4.6 Article

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Journal

FRONTIERS IN CHEMISTRY
Volume 10, Issue -, Pages -

Publisher

FRONTIERS MEDIA SA
DOI: 10.3389/fchem.2022.833784

Keywords

perovskite; CsPbBr3; graphene oxide; anaerobic oxidation of aromatic alcohols; H2 production; photocatalysis

Funding

  1. National Natural Science Foundation of China [21905049, 21902132, 22178057]
  2. Award Program for the Minjiang Scholar Professorship
  3. Natural Science Foundation of the Fujian Province [2020J01201]
  4. Research Foundation-Flanders (FWO) [G.0B39.15, G.0B49.15, G098319N, 1280021N, 12Y7221N, 12Y6418N, VS052320N, ZW15_09-GOH6316N]
  5. KU Leuven Research Fund [C14/19/079, C3/19/046, iBOF-21-085 PERSIST]
  6. Flemish government through long term structural funding Methusalem [CASAS2, Meth/15/04]
  7. European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant [891276]

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This study demonstrates the selective oxidation of aromatic alcohols to aldehydes and hydrogen (H-2) production integrated on Pt-decorated CsPbBr3. The functionalization of CsPbBr3 with graphene oxide (GO) enhances the photoactivity of the perovskite catalyst. The introduction of GO decreases the particle size of CsPbBr3 and acts as an electron reservoir, leading to improved selectivity and H-2 evolution rate.
Metal halide perovskites (MHPs) have been widely investigated for various photocatalytic applications. However, the dual-functional reaction system integrated selective organic oxidation with H-2 production over MHPs is rarely reported. Here, we demonstrate for the first time the selective oxidation of aromatic alcohols to aldehydes integrated with hydrogen (H-2) evolution over Pt-decorated CsPbBr3. Especially, the functionalization of CsPbBr3 with graphene oxide (GO) further improves the photoactivity of the perovskite catalyst. The optimal amount of CsPbBr3/GO-Pt exhibits an H-2 evolution rate of 1,060 mu mol g(-1) h(-1) along with high selectivity (>99%) for benzyl aldehyde generation (1,050 mu mol g(-1) h(-1)) under visible light (lambda > 400 nm), which is about five times higher than the CsPbBr3-Pt sample. The enhanced activity has been ascribed to two effects induced by the introduction of GO: 1) GO displays a structure-directing role, decreasing the particle size of CsPbBr3 and 2) GO and Pt act as electron reservoirs, extracting the photogenerated electrons and prohibiting the recombination of the electron-hole pairs. This study opens new avenues to utilize metal halide perovskites as dual-functional photocatalysts to perform selective organic transformations and solar fuel production.

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