p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

作者：Xiaochen Wang, Ning Zhang, Shuohai Guo, Huishan Shang, Xuan Luo, Zhiyi Sun, Zihao Wei, Yuanting Lei, Lili Zhang, Dan Wang, Yafei Zhao, Fang Zhang, Liang Zhang, Xu Xiang, Wenxing Chen, Bing Zhang · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c03576 · 被引用次数：227 · 研究领域：Electrocatalysts for Energy Conversion、Advanced battery technologies research、Fuel Cells and Related Materials

With more flexible active sites and intermetal interaction, dual-atom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing a typical p-d orbital hybridization between p-block and d-block metal atoms may bring new avenues for manipulating the electronic properties and thus boosting the electrocatalytic activities. Herein, we report a distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual atom sites embedded on a two-dimensional C 2 N nanosheet (FeSn–C 2 N), which displays excellent oxygen reduction reaction (ORR) performance with a half-wave potential of 0.914 V in an alkaline electrolyte. Theoretical calculations further unveil the powerful p-d orbital hybridization between p-block stannum and d-block ferrum in FeSn dual atom sites, which triggers electron delocalization and lowers the energy barrier of *OH protonation, consequently enhancing the ORR activity. In addition, the FeSn–C 2 N-based Zn–air battery provides a high maximum power density (265.5 mW cm –2 ) and a high specific capacity (754.6 mA h g –1 ). Consequently, this work validates the immense potential of p-d orbital hybridization along dual-metal atom catalysts and provides new perception into the logical design of heteronuclear DACs.