Mitigating the Kinetic Hindrance of Single‐Crystalline Ni‐Rich Cathode via Surface Gradient Penetration of Tantalum
Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining exp...
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| Published in | Angewandte Chemie International Edition Vol. 60; no. 51; pp. 26535 - 26539 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Weinheim
Wiley Subscription Services, Inc
13.12.2021
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| Edition | International ed. in English |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high‐valence foreign Ta5+. The as‐obtained single‐crystalline LiNi0.8Co0.1Mn0.1O2 delivers a high specific capacity (211.2 mAh g−1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g−1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li+ kinetic hindrance of the appealing single‐crystalline Ni‐rich cathodes and will inspire peers to conduct an intensive study.
The Ta doping created some low‐valence Ni, decreasing the electrostatic repulsion between transition metal and Li+, thus the Li+ diffusion energy barrier has been decreased and the kinetic hindrance was mitigated. |
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| AbstractList | Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high‐valence foreign Ta5+. The as‐obtained single‐crystalline LiNi0.8Co0.1Mn0.1O2 delivers a high specific capacity (211.2 mAh g−1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g−1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li+ kinetic hindrance of the appealing single‐crystalline Ni‐rich cathodes and will inspire peers to conduct an intensive study. Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high‐valence foreign Ta5+. The as‐obtained single‐crystalline LiNi0.8Co0.1Mn0.1O2 delivers a high specific capacity (211.2 mAh g−1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g−1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li+ kinetic hindrance of the appealing single‐crystalline Ni‐rich cathodes and will inspire peers to conduct an intensive study. The Ta doping created some low‐valence Ni, decreasing the electrostatic repulsion between transition metal and Li+, thus the Li+ diffusion energy barrier has been decreased and the kinetic hindrance was mitigated. Single-crystalline Ni-rich cathodes are promising candidates for the next-generation high-energy Li-ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high-valence foreign Ta5+ . The as-obtained single-crystalline LiNi0.8 Co0.1 Mn0.1 O2 delivers a high specific capacity (211.2 mAh g-1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g-1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li+ kinetic hindrance of the appealing single-crystalline Ni-rich cathodes and will inspire peers to conduct an intensive study.Single-crystalline Ni-rich cathodes are promising candidates for the next-generation high-energy Li-ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li+ intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high-valence foreign Ta5+ . The as-obtained single-crystalline LiNi0.8 Co0.1 Mn0.1 O2 delivers a high specific capacity (211.2 mAh g-1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g-1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li+ kinetic hindrance of the appealing single-crystalline Ni-rich cathodes and will inspire peers to conduct an intensive study. Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate capability and low specific capacity due to the severe kinetic hindrance at the nondilute state during Li + intercalation. Herein, combining experiments with density functional theory (DFT) calculations, we demonstrate that this obstacle can be tackled by regulating the oxidation state of nickel via injecting high‐valence foreign Ta 5+ . The as‐obtained single‐crystalline LiNi 0.8 Co 0.1 Mn 0.1 O 2 delivers a high specific capacity (211.2 mAh g −1 at 0.1 C), high initial Coulombic efficiency (93.8 %), excellent rate capability (157 mAh g −1 at 4 C), and good durability (90.4 % after 100 cycles under 0.5 C). This work provides a strategy to mitigate the Li + kinetic hindrance of the appealing single‐crystalline Ni‐rich cathodes and will inspire peers to conduct an intensive study. |
| Author | Mao, Huican Meng, Xin‐Hai Sheng, Hang Yu, Xiqian Zou, Yu‐Gang Guo, Yu‐Guo Shi, Ji‐Lei Du, Ya‐Hao |
| Author_xml | – sequence: 1 givenname: Yu‐Gang surname: Zou fullname: Zou, Yu‐Gang organization: University of Chinese Academy of Sciences (UCAS) – sequence: 2 givenname: Huican surname: Mao fullname: Mao, Huican organization: Chinese Academy of Sciences – sequence: 3 givenname: Xin‐Hai surname: Meng fullname: Meng, Xin‐Hai organization: University of Chinese Academy of Sciences (UCAS) – sequence: 4 givenname: Ya‐Hao surname: Du fullname: Du, Ya‐Hao organization: Chinese Academy of Sciences – sequence: 5 givenname: Hang surname: Sheng fullname: Sheng, Hang organization: University of Chinese Academy of Sciences (UCAS) – sequence: 6 givenname: Xiqian surname: Yu fullname: Yu, Xiqian organization: Chinese Academy of Sciences – sequence: 7 givenname: Ji‐Lei surname: Shi fullname: Shi, Ji‐Lei email: jileishi@iccas.ac.cn organization: University of Chinese Academy of Sciences (UCAS) – sequence: 8 givenname: Yu‐Guo orcidid: 0000-0003-0322-8476 surname: Guo fullname: Guo, Yu‐Guo email: ygguo@iccas.ac.cn organization: University of Chinese Academy of Sciences (UCAS) |
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| Snippet | Single‐crystalline Ni‐rich cathodes are promising candidates for the next‐generation high‐energy Li‐ion batteries. However, they still suffer from poor rate... Single-crystalline Ni-rich cathodes are promising candidates for the next-generation high-energy Li-ion batteries. However, they still suffer from poor rate... |
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| SubjectTerms | Cathodes Crystal structure Crystallinity Density functional theory kinetic hindrance Li-ion batteries Lithium-ion batteries Ni-rich cathode Nickel Oxidation Specific capacity surface doping Tantalum Valence |
| Title | Mitigating the Kinetic Hindrance of Single‐Crystalline Ni‐Rich Cathode via Surface Gradient Penetration of Tantalum |
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