Journal of Power Sources 414 (2019) 366–376

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Journal of Power Sources

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Development and use of a mixed-reactant fuel cell T

a b,∗ a a a
Piotr Forysinski , Colin Oloman , Sona Kazemi , Tirdad Nickchi , Ashwin Usgaocar
a
Mantra Energy Alternatives Ltd, #202 3590 W. 41st Avenue, Vancouver, B.C, V6N 3E6, Canada
b
0798465BC Ltd, 3176 W.36th Avenue, Vancouver, B.C, V6N 2R5, Canada

HIGHLIGHTS GRAPHICAL ABSTRACT

• Acellformate/oxygen mixed-reactant fuel

with superficial power density to
4000 W m−2.
• A 19 cell formate/oxygen mixed-re-
actant fuel cell stack with power
output to 120 W.
• A 250 W electric scooter powered by
formate/oxygen mixed-reactant fuel
cells.

ARTICLE INFO ABSTRACT

Keywords: Mixed-reactant fuel cells are unconventional electrochemical power sources which use a thermodynamically
Mixed-reactant unstable mixture of fuel and oxidant. In the work described here a 2-phase mixture of alkaline potassium formate
Fuel cell (liquid)/oxygen(gas) is the fuel/oxidant combination used in the “flow-by” mode with mixed-reactant fuel cells,
Formate developed in the laboratory from a 10E-4 m2 single cell to a bipolar stack of nineteen 35E-4 m2 cells. With Pd/Ag
Electric scooter
anode/cathode catalysts, operating at 500 kPa(abs), 80 °C the single cell with a Pd load of 0.054 kg m−2 reaches
a superficial power density of 4,000 W m−2 at 10,000 A m−2. Tests of the 19 cell stack with a Pd load of
0.036 kg m−2 at 300 kPa(abs), 60 °C give power output up to 120 W, with a corresponding volumetric power
density about 400 kW m−3. To demonstrate the fuel cell performance three nominally 100 W 19 cell stacks are
wired in parallel to a 250 W electric motor to drive a modified electric scooter, with on-board fuel, oxidant and
an adult passenger, for about 15 minutes at 10 km h−1. To our knowledge this is the first time mixed-reactant
fuel cells have been used alone to power a vehicle.

1. Introduction conventional separate-reactant paradigm by combining the fuel and

The mixed-reactant fuel cell (MRFC) is an unconventional, though
not novel, electrochemical device. With conventional fuel cells the fuel
and oxidant are delivered separately to the reactor (i.e. fuel cell) and are
kept apart within each half-cell by ion exchange membranes that pass
ionic current and suppress “cross-over” of the reactants. This separation
is necessary to prevent both thermochemical reactions between the fuel
and oxidant and electrochemical reactions of each on their respective
counter-electrodes. Mixed-reactant fuel cells break from the
oxidant to enter and pass through the reactor in a single mixed stream.
Although such a fuel/oxidant mixture is thermodynamically unstable, a
mixed-reactant fuel cell can function if thermochemical reactions be-
tween fuel and oxidant are slow and the electrodes are selective against
their counter-electrode reactions. That desirable selectivity can be ap-
proached by chemical and/or physical means. The chemical approach
involves selective electrocatalysts and the physical method requires
suppressing transport of reactants to their counter-electrodes. Both
methods may be used together but neither is fully effective, with the

Corresponding author.
∗

E-mail addresses: pforysinski@yahoo.com (P. Forysinski), coloman@intergate.ca (C. Oloman), sona.kazemi@gmail.com (S. Kazemi),
tirdadn@gmail.com (T. Nickchi), ashwin.usgaocar@gmail.com (A. Usgaocar).

https://doi.org/10.1016/j.jpowsour.2018.12.081
Received 28 July 2018; Received in revised form 22 December 2018; Accepted 28 December 2018
Available online 16 January 2019
0378-7753/ © 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/BY/4.0/).
P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

Nomenclature L distance, pore length (m)

n electron stoichiometry coefficient (-)
a specific surface of three-dimensional electrode (m−1) ΔP capillary pressure (Pa)
Bo Bond number (-) R electrolyte effective ionic resistivity in 3D electrode
Ca Capillary number (-) (Ohm.m)
Cb bulk reactant concentration (mol m−3) R* inter-electrode ionic area resistance (Ohm.m2)
d characteristic dimension (m) r pore radius (m)
Ecell full-cell operating voltage (V) T temperature (K)
Eo,y,c reversible potential for reaction y on the nominal cathode t time (s)
(V SHE) V velocity (m s−1)
Eo,y,a reversible potential for reaction y on the nominal anode (V ΔV voltage drop across three-dimensional electrode (V)
SHE) dL/dt rate of liquid penetration (m s−1)
Eo standard equilibrium electrode potential at 298 K (V SHE) η y,c overpotential for reaction y on the nominal cathode (a
Eo Nernst equilibrium electrode potential at T (V SHE) negative value) (V)
F Faraday number (C mole−1) η,y,a overpotential for reaction y on the nominal anode (a po-
g gravitational acceleration (m s−2) sitive value) (V)
Hin enthalpy of feed stream w.r.t. elements at 25 °C (W) ϴ contact angle (radian)
Hout enthalpy of product stream w.r.t. elements at 25 °C (W) μ liquid viscosity (kg m−1 s−1)
I total current (A) ρ density difference between phases (kg m−3)
i net superficial current density (A m−2) σ surface tension of liquid (N m−1)
iL mass transfer limited superficial current density (A m−2) τ effective electro-active thickness of 3D electrode under
jL mass transfer limited real current density (specific ac- mass transfer control (m)
tivity) (A m−2) ECSA electrochemical surface area (m2 g−1 catalyst)
K mass transfer coefficient (m s−1) 3D three-dimensional (-)

result that one or both electrodes present a mixed-potential that lowers
the voltage and energy efficiency of the fuel cell. In practical applica-
tions this loss of fuel cell performance may be compensated by reduced
complexity, size, weight and cost of mixed-reactant vs. separate-re-
actant systems.
Under alternative names such as “membrane-less”, “single-
chamber” and “separator-free” fuel cells the simple configuration of
MRFCs has inspired many investigations into their performance and
applications, as summarized in published reviews [1,2] and illustrated
in Table 1. The examples in Table 1 include fuel/oxidant mixtures
ranging from H2/O2 to CH3OH/H2O2 and CH3OH/Fe+3, with catalyst
such as Pt, Pd, Au, Ag, RuSe, Os and FeCo, operating at temperatures

Table 1
Notable MRFC results.
Reactants Electrodes Conditions Peak performance Separator Reference

Fuel Oxidant Anode Cathode Pressure Temp Current Power

−2
kPa (abs) °C Am W m−2

Various mixed-reactant systems

H2 O2 Pt/C Ag/C 102 60 150 140 PE Grueneberg [3]
H2 O2 Pt Pt 340 NS 30 290 PB Dyer [5]
CH3OH O2 PtRu/C RuSe/C 100 90 2,000 450 PM Priestnall [6]
CH3OH O2 PtRu/C PtFe/C NS 90 4,500 1,600 Nafion Shukla [7]
C2H5OH O2 PtRu/C Pt/C 100 26 700 100 PP Zeng [8]
CH3OH Fe+3 PtRu/C C NS 90 1,000 300 Nafion Ilicic [9]
NaBH4 O2 Os/C Roll Ag/C roll 105 50 4,500 1,900 PP Aziznia [10]
CH4 O2.He Ni BSCF 100 796 19,000 7,500 SDC Hao [11]
H2 O2 Pt Pt NS NS 170 38 None Hashemi [13]
Sucrose Air Microbe/C C NS NS 0.73 0.30 None Ahmed [14]
Formate separate-reactant systems
KHCO2+KOH O2 Pd PdPt 100 90 1,000 900 (OF) Asbestos Grimes [15]
KHCO2 O2 Pd Pt NS 50 4,000 1,100 AEM Nguyen [19]
H2CO2 O2 PtRu RuSe 100 90 1,300 310 Nafion Cheng [20]
KHCO2+KOH O2 Pd/C Pt/C NS 60 6,000 3,000 AEM Tran [22]
KHCO2+KOH O2 Pd/C FeCo/C NS 80 8,000 2,500 AEM Zheng [23]
KHCO2+KOH O2 PdCeO2 FeCo/C NS 60 4,500 2,500 AEM Miller [24]
NaHCO2 H2O2 Pd Pt NS 60 8,000 5,900 Nafion Li [25]
Formate mixed-reactant systems
KHCO2+KOH O2 Pd/C Pt/C 300 50 1,700 700 None Yu [26]
NaHCO2+NaOH O2 Pd/Ni Ag/C 130 60 2,400 1,200 PP Oloman [28]
NaHCO2+NaOH NaClO Pd Au NS 20 1,400 520 None Kjeang [29]

NS = not specified, presumably ambient conditions.

SCSOFC = single chamber solid oxide fuel cell PP = hydrophilic microporous polypropylene Asb = asbestos.
AEM = anion exchange membrane OF = Ohmic free LFFC = laminar flow fuel cell SDC = samaria-doped ceria.
PM = porous membrane PE = porous polyethylene PB = pseudoboehmite
The majority of the tests in Table 1 used aqueous electrolytes in single cells of area less than 10E-4 m2 (10 cm2), with no record of fuel or oxidant conversion
(utilization).

367
P. Forysinski et al.
below 100 °C and generating superficial power densities up to about
2,000 W m−2 [3–10]. Single-chamber solid oxide fuel cells (SCSOFC)
operating above 600 °C have delivered superficial power densities up to
7,500 W m−2 [11]. Partial reaction selectivity in these fuel cells was
obtained by manipulating the intrinsic kinetics, hydrophobicity and
conditions in the electrodes, giving open-circuit potentials up to about
90% of values in the corresponding separate-reactant fuel cells. In
mixed-reactant systems the fuel and oxidant may be delivered in flow-
through or flow-by mode as a single or multiphase mixture to one or
both electrodes (anode & cathode). A separator such as an ion-exchange
membrane, porous diaphragm or plastic screen is typically installed to
prevent electronic contact between anode and cathode. Laminar flow
fuel cells (LFFC), where fuel and oxidant are separated in space by
microfluidic flow phenomena, and single-chamber microbial fuel cells
are technically not mixed-reactant systems but are included in Table 1
as membraneless devices [12–14].
Formic acid and alkali formate salts have been recognized for many
decades as electrochemical fuels in both batteries and fuel cells [15,16].
More recently the search for carbon-neutral energy systems has sti-
mulated work on direct formate fuel cells (DFFCs) in association with
the electroreduction of CO2 [17,18]. The DFFC fuels typically contain
1–4 M KHCO2 with 1–4 M KOH. Notably, the formate electro-oxidation
kinetics depend on pH (9–14), so operation without KOH roughly
halves the peak superficial power density, as does replacing O2 by air
[19].
Separate-reactant single-cell DFFCs with anion membranes operated
at ambient pressure and 60 °C have achieved superficial power densities
about 3,000 W m−2 with oxygen and 5,900 W m−2 with hydrogen
peroxide as the oxidant [18,20–25]. Mixed-reactant DFFCs have had
less attention, although recent work on a membraneless DFFC with a
fuel/oxidant mix of [KHCO2+KOH]/O2 at 300 kPa(abs), 50 °C de-
monstrated superficial power densities around 900 W m−2 at 1,700
A m−2 [26,27]. Earlier, a DFFC was operated with fluid flow orthogonal
to current as a “mixed-reactant flow-by fuel cell” (MRFBFC) with a fuel/
oxidant mix of [2M NaHCO2+2M NaOH]/O2 at 130 kPa(abs), 60 °C to
generate a superficial power density of 1,200 W m−2 at 2,400 A m−2
[28]. Formate has also been tested as fuel in LFFCs fed with separate
solutions of formate and an oxidant. For example, fuel and oxidant of
Fig. 1. Section of a single cell unit in a MRFBFC (not to scale).
368
Journal of Power Sources 414 (2019) 366–376
respectively [1.2M NaHCO2 + 1.6M NaOH] and [0.7 M
NaHClO + 1.6 M NaOH] in a LFFC showed an open circuit voltage of
1.4 V and delivered a superficial power density of 520 W m−2 under
ambient conditions [29].
The present paper records a pioneering development of mixed-re-
actant flow-by fuel cell stacks and their use to power an electric scooter.
Based on principles of electrochemistry and fluid dynamics the 18
month project proceeded in three overlapping phases:
i. Conception, fabrication and testing of single cell MRFBFCs with
fuel/oxidant mixtures of [alkaline potassium formate/oxygen gas],
ultimately delivering superficial power densities up to
4,000 W m−2.
ii. An unprecedented scale-up and assembly of 19 cell 100 W bipolar
MRFBFC “filter press” stacks.
iii. Use of the MRFBFC stacks to drive an electric scooter with a nom-
inal power of 300 W.
2. Guiding principles
The mixed-reactant flow-by fuel cell (MRFBFC) has novel features
not encountered in conventional “separate-reactant” fuel cells. The
paradigm change required for the development and practical applica-
tion of the MRFBFC was guided by the principles outlined below in
reference to Fig. 1.
Fig. 1 shows a conceptual cross-section of a single fuel cell unit used
in this work. In a bipolar stack the anode and cathode current feeders
are replaced respectively by the adjacent cathode and anode in the
series. This figure indicates a vertical orientation but the fluid flow
regime is such that with proper attention to end effects the unit can
operate in any disposition with respect to gravity. Further, both the
hydraulic and electric connections between multiple cells can be in
series or in parallel. In the work reported here vertical cells were con-
nected hydraulically in parallel and electrically in series (i.e. bipolar).
All components of the fuel cell, except the separator, are electronically
conductive with desirable low contact resistances.
P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

2.1. Electrochemistry effects may be examined in terms of the values set out in Table 3.

The electrode reactions for the formate/oxygen system used in the Bo = gd2/ Bond number (2)
present work are summarized in Table 2. Ca = µV/ Capillary number (3)
Since both reactants can be present in the anode and the cathode the p = 2 cos /r Laplace Capillary pressure (4)
electrodes set up mixed-potentials whose values depend on the re- dL/dt = r cos /(4µL) Washburn Liquid penetration rate (5)
spective competitive reaction rates. Conceptually the interaction be-
tween intrinsic kinetics and mass transport biases the mixed-potentials Values of the Bond and Capillary numbers show that capillary forces
at the electrodes to favour formate oxidation at the anode (rxn 1) and are more significant than gravity in all components, while being com-
oxygen reduction at the cathode (rxn 2). The primary anode reaction 1 parable to viscous drag in the distributor and dominating in the anode,
consumes 1 mole of HCO2− and 2 moles of OH−, supplying 2 Faradays cathode and separator. The capillary pressures indicate that, under
of charge to the primary cathode reaction 2 which consumes 0.5 mole static conditions, aqueous electrolyte solutions fully wet the porous Pd
O2 and generates 2 moles OH−. In this simplified scenario the OH− anode, are strongly rejected by the hydrophobic surface layer of the
consumed at the anode is balanced by that transferred through the cathode and are absorbed in the separator which then presents sub-
separator from the adjacent cathode to give a full-cell equilibrium po- stantial resistance to penetration by gas. However, reactant contact
tential of 1.22 V at 25 °C (rxn 3) with zero net consumption of H2O. In with the electrodes under dynamic conditions in an operating fuel cell
practice the mixed-potentials lower the open-circuit voltage to a degree is more complex and depends on the two-phase flow regime in the
depending on the effectiveness of the electrodes, while excess hydro- distributor coupled to the rates of fluid penetration to the electro-active
xide tends to raise the cell voltage by converting HCO3− to CO3−with zones of the electrodes. Electrolyte solution can move rapidly into the
the resulting overall cell reaction 4. The simple stoichiometry of Table 2 anode and out of the cathode by capillary effects but this desirable
belies complex processes in which the rates of transport of formate, condition can be upset by excessive gas flux and pressure gradient in
hydroxide and oxygen into the electrodes and across the separator the distributor, which displaces liquid fuel from the anode and/or
would control the electrode potentials and/or kinetics [19,30]. drives it into the cathode.
Intrinsic selectivity of the respective anode and cathode reactions 1
and 2 is desirable but not necessary here [31]. Both electrode reactions
can occur on the nominal anode and nominal cathode. In the mixed 2.3. Fluid distribution and cell performance
formate/oxygen system these reactions are each intrinsically fast on
palladium with specific activities about 30 A m−2 Pd at 25 °C [32–34]. Apart from providing a flow path for the reactants the distributors
Reactions 1 and 2 are respectively intrinsically fast (50 A m−2 Ag) and function to provide an ionically insulated electronic connection be-
relatively slow on silver [35,36]. However reaction 2 is suppressed on tween bipolar cells. Ionic insulation is critical for bipolar operation and
the nominal anode (Pd) by the constraint on oxygen mass transfer is approached with a gas-continuous 2-phase flow regime through the
through the wetted porous hydrophilic electrode, while transport of distributor, which prevents liquid ionic paths forming between opposed
fuel to the bulk cathode (Ag) is prevented by an electronically con- electrodes. The 2 mm thick expanded metal distributor mesh presents a
ductive porous hydrophobic layer between the cathode and fluid dis- “microchannel” flow path for the liquid/gas mixture with an effective
tributor. Fuel solution can penetrate the hydrophilic micro-porous se- hydraulic diameter about 1 mm. Although many factors, such as the
parator to reach the face of the cathode which is intrinsically selective feed mixer geometry, interfacial tensions and liquid/solid contact an-
for reaction 2 over reaction 1. An ion membrane separator would be gles affect fluid dynamics in the distributor the 2-phase flow regimes
needed here if the cathode did not intrinsically favour reaction 2. called “churn”, “slug-annular” and/or “annular” may be expected in the
This configuration can be modeled as a continuous plug-flow elec- present situation, where gas/liquid superficial velocity ratios range
trochemical reactor, using four simultaneous non-linear voltage bal- from about 10 to 50 [40]. In any case proper operation of the MRFBFC
ances, one for each anode-cathode couple [30]. stack requires careful attention to the disposition of the feed nozzle(s)
Ecell = Eoc,y – Eoa,y + ηc,y – ηa,y – iR* (1) and distribution of fluids over the bipolar cells.
When capillary and fluid dynamic effects in the MRFBFC bring re-
[N.B. All quantities are defined in the Nomenclature] actants to their respective electrodes the performance of the fuel cell
will depend on behaviour in the three-dimensional (3D) electrodes.
Since the reactor design does not allow cooling a model should in-
With fast intrinsic kinetics [31–35], an anode specific surface of about
clude coupled material and energy balances to follow the reactant
4,000 m−1, cathode ECSA ≈ 50 m2g-1 Ag, 1 M formate, oxygen at
conversion and temperature through the cells under adiabatic condi-
300 kPa(abs) and ΔV = 0.1 V the mass transfer limiting anode and
tions. In practise such a model would engage three-dimensional elec-
cathode superficial current densities at 25 °C, estimated from equations
trodes and involve the numerical solution of coupled partial differential
(6)–(8) are respectively about 8,000 and 10,000 A m−2. These values
equations [37] with many parameters of unknown value. That complex
would change with temperature as it affects practically every property
analysis is beyond the scope of the present work but useful information
and parameter in an operating MRFBFC.
for design of the MRFBFC can be found in simple equations associated
with interfacial phenomena [38] and electrochemical engineering [39].
Table 2
2.2. Capillarity Stoichiometry in the alkaline formate/oxygen MRFBFC.
Rxn Stoichiometry Eo, 298 K, dEo/dT
Capillary phenomena are exploited in the MRFBFC to suppress the pH = 14
transfer of fuel and oxidant to their respective counter-electrodes and to
V SHE V K−1
prevent ionic short circuits between bipolar cells. Two-phase flow of the
fuel/oxidant mixture through the fluid distributors delivers both fuel 1 Anode HCO3− +H2O + 2e− ← HCO2− + −0.82 -2E-4
(liquid) and oxidant (gas) to the exposed “outside” surfaces of the 2OH−
anode and the cathode. Access of the reactants to the “inside” electro- 2 Cathode 1/2O2 + H2O + 2e− → 2OH− +0.40 -1E-3
3 Overall HCO2− + 1/2O2 → HCO3− +1.22 -5E-4
active fields of the 3D electrodes is determined primarily by the ca-
4 Overall HCO2− + OH− + 1/2O2 → +1.33 (excs -8E-4
pillary pressures, rates of fluid penetration in the porous electrodes [38] CO3−- + H2O OH−)
and the distributor flow regime. The significance of these capillary

369
P. Forysinski et al.
Table 3
Capillary effects in porous media with aqueous solutions vs. oxygen gas – see Table 4.
Item Material Thickness Porosity
MRFBFC m %
Distributor Ni mesh 2E-3 90
Anode Pd/Ni foam 7E-4 94
Cathode PTFE/C/Ag 5E-4 NA
Separator PP micropore 2E-4 70
jL = nFKCb mass transfer limiting real current density
= (2 V/aRjL )0.5 effective electro
active thickness in 3D electrode
iL = jL a mass transfer limited superficial current density (8)
2.4. Temperature
The effect of temperature on performance is particularly significant
in a bipolar mixed-reactant fuel cell stack. With no provision for in-
ternal cooling a bipolar stack operates under nearly adiabatic condi-
tions in which stack performance depends on complex interactions
among several variables. This situation is illustrated in Fig. 2 by the
relation between temperature, current density and reactant conversion
estimated from a material balance coupled with an energy balance in an
idealised adiabatic process at steady state.
0 = Hin H out IEcell adiabatic energy balance (9)
The intuitive understanding of fuel cell performance is made diffi-
cult here by the many interacting factors affecting the non-linear
system.
Power density in the MRBFFC typically increases with the tem-
perature, which is determined primarily by Joule heating versus the
sensible plus latent heats exchanged with the flowing fluids, and is
limited by the durability of reactor materials. Depending on the elec-
trolyte composition, oxidant gas flow and pressure, at temperatures
above 80 °C the endothermic latent heat of vaporization of water con-
tributes a large “cooling” affect in the energy balance, which predicts
temperatures approaching 130 °C in 4 M electrolytes under 300 kPa
(abs) at 12,000 A m−2. With robust reactor materials such high tem-
peratures may substantially improve the MRFBFC performance relative
to that recorded in the present work where the temperature is limited to
80 °C.
The principles outlined above were used to guide the experimental
work described below.
3. Experimental methods
The reactor design, component materials, reactants and operating
conditions initially chosen for this project were derived from prior work
with flat “filter-press” and cylindrical Swiss-roll MRFBFCs [28,41].
Fig. 3 is a flowsheet for the laboratory set-up of a vertically oriented
bipolar MRFBFC with a spray feed and Table 4 lists the components of a
100 W (nominal) 19 cell bipolar stack developed in this work. All
components of Table 4 were used as received, except the anodes which
were prepared in-house by electro-less deposition of palladium from
palladium chloride on compressed nickel foam, in an aqueous acid
solution with formaldehyde as a reducing agent. The apparatus of Fig. 3
was used to test a variety of MRFBFC manifestations, from single cells
and 3 cell stacks with 25 mm by 40 mm (10E-4 m2) electrodes, up to the
19 cell unit of Table 4 which was installed in the modified scooter de-
scribed below. The fuel cells and electric scooter were designed and
assembled in the Vancouver B.C. laboratory of Mantra Energy Alter-
natives Ltd. and the vehicle, named the “Spark”, was tested with an
adult rider on a horizontal pathway.
Journal of Power Sources 414 (2019) 366–376
Pore Bo Ca ΔP dL/dt
diam m - - Pa m s−1
5E-3 1.3E-1 1.0E-3 5.4E1 0.19
1E-4 1.3E-3 3.0E-5 3.1E3 5.4
NA 1.3E-3 3.0E-5 −1.1E3 −1.9
1E-5 1.3E-5 3.0E-6 3.1E4 0.27
(6) In all tests the fuel cells were oriented vertically and suspended by
(7) nickel rods inside a cylinder fabricated initially from 4 inch clear PVC
and later 4 inch stainless steel pipe, with an outlet throttle valve for
pressure control. A 3D-printed shroud in ABS plastic was used to pre-
vent the fuel/oxidant mixture from bypassing the stack. In tests with a
single cell the liquid fuel was dripped from a manifold to the top of the
cell while the multi-cell stacks were fed by a conical spray misting
nozzle [42], as in Fig. 3. The MRFBFC stack has no provision for cooling
except via sensible heat, heat of vaporization of the 2-phase reactant
stream and heat transfer through the container wall.
In laboratory operation the liquid fuel was fed from a calibrated
peristaltic pump, whereas for the scooter (described below) the fuel was
driven from the fuel tank by compressed oxygen. Oxygen gas was de-
livered either through the spray nozzle or at the top of the vessel ad-
jacent to the fuel in the case that separate liquid and gas feeds were
required for individual flow control.
The two-phase fuel/oxidant mixture flowed downward through the
fuel cell to be discharged from the bottom of the containment vessel
into a phase separator which also served to hold the spent fuel. Exhaust
gas was passed through a de-misting filter and released. The internal
pressure and temperature were measured respectively by a Bourdon
gauge and by a thermocouple attached to one nickel end-plate. A load
bank (BK Precision 8514) was used in the laboratory to record the
MRFBFC polarisation curves for a variety of operating conditions. Apart
from the MRFBFC stack only nickel, stainless steel 304, ABS, PVC,
polypropylene, epoxy resin, EPDM and Teflon were used in this
equipment.
The fuel and oxidant used in the tests recorded here were respec-
tively an aqueous solution of [2M NaHCO2 or KHCO2 + 2 M NaOH or
KOH] and [99 vol % O2 gas], with flow rates of approximately
0.01–0.2 L min−1 and 0.4–5 SL min−1 respectively, per vessel. Pressure
in the containment vessel was manually controlled up to 500 kPa(abs),
with temperatures up to 80 °C. For some laboratory tests the fuel was
recycled and/or preheated, whereas operation of the scooter involved a
Fig. 2. Estimated adiabatic temperature in an operating MRFBFC stack.
Conditions: MRFBFC bipolar stack, 19 cells each 35E-4 m2 (35 cm2), fuel [2M
KHCO2+2M KOH]aq varied flow, oxidant O2(g) 5 SL min−1, pressure 300 kPa
(abs), feed temperature 25 °C. Power out 90–190 W.
370
P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

Fig. 3. MRFBFC laboratory test flowsheet.

single pass of both fuel and oxidant. 4. Results and discussion

After the experimental development, assembly and testing phase
outlined above three of the nominally 100 W 19 cell MRFBFC cell stacks
described in Table 4 were fixed with spray nozzles into separate 0.15 m
high containment vessels fabricated from flanged 4 inch Schedule 40
PVC pipe and assembled in the power train of a modified scooter. The
three stacks were wired in parallel to a VFK 400W DC-DC voltage
booster connected to the scooter's 24 V DC motor, with a throttle con-
trol plus a selection of thermistors in series to reduce start-up load. The
voltage booster's output and input ratings, respectively 17 A at 24 V and
10 V, limited the output power to ca. 400 W and prevented fuel cell
draw-down by an excessive load. The scooter was subsequently tested
on a level path with a single adult rider.
Figs. 4 and 5 are respectively a flowsheet and schematic diagram of
this novel electric scooter and its main features are summarized in
Table 5.
The electrochemical and capillary features outlined in Section 2
combine in practise with physical factors such as those listed in Table 6
to determine the performance of the MRFBFC.
Fig. 6 shows an initial polarization curve from a single cell MRFBFC
obtained in the stainless steel containment vessel near the end of the
experimental program. Most of the design and operational problems
had been resolved at this stage of the work in experimental runs up to
2 h. The data of Fig. 6 and of several similar runs show an open-circuit
potential about 0.9 V/cell, versus the standard thermodynamic value of
1.22 V, and a mass transfer limited superficial current density appar-
ently exceeding 14,000 A m−2 (1,400 mA cm−2). The linear feature of
Fig. 6 reflects the fuel cell kinetic regime complimented by nearly
adiabatic conditions which drive a positive feedback, where a rising
current density provokes Joule heating that increases the local

Table 4
Components of a nominal 100 W MRFBFC stack.
Item Material Dimensions Porosity/pore size Catalyst Source

-2
H x L x T mm %/mm kgm

Anodes Pd on Ni foam 70 x 50 x 0.7 94/0.1 approx. 0.036 In-house

Cathodes Ag/C/Ni/PTFE GDE 70 x 50 x 0.5 NA NA Oxag, Gaskatel GmbH
Separators Polypropylene 75 x 60 x 0.2 70/NA approx. Zero Viledon® Freudenburg Non-Wovens
Distributors Expanded Ni mesh 70 x 50 x 2.0 90/5 approx. Zero Dexmet Corp.
Single cell As above 70 x 50 x 4.0 – As above As above
End plates Nickel 200 70 x 50 x 1.5 Zero Zero McMaster-Carr
Stack 19 cells, bipolar 70 x 50 x 70 As above As above In-house
Spray nozzle Stainless steel Orifice diameter 0.25 mm Stainless filter with ABS plastic retainer Zero McMaster-Carr

H height, L length, T thickness. NA = not available. Active superficial area per cell = 35E-4 m2 (35 cm2).
Bolted nickel end plates served as the anode and cathode current collectors.

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P. Forysinski et al.
Fig. 4. Electric scooter flowsheet.
temperature of the reactant mixture. The strong effect of temperature is
recorded in Fig. 7, which shows the superficial power density at 3,500
A m−2 increasing from about 1,200 W m−2 to 2,200 W m−2 as the
temperature rises from 23 to 60 °C, with a peak power density ex-
ceeding 3,500 W m−2 at 80 °C. With the “extra Pd” loading on the
anode (0.054 kg m−2) at 80 °C the results of Figs. 6 and 7 show the
possibility of obtaining superficial current and power densities from the
MRFBFC respectively exceeding 10,000 A m−2 and 4,000 W m−2
(1,000 mA cm−2 and 400 mW cm−2). The high catalyst loads recorded
in Figs. 6 and 7 (0.036–0.054 kg Pd m−2) result from a few months of
trial and error experimentation with a simple electro-less deposition
process. No attempt was made to optimize the anodes with respect to
the interacting effects of Pd load, thickness, pore size and porosity that
determine its performance. Further work with the catalyst support and
morphology may be expected to give a substantial reduction in Pd load
on the anode [32].
The full power parabolas were not recorded in many of the tests due
to limitations in the load bank and/or internal shorts from “burn-out” of
the polypropylene separators above 80 °C, along with time constraints
that made testing beyond peak power a low priority.
In Figs. 6 and 7 and the discussion below the performance metrics
are estimated as:
Superficial current density = [Current] / [Superficial anode area per
cell]
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Journal of Power Sources 414 (2019) 366–376
Superficial power density = [Current][Stack voltage] / {[Superficial
anode area per cell][Number of cells in stack]}
Volumetric power density = [Current][Stack voltage] / [Stack volume,
excluding end plates]
With superficial power density up to about 4,000 W m−2
(400 mW cm−2) at 10,000 A m−2 (1,000 mA cm−2) the single cell re-
sults of Figs. 6 and 7 compare favorably with previously published
values for both conventional separate-reactant fuel cells fuelled with
alkaline formate [18,23] and with mixed-reactant fuel cells using var-
ious fuels [1]. Based on a stack alone, the single cell MRFBFC peak
volumetric power density in Fig. 7 (60 °C, extra Pd) extrapolates to
about 950 kW m−3 (950 W L−1) which approaches that obtained from
contemporary PEM hydrogen/air fuel cells, albeit with a high catalyst
load and oxidant of 99 vol% oxygen at 300 kPa(abs). Tests with the
actual 19 cell stack of Table 4 at 80 °C with fuel and oxidant flows re-
spectively 150 ml min−1 and 5 SL min−1 give a peak power of about
120 W, corresponding to a volumetric power density of 400 kW m−3
(400 W L−1), with an internal resistance from about 20 to 200 mi-
croOhm m2. The lower stack power is probably due to inter-cell mis-
matches such as those caused by a non-uniform distribution of reactants
between cells, with consequent variation in local operating conditions
[43].
Temporal stability in operation is important for any fuel cell and is
relevant to the MRFBFC. A drop in power output from an MRFBFC over
P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

Fig. 5. Exemplary electric scooter configuration with mixed-reactant fuel cells.

Table 5 time may be caused by a loss or decrease in the intrinsic activity of

Electric scooter components. catalysts and/or a change in the wettabilty of the anode and/or
Item Specifications
cathode. In particular the MRFBFC used here is vulnerable to de-
gradation in hydrophobicity of the outside face of the cathode by the
Power source 3, 19 cell MRFBFC stacks, total “nominally” 300 W flowing liquid fuel/gas oxidant mixture. A loss of hydrophobicity allows
Fuel [2M KHCO2+2M KOH]aq (Sigma) liquid to enter the cathode and block the transfer of oxygen to the active
Oxidant 99.6 vol% O2 gas, 2.6 grade from Praxair
Fuel tank Capacity 2.4 L
cathode surface adjacent to the anode. The corresponding drop in
O2 tank Capacity 2.25 L, 124 bar rating, filled to ca. 3.5 MPa performance depends on the quality of the cathode and is accelerated
Exhaust tank Capacity 2.4 L by increasing temperature. As illustrated in Fig. 8 continuous operation
Motor DC 24 Volt, 250 W nominal (Razor E300) of an MRFBFC at 1,000 A m−2 (100 mA cm−2) over 4 h showed a slow
DC booster 10–36 V boosted and stabilised at 24 V (VFK 400W Q24-S24, CUI
drop in performance, in this case about 20 W m−2 h−1. This decrease in
Inc.)
Total weight Approx. 50 kg performance may also be due in part to a loss of Pd and/or hydro-
philicity in the anode. Electrode effects of this sort, occasional small
shorts from overheating and problems in replicating the factors of
Table 6 Table 6 are responsible for difficulties with reproducibility of the
Factors affecting performance of the MRFBFC. MRFBFC experimental results.
Apart from the above difficulties, the operation of the electric
Number of cells in stack
Materials Electrical, mechanical and thermal properties of solid scooter was compromised by a last-minute plumbing problem that shut-
components down one of the three MRFBFC stacks. Nonetheless the scooter was able
Dimensions Width, height, thickness, compression of each cell to carry an adult driver over a distance of several hundred meters on a
Electrodes Thickness, porosity, pore size, interfacial properties, level path at speeds up to about 10 km h−1. The fuel and oxygen con-
end effects
Catalysts Load, morphology, distribution
sumption of respectively about 10 L h−1 (no recycle) and 300 SL hr−1
Separator Thickness, porosity, pore size, wettability means that the range of the scooter is limited by the capacity of the fuel
Fluid distributor Thickness, porosity, pore size, contact angle and oxygen feed tanks to about 2 km. That 15 min test, which may be
Feed Composition, gas/liquid ratio, 2-phase fluid the first time a mixed-reactant fuel cell has been used to power a ve-
distribution
hicle, demonstrates a “proof of concept” for the MRFBFC but is in-
Conditions Fluid flow rates, pressure, temperature, time
adequate with regard to the practical application of such a fuel cell for

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P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

Fig. 6. MRFBFC polarization curve. Conditions: Single cell, 10E-4 m2 (10 cm2), fuel [2 MKCHO2 + 2 M KOH] @ 50 ml min−1, oxidant O2 @ 0.4 SLmin−1, pressure
500 kPa(abs), temperature 80 °C, Pd load 0.054 kg m−2 (5.4 mg cm−2).

transportation. In principle the range could be increased about 10 fold
by raising the fuel concentration and oxidant tank pressure (e.g. to 10 M
and 10 MPa) while reducing the feed rates to approach 80% conversion
of the reactants. However, the utility of mixed-reactant fuel cells in
transportation is ultimately limited by the relatively low energy effi-
ciency of the reactor and energy density of aqueous fuels, making the
MRFBFC system described here better suited to stationary than mobile
applications [17].
At this early stage of development of the MRFBFC there is a major
question about its durability and useful lifetime. In any application the
longevity of the fuel cell will be determined by the operating conditions
and consequent stability of the electrodes and separator, particularly
with respect to the degradation of capillary properties and catalysts
mentioned above. That question can only be answered by long term
tests not yet done. So far a single cell has been operated at a power
density around 1,000 W m−2 for intermittent 2–3 h stretches to total
about 10 h, which is far from the thousands of hours expected of con-
temporary hydrogen/air fuel cells.
Along with power density and temporal stability any practical ap-
plication of an MRFBFC would consider the reactant cost and conver-
sion, the energy efficiency, product disposal, parasitic power losses and
complexity of the balance of plant. With merchant prices respectively
around 100, 60 and 3 US$ kmol−1 the [KHCO2, KOH]/O2 is a costly
fuel/oxidant combination, although the liquid reaction product could
potentially be used in an electrosynthetic regeneration of a KHCO2/
KOH mixture [17,46]. For comparison, conventional H2/air fuel cells

Fig. 7. Superficial power and current densities in a single cell MRFBFC. Conditions: Single cell 10E-4 m2, fuel [2 M KHCO2+2 M KOH] @ 50 ml min−1, oxidant O2 @
0.4 SL min−1, pressure 300 kPa(abs), temperature 23–80 °C, Pd load 0.036 and 0.054 kg m−2 (3.6 & 5.4 mg cm−2).

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P. Forysinski et al.
Fig. 8. Effect of time on the MRFBFC performance. Conditions: MRFBFC stack, 3 bipolar cells each 10E-4 m2, fuel [2M NaHCO2+2M KOH] @ 82 ml min−1, oxidant
O2 @ 2 SL min−1, pressure 300 kPa(abs), temperature 30 °C, OCV 2.73 V, superficial power density ca. 1,000 W m−2 (100 mW cm−2) . 4 L batch of fuel used with
continuous recycle and zero make-up.
take fuel at about 10 US$ kmol−1 with an energy efficiency near 40%
and operating cost about 0.4 US$ kWh−1. The 100 W MRFBFC stacks
used in the scooter at 0.4 V per cell give conversions of formate and
oxygen respectively about 25% and 20%, without recycle. Based on the
energy density of the fuel solution (130 kWh m−3) and cost of the
[fuel + oxygen] these values correspond to an energy efficiency around
8% and operating cost about 25 US$/kWh. However, the MRFBFC in
these tests is far from being optimized, such that improvements in the
materials, configuration and operating conditions could perhaps raise
the energy efficiency at 400 kW m−3 to near 30% with a (fuel depen-
dent) operating cost below 8 US$ kWh−1.
A more comprehensive examination of the viability of the MRFBFC
system would consider the trade-off between capital and operating
costs. There are many factors to consider here, for example the catalyst
price, electrode durability and fuel cell operating conditions, whose
interactions are crudely summarized in equation (10).
Cost = (catalyst price)(catalyst load) / [(power density)(operating
life)] (10)
The fuel cell operating life in equation (10) will depend primarily on
the catalyst material(s) and the power density. For example, the cost
contribution for an anode loaded with 0.03 kg m−2 Pd, operating for
5,000 h at 4,000 W m−2 is estimated as:
Pd cost = (4E5 US$ kg −1
)(3E-2 kg m −2 −2
) / [(4 kW m )(5E3 h)] = 0.6
US$ kWh−1
Platinum is cheaper but is less effective than palladium as a formate
oxidation catalyst [18]. Nonetheless the anode cost might be sub-
stantially lowered by manipulating the catalyst morphology and com-
position, for example with nano-structured alloys of Pt or Pd and less
valuable metals [44,45]. Similar cost considerations apply to the fuel
cell cathode, whose lifetime is lowered by contact with liquid in the
reactant mixture. A separate-reactant system could avoid cathode
wetting but would require ion barriers between bipolar cells and might
introduce pressure differentials driving oxygen across the micro-porous
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Journal of Power Sources 414 (2019) 366–376
separators into the electro-active faces of the anodes. Accommodating
these “separate-reactant” features would call for inter-cell bipolar plates
and gas impermeable separators (Table 1) with attendant cost increases
that defeat the purpose of the MRFBFC.
The high operating costs of mixed-reactant fuel cells may be offset
by relatively low capital costs. In this regard the major potential ad-
vantages of the MRFBFC are the simplicity of its construction and its
balance of plant. There is no need of ion-selective separators or complex
sealing and flow distribution systems in the fuel cell hardware, along
with less onerous constraints on operating pressure and temperature
than for a conventional separate-reactant fuel cell. As represented in
Figs. 3 and 4 the balance of plant consists of systems for storing the
reactants and controlling their flow to the stack, effluent separation/
collection and regulation of the power delivered to the electric motor.
Handling a liquid fuel is straightforward, and humidification and
cooling are not necessary. Replacing O2 with air or O2 enriched air as an
oxidant is a possibility, although that would decrease the power density
and engender addition of a compressor to the balance of plant, with
corresponding parasitic power losses.
5. Conclusion
The work described here is a proof of concept for the mixed-reactant
flow-by fuel cell (MRFBFC) and its potential as a mobile or stationary
power source. Without optimization of the reactor design or operating
conditions a fuel/oxidant mixture of [2M K(Na)HCO2 + 2M KOH](aq)/
O2(g) used in a 10E-4 m2 single cell and in a 35E-4 m2/cell 19 cell bi-
polar stack, operating at 300 kPa(abs) and 80 °C with superficial current
densities up to 9,000 A m−2, achieved volumetric power densities of
respectively about 950 and 400 kW m−3. As well, two of the 19 cell,
100 W MRFBFC stacks were used alone to motivate an electric scooter
on a level path with on-board fuel, oxidant and an adult driver in a
15 min test run at speeds up to 10 km h−1.
At this stage of development, the MRFBFC suffers deficiencies of
high fuel cost, low energy efficiency, inconvenient effluents and short
P. Forysinski et al. Journal of Power Sources 414 (2019) 366–376

operating life which weigh heavily against the desirable simplicity and cells using different carbohydrate-rich wastewaters and different inocula, Pol. J.
relatively low cost of the fuel cell stack and balance of plant. However, Environ. Stud. 25 (2) (2016) 503–510.
[15] P. Grimes, H. Spengler, Formate ion-oxygen fuel cell, Fall Meeting Electrochem.
there are several conceptual avenues for improving MRFBFC perfor- Soc. Washington D.C. Oct. 1964.
mance, including for example: the use of different and reverse phase (L/ [16] W. Vielstich, Fuel Cells, Wiley-Interscience, London, 1970, pp. 275–280.
G → G/L) fuel/oxidant mixtures, better catalysts and feed distribution [17] T. Vo, et al., Formate: an energy storage bridge between carbon dioxide and a
formate fuel cell, ChemSusChem 8 (2015) 3853–3858.
methods, higher temperatures, more durable materials, enhanced ma- [18] L. An, R. Chen, Direct formate fuel cells – a review, J. Power Sources 320 (2016)
terial surface (wetting/non-wetting) properties and ultimately optimi- 127–139.
zation of the fuel cell and its operating system. Alternative fuels for this [19] T. Nguyen, et al., Operation of an alkaline direct formate fuel cell in the absence of
added hydroxide, Fuel Cells 13 (2013) 922–926.
application could be for example: hydrogen, ammonia, hydrazine, urea, [20] H. Cheng, W. Yuan, K. Scott, A liquid-gas phase mixed-reactant fuel cell with a
formic acid, borohydrides and ammonia borane along with oxidants RuSeW cathode electrocatalyst, J. Power Sources 183 (2) (2008) 678–681.
such as inorganic and organic redox-couples, nitrous oxide, peroxides [21] A. Bartrom, J. Haan, The direct formate fuel cell with an alkaline anion exchange
membrane, J. Power Sources 214 (2012) 68–74.
and persalts. The wide range of options for improvement and the en-
[22] T. Tran, A. Bartrom, et al., A fuel-flexible alkaline direct liquid fuel cell, Fuel Cells
couraging experimental results to-date, plus the prospect of low capital 14 (2014) 834–841.
cost, may justify future exploration of MRFBFCs for niche applications. [23] L. Zheng, Z. Tang, T. Zhao, A high performance alkaline exchange membrane direct
formate fuel cell, Appl. Energy 115 (2014) 405–410.
[24] H. Miller, et al., Improving the energy efficiency of direct formate fuel cell, Energies
Conflicts of interest 11 (2018) 369–381.
[25] Y. Li, et al., Performance of direct formate-peroxide fuel cells, J. Power Sources 287
Co-author Oloman owns the UK, Canadian and US patents for the (2015) 75–80.
[26] X. Yu, N. Manthiran, Catalyst-selective scale-able membraneless alkaline direct
mixed-reactant flow-by fuel cell. formate fuel cell, Appl. Catal. Environ B 165 (2015) 63–67.
[27] Manthiran N., Yu X., ”Membraneless direct liquid fuel cells”, PTO Patent
Acknowledgement Application WO2017123289A3,19 Oct. 2017.
[28] Oloman C., “Mixed-reactant flow-by fuel cell”, UK Patent 2474202 B, 18 July 2012
(US 8709680).
This work was carried out under licence at the Vancouver B.C. la- [29] E. Kjeang, et al., An alkaline microfluidic fuel cell based on formate and hypo-
boratory of Mantra Energy Alternatives Ltd. with funding from Mantra, chlorite bleach, Electrochim. Acta 54 (2008) 698–705.
[30] A. Aziznia, C. Oloman, E. Gyenge, Experimental advances and preliminary math-
0798465BC Ltd. (in kind) and the Government of Canada, the latter ematical modeling of a Swiss-roll mixed-reactant fuel cell, J. Power Sources 265
through Industrial R&D Fellowship (IRDF) and Mathematics of (2014) 201–213.
Information and Complex Systems (MITACS) grants for research and [31] Serov A., et al. ”Mixed-reactant fuel cells with selective electrodes”, US Patent
9812719, 07 Nov. 2017.
development.
[32] M. Choun, et al., Catalytically active highly metallic palladium on carbon support
for oxidation of HCOO-, Catal. Today 295 (2017) 26–31.
References [33] M. Doody, J. Haen, Comparison of fuel performance in novel palladium based
electro-catalysts, Colon. Acad. Alliance Undergrad. Res. J. 2 (2011) Article 10.
[34] L. Jiang, et al., Size dependent activity of palladium nanoparticles for oxygen
[1] A. Shukla, R. Raman, K. Scott, Advances in mixed-reactant fuel cells, Fuel Cells 5 (4) electroreduction in alkaline solution, J. Electrocherm. Soc. 156 (2009) B643–B649.
(2005) 436–447. [35] B. Garlyyev, et al., Engineering of highly active silver nanoparticles for oxygen
[2] M. Kuhn, T. Napporn, Single-chamber solid oxide fuel cell technology – from its electroreduction via simultaneous control over shape and size, Adv. Sustain. Syst. 1
origins to today's state of the art, Energies 3 (1) (2010) 57–134. (12) (2017) 1700117.
[3] Gruenberg G., Wicke W., Justi E., ”Generation of electrical energy”, British Patent [36] G. Orozco, et al., Electrooxidation of methanol on silver in alkaline solution, J.
GB994448, 1961. Electroanal. Chem. 495 (1) (2000) 71–78.
[4] P. Grimes, P. Fielder, J. Adam, Liquid alkaline fuel cells, Proc. 15th Power Sources [37] J. Newman, W. Tiedemann, Porous electrode theory with battery applications,
Conf. Fort Monmoth N.J. 1961, pp. 29–32. AIChE J. 21 (1) (1975) 25–41.
[5] Dyer C., ”Primary source of electrical energy using a mixture of fuel and oxidizer”, [38] R. Ross, I. Morrison, Colloidal Systems and Interfaces, Wiley, New York, 1988.
US Patent 4863813,1989. [39] F. Walsh, A First Course in Electrochemical Engineering, ECC, Romsey, 1993.
[6] M. Priestnall, et al., Compact mixed-reactant fuel cells, J. Power Sources 106 (2002) [40] K. Triplett, et al., Gas-liquid two-phase flow in microchannels Part 1: two-phase
21–32. flow patterns, Int. J. Multiphas. Flow 25 (1999) 377–394.
[7] A. Shukla, R. Raman, Methanol-resistant oxygen-reduction catalysts for direct me- [41] A. Aziznia, C. Oloman, E. Gyenge, A Swiss-roll liquid-gas mixed-reactant fuel cell, J.
thanol fuel cells, Annu. Rev. Mater. Res. 33 (2003) 155–168. Power Sources 212 (2012) 154–160.
[8] R. Zeng, P. Shen, Selective membrane electrode assemblies for bipolar-plate free [42] Oloman C., Aziznia A., Gyenge G., ”Apparatus and method for feeding a multiphase
mixed-reactant fuel cells, J. Power Sources 170 (2007) 286–290. mixture of reactantsto an electrochemical reactor”, US Patent Application 2016/
[9] A. Ilicic, D. Wilkinson, K. Faith, Advances in direct liquid redox fuel cells mixed- 0201207 A1, 14 July 2016.
reactant and in-situ regeneration opportunities, J. Electrochem. Soc. 157 (4) (2010) [43] J. Benzinger, et al., The power performance curve for engineering analysis of fuel
B529–B535. cells, J. Power Sources 155 (2006) 272–285.
[10] A. Aziznia, C. Oloman, E. Gyenge, A platinum and membrane-free Swiss-roll mixed- [44] S-H, H.-M. Liu, et al., Platinum-silver alloy nanoballoon nanoassemblies with super
reactant fuel cell, ChemSusChem 6 (2013) 847–855. catalytic activity for the formate electrooxidation, ACS Appl. Energy Mater. 1 (3)
[11] Y. Hao, et al., Recent advances in single-chamber fuel cells: experiment and mod- (2018) 1252–1258.
eling, J. Power Sources 177 (2006) 2013–2021. [45] J. Noborikawa, J. Lau, et al., Palladium-copper electrocatalyst for promotion of
[12] E. Kjeang, N. Djilali, D. Sinton, Microfluidic fuel cells: a review, J. Power Sources oxidation of formate and ethanol in alkaline media, Electrochim. Acta 137 (2014)
186 (2) (2009) 353–369. 654–660.
[13] S. Hashemi, et al., Membrane-less micro fuel cell based on two-phase flow, J. Power [46] C. Oloman, H. Li, Electrochemical processing of carbon dioxide, ChemSusChem 1
Sources 348 (2017) 212–218. (2008) 385–391.
[14] S. Ahmed, E. Roziak, H. Abdel-Halim, Performance of single-chamber microbial fuel

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