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Preparation and electrochemical properties of high-stability cathode prelithiation additive
Author NameAffiliationE-mail
JIANG Yuanyuan Zhejiang Narada Power Source Co., Ltd., Hangzhou 311300, China
School of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China 		 
TU Fangfang Zhejiang Narada Power Source Co., Ltd., Hangzhou 311300, China tuff@naradapower.com 
ZHANG Yuhong Zhejiang Narada Power Source Co., Ltd., Hangzhou 311300, China  
CHEN Shi Zhejiang Narada Power Source Co., Ltd., Hangzhou 311300, China  
XIANG Jiayuan Zhejiang Narada Power Source Co., Ltd., Hangzhou 311300, China  
XIA Xinhui School of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China  
Abstract: In this work, based on the catalytic effect of several metal oxides on the decomposition of lithium oxalate (Li2C2O4, LCO), a series of CuMnxO1+1.5x bimetallic oxides with different molar ratios (x) of Mn and Cu were synthesized via the controlled calcination of CuO-Mn2O3 mixture. The structural composition and surface morphology were characterized using the X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 adsorption-desorption isotherms, and scanning electron microscopy (SEM). The catalysts were applied in the electrochemical test of LCO at 0.05C within the voltage range of 2.5-4.5 V. Results showed that the charge specific capacity of LCO could be increased to 404.7 mAh·g-1 and delithium potential can be reduced to 4.44 V with the initial Coulombic efficiency of 1.3% over CuMn1.1O2.7 catalyst, which could match with the lithium iron phosphate (LFP) materials as a cathode prelithiation additive. The rate-determining step of LCO decomposition and the mechanism of the catalyst were revealed by density functional theory (DFT) calculations. Subsequently, a certain amount of LCO/CuMn1.1O2.7 was added to the LFP slurry, and the corresponding electrochemical performance was tested by assembling half-cells. It was found that under the optimal lithium supplement content, the initial charge capacity of the LFP electrode was 205.9 mAh·g-1, and the practical capacity utilization of LCO could reach 74.1%. Moreover, the cycle performance of LFP can also be improved by using an LCO prelithiation additive.
Keywords: lithium iron phosphate  cathode prelithiation additive  lithium oxalate  metal oxide
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JIANG Yuanyuan,TU Fangfang,ZHANG Yuhong,CHEN Shi,XIANG Jiayuan,XIA Xinhui.Preparation and electrochemical properties of high-stability cathode prelithiation additive[J].Chinese Journal of Inorganic Chemistry,2025,41(6):1101-1111.
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Chinese Journal of Inorganic Chemistry