Intensifying hydrogen spillover over silicotungstic acid decorated carbon black-supported Ru by green plasma preparation for boosting the electrocatalytic hydrogen evolution reaction

Abstract

The effective promotion of hydrogen spillover over supported Ru through rational modification of the carbon black support is pivotal to boosting the electrocatalytic hydrogen evolution reaction (HER). Herein, a Ru/SiW/CB-P electrocatalyst was synthesized by embedding ultrafine Ru nanoparticles onto silicotungstic acid (SiW) decorated carbon black (CB) using a green RF plasma method, which achieves an ultralow overpotential of 22 mV to afford a current density of 10 mA cm⁻² for the HER in 1 M KOH. Additionally, the mass activity of Ru/SiW/CB-P is 5 times that of benchmarked Pt/C at a 100 mV overpotential, and it shows remarkable durability over a considerable period of 80 h across 10 to 30 mA cm⁻². Structural characterization and operando electrochemical Raman measurement results reveal that after mild and rapid RF plasma treatment, the retained SiW in Ru/SiW/CB-P enhances the metal–support interaction, which is conducive to promoting the connection of the hydrogen-bond network between the electrode and the electrolyte, thereby accelerating the desorption and dynamic migration of the adsorbed hydrogen through hydrogen spillover. This work offers an effective avenue for intensifying hydrogen spillover and is crucial for sustainable hydrogen energy application.