Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2
ABSTRACT 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 su...
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| Format: | Article |
| Language: | English |
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Wiley
2025-06-01
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| Series: | Carbon Energy |
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| Online Access: | https://doi.org/10.1002/cey2.699 |
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| author | Peirong Li Yande Li Qi Liang Yize Niu Shun Zheng Zengqing Zhuo Yunhong Luo Bocheng Liang Dong Yang Jixiang Yin Supeng Chen Wanneng Ye Yuanyuan Pan Qinghao Li Pengfei Yu Xiaosong Liu Qiang Li |
| author_facet | Peirong Li Yande Li Qi Liang Yize Niu Shun Zheng Zengqing Zhuo Yunhong Luo Bocheng Liang Dong Yang Jixiang Yin Supeng Chen Wanneng Ye Yuanyuan Pan Qinghao Li Pengfei Yu Xiaosong Liu Qiang Li |
| author_sort | Peirong Li |
| collection | DOAJ |
| description | ABSTRACT 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 Li1.2Ni0.2Mn0.6O2. 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. |
| format | Article |
| id | doaj-art-da8f26f1d37d4221bb2e0231b9effa18 |
| institution | Kabale University |
| issn | 2637-9368 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Wiley |
| record_format | Article |
| series | Carbon Energy |
| spelling | doaj-art-da8f26f1d37d4221bb2e0231b9effa182025-08-20T03:30:02ZengWileyCarbon Energy2637-93682025-06-0176n/an/a10.1002/cey2.699Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2Peirong Li0Yande Li1Qi Liang2Yize Niu3Shun Zheng4Zengqing Zhuo5Yunhong Luo6Bocheng Liang7Dong Yang8Jixiang Yin9Supeng Chen10Wanneng Ye11Yuanyuan Pan12Qinghao Li13Pengfei Yu14Xiaosong Liu15Qiang Li16College of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaShanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaSchool of Chemistry and Chemical Engineering, in situ Center for Physical Sciences, Shanghai Jiao Tong University Global Institute of Future Technology Shanghai Jiao Tong University Shanghai ChinaAdvanced Light Source, Lawrence Berkeley National Laboratory Berkeley California USAShanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaCenter for Transformative Science ShanghaiTech University Shanghai ChinaNational Synchrotron Radiation Laboratory University of Science and Technology of China Hefei ChinaCollege of Physics, Center for Marine Observation and Communications Qingdao University Qingdao ChinaABSTRACT 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 Li1.2Ni0.2Mn0.6O2. 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.https://doi.org/10.1002/cey2.699anionic redox reactionoxygen releasesurface reorganizationTM dissolution |
| spellingShingle | Peirong Li Yande Li Qi Liang Yize Niu Shun Zheng Zengqing Zhuo Yunhong Luo Bocheng Liang Dong Yang Jixiang Yin Supeng Chen Wanneng Ye Yuanyuan Pan Qinghao Li Pengfei Yu Xiaosong Liu Qiang Li Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 Carbon Energy anionic redox reaction oxygen release surface reorganization TM dissolution |
| title | Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 |
| title_full | Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 |
| title_fullStr | Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 |
| title_full_unstemmed | Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 |
| title_short | Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2 |
| title_sort | uncovering the critical role of ni on surface lattice stability in anionic redox active li1 2ni0 2mn0 6o2 |
| topic | anionic redox reaction oxygen release surface reorganization TM dissolution |
| url | https://doi.org/10.1002/cey2.699 |
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