Strong Photothermal\nTandem Catalysis for CO<sub>2</sub> Reduction to C<sub>2</sub>H<sub>4</sub> Boosted by Zr–O–W\nInterfacial H<sub>2</sub>O Dissociation

Solar-driven CO<sub>2</sub> reduction to C<sub>2</sub> products\n(e.g., C<sub>2</sub>H<sub>4</sub>) represents a promising approach\nfor achieving carbon neutrality goals. Nevertheless, the high reaction\nbarriers associated with C–C coupling and H<sub>2</sub>O dissociation\nhinder the multistep proton-coupled electron transfer (PCET) processes.\nHerein, we report a zirconium–tungsten oxide heterostructure\nwith single atom Pt anchored on its surface (denoted as Pt/(Zr–W)O<sub><i>x</i></sub>) to promote the tandem photocatalytic conversion\nof CO<sub>2</sub> to C<sub>2</sub>H<sub>4</sub>. Specifically, CO\ngenerated at the Pt/ZrO<sub>2–<i>x</i></sub> region\nmigrates to the Pt/WO<sub>3–<i>x</i></sub> region,\nwhere the C–C coupling process is enabled. Furthermore, the\nelectron-deficient W at the Zr–O–W interface serves\nas a Lewis acid site, boosting the dissociation of H<sub>2</sub>O\nmolecules to generate active hydrogen species (*H). The abundant supply\nof *H lowers the formation barriers of the key intermediates *COOH\nand *CHO. Under the concentrated solar irradiation, the C<sub>2</sub>H<sub>4</sub> yield reaches 242 μmol·g<sup>–1</sup> in 0.5 h with an electron-based selectivity of 83.9%, and the solar-to-chemical\nenergy conversion efficiency reaches 1.17%. This work provides unique\ninsights into the design of heterostructured photocatalysts with efficient\n*H feeding for CO<sub>2</sub> reduction.