Reviving Sodium Tunnel Oxide Cathodes Based on Structural Modulation and Sodium Compensation Strategy Toward Practical Sodium‐Ion Cylindrical Battery

Author:

Liu Hanxiao12,Kong Lingyi12,Wang Hongrui3,Li Jiayang12,Wang Jingqiang12,Zhu Yanfang12,Li Hongwei12,Jian Zhuangchun12,Jia Xinbei12,Su Yu12,Zhang Shilin4,Mao Jianfeng4,Chen Shuangqiang12,Liu Yang12,Chou Shulei12ORCID,Xiao Yao12ORCID

Affiliation:

1. College of Chemistry and Materials Engineering Wenzhou University Wenzhou 325035 P. R. China

2. Wenzhou Key Laboratory of Sodium‐Ion Batteries Wenzhou University Technology Innovation Institute for Carbon Neutralization Wenzhou 325035 P. R. China

3. College of Science National University of Defense Technology Changsha 410073 P. R. China

4. School of Chemical Engineering & Advanced Materials University of Adelaide Adelaide SA 5005 Australia

Abstract

AbstractAs a typical tunnel oxide, Na0.44MnO2 features excellent electrochemical performance and outstanding structural stability, making it a promising cathode for sodium‐ion batteries (SIBs). However, it suffers from undesirable challenges such as surface residual alkali, multiple voltage plateaus, and low initial charge specific capacity. Herein, an internal and external synergistic modulation strategy is adopted by replacing part of the Mn with Ti to optimize the bulk phase and construct a Ti‐containing epitaxial stabilization layer, resulting in reduced surface residual alkali, excellent Na+ transport kinetics and improved water/air stability. Specifically, the Na0.44Mn0.85Ti0.15O2 using water‐soluble carboxymethyl cellulose as a binder can realize a capacity retention rate of 94.30% after 1,000 cycles at 2C, and excellent stability is further verified in kilogram large‐up applications. In addition, taking advantage of the rich Na content in Prussian blue analog (PBA), PBA‐Na0.44Mn1‐xTixO2 composites are designed to compensate for the insufficient Na in the tunnel oxide and are matched with hard carbon to achieve the preparation of coin full cell and 18650 cylindrical battery with satisfactory electrochemical performance. This work enables the application of tunnel oxides cathode for SIBs in 18650 cylindrical batteries for the first time and promotes the commercialization of SIBs.

Funder

National Natural Science Foundation of China

High-end Foreign Experts Recruitment Plan of China

Key Research and Development Program of Zhejiang Province

Natural Science Foundation of Zhejiang Province

China Scholarship Council

Australian Research Council

Science and Technology Project of State Grid

Publisher

Wiley

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