Carbon-coordinated atomic cobalt directly embedded on carbon cloth for alkaline hydrogen evolution at high current density

Abstract

Electrocatalysts for high current density hydrogen evolution reaction (HER) under alkaline conditions is critical for the widespread application of water electrolysis. Carbon-supported single-atom catalysts (SACs) stabilized by N atoms have been demonstrated as efficient electrocatalysts, but mostly for acidic HER. For alkaline HER, although defective-, edge-, and dual-sites have been found to improve the adsorption pathways of the intermediates, there is still a great challenge to precisely synthesize those complex configurations in experiments to maximize the synergistic effects. Since C atom has relatively weak electronegativity than N atom, it can induce different charge redistribution of the metal atom center. However, the reported C-coordinated SACs were derived from the N-containing precursors, which could not exclude the influence of heteroatoms on the activity completely. Herein, we reported the synthesis of carbon-coordinated CoC4 sites and ultra-small Co cluster directly embedded on pure carbon cloth (Co-SA/CC) via the high temperature shockwave (HTS) method. The C atoms on the first coordination shell can tune the local electronic structure and up-shift the d-band center of the Co atom, thus strengthening H2O molecule adsorption and promoting water dissociation. The self-supporting electrode with CoC4 can lower the interfacial contact resistance, leading to higher HER performance compared with that of Pt/C at high current density (e.g. 1000 mA/cm2). These results provide a new insight into the fundamental understanding of design and synthesis of C-coordinated atomically dispersed catalytic sites.