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Li-ion Batteries
Implanting Transition Metal into Li2O-Based Cathode Prelithiation
Agent for High-Energy-Density and Long-Life Li-Ion Batteries
Yilong Chen, Yuanlong Zhu, Wenhua Zuo, Xiaoxiao Kuai,* Junyi Yao, Baodan Zhang,
Zhefei Sun, Jianhua Yin, Xiaohong Wu, Haitang Zhang, Yawen Yan, Huan Huang,
Lirong Zheng, Juping Xu, Wen Yin, Yongfu Qiu, Qiaobao Zhang, Inhui Hwang,
Cheng-Jun Sun, Khalil Amine, Gui-Liang Xu,* Yu Qiao,* and Shi-Gang Sun
Abstract: Compensating the irreversible loss of limited
active lithium (Li) is essentially important for improving
the energy-density and cycle-life of practical Li-ion
battery full-cell, especially after employing high-capacity
but low initial coulombic efficiency anode candidates.
Introducing prelithiation agent can provide additional Li
source for such compensation. Herein, we precisely
implant trace Co (extracted from transition metal oxide)
into the Li site of Li2O, obtaining (Li0.66Co0.11&0.23)2O
(CLO) cathode prelithiation agent. The synergistic
formation of Li vacancies and Co-derived catalysis
efficiently enhance the inherent conductivity and weak-
en the LiO interaction of Li2O, which facilitates its
anionic oxidation to peroxo/superoxo species and gas-
eous O2, achieving 1642.7 mAh/g~Li2O prelithiation ca-
pacity ( �980 mAh/g for prelithiation agent). Coupled
6.5 wt% CLO-based prelithiation agent with LiCoO2
cathode, substantial additional Li source stored within
CLO is efficiently released to compensate the Li
consumption on the SiO/C anode, achieving 270 Wh/kg
pouch-type full-cell with 92 % capacity retention after
1000 cycles.
Introduction
To meet the demands of high-energy/power-density applica-
tions (such as electric vehicles), improving the energy
density of lithium-ion batteries (LIBs) is becoming espe-
cially important.[1] From the cathode perspective, adjusting
the upper charging voltage of LiCoO2(LCO) from 4.2 V to
4.48 V, which capacity presents 22 % increase.[2] However,
for the entire full-cell architecture (with limited amount of
available Li source), the formation of solid electrolyte
interphase (SEI) on the anode consumes massive active
lithium ions within the entire full-cell and results in a low
initial coulombic efficiency (ICE) and bring down actual
output energy density.[3] After the evolution from commer-
cial graphite anode (ICE >90 %) to other advanced high-
capacity anode candidates (e.g. silicon-based anodes, ICE <
80 %), intensified Li loss when the formation of SEI.[4] The
capacity improvement obtained by adjusting the cathode
cut-off potential is not enough to trade off the sacrifice of
active lithium in the initial cycling of the anode, which
severely limits the improvement of the energy density of
next-generation LIBs.[5]
To date, various prelithiation methods have been
developed to compensate for the Li loss from the ICE of
anode in the full-cell.[6] Cathode prelithiation is used to
[*] Y. Chen, Y. Zhu, X. Kuai, B. Zhang, J. Yin, X. Wu, H. Zhang, Y. Yan,
Y. Qiao, S.-G. Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces,
Department of Chemistry, College of Chemistry and Chemical
Engineering, Xiamen University
Xiamen, 361005 (P. R. China)
E-mail: kuaixiaoxiao@xmu.edu.cn
yuqiao@xmu.edu.cn
W. Zuo, K. Amine, G.-L. Xu
Chemical Sciences and Engineering Division, Argonne National
Laboratory
Lemont, IL 60439 (USA)
E-mail: xug@anl.gov
J. Yao
Department of Chemistr, Virginia Tech
Blacksburg, VA 24061 (USA)
Z. Sun, Q. Zhang
State Key Laboratory of Physical Chemistry of Solid Surfaces,
College of Materials, Xiamen University
Xiamen 361005, Fujian (China)
H. Huang, L. Zheng
Institute of High Energy Physics, Chinese Academy of Sciences
Beijing 100049 (P. R. China)
J. Xu, W. Yin
Institute of High Energy Physics, Chinese Academy of Sciences
Beijing 100049 (P. R. China)
and
Spallation Neutron Source Science Center
Dongguan 523803 (China)
Y. Qiu
School of Materials Science and Engineering, Dongguan University
of Technology
Guangdong 523808 (P. R. China)
I. Hwang, C.-J. Sun
X-ray Sciences Division, Argonne National Laboratory
Lemont, IL 60439 (USA)
X. Kuai, Y. Qiao
Fujian Science & Technology Innovation Laboratory for Energy
Materials of China (Tan Kah Kee Innovation Laboratory)
Xiamen 361005 (P. R. China)
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How to cite: Angew. Chem. Int. Ed. 2024,63, e202316112
doi.org/10.1002/anie.202316112
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