Strong Photothermal Tandem Catalysis for CO2 Reduction to C2H4 Boosted by Zr–O–W Interfacial H2O Dissociation

Solar-driven CO2 reduction to C2 products (e.g., C2H4) represents a promising approach for achieving carbon neutrality goals. Nevertheless, the high reaction barriers associated with C–C coupling and H2O dissociation hinder the multistep proton-coupled electron transfer (PCET) processes. Herein, we report a zirconium–tungsten oxide heterostructure with single atom Pt anchored on its surface (denoted as Pt/(Zr–W)Ox) to promote the tandem photocatalytic conversion of CO2 to C2H4. Specifically, CO generated at the Pt/ZrO2–x region migrates to the Pt/WO3–x region, where the C–C coupling process is enabled. Furthermore, the electron-deficient W at the Zr–O–W interface serves as a Lewis acid site, boosting the dissociation of H2O molecules to generate active hydrogen species (*H). The abundant supply of *H lowers the formation barriers of the key intermediates *COOH and *CHO. Under the concentrated solar irradiation, the C2H4 yield reaches 242 μmol·g–1 in 0.5 h with an electron-based selectivity of 83.9%, and the solar-to-chemical energy conversion efficiency reaches 1.17%. This work provides unique insights into the design of heterostructured photocatalysts with efficient *H feeding for CO2 reduction.