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The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H 2  and CO 2  molecules and enable efficient gas-phase CO 2  photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In 3+  ions in In 2 O 3  by single-site Bi 3+  ions, thereby enhancing the propensity to activate CO 2  molecules. The so-formed Bi x In 2-x O 3  materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In 2 O 3  itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of Bi x In 2-x O 3  also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO 2  photocatalysis, another step towards the vision of the solar CO 2  refinery.

Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation