One-step synthesis of single-site vanadium substitution in 1T-WS2 monolayers for enhanced hydrogen evolution catalysis

Metallic tungsten disulfide (WS2) monolayers have been demonstrated as promising electrocatalysts for hydrogen evolution reaction (HER) induced by the high intrinsic conductivity, however, the key challenges to maximize the catalytic activity are achieving the metallic WS2 with high concentration and increasing the density of the active sites. In this work, single-atom-V catalysts (V SACs) substitutions in 1T-WS2 monolayers (91% phase purity) are fabricated to significantly enhance the HER performance via a one-step chemical vapor deposition strategy. Atomic-resolution scanning transmission electron microscopy (STEM) imaging together with Raman spectroscopy confirm the atomic dispersion of V species on the 1T-WS2 monolayers instead of energetically favorable 2H-WS2 monolayers. The growth mechanism of V SACs@1T-WS2 monolayers is experimentally and theoretically demonstrated. Density functional theory (DFT) calculations demonstrate that the activated V-atom sites play vital important role in enhancing the HER activity. In this work, it opens a novel path to directly synthesize atomically dispersed single-metal catalysts on metastable materials as efficient and robust electrocatalysts. Ru is one of the most active metals for oxygen evolution reaction, but it quickly dissolves in acidic electrolyte particularly in nanosized form. Here the authors show that coral-like solid-solution RuIr consisting of 3nm-thick sheets with only 6at% Ir is a long-lived catalyst with high activity

Automated summary

This study demonstrates significantly enhanced hydrogen evolution reaction performance by preparing single-atom-V catalysts in 1T-WS2 monolayers. The activated V-atom sites play a vital role in enhancing the HER activity. Additionally, the coral-like solid-solution RuIr is shown to be a long-lived catalyst with high activity.