Abstract
Layered 2D materials are a vital class of electrocatalys for the hydrogen evolution reaction (HER), due to their large area, excellent activity, and facile fabrication. Theoretical caculations domenstrate, however, that only the edges of the 2D nanosheets act as active sites, while the much larger basal plane exhibits passive activity. Here, from a distinguishing perspective, RhSe2 is reported as a "3D" electrocatalyst for HER with top-class activity, synthesized by a facile solid-state method. Superior to 2D materials, multiple crystal facets of RhSe2 exhibit near-zero free energy change of hydrogen adsorption (ΔGH ), which guarantees high performance in most common morphologies. Density functional theory calculations reveal that the low-coordinated Rh atoms act as the active sites in acid, which enables the modified Kubas-mediated pathway, while the Se atoms act as the active sites in an alkaline medium. The overpotentials of HER activity of RhSe2 are measured to be 49.9 and 81.6mV at 10mA cm-2 in acid and alkaline solutions, respectively. This work paves the way to new transition metal chalcogenide catalysts.
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