4.8 Article

One-Pot Ethyl Acetate Production from Ethanol Photooxidation on Rutile TiO2(110): Strong Photon Energy Dependence

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 13, Issue 3, Pages 801-807

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c00048

Keywords

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Funding

  1. National Key R&D Program of China [2018YFE0203002]
  2. National Natural Science Foundation of China [22173041]
  3. Strategic Priority Research Program of Chinese Academy of Sciences [XDB17000000]
  4. Shenzhen Science and Technology Innovation Committee [JCYJ2019080914021660, ZDSYS20200421111001787]
  5. Guangdong Innovative & Entrepreneurial Research Team Program [2019ZT08L455, 2019JC01X091]
  6. International Partnership Program of Chinese Academy of Science [121421KYSB20170012]

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The formation of ethyl acetate from ethanol photooxidation on a rutile-TiO2 surface was investigated, and it was found that the photon energy has a significant effect on the reaction rate and product formation.
Ethyl acetate (EA) production from sequential ethanol (EtOH) photooxidation on a rutile(R)-TiO2(110) surface has been investigated by the temperature-programmed desorption (TPD) method at 355 and 266 nm. Significant EA product is detected under 266 nm irradiation, which is most likely to be formed via cross-coupling of primary dissociation products, aldehyde (CH3CHO) and ethoxy groups. On the contrary, EA formation at 355 nm is negligible. In addition, the initial rate of EA formation from EtOH at 266 nm is nearly 2 orders of magnitude faster than that at 355 nm. Quantitative analysis suggests that EA formation from sequential EtOH photooxidation on R-TiO2(110) is strongly dependent on photon energy or the energy of hot holes. This experimental result raises doubt about the traditional photocatalysis model on TiO2 where charge carriers relax to their respective band edges prior to charge transfer to adsorbates during the photocatalytic process, leading to no dependence on photon energy in TiO2 photocatalysis.

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