An Environmentally Friendly and Flexible Aqueous Zinc Battery Using an Organic Cathode

Article abstract of DOI:10.1002/anie.201807121

Rechargeable batteries have been used to power various electric devices and store energy from renewables, but their toxic components (namely, electrode materials, electrolyte, and separator) generally cause serious environment issues when disused. Such toxicity characteristic makes them difficult to power future wearable electronic devices. Now an environmentally friendly and highly safe rechargeable battery, based on a pyrene-4,5,9,10-tetraone (PTO) cathode and zinc anode in mild aqueous electrolyte is presented. The PTO-cathode shows a high specific capacity (336 mAh g^?1) for Zn²⁺ storage with fast kinetics and high reversibility. Thus, the PTO//Zn full cell exhibits a high energy density (186.7 Wh kg^?1), supercapacitor-like power behavior and long-term lifespan (over 1000 cycles). Moreover, a belt-shaped PTO//Zn battery with robust mechanical durability and remarkable flexibility is first fabricated to clarify its potential application in wearable electronic devices.

Full text of DOI:10.1002/anie.201807121

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Accepted Article
Title: Environment-Friendly and Flexible Aqueous Zinc Battery Using
an Organic Cathode
Authors: Yonggang Wang, Zhaowei Guo, Yuanyuan Ma, Xiaoli Dong,
Jianhang Huang, and Yongyao Xia
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To be cited as: Angew. Chem. Int. Ed. 10.1002/anie.201807121
Angew. Chem. 10.1002/ange.201807121
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http://dx.doi.org/10.1002/ange.201807121

Angewandte Chemie International Edition
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COMMUNICATION
Environment-Friendly and Flexible Aqueous Zinc Battery Using
an Organic Cathode
Zhaowei Guo, Yuanyuan Ma, Xiaoli Dong, Jianhang Huang, Yonggang Wang*, and Yongyao Xia
Abstract: Rechargeable batteries have been used to power various electric
devices and store energy from renewables, but their toxic components (i.e.,
electrode materials, electrolyte and separator) generally cause serious
environment issues when disused. Such toxicity characteristic makes them
difficult to power future wearable electronic devices. Herein, we report an
environment-friendly and high safe rechargeable battery, based on pyrene-
organics show very limited toxicity. However, the academic
results on this topic are rarely reported. Only very recently, Chen
et al. first reported an aqueous zinc battery using a quinone
(C4Q)-cathode, which shows
a
high energy density.[37]
Unfortunately, in this cell, an expensive fluorine-containing
membrane (i.e., Nafion film) must be used as separator to prevent
the crossover of the soluble discharge product of C4Q-cathode.
In addition, the Nafion separator must be sealed strongly to
prevent the mixture of anolyte and catholyte, which is very difficult
to be applied in flexible devices, especially when operated at the
repeated bending condition.
4
,5,9,10-tetraone (PTO) cathode and zinc anode in mild aqueous electrolyte.
It is demonstrated that the PTO-cathode shows a high specific capacity (336
-1
2+
mAh g ) for Zn storage with fast kinetics and high reversibility. Thus, the
-1
PTO//Zn full cell exhibits a high energy density (186.7 Wh kg ),
supercapacitor-like power behavior and long-term lifespan (over 1000
cycles). Moreover, a belt-shaped PTO//Zn battery with robust mechanical
durability and remarkable flexibility is first fabricated to clarify its potential
application in wearable electronic devices.
Herein, we propose an original aqueous zinc battery, which
involves a pyrene-4,5,9,10-tetraone (PTO) cathode, a zinc anode
and a mild aqueous electrolyte containing Zn2+ (Scheme 1).
Owing to the inherent insoluble characteristic of PTO and
corresponding discharge product, the conventional porous glass
fiber membrane can be directly used to separate cathode and
anode. All components of this battery are low toxic (or non-toxic),
exhibiting an environment-friendly nature (see Table S2, the
safety hazards caused by components in our battery). On
Currently, rechargeable batteries are playing an irreplaceable role
in realizing the sustainable energy based low-carbon society.[
However, almost all of these batteries contain toxic and/or
environmentally unfriendly components (see Table S1, the safety
hazards caused by components in various batteries).[7] When
disused, these batteries will result in serious environment issues.
Furthermore, the ever-increasing demand for wearable electronic
1-7]
2
+
discharging, the zinc anode is oxidized to Zn , which passes
across the electrolyte and is stored by PTO cathode through a
Zn2+ coordination reaction (Scheme 1). The charge process
reverses discharge. The charge storage mechanism of PTO
electrode and the electrochemical performance of the full cell are
investigated in detail. Furthermore, a belt-shaped and flexible
PTO//Zn battery is fabricated to demonstrate its potential
application in wearable electronic devices.
[
8-
devices stimulates exploitation of the matched power sources.
1
0]
Nevertheless, it seems impossible to use these toxic batteries
to power the future wearable electric devices that are close to
human body.
Over the past few years, aqueous Li(Na)-ion batteries have
attracted extensive attention because of the low toxicity and high
safety nature of the mild aqueous electrolyte. However, the Li(Na)
intercalation compounds generally exhibit low capacity (less than
The prepared PTO, exhibits a homogeneous and directional
nanorod morphology with 1-6 μm in length and 100-400 nm in
width (Figure S1). High purity of as-prepared PTO was confirmed
by 1H NMR and FTIR spectra (Figures S2 and S3). The
electrochemical behavior of PTO in mild acidic aqueous
-1
[7,11-17]
1
50 mAh g ) in aqueous electrolyte.
Therefore, the zinc
batteries using a mild aqueous electrolyte entered researchers’
spotlight due to the non-toxicity, high capacity and low-cost nature
of zinc anode.[
18-24]
Several cathodes materials, such as copper
electrolyte (i.e.,
2
M
ZnSO
4
)
was investigated by cyclic
hexacyanoferrate,[20]
V
O
5
[21,22]
and MnO
,[23,24] have been
-1
voltammetry (CV) experiments at a scan rate of 1 mV s with a
typical three-electrode system using Zn foil as counter and
reference electrodes. It can be observed from Figure 1a that
PTO-cathode displays two pairs of redox peaks at 1.0 V/1.17 V
2
2
coupled with zinc anode to form the rechargeable aqueous zinc
batteries. In these reports, cathodes still involve toxic and/or
environmentally unfriendly elements in their components. Very
recently, organic electrode materials have been considered as the
low-toxicity and sustainable alternative to conventional inorganic
electrode materials.[25-36] In theory, the combination of organic
cathode and zinc anode in mild electrolyte should be a promising
approach for developing low toxic battery, because some
2
+
and 0.63 V/0.85 V vs. Zn /Zn. Correspondingly, two pairs of
respective flat and slopping plateaus can be distinguished from
discharge/charge profiles in Figure 1b clearly, exhibiting a high
capacity of 336 mAh g-1 and good reversibility (Figure 1b). To
reveal the electrochemical reaction mechanism on PTO electrode,
a series of ex-situ structural and elemental characteristics have
been carried out. By comparing STEM-EDS mapping images of
PTO-cathode at pristine, fully discharged and fully recharged
states, a reversible process of Zn-element occurring/disappearing
[*]
Dr. Z. Guo, Dr. Y. Ma, Dr. X. Dong, Dr. J. Huang, Prof. Y. Wang,
Prof. Y. Xia
Department of Chemistry and Shanghai Key Laboratory of
Molecular Catalysis and Innovative Materials, Institute of New
Energy, iChEM (Collaborative Innovation Center of Chemistry for
Energy Materials), Fudan University
Shanghai 200433, China
E-mail: ygwang@fudan.edu.cn
on PTO-cathode could be obviously recognized during
a
discharge/charge cycle (Figure 1c). Furthermore, XPS
explorations of PTO-cathode during a discharge/discharge cycle
in Figure 1d manifest the appearance of Zn-element, in divalent
state, in PTO-cathode during discharge process, and
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COMMUNICATION
-1
-1
of 22.1 W kg . The achieved energy density (186.7 Wh kg ) is
comparable to recent reported aqueous zinc batteries using MnO
2
as cathode,[
21-24,37]
and is higher than conventional
and V
2
O
5
aqueous rechargeable batteries. Especially, even with an
-1
ultrahigh power density of 15.3 kW kg , the energy density can
-1
still retain a decent value of 12 Wh kg , which is close to
supercapacitor. Furthermore, when cycled at a current density of
-1
3
A g , the battery sustains a capacity retention of approximately
0% and a delivered capacity of 145 mAh g-1 over 1000 cycles,
7
along with Coulombic efficiency approaching 100% (Figure 2c),
verifying the durable cycle stability of PTO cathode.
Previous report has demonstrated that the ion-coordination
reaction may lead to the dissolution of organic electrode materials,
which requires ion exchange membrane (e.g., Nafion film) to
separate the organic cathode and zinc anode.[ Fortunately, in
our case, the ion-coordination does not cause the dissolution of
PTO electrode, and thus the eco-friendly glass fiber membrane
can be directly used as separator. Self-discharge measurements
were carried out to clarify this advantage. First, we investigated
the self-discharge at fully charged condition. In this test, the cell
was fully charged to 1.46 V at 0.2 A g-1 followed by a rest step of
37]
Scheme 1. Schematic illustration of the reversible reaction mechanism of the
aqueous PTO//Zn battery.
disappearance after recharged to 1.46 V as initial state (XPS of
all elements investigation is given in Figure S4). As is observed
in Figure 1e, on discharging (from initial state (1) to discharged to
24 hours, which was then discharged to 0.36 V at the same
-1
0
.6 V (4)), the characteristic peaks at about 1680 cm , assigned
to the stretching vibration of carbonyl group, are gradually
weakened, coinciding with the sustained coordination of Zn2+ on
carbonyl group of PTO during discharge process. While the
following charge states reverse discharge, where these peaks are
strengthened back to the pristine state ultimately (the full FTIR
spectra is given in Figure S5), demonstrating the reversible Zn2+
coordination/ uncoordination (Scheme 1). The morphology
variation of PTO after discharge and recharge is given in Figure
S6. The kinetics property of Zn-ion coordination reaction on PTO
was investigated by CV measurements at various scan rates
(
Figure S7a). The corresponding relationship between peak
-1
b
current (i, A) and scan rate (v, mV s ) is summarized as i = av ,
where a and b are constants.[38] As is shown in Figure S7b, the
calculated b values at different peaks vary from 0.7 to 0.8,
indicating a fast kinetics for Zn2+ storage.
After above charge storage mechanism investigation, PTO
cathode was combined with a zinc film anode to form a coin-type
full cell, in which a porous glass fiber membrane with adsorbed
4
electrolyte (i.e., 2 M ZnSO ) was directly used as the separator
between cathode and anode. As is shown in Figure 2a, PTO
cathode delivers a remarkably high specific capacity of 336 mAh
g-1 at a current density of 0.04 A g , and maintains specific
-1
-1
capacities of 300, 213, 162 mAh g at current densities of 0.1, 1,
A g- (The current densities and capacities are calculated based
1
5
on the mass of PTO in cathode). A respectable capacity of 113
mAh g-1 is attained even at fully charged in only 20 s
-1
Figure 1. a) CV curve at a scan rate of 1 mV s-1, and b) galvanostatic
(
corresponding to current density of 20 A g ), showing a
-
1
discharge/charge curve at a current density of 0.04 A g of PTO electrode. c)
STEM-HAADF images and STEM-EDS mapping of C, O, Zn elemental
distributions on PTO electrode at (i) pristine, (ii) fully discharged (0.36 V), and
(iii) fully recharged (1.46 V) states. Scale bar: 100 nm. d) High-resolution Zn 2p
XPS spectra of PTO electrode at pristine, fully discharged (0.36 V), and fully
recharged (1.46 V) states. e) Ex-situ FTIR spectra of PTO electrode at various
discharged (left) and charged (middle) states in a discharge/charge cycle,
corresponding to the marked points on a galvanostatic discharge/charge curve
(right).
supercapacitor-like high rate capability. The energy density and
power density of the cell were calculated with galvanostatic
discharge/charge data shown in Figure 2a, and the
corresponding results are given as Ragone plot (i.e., energy
density vs. power density) in Figure 2b (see calculation details in
supporting information). As is shown in Figure 2b, a specific
energy density up to 186.7 Wh kg-1 is achieved at a power density
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the data shown in Figure S9 and the area/volume of the belt-
shaped device (see calculation details in supporting information).
The corresponding results are given in Figure S10 as Ragone
plot. As shown in Figure S10a, this cell exhibits a maximum areal
-2
energy density of 1.55 mWh cm and a maximum power density
-2
of 67.86 mW cm , respectively. Taking the thickness into
consideration, the volumetric energy and power densities of the
belt-shaped battery can reach 38.72 mWh cm-3 and 1.70 W cm-3,
respectively (Figure S10b), which is superior to most of previous
reported flexible batteries and supercapacitors (see Table S3).
Cycle performance of the belt-shaped battery tested at a current
density of 3 A g-1 is given in Figure S11, showing a promising
cycle stability.
A series of flexibility tests were conducted by checking the
delivered capacity of the belt-shaped battery after being
repetitively bended to various degrees. By comparison of Figure
3a, there is almost no discernible capacity loss after folding the
flat battery in half for one hundred times. Besides, the delivered
capacities hardly decline under other bending situations (Figure
S12), demonstrating the good flexibility and robust mechanical
property against repeated bending. Furthermore, the belt-shaped
battery is cycled stably under successive various bending
degrees (Figure 3b). As shown in Figure 3c, 30 LEDs in parallel
also work well powered by these two batteries in-series. In
addition, one such battery could energetically drive an electric fan
(
the right in Figure 3c and Movie S1), showing its potential
Figure 2. a) Galvanostatic discharge/charge curves of the aqueous PTO//Zn full
practical application in wearable electronic devices.
cell at various current densities. b) Ragone plot. c) Cycle stability at a current
-
1
density of 3 A g . Self-discharge behaviour tested at a current density of 0.2 A
-
1
g , d) when firstly charged to 1.46 V, and then discharged to 0.36 V after rest
for 24 hours, and e) when firstly discharged to 0.36 V, and then charged to 1.46
V after rest for 24 hours.
current. The discharge after rest delivers a capacity of 284 mAh
-1
g , which is almost the same as that on charge (Figure 2d). This
result indicates that the self-discharge on charge state is
negligible. The self-discharge at fully discharged condition was
also investigated with the similar process. After discharged to 0.36
V, the cell experienced a 24 hours rest, showing a stable cell
voltage without the phenomenon of voltage increase (the right in
Figure 2e). The consequent recharge shows a capacity of 283
-1
mAh g , which is almost equal to discharge capacity before rest
the left in Figure 2e), indicating a negligible self-discharge at fully
(
discharged condition.
After coin-cell configuration tests, a two-dimensional (2D) belt-
shaped and flexible aqueous PTO//Zn battery was fabricated by
2
stacking up a PTO-cathode (1 × 5 cm ), a glass fiber separator
soaked with electrolyte (i.e., 2 M ZnSO
4
) and a Zn foil-anode (1 ×
2
5
cm ) to form a “sandwich” structure after a vacuum-sealed
process (see supporting information for experimental details and
Figure S8). As expected, the belt-shaped PTO//Zn battery
-1
delivers a high specific capacity of 337 mAh g at a current
-1
density of 0.04 A g , and retains a commendable capacity of 122
-1
mAh g when fast fully charged in 44 s (at a current density of 10
-1
Figure 3. a) Galvanostatic discharge/charge curve of the belt-shaped battery at
flat (left) and folded in half (180˚) (right) states for one hundred times. b) Cycle
stability at successive various repeated bending states at a current density of 1
A g . c) Practical demonstrations of lightening LED lights (left) and motivating
an electric fan using one such battery (right).
A g ) (Figure S9), exhibiting the good rate capability that is close
to the aqueous PTO//Zn coin cell. Considering the potential
application in wearable electronic devices, we calculated the areal
and volumetric energy/power density of the belt-shaped cell using
-1
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In summary, rechargeable batteries have permeated various
aspects of human life. In addition, they are also the promising
large-scale energy storage devices for renewables and power
sources for future smart clothes or skin. However, it is also well
known that almost all rechargeable batteries contain toxic
elements in their components, which might result in huge
environment issues when disused. The aqueous PTO//Zn battery
exhibits not only promising electrochemical performance but also
the low-toxic and environmentally friendly nature, which
potentially sheds light on the future development of batteries. On
the other hand, it should be noted that such PTO//Zn architecture
is still at the infant stage. Besides the advantage of sustainable
and low toxic nature, the organic cathode (e.g. PTO) still suffers
from the low electronic conductivity. In addition, Zn-dendrite
formation on anode in mild aqueous electrolyte solution also limits
the cycle life of the battery. Therefore, to further optimize the
performance of electrode materials, respectively, should be the
next logic step for practical application of such battery.
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Entry for the Table of Contents
COMMUNICATION
Zhaowei Guo, Yuanyuan Ma, Xiaoli
Dong, Jianhang Huang, Yonggang
Wang*, and Yongyao Xia
Page No. – Page No.
Environment-Friendly and Flexible
Aqueous Zinc Battery Using an
Organic Cathode
An environment-friendly flexible aqueous zinc battery using organic cathode exhibits superior electrochemical and flexible
performances, demonstrated as promising large-scale energy storage device and power source for wearable electronic devices.
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