Abstract
AbstractPhotoreduction of CO2into solar fuels has received great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, two single‐Cu‐atom catalysts with unique Cu configurations in phosphorus‐doped carbon nitride (PCN), namely, Cu1N3@PCN and Cu1P3@PCN were fabricated via selective phosphidation, and tested in visible light‐driven CO2reduction by H2O without sacrificial agents. Cu1N3@PCN was exclusively active for CO production with a rate of 49.8 μmolCO gcat−1 h−1, outperforming most polymeric carbon nitride (C3N4) based catalysts, while Cu1P3@PCN preferably yielded H2. Experimental and theoretical analysis suggested that doping P in C3N4by replacing a corner C atom upshifted thed‐band center of Cu in Cu1N3@PCN close to the Fermi level, which boosted the adsorption and activation of CO2on Cu1N3, making Cu1N3@PCN efficiently convert CO2to CO. In contrast, Cu1P3@PCN with a much lower Cu3delectron energy exhibited negligible CO2adsorption, thereby preferring H2formation via photocatalytic H2O splitting.
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