biostudies-literatureLi LResearch Program of Science and Technology at Universities of Inner Mongolia Autonomous RegionNatural Science Foundation of Inner Mongolia Autonomous RegionFundamental Research Funds for the Inner Mongolia Normal University8846https://www.ebi.ac.uk/biostudies/studies/S-EPMC11909170biostudies-literatureUnknown15(1)Precisely regulating active sites is vital for promoting the oxygen reduction reaction (ORR) activity. Here we reported highly active Ni-Pd co-doped N-coordinated graphene towards ORR achieved by edge termination and O doping. Our first-principles calculations demonstrated that edge termination effectively boost the ORR activity, and armchair-edge termination was energetically more favorable than zigzag-edge termination. Notably, after O doping Ni-Pd active center, armchair edge-terminated Ni-Pd active site exhibited better ORR activity, and the lowest overpotential was only 0.31 V. This improvement in activity was attributed to the shift of the d-band center of Ni atom toward the Fermi-level and the shift of the d-band center of Pd atom away from the Fermi-level, thus regulating the *OH aScientific reportsEngineering the coordination environment of Ni and Pd dual active sites for promoting the oxygen reduction reaction.PMC119091702023JBYJ0162023QN010102024MS01004NJZZ23019Wen YBai NZhang MLi LZhang RWu XfalseEngineering the coordination environment of Ni and Pd dual active sites for promoting the oxygen reduction reaction.Precisely regulating active sites is vital for promoting the oxygen reduction reaction (ORR) activity. Here we reported highly active Ni-Pd co-doped N-coordinated graphene towards ORR achieved by edge termination and O doping. Our first-principles calculations demonstrated that edge termination effectively boost the ORR activity, and armchair-edge termination was energetically more favorable than zigzag-edge termination. Notably, after O doping Ni-Pd active center, armchair edge-terminated Ni-Pd active site exhibited better ORR activity, and the lowest overpotential was only 0.31 V. This improvement in activity was attributed to the shift of the d-band center of Ni atom toward the Fermi-level and the shift of the d-band center of Pd atom away from the Fermi-level, thus regulating the *OH a2025-01-01T00:00:00Z2025 Mar2025-04-04T03:01:42.794Z2025-04-04T03:01:42.794ZS-EPMC119091704008731610.1038/s41598-025-93115-0