journal article·2023-02-10Open access

Stabilizing a Li–Mn–O Cathode by Blocking Lattice O Migration through a Nanoscale Phase Complex

Weiyuan Huang, Mingjian Zhang, Mingyuan Ge, Shunning Li, Lin Xie, Zhefeng Chen, Gang Wang, Junhao Lin, Jimin Qiu, Lei Yu, Jianguo Wen, Guo-Xi Ren, Cong Lin, Wenguang Zhao, Haibiao Chen, Feng Pan

ACS Energy Letters· Volume 8· Issue 2

Abstract

Among all intercalation cathodes for Li-ion batteries, Li–Mn–O layered oxides offer the highest initial energy density at the lowest cost, due to the joint contribution from cationic and anionic redox chemistry. However, the poor cycling capability, resulting from the continuous lattice O loss at high potentials (>4.5 V), hinders practical applications. Herein, we employed phase complex engineering to obtain a new Li–Mn–O nanohybrid cathode featuring the uniform and coherent integration of layered nanodomains and spinel nanodomains. The combination of DFT calculations, synchrotron-based transmission X-ray microscopy, in situ differential electrochemical mass spectrometry, in situ synchrotron XRD, and electrochemical tests demonstrated that the O migration path in layered nanodomains was blocked by the neighboring spinel nanodomains with a higher oxygen vacancy migration energy, thus effectively suppressing the irreversible lattice O loss at high potentials and enhancing the cycling stability in both capacity and average voltage. The strategy is experimentally demonstrated to be effective and it leads to a new path for developing stable high-energy-density cathode materials.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research

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Affiliations

School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, People’s Republic of China

School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518172, People’s Republic of China

National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United States

Department of Physics, Southern University of Science and Technology, Shenzhen 518055, Guangdong People’s Republic of China

Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, United States

State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, People’s Republic of China

Institute of Marine Biomedicine, Shenzhen Polytechnic, Shenzhen 518055, People’s Republic of China

Funding

Guangdong Science and Technology Department · Science and Technology Foundation of Shenzhen City · Development and Reform Commission of Shenzhen Municipality · National Natural Science Foundation of China · Natural Science Foundation of Guangdong Province · Soft Science Research Project of Guangdong Province

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