电子占位作为设计铁单原子电催化剂的描述符

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-04-28 DOI:10.1002/adma.202504852

Chun Pei, Guohua Yao, Ziguang Zhao, Yafei Sun, Qin Wang, Tongxin Shang, Ying Wan

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引用次数: 0

摘要

单原子催化剂的设计迫切需要定量的电子结构-性能关系。合成了电子占位在1.7 ~ 0.7之间的有序介孔碳负载铁单原子催化剂。在Fe位点的eg电子占位与氧相关中间体的催化活性/激活熵之间建立了线性关系。eg电子占比为0.7的Fe SAC改变了从*OH解吸到*OOH生成的速率决定步骤。其翻转频率约为Fe SAC位点的28倍，eg电子占用率为1.7 e，质量活度约为商用Pt/C的6.3倍。当用于锌-空气电池时，Fe SAC的功率密度为196.3 mW cm - 2，长期稳定性超过1500 h。eg电子占据描述符的发现为设计单原子电催化剂提供了有价值的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

eg Electron Occupancy as a Descriptor for Designing Iron Single-Atom Electrocatalysts

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eg Electron Occupancy as a Descriptor for Designing Iron Single-Atom Electrocatalysts

A quantitative electronic structure-performance relationship is highly desired for the design of single-atom catalysts (SACs). The Fe single-atom catalysts supported by ordered mesoporous carbon with the e_g electron occupancy from 1.7 to 0.7 are synthesized. A linear relationship has been established between the e_g electron occupancy of the Fe site and the catalytic activity/activation entropy of oxygen-related intermediates. Fe SAC with an e_g electron occupancy of 0.7 alters the rate determining step from ^*OH desorption to ^*OOH formation. The value of the turn-over frequency is ≈28 times that of the Fe SAC site with an e_g electron occupancy of 1.7 e, and the mass activity is ≈6.3 times that of commercial Pt/C. When used in a zinc–air battery, the Fe SAC gives a remarkable power density of 196.3 mW cm⁻² and a long-term stability exceeding 1500 h. The discovery of e_g electron occupancy descriptor provides valuable insights for designing single-atom electrocatalysts.

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.