Confinement Synthesis of Atomic Copper‐Anchored Polymeric Carbon Nitride in Crystalline UiO‐66‐NH 2 for High‐Performance CO 2 ‐to‐CH 3 OH Photocatalysis

Abstract Photocatalytic CO 2 reduction to value‐added fuels displays an attractive scenario to enhance energy supply and reduce global warming. We report herein the confinement synthesis of polymeric carbon nitride (PCN) incorporating with Cu single atoms (CuSAs) inside the crystalline UiO‐66‐NH 2 , which combines the merits of heterojunction photocatalysis and single‐atom catalysis (SAC) to achieve high‐performance CO 2 ‐to‐CH 3 OH conversion. A series of spectral studies displays the formation of CuSAs@PCN inside the crystalline UiO‐66‐NH 2 . Remarkably, the ternary composite shows an excellent photocatalytic turnover frequency of 4.15 mmol ⋅ h −1 ⋅ g −1 for CO 2 ‐to‐CH 3 OH conversion. Theoretical and experimental studies demonstrate the doping of CuSAs, as well as the formation of type‐II heterojunction, are causal factors to achieve CH 3 OH generation. The study provides new insights designing high‐performance photocatalyst for CO 2 conversion to fuels at atomic scale.