Abstract

AbstractThe essence of developing a Pt‐based single‐atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well‐defined and stable single Pt sites with desired electrocatalytic efficacy. Herein, we report a facile approach to generate uniformly dispersed Pt sites with outstanding HER performance via a photochemical reduction method using polyvinylpyrrolidone (PVP) molecules as the key additive to significantly simplify the synthesis and enhance the catalytic performance. The as‐prepared catalyst displays remarkable kinetic activities (20 times higher current density than the commercially available Pt/C) with excellent stability (76.3 % of its initial activity after 5000 cycles) for HER. EXAFS measurements and DFT calculations demonstrate a synergetic effect, where the PVP ligands and the support together modulate the electronic structure of the Pt atoms, which optimize the hydrogen adsorption energy, resulting in a considerably improved HER activity.

Highlights

  • The essence of developing a Pt-based single-atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well-defined and stable single Pt sites with desired electrocatalytic efficacy

  • The procedures to synthesize the PVP (K30)-coordinated Pt single-site titanium oxide nanorods encapsulated by graphitic carbon (TNR@GC) catalysts are summarized in Scheme 1; a detailed description of the reaction conditions and the properties of the catalyst support are given in the Supporting Information (Figures S1–S3) In brief, a narrow band of 365 nm ultraviolet light was introduced to indirectly reduce the Pt4+ cations via the photoexcited electron of the TiO2 substrate

  • The abundant amide functional groups of PVP serve as the coordination environment to fix the Pt atoms, and modulate the electronic structure

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Summary

Introduction

The essence of developing a Pt-based single-atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well-defined and stable single Pt sites with desired electrocatalytic efficacy. EXAFS measurements and DFT calculations demonstrate a synergetic effect, where the PVP ligands and the support together modulate the electronic structure of the Pt atoms, which optimize the hydrogen adsorption energy, resulting in a considerably improved HER activity.

Results
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