Photocatalytic CO2 conversion into valuable solar fuels is highly appealing, but lack of directional charge-transfer channel and insufficient active sites resulted in limited CO2 reduction efficiency and selectivity for most photocatalytic systems. Herein, we designed and fabricated rare-earth La single-atoms on carbon nitride with La–N charge-transfer bridge as the active center for photocatalytic CO2 reaction. The formation of La single-atoms was certified by spherical aberration-corrected HAADF-STEM, STEM-EELS, EXAFS, and theoretical calculations. The electronic structure of the La–N bridge enables a high CO-yielding rate of 92 μmol·g–1·h–1 and CO selectivity of 80.3%, which is superior to most g-C3N4-based photocatalytic CO2 reductions. The CO production rate remained nearly constant under light irradiation for five cycles of 20 h, indicating its stability. The closely combined experimental and DFT calculations clearly elucidated that the variety of electronic states induced by 4f and 5d orbitals of the La single atom and the p–d orbital hybridization of La–N atoms enabled the formation of charge-transfer channel. The La–N charge bridges are found to function as the key active center for CO2 activation, rapid COOH* formation, and CO desorption. The present work would provide a mechanistic understanding into the utilization of rare-earth single-atoms in photocatalysis for solar energy conversion.

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The alternative charge arrangement on the {010} facet of BiOCl facilitates benzyl oxidation and selectivity for benzoic acid ring-opening reactions, subsequently resulting in remarkably enhanced photocatalytic efficiency.

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Cu 2 O microparticles with controllable crystal planes and relatively high stability have been recognized as a good platform to understand the mechanism of the electrocatalytic CO 2 reduction reaction (CO 2 RR). Herein, we demonstrate that the in situ generated Cu 2 O/Cu interface plays a key role in determining the selectivity of methane formation, rather than the initial crystal plane of the reconstructed Cu 2 O microparticles. Experimental results indicate that the methane evolution is dominated on all three different crystal planes with similar Tafel slopes and longterm stabilities. Density functional theory (DFT) calculations further reveal that *CO is protonated via a similar bridge configuration at the Cu 2 O/Cu interface, regardless of the initial crystal planes of Cu 2 O. The Gibbs free energy changes (ΔG) of *CHO on different reconstructed Cu 2 O planes are close and more negative than that of *OCCOH, indicating the methane formation is more favorable than ethylene on all Cu 2 O crystal planes.