Highly Selective Coupled CO ₂ ‐to‐CO Reduction and Anisyl Alcohol Oxidation Over In Situ‐Anchored CdSe Quantum Dots on MgCdAl‐LDH

ABSTRACT Photocatalytic CO ₂ reduction reaction (CO ₂ RR) is a promising route for solar‐to‐chemical conversion, yet its performance is still limited by weak CO ₂ activation, rapid charge recombination, and the use of sacrificial reagents. Coupling CO ₂ RR with value‐added organic oxidation can improve overall redox efficiency, but it requires efficient interfacial charge transport and balanced dual‐half‐reaction kinetics. Herein, we report an in situ‐derived CdSe quantum dots/layered double hydroxide (CdSe/LDH) composite catalyst for visible light driven CO ₂ to CO reduction coupled with anisyl alcohol oxidation to pinacol, without external photosensitizers or sacrificial donors. In situ X‐ray absorption spectroscopy reveals reactant‐dependent electronic shifts under illumination, indicating dynamic interfacial charge redistribution during catalysis. Compared with the individual components, the coupled catalyst delivers approximately threefold higher CO evolution, high pinacol selectivity (∼98%), and markedly improved cycling stability under visible‐light irradiation ( λ ≥ 400 nm). This work demonstrates an in situ interface‐engineering strategy to stabilize quantum‐dot photocatalysts while promoting synergistic activity, selectivity, and durability in dual‐end photocatalytic redox coupling.