Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2

Li, Peirong; Li, Yande; Liang, Qi; Niu, Yize; Zheng, Shun; Zhuo, Zengqing; Luo, Yunhong; Liang, Bocheng; Yang, Dong; Yin, Jixiang; Chen, Supeng; Ye, Wanneng; Pan, Yuanyuan; Li, Qinghao; Yu, Pengfei; Liu, Xiaosong; Li, Qiang

doi:10.1002/cey2.699

Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li_1.2Ni_0.2Mn_0.6O₂

Journal Article · Wed Mar 19 00:00:00 EDT 2025 · Carbon Energy

DOI:https://doi.org/10.1002/cey2.699· OSTI ID:2553921

Li, Peirong ^[1]; Li, Yande ^[2]; Liang, Qi ^[1]; Niu, Yize ^[1]; Zheng, Shun ^[3]; ^[4]; Luo, Yunhong ^[2]; Liang, Bocheng ^[1]; Yang, Dong ^[1]; Yin, Jixiang ^[1]; Chen, Supeng ^[1]; Ye, Wanneng ^[1]; Pan, Yuanyuan ^[1]; Li, Qinghao ^[1]; Yu, Pengfei ^[5]; Liu, Xiaosong ^[6]; ^[1]

Qingdao University (China)
Chinese Academy of Sciences (CAS), Shanghai (China)
Shanghai Jiao Tong Univ. (China)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
ShanghaiTech University (China)
Univ. of Science and Technology of China, Hefei (China)

Anionic redox reaction (ARR) can provide extra capacity beyond transition metal (TM) redox in lithium-rich TM oxide cathodes. Practical ARR application is much hindered by the structure instability, particularly at the surface. Oxygen release has been widely accepted as the ringleader of surficial structure instability. However, the role of TM in surface stability has been much overlooked, not to mention its interplay with oxygen release. Herein, TM dissolution and oxygen release are comparatively investigated in Li_1.2Ni_0.2Mn_0.6O₂. Ni is verified to detach from the lattice counter-intuitively despite the overwhelming stoichiometry of Mn, facilitating subsequent oxygen release of the ARR process. Intriguingly, surface reorganization occurs following regulated Ni dissolution, enabling the stabilization of the surface and elimination of oxygen release in turn. Accordingly, a novel optimization strategy is proposed by adding a relaxation step at 4.50 V within the first cycle procedure. Battery performance can be effectively improved, with voltage decay suppressed from 3.44 mV/cycle to 1.60 mV/cycle, and cycle stability improved from 66.77% to 90.01% after 100 cycles. This work provides new perspectives for clarifying ARR surface instability and guidance for optimizing ARR performance.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2553921

Journal Information:: Carbon Energy, Journal Name: Carbon Energy Journal Issue: 6 Vol. 7; ISSN 2637-9368

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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TM dissolution
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oxygen release
surface reorganization

Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2

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Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li_1.2Ni_0.2Mn_0.6O₂