Abstract
Metal halide perovskites (MHPs) have been widely investigated for various photocatalytic applications. However, the dual-functional reaction system integrated selective organic oxidation with H2 production over MHPs is rarely reported. Here, we demonstrate for the first time the selective oxidation of aromatic alcohols to aldehydes integrated with hydrogen (H2) 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 H2 evolution rate of 1,060 μmol g−1 h−1 along with high selectivity (>99%) for benzyl aldehyde generation (1,050 μmol g−1 h−1) under visible light (λ > 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.
Highlights
The selective oxidation of alcohols to carbonyls represents one of the most important reactions in both the fine chemical industry and laboratory research (Shibuya et al, 2011; Yang and Xu, 2013; Sharma et al, 2016; Xue Yang et al, 2017; Liu et al, 2018a; Huang et al, 2018; Li et al, 2020; Shang et al, 2021); the carbonyl products are widely used intermediates and precursors for the manufacture of perfumes, pharmaceuticals, and dyes (Liu et al, 2015; Agosti et al, 2020; Xia et al, 2020; Shang et al, 2021)
Owing to the addition of GO, the light absorption of CPB/GO composites in the region of visible light (550–800 nm) gradually enhances with the increase in the weight ratios of GO, and the colors of the samples change from yellow to brown (Supplementary Figure S2), which can be attributed to the significant background absorption of GO (Xu et al, 2011)
The absorption edges for CsPbBr3 and CPB/GO are around 548 nm, which correlates with the intrinsic absorption of the material (Supplementary Figure S3)
Summary
The selective oxidation of alcohols to carbonyls represents one of the most important reactions in both the fine chemical industry and laboratory research (Shibuya et al, 2011; Yang and Xu, 2013; Sharma et al, 2016; Xue Yang et al, 2017; Liu et al, 2018a; Huang et al, 2018; Li et al, 2020; Shang et al, 2021); the carbonyl products are widely used intermediates and precursors for the manufacture of perfumes, pharmaceuticals, and dyes (Liu et al, 2015; Agosti et al, 2020; Xia et al, 2020; Shang et al, 2021). Coupling the oxidative dehydrogenation of alcohols with reductive hydrogen production is challenging Within this context, the advancement of photocatalytic anaerobic oxidation technology in recent years provides a promising strategy. The advancement of photocatalytic anaerobic oxidation technology in recent years provides a promising strategy This approach utilizes photogenerated holes to oxidize organics while employing photoelectrons to reduce the removed protons to produce H2, completing the oxidative–reductive coupled reaction (Weng et al, 2016; Han et al, 2017; Zhou et al, 2020; Peixian Li et al, 2021). The perovskite shows a long carrier lifetime of tens to hundreds of μs and diffusion length of μm levels, providing more opportunities for the diffusion and utilization of photoinduced holes and electrons (Dong et al, 2015; Bi et al, 2016) In this context, these unique features enable the metal halogen perovskite to be an appealing candidate for the organic conversion-coupled hydrogen production reaction, but the research is still rarely reported so far. Where C0 is the initial concentration of aromatic alcohols, and CA and CAD are the concentrations of aromatic alcohols and aldehydes measured after the photocatalytic reaction for a specific time, respectively
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