Rational Design of Ultrafine Pt Nanoparticles with Strong Metal-Support Interaction for Efficient Hydrogen Evolution

Hydrogen evolution reaction (HER) plays an indispensable role in hydrogen economy. However, the development of highly active and durable Pt catalysts remains a great challenge. A homogenously-dispersed, ultrafine and chemically anchored Pt-based catalyst is successfully synthesized with the regulation of -SH groups tethered to SBA-15 template. The -SH not only regulates the particle size of Pt, but also modifies the chemical environment of the carbon support by converting itself into heteroatom-S. The obtained catalyst (Pt/OMCSH) exhibits superior HER catalytic activity (15.4 mV at 10 mA cm-2; 28.4 mV dec-1; 1.0 M KOH) and stability to benchmark samples and most of the previously reported Pt-based electrocatalysts. First-principles calculations reveal that the presence of S in the carbon support regulates the electronic structure of Pt and strengthens the metal-support interaction, thus boosting the reaction kinetics and enhancing the stability of Pt/OMCSH catalyst for HER. Under the control of -SH groups attached to SBA-15 template, a homogeneously dispersed, ultrafine and chemically anchored Pt-based catalyst is successfully prepared. In addition to controlling Pt particle size, the -SH also alters the chemical environment of the carbon support through doping by converting itself heteroatom-S. Finally, the obtained Pt/OMCSH catalyst shows a better HER catalytic activity and stability than benchmark samples. Experimental results and first-principles simulations all indicate that S as heteroatom not only adjusts Pt electronic structure, but also enhances the metal-support interaction. image