1T-MoS2 Coordinated Bimetal Atoms as Active Centers to Facilitate Hydrogen Generation

Abstract

Anchoring single metal atoms has been demonstrated as an effective strategy to boost the catalytic performance of non-noble metal 1T-MoS2 towards hydrogen evolution reaction (HER). However, the dual active sites on 1T-MoS2 still remain a great challenge. Here, first-principles calculations were performed to systematically investigate the electrocatalytic HER activity of single and dual transition metal (TM) atoms bound to the 1T-MoS2 monolayer (TM@1T-MoS2). The resulted Ti@1T-MoS2 exhibits excellent structural stability, near-thermoneutral adsorption of H* and ultralow reaction barrier (0.15 eV). It is a promising single metal atom catalyst for HER, outperformed the reported Co, Ni and Pd anchoring species. Surprisingly, by further introducing Pd atoms coordinated with S atoms or S vacancies on the Ti@1T-MoS2 surface, the resulted catalyst not only maintains the high HER activity of Ti sites, but also achieves new dual active moiety due to the appropriate H* adsorption free energy on Pd sites. This work is of great significance for realizing dual active centers on 1T-MoS2 nanosheets and offers new thought for developing high-performance electrocatalysts for HER.

Solving the Trifunctional Activity Challenge of Catalysts in Unitized Regenerative Fuel Cells via 1T-MoS2-Coordinated Single Pd Atoms

“…Specifically, the metallic 1T-MoS 2 nanosheet exhibits high conductivity, low cost, and intrinsic HER activity. , It performs well as an electrocatalyst toward HER in acidic solution. , The sulfur on the outer surface of 1T-MoS 2 catalyzes the generation of hydrogen from free protons, like those generated from the water splitting in the OER. By anchoring single Pd atoms, our previous DFT results found that the S atom near Pd becomes more activated for HER . Also, the experimental and theoretical studies of Lau et al demonstrated that the immobilization of single Pd atoms on the 1T-MoS 2 basal plane can greatly promote the proton reduction step from water splitting to produce hydrogen and render it non-rate-limiting, further improving the kinetic rate and efficiency of 1T-MoS 2 for HER.…”

“…By anchoring single Pd atoms, our previous DFT results found that the S atom near Pd becomes more activated for HER. 43 Also, the experimental and theoretical studies of Lau et al 22 demonstrated that the immobilization of single Pd atoms on the 1T-MoS 2 basal plane can greatly promote the proton reduction step from water splitting to produce hydrogen and render it non-rate-limiting, further improving the kinetic rate and efficiency of 1T-MoS 2 for HER. In concert with the newfound OER and ORR catalytic capability on the Pd site, Pd@1T-MoS 2 is a promising trifunctional electrocatalyst for HER, OER, and ORR.…”

The Advanced Progress of MoS2 and WS2 for Multi-Catalytic Hydrogen Evolution Reaction Systems

“…It will not only address human daily needs but also enhance the energy security of all countries and reduce international conflicts caused by the fossil energy crisis, thereby promoting harmonious global development, enhancing sustainability and reducing pollution [1][2][3]. Ultrathin MoS 2 nanosheet is a typical material in transition metal sulfide systems attracting extensive attention in recent years, possessing superior structural and photocatalytic properties, and becoming a substitute for platinum in highly active hydrogen production reactions [4,5].…”