Coordination engineering for iron-based hexacyanoferrate as a high-stability cathode for sodium-ion batteries

Author:

Zhong Jiang1ORCID,Xia Lirong2,Chen Song1,Zhang Zhengwei3,Pei Yong2,Chen Hao1,Sun Hongtao4ORCID,Zhu Jian15,Lu Bingan1ORCID,Zhang Yinghe6

Affiliation:

1. State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, School of Physics and Electronics, Hunan Key Laboratory of Two-Dimensional Materials, Engineering Research Center of Advanced Catalysis of the Ministry of Education, Hunan University, Changsha 410082, People’s Republic of China

2. Department of Chemistry, Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education, Xiangtan University, Xiangtan 411105, People’s Republic of China

3. Hunan Key Laboratory of Nanophotonics and Devices, School of Physics and Electronics, Central South University, Changsha 410083, People’s Republic of China

4. The Harold and Inge Marcus Department of Industrial Engineering, The Pennsylvania State University, State College, University Park, PA 16802

5. Shenzhen Research Institute, Hunan University, Shenzhen 518000, People’s Republic of China

6. School of Civil and Environmental Engineering, Harbin Institute of Technology, Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application, Shenzhen 518055, People’s Republic of China

Abstract

Iron-based hexacyanoferrate (Fe-HCF) are promising cathode materials for sodium-ion batteries (SIBs) due to their unique open-channel structure that facilitates fast ion transport and framework stability. However, practical implementation of SIBs has been hindered by low initial Coulombic efficiency (ICE), poor rate performance, and short lifespan. Herein, we report a coordination engineering to synthesize sodium-rich Fe-HCF as cathodes for SIBs through a uniquely designed 10-kg-scale chemical reactor. Our study systematically investigated the relationship between coordination surroundings and the electrochemical behavior. Building on this understanding, the cathode delivered a reversible capacity of 99.3 mAh g −1 at 5 C (1 C = 100 mA g −1 ), exceptional rate capability (51 mAh g −1 even at 100 C), long lifespan (over 15,000 times at 50 C), and a high ICE of 92.7%. A full cell comprising the Fe-HCF cathode and hard carbon (HC) anode exhibited an impressive cyclic stability with a high-capacity retention rate of 98.3% over 1,000 cycles. Meanwhile, this material can be readily scaled to the practical levels of yield. The findings underscore the potential of Fe-HCF as cathodes for SIBs and highlight the significance of controlling nucleation and morphology through coordination engineering for a sustainable energy storage system.

Publisher

Proceedings of the National Academy of Sciences

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