Design of Multifunctional Electrocatalysts for ORR/OER/HER/HOR: Janus Makes Difference

Abstract Multifunctional electrocatalysts for hydrogen evolution reaction (HER), hydrogen oxidation reaction (HOR), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) have broad application prospects; However, realization of such kinds of materials remain difficulties because it requires the materials to have not only unique electronic properties, but multiple active centers to deal with different reactions. Here, employing density functional theory (DFT) computations, it is demonstrated that by decorating the Janus‐type 2D transition metal dichalcogenide (TMD) of TaSSe with the single atoms, the materials can achieve multifunctionality to catalyze the ORR/OER/HER/HOR. Out of sixteen catalytic systems, Pt‐V S (i.e., Pt atom embedded in the sulfur vacancy), Pd‐V Se , and Pt‐V Se @TaSSe are promising multifunctional catalysts with superior stability. Among them, the Pt‐V S @TaSSe catalyst exhibits the highest activity with theoretical overpotentials η ORR = 0.40 V, η OER = 0.39 V, and η HER/HOR = 0.07 V, respectively, better than the traditional Pt (111), IrO 2 (110). The interplays between the catalyst and the reaction intermediate over the course of the reaction are then systematically investigated. Generally, this study presents a viable approach for the design and development of advanced multifunctional electrocatalysts. It enriches the application of Janus, a new 2D material, in electrochemical energy storage and conversion technology.