In Situ Reconstruction of Ag‐Doped Ni ₂ P Electrocatalyst for Hydrogen Evolution and Value‐Added Acrylamide Conversion

Concurrent remediation of organic pollutants in wastewater and energy‐efficient hydrogen production is a highly attractive yet challenging dual strategy. Acrylamide (AA), depolymerized from polyacrylamide under natural conditions such as UV radiation and elevated temperatures, causes severe environmental pollution. Herein, in situ reconstructed Ag‐doped Ni 2 P nanosheets on Ni foam (CV‐Ag‐Ni 2 P/NF) are developed as a bifunctional catalyst. This catalyst exhibits high activity for the AA oxidation reaction (AOR) while enabling energy‐efficient hydrogen evolution reaction (HER). After electrochemical operation, the initial zipper‐like morphology transforms into spherical features with interspersed rod‐like particles, providing a larger electrochemical surface area and more active sites. Particularly, a potential of 1.82 V delivers 100 mA cm −2 in the two‐electrode AOR system. Remarkably, 79.3% AA removal was achieved after 24 h at 50 mA cm −2 . Meanwhile, ethanol generated at the anode serves as a value‐added product. Density functional theory (DFT) calculations reveal that Ag atoms are the active sites for AA degradation and ethanol formation, with favorable adsorption energies. We propose a plausible AOR catalytic mechanism and reveal the key roles of Ag and Ni in H* adsorption and reduction of AA dehydrogenation energy, which offers a promising way of coupling AOR with HER to reduce energy consumption while producing high‐value products.