the Nernst equation, particularly due to the higher diffusion rates 49
of pure oxygen if compared to the oxygen/nitrogen mixture. In 50

∗
addition, a fuel cell operating with air requires fans or compressors 51
Corresponding author. Tel.: +39 90 624 231; fax: +39 90 624 247.
to feed air through the fuel cell, resulting in additional parasitic 52
E-mail address: irene.gatto@itae.cnr.it (I. Gatto).

http://dx.doi.org/10.1016/j.jechem.2016.01.017
2095-4956/© 2016 Science Press and Dalian Institute of Chemical Physics. All rights reserved.

Please cite this article as: F.V. Matera et al., Fuel cell performance assessment for closed-loop renewable energy systems, Journal of
Energy Chemistry (2016), http://dx.doi.org/10.1016/j.jechem.2016.01.017
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Table 1. Performed test conditions.

Test T (°C) RH (%) P (bar) H2 /O2 (stoichiometry)

1 80 100 3 1.1/1.1
2 80 100 3 1.2/1.2
3 80 100 3 1.2/1.5
4 80 100 3 1.5/1.5
5 80 100 3 1.2/2.0
6 60 100 3 1.2/1.5
7 80 75 3 1.2/1.5
8 60 75 3 1.2/1.5
9 80 50 3 1.2/1.5
10 60 50 3 1.2/1.5

Several conditions were investigated varying the cell temperature 96

from 60 to 80 °C, the reactants stoichiometry between 1.1 and 2.0 97
and the RH between 50% and 100%. In Table 1, all the performed 98

Fig. 1. Single cell and laboratory connection.

tests are summarized. 99
The cell resistance (Rcell ) was measured with an Agilent 100
milliohm meter by a static method at a frequency of 1 kHz. 101
53 losses, meanwhile passive air supply based on natural convection
54 may be only used for very low-power applications usually featured 4. Results and discussion 102
55 from a poor performance. In order to best identify the criticalities,
56 an experimental test campaign has been conducted to finalize the This study was carried out to verify the possible application 103
57 system configuration. So, a standard single cell using commercial of PEFC in a closed-loop system and to individuate the optimal 104
58 components has been connected to a test station and tested in stack operative conditions. In fact, testing conditions were far from 105
59 different conditions of T, P, RH with O2 as an oxidant. This should those of a standard single cell characterization reference, whereas 106
60 lead to identify the critical aspects of the technology to be over- the application is very different from the typical application of 107
61 come in the future development of the fuel cell technologies. The a PEFC system. While useful for qualitative comparisons between 108
62 results of these experiments helped the successive design of the cells, this data are generally not very representative of a stack per- 109
63 fuel cell stack, the fuel cell size developed to provide a nominal formance, which needs further developments, especially on the en- 110
64 power of 300 W with a single cell voltage of 0.65–0.8 V. gineering side [13–18]. 111
When operating in a closed-loop configuration, without any 112
65 2. Experimental external humidification system, the RH at the stack inlet can 113
significantly vary depending from the power output, from 100% 114
66 A commercial MEA, purchased from IRD fuel cells, was used (stand-by or low power operation with a non-zero minimum 115
67 for this investigation. It was selected, among several commercial recirculation flow) to very low values (i.e. 17% at 1,2 stoich. or 116
68 MEAs, after a successful testing in H2 /O2 conditions. IRD-FC MEA is 33% at 1,5 stoich.). This can be calculated considering the fuel cell 117
69 a catalyst coated membrane (CCM) on the reinforced Nafion mem- mass and heat capacity, heat losses along the gas pipeline and the 118
70 brane XL-100. Pt loadings of 0.6 mg/cm2 and 0.3 mg/cm2 , for cath- operation temperature. The gas phase at the anode and cathode 119
71 ode and anode respectively, were used and a carbon felt based on outlet can be assumed to have the fuel cell temperature, because 120
72 a Gas Diffusion Layer (GDL) Sigracet24BC (SGL Group) was applied the fuel cell is maintained at a fixed temperature, either by means 121
73 to the CCM. of electrical heaters (in case of a single cell) or an external cooling 122
circuit (in case of a stack) and the mass of the fuel cell is much 123
74 3. Electrochemical characterization
greater than that of the gas inside the cell. The gas at the fuel cell 124
outlet has the same temperature of the fuel cell and the gas is 125
75 MEAs were tested in a 25 cm2 single cell. The channel flow fully saturated by water (with a significant liquid phase). The gas 126
76 design is a combination between serpentine and parallel channel
coming from the storage vessel has the ambient temperature and 127
77 configurations and it is based on the same design of the fuel cell
its RH can be assumed equal to zero. The temperature and the RH 128
78 stack to be developed. Single cell plates were realized by machin- of the gas resulting from the mixing of the recirculated and the 129
79 ing graphite (XM9612 graphite grade, SGL Carbon) with a thickness
fresh gas from the storage vessel can be calculated from mass and 130
80 of 10 mm and channel dimensions of 1.2 × 1.0 mm. Current collec-
energy balance: 131
81 tors were realized in copper and protected against oxidation inter-
82 posing a flexible graphite sheet between the copper and graphite ṁ1 (g ) · cp (g ) · (1 + α ) · (T1 + T2 ) + ṁ2 (v ) · c p (w ) · T2
83 plates. Single cell tests were performed by a PC-controlled fuel cell = ((ṁ1 (g ) · c p (g ) · (1 + α ) + ṁ2 (v ) · c p (w )) · T3 − ṁ3 (l ) · r
84 test station. A bubble gas humidifying system was used to man-
·
85 age the gases relative humidity (RH) levels varying the humidifier where, mi (g ) is the mass flow of the gas. When i = 1, the gas 132
86 bottles temperature. In Fig. 1, an image of the single cell and the comes from the storage vessel; when i = 2, the gas comes from 133
87 connection to the test station was reported. the recirculation loop; when i = 3, the gas is the sum of gases 134
88 Moreover, Fig. 2 shows a scheme of the Balance of Plant imple- coming from storage vessel and recirculation loop at the fuel cells 135
89 mented for the experimental tests. inlet (kg/s); cp (x ) is the specific heat of the gas (x = g) or the 136
90 The reference working conditions of the cell were based on the water (x = w) (J/kg/K); α is the difference between the actual gas 137
91 following standard conditions of a PEFC: Tcell = 80 °C, PH2/O2 = 3 bar, flow and the stoichiometric value divided by the stoichiometric 138
92 H2 /O2 stoichiometry = variable, and RH = 100%. To simulate a value and it represents the gas utilization factor. α = 0 indicates an 139
93 closed loop system and investigate the most favorable operating actual flow equal to the stoichiometric flow, while 0.5 indicates an 140
94 conditions, single cell I–V polarization curves were carried out at actual flow which is 50% higher than the stoichiometric one (adi- 141
95 PH2 /PO2 = 3.0/3.0 with a fixed stoichiometry for fuel and oxidant. mensional); T is the temperature (°C) of the gas coming from the 142

Please cite this article as: F.V. Matera et al., Fuel cell performance assessment for closed-loop renewable energy systems, Journal of
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Fig. 2. Scheme of simplified BoP for experimental set up.

Fig. 3. Scheme of closed-loop system.

143 storage vessel (i = 1, which is assumed to be the ambient tempera- flow of the condensed liquid phase water, due to the decrease of 149
144 ture), the recirculation loop (i = 2, which is the stack temperature) the temperature T3 below the dew-point in the mixture between 150
145 or the resulting mixture at the fuel cells inlet (i = 3, which is the the gas coming from the storage vessel and the recirculated gas 151
·
146 unknown variable and depends also on condensation phase); m2 (kg/s); r is the latent heat of the water (J/kg). 152
147 (v ) is the mass flow of the vapor phase in the recirculated gas, Considering the testing conditions required to vary the stack 153
· output power from stand-by to full power, RH has been fixed to 154
148 after the removal of the liquid phase (kg/s); m3 (l ) is the mass

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Fig. 4. I–V curves comparison in H2 /air standard conditions and in H2 /O2 .

Table 2. Cell potential at different current densities in different cell conditions.

Conditions Potential (V @250 mA/cm2 ) Potential (V @500 mA/cm2 ) Potential (V @1000 mA/cm2 ) Potential (V @1500 mA/cm2 )

H2 /air 0.800 0.717 0.551 0.153

H2 /O2 0.827 0.761 0.652 0.548

155 an average value of 50% for the single cell testing. Besides, the gas the H2 /O2 is not a constant along the polarization curve, but it in- 184
156 at the stack outlet has a significant amount of liquid water, hence a creases with the increase of current density. 185
157 phase separation tank (Figs. 2 and 3) has been inserted in both the From the voltage values reported in Table 2, at four current 186
158 single cell (to avoid back pressure flooding) and the closed loop density values, it is possible to calculate an improvement of 27 mV 187
159 system (to remove the liquid phase and leave only a fully humidi- up to 101 mV (at 250 and 1000 mA/cm2 , respectively) when the 188
160 fied gas in the recirculation loop). stoichiometry ratio is higher or equal to 1.2/2.0, that drastically in- 189
161 The main differences between a standard and a closed-loop creases (395 mV at 1500 mA/cm2 ) when operating in the diffusion 190
162 PEFC based system are: region of the polarization plot. 191
The real gain is measured at 1 A/cm2 , because, at this current 192
163 • in the closed-loop system pure hydrogen and oxygen are sup- density value, the same gas stoichiometry was obtained; in this 193
164 plied as reactants, instead of air (at the cathode); case, an increment of the performance of about 100 mV working 194
165 • both gases are not humidified before being supplied to the fuel with a pure oxidant was recorded, but it is evident that the fuel 195
166 cell, but the waste humidified reactants are re-circulated, re- cell performance strongly depends on the used gas flows. There- 196
167 sulting in a humidification level usually lower than 100%; fore, the first step of this study was to individuate the more suit- 197
168 • the enhanced performance of a hydrogen–oxygen stack pro- able stoichiometry ratios. 198
169 duces an excess heat that requires an efficient cooling system;
170 therefore it can be more convenient to work at lower current 4.1. Influence of reactant gas stoichiometry 199
171 densities.
This analysis was performed at 100% RH and 80 °C. The hydro- 200
172 In Fig. 3(a), scheme of the closed-loop system was reported. gen stoichiometry was varied from 1.1 to 1.5 and the oxygen stoi- 201
173 At the beginning of the experimental activity, a standard I–V chiometry was varied from 1.2 to 2.0. The electrochemical behavior 202
174 curve, obtained in H2 /air with a variable stoichiometry wherein the is shown in Fig. 5 and the electrochemical parameters, in terms of 203
175 gas flow is calculated to have 1.2/2.0 stoich. for H2 /air at 1.0 A/cm2 , cell resistance and cell voltage at two different current densities, 204
176 has been compared to a I–V curve, obtained in H2 /O2 with a fixed are reported in Table 3. The cell resistance increases by increasing 205
177 stoichiometry (1.2/2.0). The hydrogen–air performance was shown the reactants gas flow, because an excess of gas dries the Nafion 206
178 to give a more complete overview of the changes using oxygen in- ionomer in the catalyst layer and in the membrane. On the con- 207
179 stead of air (dilution effects at the cathode). trary, when the gas flow is too low (1.1/1.1, 1.2/1.2), a depletion of 208
180 This comparison is shown in Fig. 4. The slope of the H2 /O2 reagents produces significant problems in the diffusion region with 209
181 curve is different from the H2 /air one, not only because a pure re- a marked decay of performance. 210
182 actant is used, but also for the constant stoichiometry that ensures As result of this analysis, a gas flow stoichiometry of 1.2 for hy- 211
183 the same gas utilization at each current value. In fact, the gain in drogen and 1.5 and 2.0 for oxygen was selected taking into account 212

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Fig. 5. Influence of reactant gas stoichiometry at 80 °C 100% RH.

Fig. 6. Influence of RH% at 80 °C and 1.2/1.5 stoichiometry.

Table 3. Electrochemical data at different O2 stoichiometry.

Condition (H2 /O2 stoich.) Rcell ( cm2 ) Voltage (V @250 mA/cm2 ) Voltage (V @500 mA/cm2 )

1.1/1.1 0.142 0.670 0

1.2/1.2 0.145 0.853 0.739
1.2/1.5 0.147 0.850 0.779
1.5/1.5 0.145 0.845 0.637
1.2/2.0 0.152 0.827 0.761

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Fig. 7. Influence of RH% at 80 °C and 1.2/2.0 stoichiometry.

Table 4. Electrochemical data at different RH%.

Condition (H2 /O2 stoich.) RH (%) Rcell ( cm2 ) Voltage (V @250 mA/cm2 ) Voltage (V @500 mA/cm2 )

1.2/1.5 100 0.147 0.850 0.779

1.2/1.5 75 0.187 0.774 0.636
1.2/1.5 50 0.240 0.677 0.374
1.2/2.0 100 0.152 0.827 0.761
1.2/2.0 75 0.225 0.775 0.663
1.2/2.0 50 0.267 0.703 0.520

Fig. 8. Influence of T and gas flow stoichiometry at 50% RH.

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Fig. 9. Cell voltage behavior as a function of RH% at different O2 flows and cell temperatures.

213 the obtained performance in the region of potential interest (0.65– (Fig. 9), it is evident that, the performance at 80 °C linearly de- 247
214 0.8 V). creases with the relative humidity decrease, while no significant 248
change in the performance with RH < 75% was observed at 60 °C, 249

215 4.2. Influence of RH% assuring a less sensitivity to humidity of the fuel cell. 250
The oxidant flow has a little influence in these conditions, be- 251

216 The influence of relative humidity was investigated using the cause a lower cell temperature mitigates the negative effect of low 252

217 previous selected gas flows. Polarization curves were recorded humidity, therefore a stoichiometry of 1.2/1.5 seems to be reason- 253

218 varying the relative humidity at both sides of the cell. Figs. 6 and able to ensure a more controlled dehydration of the membrane. 254

219 7 show a comparison of I–V curves recorded at different RH% for Moreover a cell temperature of 60 °C with a RH = 50% is a good 255

220 an oxidant stoichiometry of 1.5 and 2.0, respectively. It is evident compromise between application requirements, performance and 256

221 that a RH decrease causes a decay of performance for both the ox- durability. The results of this study have oriented the development 257

222 idant gas stoichiometries. From the electrochemical data reported of a H2 /O2 stack for a closed loop system with a 700 W of Nominal 258

223 in Table 4, it is possible to notice that a higher flow (2.0) in- Power finalized to space applications. 259

224 creases the cell resistance; this effect is mainly due to the Ohmic
225 losses derived from the membrane dehydration with a consequent 5. Conclusions 260
226 decrease in proton conductivity. Nevertheless, at high flow, the
227 performance at low humidity improves; in fact, reducing humid- This work represents the initial step for pure H2 /O2 fuel cell op- 261
228 ity from RH = 100% to RH = 50%, losses in cell potential of about eration in closed-loop systems. An investigation on the influence 262
229 15% and 32% (at 250 mA/cm2 and 500 mA/cm2 , respectively) were of reactant gases stoichiometry, relative humidity and cell temper- 263
230 recorded for oxygen stoichiometry = 2.0 against a loss of about 21% ature was carried out. A gases utilization of 1.2/1.5 for fuel and 264
231 and 52% at the same current density value for oxygen stoichiome- oxidant, respectively, was found to be as a good compromise for 265
232 try = 1.5. closed-loop operation. As expected, a performance reduction was 266
233 As low humidity operation is a design parameter for a closed- observed decreasing the relative humidity of the reactant gases 267
234 loop system, the study was focused at RH = 50%. Under this condi- from 100%RH to 50%. This behavior was confirmed both at 80 °C 268
235 tion, the influence of temperature was investigated with the aim of and 60 °C as cell temperatures. Furthermore, this trend is more ev- 269
236 decreasing the cell temperature and improving the cooling system ident at high current density. For this reason, it is necessary to se- 270
237 efficiency. lect the most appropriate operative conditions as a function of a 271
real application of the system. 272

238 4.3. Influence of temperature

References 273

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