Photocatalytic ethane conversion on rutile TiO₂(110): identifying the role of the ethyl radical

Li, Fangliang1,2; Lai, Yuemiao1,2; Zeng, Yi1,2; Chen, Xiao1,2; Wang, Tao1,2; Yang, Xueming1,2,3,4; Guo, Qing1,2

2023-11-01

10.1039/d3sc05623f

CHEMICAL SCIENCE   影响因子和分区

2041-6520

2041-6539

Oxidative dehydrogenation of ethane (C2H6, ODHE) is a promising approach to producing ethene (C2H4) in the chemical industry. However, the ODHE needs to be operated at a high temperature, and realizing the ODHE under mild conditions is still a big challenge. Herein, using photocatalytic ODHE to obtain C2H4 has been achieved successfully on a model rutile(R)-TiO2(110) surface with high selectivity. Initially, the C2H6 reacts with hole trapped O-Ti(-) centers to produce ethyl radicals , which can be precisely detected by a sensitive TOF method, and then the majority of the radicals spontaneously dehydrogenate into C2H4 without another photo-generated hole. In addition, parts of the radicals rebound with diversified surface sites to produce C-2 products via migration along the surface. The mechanistic model built in this work not only advances our knowledge of the C-H bond activation and low temperature C2H6 conversion, but also provides new opportunities for realizing the ODHE with high C2H4 efficiency under mild conditions.

SCI ; EI

英语

NI论文

第一 ; 通讯

National Natural Science Foundation of China["2022YFA1503102","2018YFE0203002"] ; National Key R&D Program of China["22173041","22103033","22103031","22173042","21973037"] ; National Natural Science Foundation of China[XDB17000000] ; Strategic Priority Research Program of Chinese Academy of Sciences["20220814164755002","ZDSYS20200421111001787"] ; Shenzhen Science and Technology Innovation Committee["2019ZT08L455","2019JC01X091"] ; Guangdong Innovative & Entrepreneurial Research Team Program[121421KYSB20170012] ; International Partnership Program of Chinese Academy of Sciences[2021ZD0303304]

Chemistry

Chemistry, Multidisciplinary

WOS:001115660600001

ROYAL SOC CHEMISTRY

20235115233585

Chemical bonds ; Dehydrogenation ; Ethane ; Ethylene ; Oxide minerals ; Temperature ; Titanium dioxide

Minerals:482.2 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Chemical Engineering, General:805

Web of Science

1.Southern Univ Sci & Technol, Shenzhen Key Lab Energy Chem, Shenzhen 518055, Guangdong, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian Inst Chem Phys, Dalian 116023, Liaoning, Peoples R China
4.Hefei Natl Lab, Hefei 230088, Peoples R China

Li, Fangliang,Lai, Yuemiao,Zeng, Yi,et al. Photocatalytic ethane conversion on rutile TiO₂(110): identifying the role of the ethyl radical[J]. CHEMICAL SCIENCE,2023,15:307-316.

Li, Fangliang.,Lai, Yuemiao.,Zeng, Yi.,Chen, Xiao.,Wang, Tao.,...&Guo, Qing.(2023).Photocatalytic ethane conversion on rutile TiO₂(110): identifying the role of the ethyl radical.CHEMICAL SCIENCE,15,307-316.

Li, Fangliang,et al."Photocatalytic ethane conversion on rutile TiO₂(110): identifying the role of the ethyl radical".CHEMICAL SCIENCE 15(2023):307-316.