biostudies-literatureUnknown17(1)Wang CArtificial carbon fixation is a promising pathway for achieving the carbon cycle and environment remediation. However, the sluggish kinetics of oxygen evolution reaction (OER) and poor selectivity of CO₂ reduction seriously limited the overall conversion efficiencies of solar energy to chemical fuels. Herein, we demonstrated a facile and feasible strategy to rationally regulate the coordination environment and electronic structure of surface-active sites on both photoanode and cathode. More specifically, the defect engineering has been employed to reduce the coordination number of ultrathin FeNi catalysts decorated on BiVO₄ photoanodes, resulting in one of the highest OER activities of 6.51 mA cm^-2 (1.23 V_RHE, AM 1.5G). Additionally, single-atom Nano-micro letters184https://www.ebi.ac.uk/biostudies/studies/S-EPMC11904044biostudies-literatureHighly Active Oxygen Evolution Integrating with Highly Selective CO<sub>2</sub>-to-CO Reduction.PMC11904044Wang CGeng LBi YfalseHighly Active Oxygen Evolution Integrating with Highly Selective CO<sub>2</sub>-to-CO Reduction.Artificial carbon fixation is a promising pathway for achieving the carbon cycle and environment remediation. However, the sluggish kinetics of oxygen evolution reaction (OER) and poor selectivity of CO₂ reduction seriously limited the overall conversion efficiencies of solar energy to chemical fuels. Herein, we demonstrated a facile and feasible strategy to rationally regulate the coordination environment and electronic structure of surface-active sites on both photoanode and cathode. More specifically, the defect engineering has been employed to reduce the coordination number of ultrathin FeNi catalysts decorated on BiVO₄ photoanodes, resulting in one of the highest OER activities of 6.51 mA cm^-2 (1.23 V_RHE, AM 1.5G). Additionally, single-atom 2025-01-01T00:00:00Z2025 Mar2026-03-27T16:46:00.726Z2025-04-03T23:26:33.226ZS-EPMC119040444007498810.1007/s40820-025-01688-2