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An almost full reversible lithium-rich cathode: Revealing the mechanism of high initial coulombic efficiency

查看全文 作　　者：Dong [1]Luo;Jianming [2]Fan;Zhuo [1]Yao;Huixian [1]Xie;Jiaxiang [1]Cui;Yajun [1]Yang;Xiaokai [1]Ding;Jiapeng [3]Ji;Shuxing [1]Wu;Ming [3]Ling;Chenyu [1]Liu;Zhan [1]Lin 高影响力作者 机构地区：[1]Guangzhou Key Laboratory of Clean Transportation Energy Chemistry,School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou 510006,Guangdong,China;[2]Fujian Provincial Key Laboratory of Clean Energy Materials,College of Chemistry and Materials,Longyan University,Longyan 364012,Fujian,China;[3]Key Laboratory of Biomass Chemical Engineering of Ministry of Education,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,Zhejiang,China高影响力机构 出　　处：《Journal of Energy Chemistry》索引2021年第30卷第11期,共8页高影响力期刊 基　　金：We thank the funding supports of the National Natural Science Foundation of China(Project Nos.51874104 and 52004070);the Key Technology and Supporting Platform of Genetic Engineering of Materials under States Key Project of Research and Development Plan of China(Project No.2016YFB0700600).The authors thank Cheng-Hao Chuang for the assistant with X-ray spectroscopy measurement. 摘　　要：Low initial Coulombic efficiency (ICE) is an important impediment to practical application of Li-rich layered oxides (LLOs), which is due to the irreversible oxygen release. It is generally considered that surface oxygen vacancies are conducive to the improvement of ICE of LLOs. To reveal the relation of oxygen vacancies and ICE, sample PLO (Li-Mn-Cr-O) and its treated product (TLO) are comprehensive investigated in this work. During the treated process, part of oxygen atoms return to original constructed vacancies. It makes oxygen vacancies in sample TLO much poorer than those in sample PLO, and induces the formation of Li-poor spinel-layered integrated structure. Electrochemical measurement indicates the ICE of sample PLO is only 80.8%, while sample TLO is almost full reversible with the ICE of ~97.1%. In term of high-energy X-ray diffraction, scanning transmission electron microscopy, X-ray photoelectron spectroscopy and synchrotron hard/soft X-ray absorption spectroscopy, we discover that the ICE is difficult to be improved significantly just by building oxygen vacancies. LLOs with high ICE not only have to construct suitable oxygen vacancies, but also require other components with Li-poor structure to stabilize oxygen. This work provides deep insight into the mechanism of high ICE, and will contribute to the design and development of LLOs for next-generation high-energy lithium-ion batteries. 关 键 词：Li-ion batteries Li-rich layered oxides Initial coulombic efficiency Oxygen vacancies
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