Rare Earth Er-Nd Dual Single-Atomic Catalysts for Efficient Visible-light Induced CO Reduction to CHOH (n=1, 2).

Efficient synthesis of CHOH (n=1, 2) via photochemical CO reduction holds promise for achieving carbon neutrality but remains challenging. Here, we present rare earth dual single atoms (SAs) catalysts containing ErN and NdN moieties, fabricated via an atom-confinement and coordination method. The dual Er-Nd SAs catalysts exhibit unprecedented generation rates of 1761.4 μmol g h and 987.7 μmol g h for CHCHOH and CHOH, respectively. Through a combination of theoretical calculation, XAFS analysis, aberration-corrected HAADF-STEM, and in-situ FTIR spectroscopy, we demonstrate that the Er SAs facilitate charge transfer, serving as active centers for C-C bond formation, while Nd SAs provide the necessary *CO for C-C coupling in CHOH synthesis under visible light. Furthermore, the experiment and DFT calculation elucidate that the variety of electronic states induced by 4 f orbitals of the Er SAs and the p-f orbital hybridization of Er-N moieties enable the formation of charge-transfer channel. Therefore, this study sheds light on the pivotal role of *CO adsorption in achieving efficient conversion from CO to CHOH (n=1, 2) via a novel rare earth-based dual SAs photocatalysis approach.