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Title: Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries

Abstract

The formation of solid-electrolyte interphase (SEI) in “water-in-salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long-term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both anode and cathode surfaces, and enables LiMn2O4||L-TiO2 full cells with high specific capacity (157 mAh g–1 at 1 C), long-term cycling stability (80% capacity retention within 200 cycles at 1 C), and high rate capability (79 mAh g–1 at 30 C). The in situ electropolymerization found in this work provides an alternative and highly effective strategy to design protective interphases at the negative and positive electrodes for high-voltage aqueous batteries of lithium-ion or beyond.

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [6];  [7];  [3];  [2];  [2];  [8]; ORCiD logo [7]
  1. Forschungszentrum Juelich (Germany). Helmholtz-Institut Münster
  2. Army Research Lab., Adelphi, MD (United States)
  3. Peking Univ., Shenzhen (China)
  4. Sichuan Univ., Chengdu (China)
  5. Southern University of Science and Technology (SUSTech), Shenzhen (China)
  6. University of Muenster (Germany)
  7. Forschungszentrum Juelich (Germany). Helmholtz-Institut Münster; Politecnico di Milano (Italy)
  8. Forschungszentrum Juelich (Germany). Helmholtz-Institut Münster; University of Muenster (Germany)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Sponsoring Org.:
USDOE; US Army Research Laboratory (USARL)
OSTI Identifier:
1981439
Grant/Contract Number:  
AC02-06CH11357; W911NF-19-2-0046
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 18; Journal Issue: 5; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; "water-in-salt" electrolytes; cathode-electrolyte interphases; high-voltage aqueous lithium-ion batteries; in situ electropolymerization; solid-electrolyte interphases

Citation Formats

Hou, Xu, Pollard, Travis P., Zhao, Wenguang, He, Xin, Ju, Xiaokang, Wang, Jun, Du, Leilei, Paillard, Elie, Lin, Hai, Xu, Kang, Borodin, Oleg, Winter, Martin, and Li, Jie. Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries. United States: N. p., 2021. Web. doi:10.1002/smll.202104986.
Hou, Xu, Pollard, Travis P., Zhao, Wenguang, He, Xin, Ju, Xiaokang, Wang, Jun, Du, Leilei, Paillard, Elie, Lin, Hai, Xu, Kang, Borodin, Oleg, Winter, Martin, & Li, Jie. Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries. United States. https://doi.org/10.1002/smll.202104986
Hou, Xu, Pollard, Travis P., Zhao, Wenguang, He, Xin, Ju, Xiaokang, Wang, Jun, Du, Leilei, Paillard, Elie, Lin, Hai, Xu, Kang, Borodin, Oleg, Winter, Martin, and Li, Jie. Wed . "Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries". United States. https://doi.org/10.1002/smll.202104986. https://www.osti.gov/servlets/purl/1981439.
@article{osti_1981439,
title = {Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries},
author = {Hou, Xu and Pollard, Travis P. and Zhao, Wenguang and He, Xin and Ju, Xiaokang and Wang, Jun and Du, Leilei and Paillard, Elie and Lin, Hai and Xu, Kang and Borodin, Oleg and Winter, Martin and Li, Jie},
abstractNote = {The formation of solid-electrolyte interphase (SEI) in “water-in-salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long-term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both anode and cathode surfaces, and enables LiMn2O4||L-TiO2 full cells with high specific capacity (157 mAh g–1 at 1 C), long-term cycling stability (80% capacity retention within 200 cycles at 1 C), and high rate capability (79 mAh g–1 at 30 C). The in situ electropolymerization found in this work provides an alternative and highly effective strategy to design protective interphases at the negative and positive electrodes for high-voltage aqueous batteries of lithium-ion or beyond.},
doi = {10.1002/smll.202104986},
journal = {Small},
number = 5,
volume = 18,
place = {United States},
year = {Wed Dec 01 00:00:00 EST 2021},
month = {Wed Dec 01 00:00:00 EST 2021}
}

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