Low-Temperature C-H Bond Activation via Photocatalysis: Highly Efficient Ethylbenzene Dehydrogenation into Styrene on Rutile TiO2(110)

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

2022-09-01

10.1021/acs.jpclett.2c02269

Journal of Physical Chemistry Letters   Impact Factor & Quartile

1948-7185

The direct dehydrogenation of hydrocarbons to olefins under mild conditions is an atom-economical but challenging route. Here, we have investigated photocatalytic ethylbenzene dehydrogenation into styrene on rutile(R)-TiO2(110) using the temperature-programmed desorption (TPD) method. The results demonstrate that photocatalytic ethylbenzene dehydrogenation into styrene occurs on R-TiO2(110) in a stepwise manner, in which the initial alpha-C-H bond cleavage occurs facilely under UV irradiation via a possible homolytic hydrogen atom transfer process and then is followed by the second C-H bond cleavage induced by either photocatalysis at similar to 120 K or thermocatalysis at >400 K. With preadsorbed oxygen atoms to eliminate hydrogen atoms from ethylbenzene dehydrogenation and excess electrons on the surface, the yield of styrene is largely enhanced by about 4 times. The results not only demonstrate a photocatalytic route for ethylbenzene dehydrogenation into styrene on R-TiO2(110) but also advance our understanding of the photocatalytic activation of the saturated C-H bond with TiO2.

SCI

English

NI Journal Papers

First ; Corresponding

National Key R&D Program of China[2018YFE0203002] ; National Natural Science Foundation of China (NSFC Center for Chemical Dynamics)["22173041","22103033","22103031","22173042","21973037"] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDB17000000] ; Shenzhen Science and Technology Innovation Committee["JCYJ2019080914021660","ZDSYS20200421111001787"] ; Guangdong Innovative & Entrepreneurial Research Team Program["2019ZT08L455","2019JC01X091"] ; International Partnership Program of the Chinese Academy of Science[121421KYSB20170012] ; Innovation Program for Quantum Science and Technology[2021ZD0303304]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000863619700001

AMER CHEMICAL SOC

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, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China
4.Hefei Natl Lab, Hefei 230088, Anhui, Peoples R China

Li, Fangliang,Chen, Xiao,Lai, Yuemiao,et al. Low-Temperature C-H Bond Activation via Photocatalysis: Highly Efficient Ethylbenzene Dehydrogenation into Styrene on Rutile TiO2(110)[J]. Journal of Physical Chemistry Letters,2022.

Li, Fangliang,Chen, Xiao,Lai, Yuemiao,Wang, Tao,Yang, Xueming,&Guo, Qing.(2022).Low-Temperature C-H Bond Activation via Photocatalysis: Highly Efficient Ethylbenzene Dehydrogenation into Styrene on Rutile TiO2(110).Journal of Physical Chemistry Letters.

Li, Fangliang,et al."Low-Temperature C-H Bond Activation via Photocatalysis: Highly Efficient Ethylbenzene Dehydrogenation into Styrene on Rutile TiO2(110)".Journal of Physical Chemistry Letters (2022).