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Efficient Photocatalytic CH4-to-Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles
Quan Zhang1,2, Chao Yang1, Yangshen Chen1
1Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438, China.
This study introduces a novel gold-nanoparticle-functionalized bismuth vanadate (BiVO4@Au) photocatalyst for converting methane (CH4) to ethanol. The catalyst enhances ethanol selectivity by controlling hydroxyl radical (⋅OH) levels, achieving high yields at ambient conditions.
Area of Science:
- Materials Science
- Photocatalysis
- Green Chemistry
Background:
- Selective oxidation of methane (CH4) to multi-carbon products like ethanol is highly desirable but challenging due to the inert C-H bond.
- Hydroxyl radicals (⋅OH) are crucial for CH4 activation but can lead to over-oxidation, forming undesirable C1 products instead of ethanol.
- Developing photocatalysts that can selectively activate CH4 and promote C-C coupling is essential for efficient ethanol synthesis.
Purpose of the Study:
- To develop a highly selective photocatalyst for converting CH4 to ethanol under ambient conditions.
- To investigate the role of surface-modified gold nanoparticles (Au) on BiVO4 in controlling reactive oxygen species and enhancing ethanol selectivity.
- To optimize the photocatalytic system for improved CH4-to-ethanol conversion efficiency and stability.
Main Methods:
- Synthesis of BiVO4 photocatalyst functionalized with Au nanoparticles (BiVO4@Au).
- Photocatalytic oxidation of CH4 using the developed BiVO4@Au catalyst under ambient conditions.
- Utilizing a gas-diffusion layer to enhance CH4 transport to the photocatalytic interface.
- Characterization of reactive oxygen species (ROS) and reaction intermediates to understand the reaction mechanism.
Main Results:
- The BiVO4@Au photocatalyst demonstrated efficient CH4 activation and selective oxidation to ethanol.
- Surface functionalization with Au nanoparticles helped generate methyl radicals (⋅CH3) and consume ⋅OH, enhancing the ⋅CH3/⋅OH ratio.
- The use of a gas-diffusion layer further improved ethanol selectivity and production rates.
- Achieved a peak ethanol yield of 680 μmol·g-1·h-1 with 86% selectivity and >100 hours of stable photoconversion.
Conclusions:
- The BiVO4@Au photocatalyst provides an effective strategy for selective CH4-to-ethanol conversion.
- In situ generation and modulation of ⋅OH levels are critical for promoting C-C coupling and suppressing over-oxidation.
- This approach offers a promising pathway for sustainable production of multi-carbon chemicals from methane.
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