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...

Full description

Saved in:
Bibliographic Details
Published in:Angewandte Chemie International Edition 2021-12, Vol.60 (51), p.26535-26539
Main Authors: Zou, Yu‐Gang, Mao, Huican, Meng, Xin‐Hai, Du, Ya‐Hao, Sheng, Hang, Yu, Xiqian, Shi, Ji‐Lei, Guo, Yu‐Guo
Format: Article
Language:English
Subjects:
Batteries
Cathodes
Crystal structure
Crystallinity
Density functional theory
Durability
kinetic hindrance
Li-ion batteries
Lithium-ion batteries
Ni-rich cathode
Nickel
Oxidation
Specific capacity
surface doping
Tantalum
Valence
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary: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.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202111954