journal article·2023-07-13

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

Yuemiao Lai, Yi Zeng, Fangliang Li, Xiao Chen, Tao Wang, Xueming Yang, Qing Guo

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Abstract

Direct dehydrogenation of alkanes under mild conditions offers a green route to produce valuable olefins, but realizing C–H bond activation at a low temperature presents a significant challenge. Here, photocatalytic ethylbenzene conversion into styrene has been achieved by one hole on rutile (R)–TiO 2 (100) at 80 K under 257 and 343 nm irradiation. Although the rates of the initial α-C–H bond activation are nearly the same at the two wavelengths, the rate of the β-C–H bond cleavage is strongly dependent upon hole energy, leading to the much higher yield of 290 K styrene formation at 257 nm, which raises doubt about the simplified TiO 2 photocatalysis model in which excess energy of the charge carrier is useless and highlights the importance of intermolecular energy redistribution in photocatalytic reactions. The result not only advances our understandings in low-temperature C–H bond activation but also calls for the development of a more sophisticated photocatalysis model.
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Research context

OpenAlex topics: TiO2 Photocatalysis and Solar Cells · Advanced Photocatalysis Techniques · Catalytic Processes in Materials Science

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Shenzhen Key Laboratory of Energy Chemistry & Department of Chemistry, Southern University of Science and Technology, Shenzhen, Guangdong 518055, People’s Republic of China

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, People’s Republic of China

Hefei National Laboratory, Hefei, Anhui 230088, People’s Republic of China

Funding

Guangdong Province Introduction of Innovative R&D Team · Ministry of Science and Technology of the People's Republic of China · National Key Research and Development Program of China · Science, Technology and Innovation Commission of Shenzhen Municipality · National Natural Science Foundation of China · Chinese Academy of Sciences

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