Ultra-Fast Synthesis of Highly Dispersed Pt Nanoclusters Anchored on Sulfur-Doped Porous Carbon Carriers by Nanosecond Pulsed Laser for Hydrogen Evolution Reaction

Nanosecond pulsed laser irradiation is employed for synthesis of highly active and stable Pt-based electrocatalysts by anchoring Pt nanoclusters on porous sulfur-doped carbon supports (L-Pt/SC). Strong metal-support interaction (SMSI) between Pt and S induces a local charge rearrangement and modulates the electronic structure of Pt surroundings, thus boosting the reaction kinetics and enhancing stability in long-term hydrogen evolution reaction (HER). The L-Pt/SC catalyst exhibits high activity toward HER, with an overpotential of 23 mV at current densities reaching 10 mA cm^-2 and a Tafel slope of 24 mV dec^-1. The unit mass activity of L-Pt/SC is calculated to be -10.8 A cm^-2 mg_Pt ^-1 at an applied voltage of -0.3 V versus RHE. In situ Raman spectra reveals that L-Pt/SC catalyst exhibits fast hydrogen production efficiency and its electrocatalytic HER process is determined by the Tafel step. Density functional theory calculations suggest the strong bonding energy between SC and Pt induces the formation of smaller nanoclusters of L-Pt/SC during fast pulsed laser preparation, which increases the effective contact area during the HER process thereby increasing the activity per unit mass.