Manipulating the Dispersed Domain of Pinning Dopants in Layered Oxide Cathodes for Sodium‐Ion Batteries
Abstract
ABSTRACT Layered oxide cathodes are primary candidates for high‐performance sodium‐ion batteries, which often suffer from structural degradation during deep Na + (de)intercalation processes. Incorporating electrochemically inactive cations into the transition metal (TM) layers has emerged as a mainstream strategy to enhance structural stability through the so‐called pinning effect. However, the microstructural heterogeneity of inactive cations within the TM layers and the spatial extent of their influence remain poorly understood. In this work, we regulate the pinning domain by modulating configurational entropy of inactive ions (S config ‐I), thereby promoting their dispersion and maximizing the spatial extent of the pinning effect. Additionally, we establish a correlation between S config ‐I and local structural fluctuations using quantitative experimental analyses. Compared with samples lacking sufficient pinning domains, the sample with 21% S config ‐I (denoted as S‐I‐21%) exhibits markedly improved structural homogeneity and optimally dispersed pinning dopants. Accordingly, S‐I‐21% delivers a high reversible capacity of 145 mAh g −1 and maintains ∼80% capacity retention after 500 cycles within a wide voltage window (2.0−4.3 V). These findings highlight the effect domain of dopants and their role in regulating structural chemistry, providing design principles for robust layered cathodes.
Article Details
Authors (14)
Ziheng Zhang
Machuan Hou
State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Academy of Advanced Interdisciplinary Studies College of Chemistry Nankai University Tianjin China
Jiangtao Yu
Frontiers Science Center for New Organic Matter, State Key Laboratory of Advanced Chemical Power Sources, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Academy of Advanced Inter Disciplinary Studies, College of Chemistry
Peixin Jiao
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (MOE), College of Chemistry
Jing Liu
Yanxia Deng
State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Academy of Advanced Interdisciplinary Studies College of Chemistry Nankai University Tianjin China
Meihong Che
State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Academy of Advanced Interdisciplinary Studies College of Chemistry Nankai University Tianjin China
Jiahua Zhao
Zixin Liang
School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing China
Lunhua He
Limin Zhou
School of Energy and Power Engineering
Zhenhua Yan
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry
Jun Chen
Kai Zhang