journal article·2025-01Open access

Quantitative Identification of Dopant Occupation in Li‐Rich Cathodes

Tianhao Wu, Xu Zhang, Yuqiang Li, Haozhe Du, Tongchao Liu, Yubo Yang, Zihe Zhang, Xiaosong Liu, Qingzhen Huang, Yang Ren, Jiangtao Qu, Shu Zhao, Boya Wang, Rongkun Zheng, Khalil Amine, Haijun Yu

Advanced Materials· Volume 37· Issue 3

Abstract

Abstract Elemental doping is widely used to improve the performance of cathode materials in lithium‐ion batteries. However, macroscopic/statistical investigation on how doping sites are distributed in the material lattice, despite being a key prerequisite for understanding and manipulating the doping effect, has not been effectively established. Herein, to solve this predicament, a universal strategy is proposed to quantitatively identify the locations of Al and Mg dopants in lithium‐rich layered oxides (LLOs). Solid evidence confirms that Al prefers to occupy the transition metal (TM) layer, while Mg evenly occupies both TM and Li layers. As a result, Mg significantly reduces the thickness of LiO2 slabs at room temperature, which will increase the energy barrier of oxygen activation and enhance the structure stability of LLOs. The suppressed oxygen activity in Mg‐doped LLO can be kinetically unlocked at 55 °C. The different characteristics of Al and Mg enlighten an Al/Mg co‐doping strategy to optimize LLOs, which significantly improves the cycle performance while lifting the capacity. These insights from the quantitative identification of doping sites shed light on the manipulation of doping effects toward better cathodes.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Extraction and Separation Processes

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Advanced Battery Materials and Devices College of Materials Science and Engineering Beijing University of Technology Beijing 100124 P. R. China

Key Laboratory of Advanced Functional Materials (Beijing University of Technology) Ministry of Education Beijing 100124 P. R. China

Chemical Sciences and Engineering Division Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA

Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai 200050 P. R. China

NIST Center for Neutron Research National Institute of Standards and Technology Gaithersburg MD 20899 USA

Department of Physics and Centre for Neutron Scattering City University of Hong Kong Hong Kong 999077 P. R. China

Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 P. R. China

Aerospace Mechanical and Mechatronic Engineering The University of Sydney Sydney NSW 2006 Australia

School of Physics The University of Sydney Sydney NSW 2006 Australia

Funding

National Natural Science Foundation of China · Vehicle Technologies Office · Key Technologies Research and Development Program · Beijing Municipal Natural Science Foundation

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