Constructing Pt Clusterson Oxidation-FunctionalizedCarbon Nanotubes for Robust Electrocatalytic Hydrogen Production

Enhancing the activity and stability of platinum-based electrocatalysts for the hydrogen evolution reaction (HER) is critical for efficient water electrolysis. In this study, an efficient and scalable approach via electron-beam irradiation is employed to induce the chemical reduction of Pt ions and construct the coordination environment of Pt clusters. Two nanotube-supported Pt catalysts (Pt/CNT-O and Pt/CNT) are studied to probe the support effects on regulating the structure and electronic state of Pt by combining electrocatalytic measurements, catalyst characterizations, kinetic analysis, and density functional theoretical calculations. The Pt/CNT-O catalyst shows superior HER mass activity and durability after prolonged 6000 cycles testing compared to the Pt/CNT catalyst. This robust hydrogen evolution activity is ascribed to the more Pt(111) facets as well as favorable Pt₄–Cl/C–O active sites toward desirable Pt 4f binding energy and Gibbs free energy for HER. These insights could guide the rational design and surface-interface tuning of carbon-supported Pt-based electrocatalysis for sustainable hydrogen energy production.