Tunable Pt-Ni Interaction Induced Construction of Disparate Atomically Dispersed Pt Sites for Acidic Hydrogen Evolution

Developing cost-effective Pt-based electrocatalysts forthe hydrogenevolution reaction (HER) is highly urgent. Herein, we report novelelectrocatalysts with individually dispersed Pt active sites and tunablePt-Ni interaction decorated on carbon-wrapped nanotube frameworks(Pt/Ni-DA). Pt/Ni-DA exhibits superior HER performance at low Pt concentrationswith an ultralow overpotential of 18 mV at 10 mA cm(-2) and an ultrahigh mass activity of 2.13 A mg(Pt) (-1) at an overpotential of 50 mV, which is about four times higher thanthat of commercial Pt/C. X-ray absorption fine structure (XAFS) confirmsthe extension of Pt from the Ni surface to the Ni bulk phase. Mechanisticresearch and density functional theory (DFT) calculations collectivelyreveal that the dispersibility and distribution of Pt atoms in Niregulate the electronic configuration of Pt sites, optimizing thebinding energy of reaction intermediates and facilitating electrontransfer during the HER process. This work highlights the importanceof the electronic structure alternation through the accommodationeffect toward enhanced catalytic performance in HER.

Automated summary

In this study, novel electrocatalysts with individually dispersed Pt active sites and tunable Pt-Ni interaction were developed. The Pt/Ni-DA catalyst exhibited superior performance for the hydrogen evolution reaction (HER), with an ultralow overpotential of 18 mV at 10 mA cm(-2) and an ultrahigh mass activity of 2.13 A mg(Pt) (-1) at an overpotential of 50 mV, which is about four times higher than that of commercial Pt/C. X-ray absorption fine structure (XAFS) confirmed the diffusion of Pt from the Ni surface to the Ni bulk phase. Mechanistic research and density functional theory (DFT) calculations revealed that the dispersibility and distribution of Pt atoms in Ni regulate the electronic configuration of Pt sites, optimizing the binding energy of reaction intermediates and facilitating electron transfer during the HER process. This work highlights the importance of electronic structure alteration through the accommodation effect for enhanced catalytic performance in HER.