Intensifying Interfacial Reverse Hydrogen Spillover for Boosted Electrocatalytic Nitrate Reduction to Ammonia

Abstract Rational regulation of active hydrogen (*H) behavior is crucial for advancing electrocatalytic nitrate reduction reaction (NO 3 RR) to ammonia (NH 3 ), yet in‐depth understanding of the *H generation, transfer, and utilization remains ambiguous, and explorations for *H dynamic optimization are urgently needed. Herein we engineer a Ni 3 N nanosheet array intimately decorated with Cu nanoclusters (NF/Ni 3 N−Cu) for remarkably boosted NO 3 RR. From comprehensive experimental and theoretical investigations, the Ni 3 N moieties favors water dissociation to generate *H, and then *H can rapidly transfer to the Cu via unique reverse hydrogen spillover mediating interfacial Ni−N−Cu bridge bond, thus increasing…

• NN
  National Natural Science Foundation of China

  Award: U21A2077