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

被引:3
作者
Sun, Rulin [1 ]
Liu, Xinlu [1 ]
Chen, Xiao [2 ,3 ]
Che, Li [1 ]
Yang, Xueming [2 ,3 ,4 ]
Guo, Qing [2 ,3 ]
机构
[1] Dalian Maritime Univ, Coll Environm Sci & Engn, Dalian 116026, Liaoning, Peoples R China
[2] Southern Univ Sci & Technol, Shenzhen Key Lab Energy Chem, Shenzhen 518055, Guangdong, Peoples R China
[3] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
[4] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2022年 / 13卷 / 03期
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
PHOTOCATALYTIC OXIDATION; METHYL FORMATE; METHANOL; SURFACE; DISSOCIATION; ADSORPTION; MECHANISM; WATER; PHOTOREACTION; DECOMPOSITION;
D O I
10.1021/acs.jpclett.2c00048
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:801 / 807
页数:7
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