Cobalt and Aluminum Co-Optimized 1T Phase MoS2 with Rich Edges for Robust Hydrogen Evolution Activity

Water electrolysis is an effective method of obtaining hydrogen energy, which is the key to achieve the global “carbon neutrality” goal. Molybdenum disulfide (MoS2) with a layered structure is considered to be a competitive hydrogen evolution reaction (HER) catalyst. However, until now, metal-atom-modified 1T-phase MoS2 with rich edge active sites has rarely been reported. Herein, we first report Co and Al co-optimized 1T-phase MoS2 (CA-1T-MoS2) with rich edge active sites using a simple one-step ball-milling method. The CA-1T-MoS2 exhibits an outstanding HER performance with an overpotential value of 102 mV at 10 mA cm–2 in 1.0 M KOH. The density functional theory (DFT) results prove that the introduction of Co and Al atoms on the rich edges of 1T-MoS2 provides rich active sites, improves the electrical conductivity, accelerates the distortion of H2O to generate H* and reduces the adsorption energy of hydrogen. Thus, CA-1T-MoS2 exhibits a prominent HER performance. This work provides a novel strategy for the simple preparation of metal-atom-modified 2D transition-metal sulfide HER catalysts with rich edge active sites.