Enhanced hydrogen evolution performance by covalent-linked ultrafine, uniform Pt nanoparticles with doped sulfur atoms in three-dimensional graphene

Abstract Highly efficient and stable electrocatalyst for hydrogen evolution reaction (HER) is essential for the application of green hydrogen energy. To date, platinum -based materials are the most efficient electrocatalyst. Developing inexpensive electrocatalyst with low Pt loading and high platinum utilization efficiency is one of effective strategies to lower the cost of platinum -based electrocatalyst. In this paper, it was demonstrated that ultrafine and uniform distribution platinum nanoparticles could be synthesized on three-dimensional sulfur-doped graphene materials (Pt/3DSG) via covalent cross-linking between platinum and doped sulfur atoms. The high conductive 3DSG not only facilitates the electron transport but also serves as a template for depositing ultrafine and uniform platinum nanoparticles. The Pt/3DSG with low Pt loading (3.1 wt%) delivers extremely outstanding HER performance, which is superior to the commercial 20 wt% Pt/C catalyst. The turnover frequencies (TOFs) of Pt/3DSG can reach 1.12 s −1 , which is larger than that of 20% Pt/C (0.71 s −1 ). Furthermore, the stability is also superior than that of Pt/C. This work provides a rational design strategy for highly efficient and stable electrocatalysts with low loading and high utilization of precious metal.