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Title: A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm–2 and 20 mAh cm–2

Abstract

Metal anodes represent as a prime choice for the coming generation rechargeable batteries with high energy density. However, daunting challenges including electrode volume variation and inevitable side reactions preclude them from becoming a viable technology. Here, a facile replacement reaction was employed to fabricate a three-dimensional (3D) interdigitated metal/solid electrolyte composite electrode, which not only provides a stable host structure for buffering the volume change within the composite but also prevents side reactions by avoiding the direct contact between active metal and liquid electrolyte. As a proof-of-concept demonstration, a 3D interdigitated zinc (Zn) metal/solid electrolyte architecture was fabricated via a galvanic replacement reaction between Zn metal foil and indium (In) chloride solution followed by electrochemical activation, featuring the interdigitation between metallic Zn and amorphous indium hydroxide sulfate (IHS) with high Zn2+ conductivity (56.9 ± 1.8 mS cm–1), large Zn2+ transference number (0.55), and high electronic resistivity [(2.08 ± 0.01) × 103 Ω cm]. The as-designed Zn/IHS electrode sustained stable electrochemical Zn plating/stripping over 700 cycles with a record-low overpotential of 8 mV at 1 mA cm–2 and 0.5 mAh cm–2. More impressively, it displayed cycle-stable performance with low overpotential of 10 mV under ultrahigh current density and areal capacity (20more » mA cm–2, 20 mAh cm–2), which outperformed all the reported Zn metal electrodes in mild aqueous electrolyte. The fabrication of interdigitated metal/solid electrolyte was generalized to other metal pairs, including Zn/Sn and Zn/Co, which provide inspiration for next-generation Zn metal batteries with high energy density and reversibility.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]
  1. Huazhong Univ. of Science and Technology, Wuhan (China)
  2. Tsinghua Univ., Beijing (China)
  3. Agency for Science, Technology and Research (A*STAR) (Singapore)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1766786
Alternate Identifier(s):
OSTI ID: 1776636
Report Number(s):
BNL-221049-2021-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
SC0012704; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 143; Journal Issue: 8; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; batteries; interphase; solid electrolytes; metals; electrodes; electrochemical cells; electrolytes

Citation Formats

Cai, Zhao, Ou, Yangtao, Zhang, Bao, Wang, Jindi, Fu, Lin, Wan, Mintao, Li, Guocheng, Wang, Wenyu, Wang, Li, Jiang, Jianjun, Seh, Zhi Wei, Hu, Enyuan, Yang, Xiao-Qing, Cui, Yi, and Sun, Yongming. A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm–2 and 20 mAh cm–2. United States: N. p., 2021. Web. doi:10.1021/jacs.0c11753.
Cai, Zhao, Ou, Yangtao, Zhang, Bao, Wang, Jindi, Fu, Lin, Wan, Mintao, Li, Guocheng, Wang, Wenyu, Wang, Li, Jiang, Jianjun, Seh, Zhi Wei, Hu, Enyuan, Yang, Xiao-Qing, Cui, Yi, & Sun, Yongming. A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm–2 and 20 mAh cm–2. United States. https://doi.org/10.1021/jacs.0c11753
Cai, Zhao, Ou, Yangtao, Zhang, Bao, Wang, Jindi, Fu, Lin, Wan, Mintao, Li, Guocheng, Wang, Wenyu, Wang, Li, Jiang, Jianjun, Seh, Zhi Wei, Hu, Enyuan, Yang, Xiao-Qing, Cui, Yi, and Sun, Yongming. Wed . "A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm–2 and 20 mAh cm–2". United States. https://doi.org/10.1021/jacs.0c11753. https://www.osti.gov/servlets/purl/1766786.
@article{osti_1766786,
title = {A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm–2 and 20 mAh cm–2},
author = {Cai, Zhao and Ou, Yangtao and Zhang, Bao and Wang, Jindi and Fu, Lin and Wan, Mintao and Li, Guocheng and Wang, Wenyu and Wang, Li and Jiang, Jianjun and Seh, Zhi Wei and Hu, Enyuan and Yang, Xiao-Qing and Cui, Yi and Sun, Yongming},
abstractNote = {Metal anodes represent as a prime choice for the coming generation rechargeable batteries with high energy density. However, daunting challenges including electrode volume variation and inevitable side reactions preclude them from becoming a viable technology. Here, a facile replacement reaction was employed to fabricate a three-dimensional (3D) interdigitated metal/solid electrolyte composite electrode, which not only provides a stable host structure for buffering the volume change within the composite but also prevents side reactions by avoiding the direct contact between active metal and liquid electrolyte. As a proof-of-concept demonstration, a 3D interdigitated zinc (Zn) metal/solid electrolyte architecture was fabricated via a galvanic replacement reaction between Zn metal foil and indium (In) chloride solution followed by electrochemical activation, featuring the interdigitation between metallic Zn and amorphous indium hydroxide sulfate (IHS) with high Zn2+ conductivity (56.9 ± 1.8 mS cm–1), large Zn2+ transference number (0.55), and high electronic resistivity [(2.08 ± 0.01) × 103 Ω cm]. The as-designed Zn/IHS electrode sustained stable electrochemical Zn plating/stripping over 700 cycles with a record-low overpotential of 8 mV at 1 mA cm–2 and 0.5 mAh cm–2. More impressively, it displayed cycle-stable performance with low overpotential of 10 mV under ultrahigh current density and areal capacity (20 mA cm–2, 20 mAh cm–2), which outperformed all the reported Zn metal electrodes in mild aqueous electrolyte. The fabrication of interdigitated metal/solid electrolyte was generalized to other metal pairs, including Zn/Sn and Zn/Co, which provide inspiration for next-generation Zn metal batteries with high energy density and reversibility.},
doi = {10.1021/jacs.0c11753},
journal = {Journal of the American Chemical Society},
number = 8,
volume = 143,
place = {United States},
year = {Wed Feb 17 00:00:00 EST 2021},
month = {Wed Feb 17 00:00:00 EST 2021}
}

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