Low-Temperature Ethylbenzene Conversion on Rutile TiO2(100) via Photocatalysis: The Strong Photon Energy Dependence

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

2023-07-01

10.1021/acs.jpclett.3c01491

JOURNAL OF PHYSICAL CHEMISTRY LETTERS   影响因子和分区

1948-7185

Direct dehydrogenation of alkanesunder mild conditionsoffersa green route to produce valuable olefins, but realizing C-Hbond activation at a low temperature presents a significant challenge.Here, photocatalytic ethylbenzene conversion into styrene has beenachieved by one hole on rutile (R)-TiO2(100) at80 K under 257 and 343 nm irradiation. Although the rates of the initial & alpha;-C-H bond activation are nearly the same at the twowavelengths, the rate of the & beta;-C-H bond cleavage is stronglydependent upon hole energy, leading to the much higher yield of 290K styrene formation at 257 nm, which raises doubt about the simplifiedTiO(2) photocatalysis model in which excess energy of thecharge carrier is useless and highlights the importance of intermolecularenergy redistribution in photocatalytic reactions. The result notonly advances our understandings in low-temperature C-H bondactivation but also calls for the development of a more sophisticatedphotocatalysis model.

SCI ; EI

英语

NI论文

第一 ; 通讯

National Key Ramp;D Program of China[2018YFE0203002] ; National Natural Science Foundation of China["22173041","22173042","22103033","22103031","21973037"] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDB17000000] ; Shenzhen Science and Technology Innovation Committee["20220814164755002","ZDSYS20200421111001787"] ; Guangdong Innovative amp; Entrepreneurial Research Team Program["2019ZT08L455","2019JC01X091"] ; 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:001021462200001

AMER CHEMICAL SOC

20232914412443

Chemical activation ; Ethylbenzene ; Oxide minerals ; Photocatalysis ; Styrene ; Temperature

Minerals:482.2 ; Thermodynamics:641.1 ; Light/Optics:741.1 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2

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

Lai, Yuemiao,Zeng, Yi,Li, Fangliang,et al. Low-Temperature Ethylbenzene Conversion on Rutile TiO2(100) via Photocatalysis: The Strong Photon Energy Dependence[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2023,14(27):6286-6294.

Lai, Yuemiao.,Zeng, Yi.,Li, Fangliang.,Chen, Xiao.,Wang, Tao.,...&Guo, Qing.(2023).Low-Temperature Ethylbenzene Conversion on Rutile TiO2(100) via Photocatalysis: The Strong Photon Energy Dependence.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,14(27),6286-6294.

Lai, Yuemiao,et al."Low-Temperature Ethylbenzene Conversion on Rutile TiO2(100) via Photocatalysis: The Strong Photon Energy Dependence".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 14.27(2023):6286-6294.