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Supporting Information
Durable, Flexible Self-standing Hydrogel Electrolyte
Enabling High-safety Rechargeable Solid-state Zinc Metal
Battery Qi Hana,b, Xiaowei Chi*,a, Shuming Zhanga,b, Yunzhao Liua,b, Biao Zhoua,b, Jianhua Yanga, Yu Liu*,aa Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, Chinab University of Chinese Academy of Sciences, 19 Yuquan Road, Beijing 100049, China
This file includes characterization of the materials, supplementary figures S1-S18.
Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A.This journal is © The Royal Society of Chemistry 2018
Fig. S1 Photographs of transformation of flowable gelation hydrogel electrolytes solution (gelatin dissolved in 0.5 M Li2SO4 and 0.5 M ZnSO4 aqueous solution) to solidified GHEs: (a) after heating; (b) after freezing, illustrating the reversible flowability of gelation electrolyte.
30 40 50 60
Temperature (°C)
Tg=38.4 °C
Exot
herm
ic
Fig. S2 DSC curve of the gelatin hydrogel electrolyte (GHE)
Fig. S3 Schematic diagram of the formation of network in GHEs. (a) Gelatin randomly dispersed in solution (upon heating), (b) Gelatin solidified to hydrogel (upon freezing).
Fig. S4 Photographs of GHEs. (a) Gelatin electrolyte separator, (b) Thick gelatin electrolyte under bending condition.
0 1 2 3 4 5
8
10
12
Z (n
m)
X (m)1 µm
(a) (b)
Fig. S5 (a) AFM image (5 µm×5 µm) of the GHE film; (b) Height profile at Y=2.5
µm in the section of (a)
-1.06 -1.04 -1.02 -1.00-8
-6
-4
-2
log
i (A
cm-2
)
Potential (V) vs SCE
AE GHE
Fig. S6 Tafel plots of the Zn anode in AE and GHE
0 200 400 600 800 1000 1200-0.6
-0.4
-0.2
0.0
0.2
0.4
0.6
Volta
ge (V
)
Cycle time (h)
0.1mA cm-2
Fig. S7 Galvanostatic cycling tests of solid-state Zn/GHE/Zn symmetric cell at 0.1 mA cm−2.
0 100 200 300 4000
100
200
After 800 h-Z''
()
Z' ()
Fig. S8 EIS plot of Zn/GHE/Zn battery after cycling for 800 h.
Fig. S9 SEM images of pristine AGM: (a) surface and (b) cross-section.
10 µm
1 µm
10 µm
1 µm
(a)
(b)
(c)
(d)
Fig. S10 SEM images of the GHEs before (a, b) and after (c, d) cycling in the symmetric cells
5 µm
(a) (b)
Zn
Fig. S11 (a) SEM image of the GHE after cycling; (b) mapping image of Zn element
0 50 100 150 20040
60
80
100
120
140
Coulombic efficiency (%
)
Cycle Number
Capa
city
(mAh
g1
)
100 mA g1
80
85
90
95
100
105
Fig. S12 Cycling performance of Zn/GHE/LMO full cells at a current density of 100 mA g1
(a) (b)
0 100 2000
50
100After 1 cycleAfter 100 cycles
-Z''
()
Z' (1.4 1.6 1.8 2.0 2.2
-0.8
-0.4
0.0
0.4
0.8
Potential (V) vs.Zn2+/Zn
0.5 mV s-1
Curr
ent d
ensit
y (m
A cm
-2)
0.1 mV s-1 0.2 mV s-1 0.5 mV s-1
0.1 mV s-1
Fig. S13 Electrochemical characterizations of solid-state Zn/GHE/LMO batteries: (a) CV curves at different scanning rates; (b) EIS plots at different cycles.
(b)(a)
0 20 40 60 80 10020
40
60
80
100
120
140
25 mA g-1
Cycle Number
Capa
city
Rent
entio
n (%
)
80
85
90
95
100
Coulombic efficiency (%
)
Fig. S14 (a) Cycle performance of Zn/LMO battery with AE at 25 mA g−1; (b) photographs of Zn/LMO batteries with AE and GHE after 100 cycles.
0 5 10 15 201.2
1.4
1.6
1.8
2.0
2.2 2 batteries in parallel Single battery
Volta
ge (V
)
Time (h)0 4 8 12
1.2
1.62.0
2.42.8
3.2
3.64.0
4.4
Volta
ge (V
)
Time (h)
2 batteries in series Single battery
(a) (b)
Fig. S15 Galvanostatic charge-discharge curves of two batteries connected in (a) parallel and (b) serial.
0 50 100 150 200 250
1.4
1.6
1.8
2.0
2.2
246 247 248 249 250
1.4
1.6
1.8
0 2 4 6
1.6
1.8
2.0
2.2Columbic efficiency : 60.35%, 49.19%
Rest 240 h
Pote
ntia
l (V)
vs Z
n2+ /Z
n
Time (h)
GHE AE
1.8052 V
1.8493 V
Fig. S16 Comparison of self-discharge performances of batteries based on AE and GHE.
Fig. S17 Photograph of GHE soaked in pure water (a) and water added with several drops of 1 M BaCl2 solution (b).
Fig. S18 Photographs of interdigitated Zn/GHE/LMO solid-state battery at different conditions.