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Title: Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries

Abstract

Owing to their high specific capacity and suitably low operating potential, silicon-based anodes are an attractive alternative to graphite in next-generation lithium-ion batteries. However, silicon anodes suffer from low initial coulombic efficiency and fast capacity decay, limiting their widespread application. Pre-lithiation strategies are highly appealing to compensate for irreversible active lithium loss and to boost the cell energy density. In this work, we maximize the cell energy density by direct pre-lithiation of the NMC (LiNi0.5Mn0.3Co0.2O2) cathode to Li1+xNMCO2 without introducing inactive deadweight to either electrode. First, we demonstrate that Li1+xNMCO2 can be synthesized chemically, via reaction between NMC and lithium napthalide, and electrochemically. The NMC cathode is tolerant of a one-time over-lithiation up to 60 mA h gNMC-1, giving capacity retention on par with untreated NMC in half cell electrochemical cycling. Using synchrotron X-ray absorption spectroscopy (ex situ) and diffraction (in situ), we demonstrate that higher amounts of over-lithiation lead to local structure distortion – driven by transition metal reduction to Jahn–Teller active Mn3+ and Co2+ – as well as bulk structural hysteresis during over-lithiation and layer “buckling” that increases the amount of lithium extracted from the structure in the charged state. The Li1+xNMCO2 with low-to-moderate over-lithiation capacity (23, 46,more » and 70 mA h gNMC-1) is proven to be a highly effective dual-purpose lithium source and cathode material in full cell tests with a commercially relevant Si–graphite anode. These cells show higher capacity, superior cycle life, and improved coulombic efficiencies when compared to those with stoichiometric NMC cathodes. Finally, this study introduces a new and simple method to pre-lithiate layered transition metal oxide cathodes, opening up new possibilities for the development of high energy density lithium-ion batteries with next-generation anodes.« less

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2];  [2];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Cambridge (United Kingdom)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE
OSTI Identifier:
1798133
Alternate Identifier(s):
OSTI ID: 1784357
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 9; Journal Issue: 21; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Dose, Wesley M., Kim, Soojeong, Liu, Qian, Trask, Stephen E., Dunlop, Alison R., Ren, Yang, Zhang, Zhengcheng, Fister, Timothy T., and Johnson, Christopher S. Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries. United States: N. p., 2021. Web. doi:10.1039/d1ta01290h.
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Dose, Wesley M., Kim, Soojeong, Liu, Qian, Trask, Stephen E., Dunlop, Alison R., Ren, Yang, Zhang, Zhengcheng, Fister, Timothy T., & Johnson, Christopher S. Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries. United States. https://doi.org/10.1039/d1ta01290h
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Dose, Wesley M., Kim, Soojeong, Liu, Qian, Trask, Stephen E., Dunlop, Alison R., Ren, Yang, Zhang, Zhengcheng, Fister, Timothy T., and Johnson, Christopher S. Fri . "Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries". United States. https://doi.org/10.1039/d1ta01290h. https://www.osti.gov/servlets/purl/1798133.
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@article{osti_1798133,
title = {Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries},
author = {Dose, Wesley M. and Kim, Soojeong and Liu, Qian and Trask, Stephen E. and Dunlop, Alison R. and Ren, Yang and Zhang, Zhengcheng and Fister, Timothy T. and Johnson, Christopher S.},
abstractNote = {Owing to their high specific capacity and suitably low operating potential, silicon-based anodes are an attractive alternative to graphite in next-generation lithium-ion batteries. However, silicon anodes suffer from low initial coulombic efficiency and fast capacity decay, limiting their widespread application. Pre-lithiation strategies are highly appealing to compensate for irreversible active lithium loss and to boost the cell energy density. In this work, we maximize the cell energy density by direct pre-lithiation of the NMC (LiNi0.5Mn0.3Co0.2O2) cathode to Li1+xNMCO2 without introducing inactive deadweight to either electrode. First, we demonstrate that Li1+xNMCO2 can be synthesized chemically, via reaction between NMC and lithium napthalide, and electrochemically. The NMC cathode is tolerant of a one-time over-lithiation up to 60 mA h gNMC-1, giving capacity retention on par with untreated NMC in half cell electrochemical cycling. Using synchrotron X-ray absorption spectroscopy (ex situ) and diffraction (in situ), we demonstrate that higher amounts of over-lithiation lead to local structure distortion – driven by transition metal reduction to Jahn–Teller active Mn3+ and Co2+ – as well as bulk structural hysteresis during over-lithiation and layer “buckling” that increases the amount of lithium extracted from the structure in the charged state. The Li1+xNMCO2 with low-to-moderate over-lithiation capacity (23, 46, and 70 mA h gNMC-1) is proven to be a highly effective dual-purpose lithium source and cathode material in full cell tests with a commercially relevant Si–graphite anode. These cells show higher capacity, superior cycle life, and improved coulombic efficiencies when compared to those with stoichiometric NMC cathodes. Finally, this study introduces a new and simple method to pre-lithiate layered transition metal oxide cathodes, opening up new possibilities for the development of high energy density lithium-ion batteries with next-generation anodes.},
doi = {10.1039/d1ta01290h},
journal = {Journal of Materials Chemistry. A},
number = 21,
volume = 9,
place = {United States},
year = {Fri May 21 00:00:00 EDT 2021},
month = {Fri May 21 00:00:00 EDT 2021}
}
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