Multi-angle tracking synthetic kinetics of phase evolution in Li-rich Mn-based cathodes

Xu, Shenyang1; Chen, Zhefeng1; Zhao, Wenguang1; Ren, Wenju1,2; Hou, Chenxin1; Liu, Jiajie1; Wang, Wu3; Yin, Chong4; Tan, Xinghua1; Lou, Xiaobing5; Yao, Xiangming1; Gao, Zhihai1; Liu, Hao6; Wang, Lu1; Yin, Zuwei1; Qiu, Bao7; Hu, Bingwen5; Li, Tianyi8; Dong, Cheng1; Pan, Feng1; Zhang, Mingjian9

2024-06-04

10.1039/d3ee04199a

ENERGY & ENVIRONMENTAL SCIENCE   影响因子和分区

1754-5692

1754-5706

As commercial cathodes with the highest practical capacity, the structural nature of Li-rich Mn-based (LMR) cathodes, composite or solid solution, is still under debate. Due to the extreme structural similarity of two layered-phase components, namely, the monoclinic phase (C2/m) and rhombohedral phase (R (3) over barm), no single tool can resolve this concern alone. Herein, we combined multiple advanced techniques to comprehensively study the structural changes during synthesis of LMR cathodes from different aspects such as the elemental distribution, local structure, long-range structure, and short-range structure, revealing a clear process from the formation of two phases to the gradual phase fusion and eventually to a nearly solid solution. Particularly, X-ray pair distribution function (PDF) analysis combined with theoretical simulations reveals for the first time that the transition metal (TM)-TM distance increases with the progress of the phase fusion, which makes the short-range structural change in TM-TM atomic pairs an effective parameter for judging the extent of phase fusion. Eventually, excellent electrochemical performance was achieved by balancing capacity and cycling stability through adjusting the phase fusion to a medium extent in lithium and sodium two layered-phase components. This study establishes an approach to investigate the structural evolution in the complicated multiple-phase system and provides valuable insights into the design and optimization of cathodes by tuning the phase fusion extent.

SCI ; EI

英语

其他

National Natural Science Foundation of China-Guangdong Joint Fund[52172175] ; National Natural Science Foundation of China[JCYJ20210324130812033] ; Shenzhen Science and Technology Research Grant[ZDSYS20200922160400001] ; Shenzhen Key Laboratory of Eco-materials and Renewable Energy["2019ZT08L101","RCTDPT-2020-001"] ; Program from Guangdong Introducing Innovative and Entrepreneurial Teams[2021B1515130002] ; Basic and Applied Basic Research Foundation of Guangdong Province[1922018] ; Chemistry and Chemical Engineering Guangdong Laboratory[DE-AC02-06CH11357]

Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology

Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences

WOS:001215596000001

ROYAL SOC CHEMISTRY

Web of Science

1.Peking Univ, Sch Adv Mat, Shenzhen Grad Sch, Shenzhen 518055, Peoples R China
2.Chongqing Univ Posts & Telecommun, Sch Adv Mfg Engn, Chongqing 400065, Peoples R China
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen Key Lab Thermoelectr Mat, Shenzhen 518055, Peoples R China
4.Ningbo Ronbay Lithium Battery Mat Co Ltd, Ningbo 315400, Peoples R China
5.East China Normal Univ, Sch Phys & Elect Sci, Shanghai Key Lab Magnet Resonance, State Key Lab Precis Spect, Shanghai 200241, Peoples R China
6.Karlsruhe Inst Technol, Inst Appl Mat, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany
7.Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Peoples R China
8.Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
9.Chinese Univ Hong Kong, Sch Sci & Engn, Shenzhen 518172, Guangdong, Peoples R China

Xu, Shenyang,Chen, Zhefeng,Zhao, Wenguang,et al. Multi-angle tracking synthetic kinetics of phase evolution in Li-rich Mn-based cathodes[J]. ENERGY & ENVIRONMENTAL SCIENCE,2024,17(11).

Xu, Shenyang.,Chen, Zhefeng.,Zhao, Wenguang.,Ren, Wenju.,Hou, Chenxin.,...&Zhang, Mingjian.(2024).Multi-angle tracking synthetic kinetics of phase evolution in Li-rich Mn-based cathodes.ENERGY & ENVIRONMENTAL SCIENCE,17(11).

Xu, Shenyang,et al."Multi-angle tracking synthetic kinetics of phase evolution in Li-rich Mn-based cathodes".ENERGY & ENVIRONMENTAL SCIENCE 17.11(2024).