Super‐Coordinated Nickel N4Ni1O2Site Single‐Atom Catalyst for Selective H2O2Electrosynthesis at High Current Densities

Abstract Electrochemical production of hydrogen peroxide (H 2 O 2 ) from O 2 on single‐atom catalysts has attracted great attention, yet the quest for robust catalysts is driven by achieving >90 % Faradaic efficiency (FE) under industrial‐relevant current densities (>100 mA cm −2 ). Herein we synthesize a catalyst that contains single nickel site coordinated by four nitrogen and two oxygen atoms (i.e., N 4 Ni 1 O 2 ) via involving carboxyl functionalized multiwall carbon nanotubes as a substrate to provide extra O coordination to the regular NiN 4 site. It has a cathodic energy efficiency of approximately 82 % and a H 2 O 2 FE of around 96 % at 200 mA cm −2 current density, outperforming the reported single‐atom catalysts for H 2 O 2 electrosynthesis.