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Title: A redox-active organic cation for safer high energy density Li-ion batteries

Abstract

Ni-rich layered cathode materials are at the forefront to be deployed in high energy density Li-ion batteries for the automotive market. However, the intrinsic poor structural and interfacial stability during overcharging could trigger violent thermal failure, which severely limits their wide application. To protect the Ni-rich cathode from overcharging, we firstly report a redox-active cation, thioether-substituted diaminocyclopropenium, as an electrolyte additive to limit the cell voltage within the safe value during overcharging. The organic cation demonstrates a record-breaking electrochemical reversibility at ~4.55 V versus Li+/Li and solubility (0.5 M) in carbonate-based electrolyte. The protection capability of the additive was explored in two cell chemistries: a LiNi0.8Co0.15Al0.05O2/graphite cell and a LiNi0.8Co0.15Al0.05O2/silicon–graphene cell with areal capacities of ~2.2 mA h cm-2 and ~3 mA h cm-2, respectively. With 0.2 M addition, the LiNi0.8Co0.15Al0.05O2/graphite cell survived 54 cycles at 0.2C with 100% overcharge. Moreover, the cell can carry an utmost 4.4 mA cm-2 (2C) with 100% overcharge and a maximum capacity of 7540% SOC at 0.2C.

Authors:
 [1];  [2]; ORCiD logo [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
  2. Cornell Univ., Ithaca, NY (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1799555
Alternate Identifier(s):
OSTI ID: 1646936
Grant/Contract Number:  
EE0008859
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 8; Journal Issue: 33; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Chemistry; Energy & Fuels; Materials Science

Citation Formats

Ji, Weixiao, Huang, He, Huang, Xingkang, Zhang, Xiaoxiao, Zheng, Dong, Ding, Tianyao, Chen, Junhong, Lambert, Tristan H., and Qu, Deyang. A redox-active organic cation for safer high energy density Li-ion batteries. United States: N. p., 2020. Web. doi:10.1039/d0ta06133f.
Ji, Weixiao, Huang, He, Huang, Xingkang, Zhang, Xiaoxiao, Zheng, Dong, Ding, Tianyao, Chen, Junhong, Lambert, Tristan H., & Qu, Deyang. A redox-active organic cation for safer high energy density Li-ion batteries. United States. https://doi.org/10.1039/d0ta06133f
Ji, Weixiao, Huang, He, Huang, Xingkang, Zhang, Xiaoxiao, Zheng, Dong, Ding, Tianyao, Chen, Junhong, Lambert, Tristan H., and Qu, Deyang. Sun . "A redox-active organic cation for safer high energy density Li-ion batteries". United States. https://doi.org/10.1039/d0ta06133f. https://www.osti.gov/servlets/purl/1799555.
@article{osti_1799555,
title = {A redox-active organic cation for safer high energy density Li-ion batteries},
author = {Ji, Weixiao and Huang, He and Huang, Xingkang and Zhang, Xiaoxiao and Zheng, Dong and Ding, Tianyao and Chen, Junhong and Lambert, Tristan H. and Qu, Deyang},
abstractNote = {Ni-rich layered cathode materials are at the forefront to be deployed in high energy density Li-ion batteries for the automotive market. However, the intrinsic poor structural and interfacial stability during overcharging could trigger violent thermal failure, which severely limits their wide application. To protect the Ni-rich cathode from overcharging, we firstly report a redox-active cation, thioether-substituted diaminocyclopropenium, as an electrolyte additive to limit the cell voltage within the safe value during overcharging. The organic cation demonstrates a record-breaking electrochemical reversibility at ~4.55 V versus Li+/Li and solubility (0.5 M) in carbonate-based electrolyte. The protection capability of the additive was explored in two cell chemistries: a LiNi0.8Co0.15Al0.05O2/graphite cell and a LiNi0.8Co0.15Al0.05O2/silicon–graphene cell with areal capacities of ~2.2 mA h cm-2 and ~3 mA h cm-2, respectively. With 0.2 M addition, the LiNi0.8Co0.15Al0.05O2/graphite cell survived 54 cycles at 0.2C with 100% overcharge. Moreover, the cell can carry an utmost 4.4 mA cm-2 (2C) with 100% overcharge and a maximum capacity of 7540% SOC at 0.2C.},
doi = {10.1039/d0ta06133f},
journal = {Journal of Materials Chemistry. A},
number = 33,
volume = 8,
place = {United States},
year = {Sun Jun 21 00:00:00 EDT 2020},
month = {Sun Jun 21 00:00:00 EDT 2020}
}

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