Zhong Jiang, Xia Lirong, Chen Song, Zhang Zhengwei, Pei Yong, Chen Hao, Sun Hongtao, Zhu Jian, Lu Bingan, Zhang Yinghe
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.
Department of Chemistry, Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education, Xiangtan University, Xiangtan 411105, People's Republic of China.
Proc Natl Acad Sci U S A. 2024 Jul 30;121(31):e2319193121. doi: 10.1073/pnas.2319193121. Epub 2024 Jul 25.
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 at 5 C (1 C = 100 mA g), exceptional rate capability (51 mAh g 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.
铁基六氰合铁酸盐（Fe-HCF）因其独特的开放通道结构有利于快速离子传输和骨架稳定性，是钠离子电池（SIB）颇具前景的正极材料。然而，SIB的实际应用受到低初始库仑效率（ICE）、较差的倍率性能和短寿命的阻碍。在此，我们报道了一种配位工程，通过独特设计的10千克规模化学反应器合成富钠Fe-HCF作为SIB的正极。我们的研究系统地研究了配位环境与电化学行为之间的关系。基于这一认识，该正极在5C（1C = 100 mA g）下具有99.3 mAh g的可逆容量、出色的倍率性能（即使在100C时也有51 mAh g）、长寿命（在50C下超过15000次循环）以及92.7%的高ICE。由Fe-HCF正极和硬碳（HC）负极组成的全电池表现出令人印象深刻的循环稳定性，在1000次循环中具有98.3%的高容量保持率。同时，这种材料可以很容易地扩大到实际生产水平。这些发现强调了Fe-HCF作为SIB正极的潜力，并突出了通过配位工程控制成核和形态对于可持续储能系统的重要性。
