Designing asymmetrical TMN4 sites via phosphorus or sulfur dual coordination as high-performance electrocatalysts for oxygen evolution reaction

Zhe Xue; Rui Tan; Jinzhong Tian; Hua Hou; Xinyu Zhang; Yuhong Zhao

doi:10.1016/j.jcis.2024.04.095

Designing asymmetrical TMN₄ sites via phosphorus or sulfur dual coordination as high-performance electrocatalysts for oxygen evolution reaction

J Colloid Interface Sci. 2024 Aug:667:679-687. doi: 10.1016/j.jcis.2024.04.095. Epub 2024 Apr 20.

Authors

Zhe Xue¹, Rui Tan², Jinzhong Tian³, Hua Hou⁴, Xinyu Zhang⁵, Yuhong Zhao⁶

Affiliations

¹ School of Materials Science and Engineering, Collaborative Innovation Center of Ministry of Education and Shanxi Province for High-performance Al/Mg Alloy Materials, North University of China, Taiyuan 030051, China; State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, Hebei, China.
² College of Physics and Electronics Engineering, Hengyang Normal University, Hengyang 421002, China.
³ School of Materials Science and Engineering, Collaborative Innovation Center of Ministry of Education and Shanxi Province for High-performance Al/Mg Alloy Materials, North University of China, Taiyuan 030051, China.
⁴ School of Materials Science and Engineering, Collaborative Innovation Center of Ministry of Education and Shanxi Province for High-performance Al/Mg Alloy Materials, North University of China, Taiyuan 030051, China; School of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China.
⁵ State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, Hebei, China. Electronic address: xyzhang@ysu.edu.cn.
⁶ School of Materials Science and Engineering, Collaborative Innovation Center of Ministry of Education and Shanxi Province for High-performance Al/Mg Alloy Materials, North University of China, Taiyuan 030051, China; Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China. Electronic address: zhaoyuhong@nuc.edu.cn.

PMID: 38670011
DOI: 10.1016/j.jcis.2024.04.095

Abstract

The development ofhighly efficient oxygen evolution reaction (OER) catalysts based on more cost-effective and earth-abundant elements is of great significance and still faces a huge challenge. In this work, a series of transition metal (TM)embedding a newly-defined monolayer carbon nitride phase is theoretically profiled and constructed as a catalytic platform for OER studies. Typically, a four-step screening strategy was proposed to rapidly identified high performance candidates and the coordination structure and catalytic performance relationship was thoroughly analyzed. Moreover, the eliminating criterion was established to condenses valid range based on the Gibbs free energy of OH*. Our results reveal that the as-constructed 2FeCN/P exhibits superior activity toward OER with an ultralow overpotential of 0.25 V, at the same time, the established 3FeCN/S configuration performed well as abifunctional OER/ORR electrocatalysis with extremely low overpotential η^OER/η^ORR of 0.26/0.48 V. Overall, this work provides an effective framework for screening advanced OER catalysts, which can also be extended to other complex multistep catalytic reactions.

Keywords: Asymmetrical structure; Carbon nitride; Density functional theory; Electrocatalysis; Fe–N–C; Single-atom catalysis.