Abstract
The development of highly active and stable cathodes in alkaline solutions is crucial for promoting the commercialization of anion exchange membrane (AEM) electrolyzers, yet it remains a significant challenge. Herein, we synthesized atomically dispersed CoP4 moieties (CoP4-SSC) immobilized on ultrathin carbon nanosheets via a phosphidation exfoliation strategy at medium temperature. The thermodynamic formation process of the Co-P moieties was elucidated using X-ray absorption spectroscopy (XAS) and theoretical calculations. Remarkably, the resulting CoP4-SSC electrocatalyst exhibited outstanding activity for alkaline hydrogen evolution, with a low overpotential of 52 mV at 10 mA cm-2 and a turnover frequency of up to 23.83 s-1. Moreover, the AEM electrolyzer fabricated with CoP4-SSC achieved a current density of 1 A cm-2 under an applied voltage of only 1.94 V, showing negligible degradation after 500 h of continuous electrocatalysis. A series of operando characterizations and density functional theory calculations revealed that the atomically dispersed Co-P moieties formed a nanointerface of [P-*H···H2O*-Co], which facilitates water dissociation during the Volmer-Heyrovsky pathway.
Published Version
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