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

Yu-Jie Wang; Gui-Lin Zhuang; Jiang-Wei Zhang; Fang Luo; Xin Cheng; Fu-Li Sun; Shan-Shan Fu; Tong-Bu Lu; Zhi-Ming Zhang

doi:10.1002/anie.202216592

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

Angew Chem Int Ed Engl. 2023 Feb 1;62(6):e202216592. doi: 10.1002/anie.202216592. Epub 2022 Dec 28.

Authors

Yu-Jie Wang^{1

2}, Gui-Lin Zhuang³, Jiang-Wei Zhang⁴, Fang Luo¹, Xin Cheng², Fu-Li Sun³, Shan-Shan Fu², Tong-Bu Lu², Zhi-Ming Zhang^{1

2}

Affiliations

¹ Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education, Northeast Normal University, Jilin, 130024, China.
² Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin, 300384, China.
³ Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, China.
⁴ College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021, P. R. China.

PMID: 36478491
DOI: 10.1002/anie.202216592

Abstract

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.

Keywords: CO2 Photoreduction; Polyoxometalate; Polyoxovanadate; Single-Atom-Site Catalyst.

Abstract

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