Single transition metal-decorated C4N/MoS2 heterostructure for boosting oxygen reduction, oxygen evolution, and hydrogen evolution

Qifang Liu; Xiuyun Zhao; Xin Chen

doi:10.1016/j.jcis.2023.06.039

Single transition metal-decorated C₄N/MoS₂ heterostructure for boosting oxygen reduction, oxygen evolution, and hydrogen evolution

J Colloid Interface Sci. 2023 Oct 15:648:787-797. doi: 10.1016/j.jcis.2023.06.039. Epub 2023 Jun 12.

Authors

Qifang Liu¹, Xiuyun Zhao², Xin Chen³

Affiliations

¹ Center for Computational Chemistry and Molecular Simulation, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China.
² Department of Technical Physics, University of Eastern Finland, Kuopio 70211, Finland.
³ Center for Computational Chemistry and Molecular Simulation, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China; State Key Laboratory of Oil & Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China. Electronic address: chenxin830107@pku.edu.cn.

PMID: 37327622
DOI: 10.1016/j.jcis.2023.06.039

Abstract

Multifunctional electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution (HER) are required preconditions for the development of a highly promising new green energy conversion and storage technology. Herein, a comprehensive computation of the ORR, OER and HER catalytic performance for the pristine and metal-decorated C₄N/MoS₂ (TM-C₄N/MoS₂) is researched using density functional theory. Remarkably, Pd-C₄N/MoS₂ exhibits distinguished bifunctional catalytic performance with lower ORR/OER overpotentials of 0.34/0.40 V. Rh-C₄N/MoS₂ is the prospective trifunctional catalyst with the low ORR/OER/HER overpotentials of 0.48/0.55/-0.16 V, but its electrochemical stability needs to be further improved. Furthermore, the strong correlation between intrinsic descriptor (φ) and adsorption free energy of *OH verifies that the catalytic activity of TM-C₄N/MoS₂ is affected by active metal and surrounding coordination environment. The heap map has summarized the correlations of d-band center, adsorption free energy of reaction species, and φ as the vital parameter for ORR/OER overpotentials of designing catalysts. The electronic structure analysis uncovers the activity enhancement is due to the adjustable adsorption behavior of reaction intermediates on TM-C₄N/MoS₂. This finding paves the way to develop high-activity and multifunctional catalysts, making them suitable for multifunctional applications in the forthcoming critically needed green energy conversion and storage technologies.

Keywords: Catalytic activity; Density functional theory; Heterojunction; Multifunctional electrocatalyst; Single atom catalyst.