Abstract
Engineering of the catalysts' structural stability and electronic structure could enable high-throughput H2 production over electrocatalytic water splitting. Herein, a double-shell interlayer confinement strategy is proposed to modulate the spatial position of Ru nanoparticles in hollow carbon nanoreactors for achieving tunable sizes and electronic structures toward enhanced H2 evolution. Specifically, the Ru can be anchored in either the inner layer (Ru-DSC-I) or the external shell (Ru-DSC-E) of double-shell nanoreactors, and the size of Ru is reduced from 2.2 to 0.9 nm because of the double-shell confinement effect. The electronic structures are efficiently optimized thereby stabilizing active sites and lowering the reaction barrier. According to finite element analysis results, the mesoscale mass diffusion can be promoted in the double-shell configuration. The Ru-DSC-I nanoreactor exhibits a much lower overpotential (η10 = 73.5 mV) and much higher stability (100 mA cm-2). Our work might shed light on the precise design of multishell catalysts with efficient refining electrostructures toward electrosynthesis applications.