Enhancing
catalytic activity by decorating noble metals in catalysts
provides an opportunity for promoting the electrocatalytic hydrogen
evolution reaction (HER) application. However, there are few systematic
studies on regulating the structures of noble metals in catalytic
materials and investigating their influence on HER. Herein, Pt catalysts
with different structures including single atoms (SAs), clusters,
and nanoparticles well-controllably anchored on VS2 nanosheets
through a cost-effective optothermal method are reported, and their
HER performance is studied. The most efficient Pt-decorated VS2 catalyst (with both Pt SAs and clusters) delivers an overpotential
of 77 mV at 10 mA cm–2, close to that of Pt/C (48
mV). However, the optimal mass activity of Pt (normalizing to Pt content)
is obtained from only SA Pt-decorated VS2 (i.e., 22.88 A mgPt
–1 at 200 mV) and is 12
times greater than that of the Pt/C (1.87 A mgPt
–1), attributed to the greatly enhanced Pt utilization. Additionally,
the theoretical simulations reveal that Pt SA decoration makes the
adsorption free energy of H* closer to the thermoneutral value and
improves the charge-transfer kinetics, significantly enhancing HER
activity. This work offers a pathway to prepare the desired catalyst
based on synergy of Pt structures and VS2 and reveals the
intrinsic mechanism for enhancing catalytic activity, which is important
for HER applications.