Structure-Driven Performance Enhancement in Palladium-Graphene Oxide Catalysts for Electrochemical Hydrogen Evolution.

Graphene oxide (GO) has recently gained significant attention in electrocatalysis as a promising electrode material owing to its unique physiochemical properties such as enhanced electron transfers due to a conjugated π-electron system, high surface area, and stable support for loading electroactive species, including metal nanoparticles. However, only a few studies have been directed toward the structural characteristics of GO, elaborating on the roles of oxygen-containing functional groups, the presence of defects, interlayer spacing between the layered structure, and nonuniformity in the carbon skeleton along with their influence on electrochemical performance. In this work, we aim to understand these properties in various GO materials derived from different graphitic sources. Both physiochemical and electrochemical characterization were employed to correlate the above-mentioned features and explore the effect of the location of the palladium nanoparticles (Pd NPs) on various GO supports for the hydrogen evolution reaction (HER). The interaction of the functional groups has a crucial role in the Pd dispersion and its electrochemical performance. Among the different GO samples, Pd supported on GO derived from graphene nanoplate (GNP), Pd/GO-GNP, exhibits superior HER performance; this could be attributed to the optimal balance among particle size, defect density, less in-plane functionalities, and higher electrochemical surface area. This study, thus, helps to identify the optimal conditions that lead to the best performance of Pd-loaded GO, contributing to the design of more effective HER electrocatalysts.