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Highly efficient visible-light photocatalytic ethane oxidation into ethyl hydroperoxide as a radical reservoir.

ABSTRACT: Photocatalytic ethane conversion into value-added chemicals is a great challenge especially under visible light irradiation. The production of ethyl hydroperoxide (CH₃CH₂OOH), which is a promising radical reservoir for regulating the oxidative stress in cells, is even more challenging due to its facile decomposition. Here, we demonstrated a design of a highly efficient visible-light-responsive photocatalyst, Au/WO₃, for ethane oxidation into CH₃CH₂OOH, achieving an impressive yield of 1887 μmol g_cat ^-1 in two hours under visible light irradiation at room temperature for the first time. Furthermore, thermal energy was introduced into the photocatalytic system to increase the driving force for ethane oxidation, enhancing CH₃CH₂OOH production by six times to 11 233 μmol g_cat ^-1 at 100 °C and achieving a significant apparent quantum efficiency of 17.9% at 450 nm. In addition, trapping active species and isotope-labeling reactants revealed the reaction pathway. These findings pave the way for scalable ethane conversion into CH₃CH₂OOH as a potential anticancer drug.

SUBMITTER: Zhu Y

PROVIDER: S-EPMC8179680 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Redox mediators in visible light photocatalysis: photocatalytic radical thiol-ene additions.

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Metal-Organic Framework-Derived ZnO/ZnS Heteronanostructures for Efficient Visible-Light-Driven Photocatalytic Hydrogen Production.

Project description:Developing highly active, recyclable, and inexpensive photocatalysts for hydrogen evolution reaction (HER) under visible light is significant for the direct conversion of solar energy into chemical fuels for various green energy applications. For such applications, it is very challenging but vitally important for a photocatalyst to simultaneously enhance the visible-light absorption and suppress photogenerated electron-hole recombination, while also to maintain high stability and recyclability. Herein, a metal-organic framework (MOF)-templated strategy has been developed to prepare heterostructured nanocatalysts with superior photocatalytic HER activity. Very uniquely, the synthesized photocatalytic materials can be recycled easily after use to restore the initial photocatalytic activity. It is shown that by controlling the calcination temperature and time with MOF-5 as a host and guest thioacetamide as a sulfur source, the chemical compositions of the formed heterojunctions of ZnO/ZnS can be tuned to further enhance the visible-light absorption and photocatalytic activity. The nanoscale heterojunction ZnO/ZnS structural feature serves to reduce the average free path of charge carriers and improve the charge separation efficiency, thus leading to significantly enhanced HER activity under visible-light irradiation (? > 420 nm) with high stability and recyclability without any cocatalyst.

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Project description:Constructing the heterojunctions or designing the novel nanostructures are thought as effective methods to improve photocatalytic activities of semiconductors. Herein, a one-step green route was developed to fabricate bismuth oxyiodide/activated carbon (BiOI/C) composite. The prepared BiOI/C exhibit obviously red shifts and increased absorption range of visible light. The presence of Bi-C bonds confirms the heterojunction, on account of which the BiOI nanosheets tightly grew on the surface of carbon and subsequently provided the hierarchical structure, sufficient interfacial interaction and high specific surface area. Significantly, the sufficient interracial interaction is beneficial to the detachment of electrons (e-)-holes (h+) pairs and the Bi-C bonds work like a bridge to rapidly transmit the e- from BiOI to carbon. What's more, the hierarchical structure of BiOI/C efficiently shortened the diffusion pathways of pollutants and the high SBET provided more exposed reaction sites. Benefiting from multiple synergistic effects, the as-prepared BiOI/C exhibited enhanced photocatalytic activities in degrading Rhodamine B (RhB) solution under visible light irradiation. The degradation rate of optimized BiOI/C reaches up to 95% in 120 min, and the efficiency is 3.36 times higher than pure BiOI. This study provides a promising strategy that activated carbon can be utilized in highly-efficiency photocatalysts.

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