Co-Dissolved Isostructural Polyoxovanadates to Construct Single-Atom-Site Catalysts for Efficient CO₂ Photoreduction

We explored a co-dissolved strategy to embed mono-dispersed Pt center into V₂ O₅ support via dissolving [PtV₉ O₂₈ ]^7- into [V₁₀ O₂₈ ]^6- aqueous solution. The uniform dispersion of [PtV₉ O₂₈ ]^7- in [V₁₀ O₂₈ ]^6- solution allows [PtV₉ O₂₈ ]^7- to be surrounded by [V₁₀ O₂₈ ]^6- clusters via a freeze-drying process. The V centers in both [PtV₉ O₂₈ ]^7- and [V₁₀ O₂₈ ]^6- were converted into V₂ O₅ via a calcination process to stabilize Pt center. These double separations can effectively prevent the Pt center agglomeration during the high-temperature conversion process, and achieve 100 % utilization of Pt in [PtV₉ O₂₈ ]^7- . The resulting Pt-V₂ O₅ single-atom-site catalysts exhibit a CH₄ yield of 247.6 μmol g^-1  h^-1 , 25 times higher than that of Pt nanoparticle on the V₂ O₅ support, which was accompanied by the lactic acid photooxidation to form pyruvic acid. Systematical investigations on this unambiguous structure demonstrate an important role of Pt-O atomic pair synergy for highly efficient CO₂ photoreduction.