Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.150
Publication date: 23rd September 2021
Photoelectrochemical (PEC) oxidation of alcohol to the value-added aldehyde using semiconductor materials has been one of the promising approaches for green chemistry synthesis. It offers a low-temperature and low-pressure reaction environment to replace high pressure and high energy consumption of the industrial approach using silver catalysis. However, such reaction has been overlooked in the PEC research since alcohol is often used as hole scavengers and the product of this oxidation has not been attracted great attention. In addition, the aldehyde product, as the result of the highly selective oxidation product from alcohol PEC oxidation[1], is still highly reductive. Therefore, the reason that the oxidative photogenerated holes in hematite could not further oxidize aldehyde still remains unclear.
My presentation will primarily focus upon the acetaldehyde formation from PEC ethanol oxidation and its over-oxidation by the highly oxidative photogenerated holes in hematite photoanodes. The kinetic competition of alcohol oxidation and aldehyde oxidation will be primarily elucidated based on operando-spectroelectrochemical measurements[2]. In addition, the Ahhrenius relationship will also be established to elucidate how we can achieve highly selective aldehyde formation by linking thermodynamic and kinetic information learnt from such optical spectroscopies. On the other hand, the challenges in photo-oxidation of organics for the application of water purification will be discussed in detail in terms of the thermodynamic driving force and the reaction kinetics of the photocatalysts.
The author acknowledges the Fundamental Research Funds for the Central Universities No. 2232020G-04 and the Donghua University Research Fellowship Starting Grant.
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