i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 4 ( 2 0 1 9 ) 7 5 3 8 e7 5 4 3

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Understanding mass and charge transports to

create anion-ionomer-free high-performance
alkaline direct formate fuel cells

Xianda Sun a, Yinshi Li a,b,*

a
Key Laboratory of Thermo-Fluid Science and Engineering of MOE, School of Energy and Power Engineering, Xi'an
Jiaotong University, Xi'an, Shaanxi, 710049, China
b
Xi'an Jiaotong University Shenzhen Research School, Shenzhen, Guangdong, 518057, China

article info abstract

Article history: The disadvantage of anion ionomer that possesses low hydroxide conductivity, and ther-
Received 7 November 2018 mal and chemical instability hinders the development of the high-performance anion-
Received in revised form exchange membrane direct liquid fuel cells. Instead of adding additional base and syn-
23 January 2019 thesizing high-conductivity ionomer material, by gaining insight into species transports,
Accepted 26 January 2019 herein, we propose an anion-ionomer-free anion-exchange membrane direct formate fuel
Available online 21 February 2019 cell (AEM DFFC). Experimental result reveals that this conceptual anion-ionomer-free AEM
DFFC can operate stably within a 6-h constant-current discharge at 10 mA cm
2, mainly
Keywords: because formate hydrolysis renders a high OH
conductivity. It was also found that the
Fuel cell anion-ionomer-free AEM DFFC yields a peak power density as high as 41 mW cm
2 at 40  C,
Direct formate fuel cell 40% higher than that of the conventional quaternary ammonia polysulfone anion-ionomer
Formate oxidation reaction AEM DFFC. This can be attributed to the fact that the OH
-containing formate solution
Anion exchange membrane facilitates the mass and charge transports, thereby enlarging the triple-phase boundary for
Anion ionomer both anodic formate oxidation reaction and cathodic oxygen reduction reaction.
© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

exchange membrane direct liquid fuel cells (AEM DLFCs)

Introduction
The growing crisis of both energy shortage and environmental
pollution is driving people to pursue a sustainable and clean
substitute of the conventional fossil energy [1e5]. Fuel cell has
been recognized as one of the most ideal approaches to solve
these problems by directly converting chemical energy into
electricity with high energy-conversion efficiency and low/
zero emission [6e10]. Currently, with the increase in the de-
mand for portable and mobile applications, alkaline anion-
have received ever-increasing attention [11e16], primarily
because they possess unique advantages as compared with
proton exchange membrane fuel cells (PEMFCs): i) quick
electro-kinetics even using Pt-/metal-free catalysts [17e19], ii)
the increased fuel utilization and the alleviated water flooding
caused by the opposite electro-osmosis [20,21], and iii) weak
corrosion towards electrode materials [22,23].
Over the past decade, considerable progress has been
made in the development of AEM DLFCs [24e27]. The AEM
direct methanol fuel cell (DMFC) [28] that consumes 1.0 M

* Corresponding author. Key Laboratory of Thermo-Fluid Science and Engineering of MOE, School of Energy and Power Engineering, Xi'an
Jiaotong University, Xi'an, Shaanxi, 710049, China.
E-mail address: ysli@mail.xjtu.edu.cn (Y. Li).
https://doi.org/10.1016/j.ijhydene.2019.01.240
0360-3199/© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 4 ( 2 0 1 9 ) 7 5 3 8 e7 5 4 3
methanol with 2.0 M KOH can produce a peak power density
as high as 168 mW cm
2, which is comparable to PEM DMFC.
When 3.0 M ethanol mixed with 5.0 M KOH was injected into
the fuel tank of the passive AEM direct ethanol fuel cell (DEFC)
stack [26], a peak power density of 38 mW cm
2 was achieved.
Recently, an AEM direct ascorbate fuel cell (DAFC) was
demonstrated [29], which yields a peak power density of
73 mW cm
2 when feeding 1.0 M ascorbic acid and 1.0 M KOH
to the anode, higher than the PEM direct ascorbic acid fuel cell.
Although appealing, it should be pointed out that the addi-
tional liquid electrolyte (typically KOH/NaOH) requires to be
added to the fuel solution to enhance ionic conductivity and
accelerate fuel oxidation reaction [20]. It has been demon-
strated that with the aid of the additional alkali, the peak
power density of AEM DLFC can be increased by an order of
magnitude [26]. However, adding additional alkali to the fuel
solution directly lowers system energy density [8]. Therefore,
it is essential to develop the AEM DLFC without the assistance
of the additional liquid electrolyte. Among fuels, formate
[30e33] is considered to be one of the most promising fuels for
AEM DLFCs because of its unique features of non-flammable,
non-toxic, and low cost, in addition to its renewability that
can be easily produced from electrochemical reduction of
carbon dioxide [34,35]. More importantly, formate oxidation is
independent on pH between 9 and 14. As a result, the alkaline
anion-exchange membrane direct formate fuel cell (AEM
DFFC) in the absence of additional alkali was developed [36].
To improve cell performance, an alkaline AEM direct formate-
peroxide fuel cell (DFPFC) was also proposed, and the proof-of-
concept AEM DFPFC shows a half-hour constant-current
discharge even eliminating the additional liquid electrolytes
from both anode and cathode electrodes [37]. However, there
still exists an unavoidable issue: the state-of-the-art anion
ionomer that is used to build the triple-phase boundary for
electrode reactions possesses the disadvantages of low hy-
droxide conductivity, and the thermal and chemical insta-
bility, thereby leading to the low electrode performance and
instable long-time discharge [38e42].
Clearly, the challenge of developing high-performance and
stable AEM DLFCs remains on how to break through the lim-
itation of the current anion ionomer. Rather than focusing on
the improvement of the anion ionomer material, the objective
of the present work is to meet the electrode reactions by dig-
ging into species transports. To this end, an anion-ionomer-
free alkaline anion-exchange membrane direct formate fuel
cell (AEM DFFC) is proposed and tested. It has been demon-
strated that the anion-ionomer-free AEM DFFC can operate
steadily without additional alkaline electrolyte and anion
ionomer.
Experimental
Materials
Potassium formate (HCOOK), potassium hydroxide (KOH) and
ethanol (CH3CH2OH) were purchased from Aladdin. Palla-
dium chloride (PdCl2), sodium borohydride (NaBH4) and
polytetrafluoroethylene (PTFE) were from Sigma-Aldrich.
Quaternary ammonia polysulfone (QAPS) anion ionomer
7539
and anion-exchange membrane were from Hephasenergy.
Carbon black and carbon paper were respectively obtained
from Cabot and Toray.
Membrane electrode assembly (MEA) preparation
The MEA consists of an anode electrode, a QAPS anion-
exchange membrane and a cathode electrode. Both anode
and cathode electrodes are composed of a gas diffusion layer
(GDL) and a catalyst layer (CL). The GDL contains a carbon-
paper supporting layer, a micro-porous layer (MPL). The MPL
ink made up of 4.0-mg cm
2 carbon black (Vulcan XC-72) and
40-wt.% PTFE was directly sprayed onto carbon paper to form
GDL. The catalyst ink combines Pd/C and binder (PTFE or
QAPS) using ethanol as the dispersion solvent. The Pd/C
catalyst was synthesized by the simultaneous reduction
method using NaBH4 as a reductant [8]. After stirred in an
ultrasonic bath for 15 min, the catalyst ink was brushed on the
GDL to form electrode. The catalyst loading for all of the
electrodes was controlled at 2 mg cm
2, while the binder
content was 10 wt%.
Electrochemical characterization
Cyclic voltammetry (CV) experiments were carried out by
electrochemical workstation (CHI 760E) in a conventional
three-electrode electrochemical cell. The as-prepared elec-
trode was used as the working electrode. The active area and
Pd loading of working electrode were respectively 0.25 cm2
and 60 mg. The counter electrode and the reference electrode
were a Pt foil and an Hg/HgO (MMO, 1.0 M KOH, 0.098 V vs.
SHE), respectively. The electrochemical experiments were
conducted in 1 M KOH solution with and without 1 M HCOOK
at a scan rate of 20 mV s
1. The solution was bubbled with
nitrogen gas for 30 min before each testing to remove the
dissolved oxygen.
Measurement instrumentation and test conditions
An electrochemical workstation (Arbin BT-G, Arbin Instru-
ment Inc.) was applied to collect the polarization curves. The
aqueous solution of HCOOK was supplied to anode by a peri-
staltic pump at a flow rate of 1.0 mL min
1. At the cathode,
99.5% pure oxygen without humidification was fed by a mass
flow controller (Omega FMA series, USA) at a flow rate of 100
sccm (standard cubic centimeters per minute). The cell
resistance was measured by the d.c.-pulse method. An elec-
trical heating rod was used to control the operating temper-
ature at 40  C.
Results and discussion
The anion-ionomer-free AEM DFFC comprises an anion-
exchange membrane sandwiched between two electrodes as
demonstrated in Fig. 1. Instead of using the conventional
functionalized anion-ionomer, the neutral-polymer is incor-
porated into catalyst layer to bind the catalytic nanoparticles
to prepare both anode and cathode electrodes. To observe the
feasibility, the constant-current discharging behavior of
7540 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 4 ( 2 0 1 9 ) 7 5 3 8 e7 5 4 3
Fig. 1 e Schematic illustration of the anion-ionomer-free anion-exchange membrane direct formate fuel cell.
anion-ionomer-free AEM DFFC was conducted at 40  C as
shown in Fig. 2. As seen, when 2.0 M HCOOK aqueous solution
and pure oxygen gas were respectively supplied into anode
and cathode, the cell discharges stably within 6-h continuous
operation at 10 mA cm
2 in the absence of additional alkaline
electrolyte and anion ionomer, which confirms the feasibility
Fig. 2 e Constant-current discharging behavior of the
anion-ionomer-free AEM DFFC. Anode fuel: KCOOH, 2.0 M,
1.0 mL min¡1; Cathode oxidant: oxygen, 100 sccm, at
ambient pressure; Anode electrode: 2.0 mgPd cm¡2 Pd/C,
10 wt% PTFE; Cathode electrode: 2.0 mgPd cm¡2 Pd/C, 10 wt
% PTFE; AEM: QAPS membrane; Operating temperature:
40  C.
of anion-ionomer-free AEM DFFC. This is mainly because: i)
On anode, formate hydrolysis occurs according to:
HCOO
þ H2 O#HCOOH þ OH
(1)
Equation (1) reveals that the formate hydrolysis can pro-
duce OH
ions. The OH
-containing formate solution, on one
hand, provides one-third OH
ions for the formate oxidation
reaction (FOR) [43], i.e.:
HCOO
þ 2OH
/HCO

3 þ H2 O þ 2e


(2)
on the other hand, offers the charge transport media for OH

conduction, thereby establishing the triple-phase boundary
without the aid of additional alkaline and the anion ionomer;
ii) On cathode, the oxygen reduction reaction (ORR) takes
place:
1
O2 þ H2 O þ 2e
/2OH
(3)
2
Equation (3) indicates that the ORR is associated with the
liquid-gas two-phase flow. Previous work [13] has demon-
strated that the cathode flooding occurs in an AEM DLFC,
owing to the fact that the diffusion flux of the liquid water
from anode to cathode outweighs the total water flux due to
both the ORR and electro-osmotic drag (EOD). The accumula-
tion of liquid water in cathode catalyst layer increases the
oxygen transport resistance. The addition of the hydrophobic
PTFE in cathode catalyst layer facilitates the oxygen and water
transports, and thus improving cell performance.
Cell performances of AEM DFFC with different electrodes
were investigated as shown in Fig. 3: PTFE-based electrodes
for anion-ionomer-free AEM DFFC and QAPS-based electrodes
for conventional anion-ionomer AEM DFFC. It can be seen
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 4 ( 2 0 1 9 ) 7 5 3 8 e7 5 4 3
Fig. 3 e Polarization and power density curves of the AEM
DFFC with and without anion ionomer. Anode: KCOOH,
1.0 M, 1.0 mL min¡1; Cathode: oxygen, 100 sccm, ambient
pressure; Operating temperature: 40  C. Anion-ionomer-
free AEM DFFC: 2.0 mgPd cm¡2 Pd/C and 10 wt% PTFE
anode þ QAPS membrane þ 2.0 mgPd cm¡2 Pd/C and 10 wt
% PTFE cathode; Anion-ionomer AEM DFFC: 2.0 mgPd cm¡2
Pd/C and 10 wt% QAPS anion ionomer anode þ QAPS
membrane þ 2.0 mgPd cm¡2 Pd/C and 10 wt% QAPS anion
ionomer cathode.
from Fig. 3 that the anion-ionomer-free AEM DFFC yields a
better cell performance than the conventional AEM DFFC
does: the peak power density of anion-ionomer-free AEM
DFFC is as high as 41 mW cm
2, 40% higher than that of the
conventional AEM DFFC. In addition, the electrocatalytic ac-
tivity of both QAPS-based electrode and PTFE-based electrode
are investigated by CV curves in 1.0 M KOH with and without
1.0 M HCOOK aqueous solution. It can be clearly observed
from Fig. 4 that PTFE-based electrode exhibits a higher redox
Fig. 4 e Cyclic voltammograms of different working
electrodes in 1.0 M KOH at a scan rate of 20 mV s¡1. PTFE-
based electrode: 60 mg Pd/C, 10 wt% PTFE; QAPS-based
electrode: 60 mg Pd/C, 10 wt% QAPS anion ionomer; Room
temperature.
7541
peak and a broader area of palladium oxide reduction. The
ECSA value of both QAPS-based electrode and PTFE-based
electrode can be evidenced by calculating the palladium
oxide reduction peak in CV curves according to the following
equation [44]:
Q
ECSA ¼ (4)
qm
where Q the coulombic charge (mC), q the charge value of
405 mC cm
2 for the reduction of palladium oxide monolayer
[45], and m the Pd loading on the working electrode (mg).
Based on this correlation, the calculated value of PTFE-based
electrode is 17.6 m2 g
1, which is 45% higher than that of
QAPS-based electrode. In addition, the stabilized CV curves for
the FOR on two mentioned electrodes in 1.0 M KOH and 1.0 M
HCOOK solution are shown in Fig. 5. The results indicate that
the maximum current generated by the PTFE-based electrode
is 26 mA, higher than that by the QAPS-based electrode with
22 mA. As a result, the PTFE-based electrode yields a remarked
catalytic activity towards FOR compared with the QAPS-based
electrode. The improved cell performance can be mainly
attributed to two aspects: i) The enhanced charge transport:
Formate hydrolysis as mentioned in Equation (1) raises the
alkalinity of anode aqueous solution, leading to increasing the
OH
conductivity, thereby alleviating the ohmic loss. It can be
proven from the cell resistance as shown in Table 1. The cell
resistance of the anion-ionomer-free AEM DFFC is
373 mU cm2, while this value goes up to 426 mU cm2 for the
conventional AEM DFFC; ii) The enhanced mass transport and
Fig. 5 e CV curves of FOR on different working electrodes in
1.0 M KOH and 1.0 M HCOOK at a scan rate of 20 mV s¡1.
PTFE-based electrode: 60 mg Pd/C, 10 wt% PTFE; QAPS-
based electrode: 60 mg Pd/C, 10 wt% QAPS anion ionomer;
Room temperature.
Table 1 e Cell resistance of the AEM DFFCs with and
without anion ionomer.
AEM DFFC Cell resistance (mU cm2)
Anion-ionomer-free 373
Anion-ionomer 426
7542 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 4 ( 2 0 1 9 ) 7 5 3 8 e7 5 4 3
Fig. 6 e Microstructure and formate oxidation reaction process diagram of (a) QAPS-based electrode and (b) PTFE-based
electrode in anion-ionomer-free anion-exchange membrane direct formate fuel cell.
the extended electrochemically active surface area (ECSA):
The SEM images of the PTFE-based electrode and anion-
ionomer-based electrode have been reported in our previous
work [46]. The corresponding microstructure and FOR process
in anion-ionomer-free AEM DFFC are shown in Fig. 6. As can
been seen that QAPS anion ionomer is inclined to cover cat-
alytic nanoparticles to form large agglomerates with low
porosity as illustrated in Fig. 6a, lowering the interaction of
catalyst/ionomer/reactant, resulting in a low triple-phase
boundary. In contrast, PTFE as a neutral polymer tends to
adhere nanoparticles together to form small agglomerates
associated with high porosity as shown in Fig. 6b, thereby
facilitating the mass transport and raising catalyst utilization.
More importantly, the OH
-containing formate solution ren-
ders the mass and charge transport media, and hence
increasing the interaction of catalyst/ion/fuel, leading to a
large triple-phase boundary. Therefore, the PTFE-based elec-
trode reduces the mass and charge transport resistances and
allows a larger ECSA than the QAPS-based electrode, sug-
gesting the potential of the anion-ionomer-free AEM DFFC.
Conclusions
To overcome the disadvantages of anion ionomer, such as low
hydroxide conductivity, and the thermal and chemical insta-
bility, presently, a prevalent solution is to add additional alkali
to anode fuel solution. Although effective, the addition of the
alkali not only lowers system energy density but also in-
creases system complexity. In this work, from the viewpoint
of species transports, we propose and develop an anion-
ionomer-free anion-exchange membrane direct formate fuel
cell. Instead of using the additional alkali and the anion ion-
omer, the formate hydrolysis allows the OH
ion to possess a
high conductivity in aqueous solution. The experimental
result demonstrated that the anion-ionomer-free AEM DFFC
discharges stably within 6 h of continuous operation at
10 mA cm
2, suggesting the conceptual feasibility. In addition,
the peak power density of anion-ionomer-free AEM DFFC is as
high as 41 mW cm
2 at 40  C, 40% higher than that of the
conventional AEM DFFC. The improved performance can be
attributed to the reduced ohmic loss and the increased elec-
trochemically active surface area. This work presents a new
way to develop the high-performance anion-exchange mem-
brane direct liquid fuel cells.
Acknowledgements
This work was supported by the National Natural Science
Foundation of China (51776156) and the Shenzhen Science
and Technology Foundation (JCYJ20170816100910119).
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