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A novel on-line electrochemical transmission infrared spectroscopy to?study the current efficiency of carbonates for?ethanol oxidation reactions in alkaline media
摘要： Research on the reaction mechanism of ethanol oxidation reaction (EOR) is important for the development of highly active EOR electro-catalysts. One of the main difficulties in the EOR study is the quantitative analysis of the non-volatile products. Conventional on-line electrochemical flowing transmission infrared spectroscopy (ETIRS) can only collect a part of the carbonate products of EOR in alkaline media, making the further quantitative study impossible. Herein, a new ETIRS system has been designed and prepared by employing a cation-exchange membrane (Nafion) in the sampling hood. The using of the Nafion membrane can prevent the anions crossing over by confining the generated carbonates in the sampling hood without diffusing into the bulk electrolyte. Therefore, the collection efficiency of the carbonate products as well as the test accuracy of the carbonate current efficiency has been significantly improved. The result of CO stripping reaction shows that ca. 100% of the carbonate product is able to be collected in alkaline media by this new system. The influence of the experimental temperature to the carbonate current efficiency has been further studied on Pt/C toward EOR in alkaline media.
关键词： Transmission infrared spectroscopy,Ethanol oxidation reaction,Platinum,Alkaline media
更新于2025-09-23 15:23:52
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Visible Light-Promoted Plasmon Resonance to Induce “Hot” Hole Transfer and Photothermal Conversion for Catalytic Oxidation
摘要： Titanium dioxide (TiO2) semiconductor photocatalysts were photosensitized to the visible spectrum with gold nanospheres (AuNSs) and gold nanorods (AuNRs) to study the ethanol photo-oxidation cycle, with an emphasis towards driving carbon-carbon (C-C) bond cleavage at low temperatures. The photocatalysts exhibited a localized surface plasmon resonance (SPR) that was harnessed to drive the complete photo-oxidation of formic acid (FA) and ethanol (EtOH) via augmented carrier generation/separation and photothermal conversion. Contributions of transverse and longitudinal localized SPR modes were decoupled by irradiating AuNSs-TiO2 and AuNRs-TiO2 with targeted wavelength ranges to probe their effects on plasmonically-assisted photocatalytic oxidation of FA and EtOH. Photocatalytic performance was assessed by monitoring the yield of gaseous products during photo-oxidation experiments using a gas chromatography-mass spectrometry-multiple headspace extraction (GC-MS-MHE) analysis method. The complete oxidation of EtOH to CO2 under visible-light irradiation was confirmed by GC-MS-MHE for both AuNSs and AuNRs on TiO2 at room temperature. Photothermal and local field enhancements were found to aid in selectively cleaving the C-C bond in EtOH to form FA, while FA was further oxidized to CO2 by plasmon-induced electron transfer mechanisms. Under visible light (>420 nm) irradiation, carrier generation/separation and photothermal conversion was achieved, resulting in the photogenerated “hot” holes driving the photo-oxidation primarily on the AuNPs. Specifically, plasmonic enhancement by AuNR-TiO2 enhances EtOH oxidation, providing a method to selectively cleave C-C bonds.
关键词： Carbon-carbon bond cleavage,Photocatalysis,Hybrid Materials,Gold nanoparticles,Ethanol oxidation,Magnetic,Formic acid oxidation,Plasmonics,TiO2,Optical
更新于2025-09-10 09:29:36