Delineating the Multifunctional Performance of Janus WSSe with Nonmetals in Water Splitting and Hydrogen Fuel Cell Applications via First-Principles Calculations

Abstract

The development of cost-effective and highly efficient multifunctional catalysts for water splitting and hydrogen fuel cells is crucial for advancing renewable energy technologies. This study employs density functional theory to investigate the electrocatalytic performance of Janus-type WSSe (JW) transition metal dichalcogenides toward the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). Additionally, the impact of nonmetal doping (NM = C, O, N, P) at the S and Se sites in the JW structure is explored. The cohesive energy of -5.82 eV/atom and minimal fluctuations in AIMD simulations over 10 ps at 300 K and 500 K confirm structural stability. Although the pristine structure exhibits a high overpotential, NM doping substantially improves catalytic performance, making it more suitable for efficient energy conversion applications. The N doped JW system demonstrates exceptional multifunctional performance, with NS@JW showing overpotentials of 0.34 V (HER), 0.18 V (OER), and 0.14 V (ORR), while NSe@JW exhibits 0.35 V (HER), 0.46 V (OER), and 0.24 V (ORR). This outstanding performance results from bonding-antibonding interactions in intermediate adsorption, as confirmed by crystal orbital Hamiltonian population analysis. This comprehensive study highlights the promise of Janus-type WSSe and emphasizes the crucial role of NM doping in boosting catalytic efficiency, offering key insights for designing cost-effective, high-performance multifunctional electrocatalysts for energy conversion.