In Situ Observation of Stepwise C-H Bond Scission: Deciphering the Catalytic Selectivity of Ethylbenzene-to-Styrene Conversion on TiO2

Lin，Haiping1,2; Wang，Zhijun3; Wang，Haochen4,8; Gao，Jianzhi1; Ding，Haoxuan5; Xu，Yong2; Li，Qing1,2; Guo，Qing4; Ma，Zhibo4; Yang，Xueming4,7; Pan，Minghu1,6

2020

10.1021/acs.jpclett.0c02729

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

1948-7185

The conversion of light alkanes to olefins is crucial to the chemical industry. The quest for improved catalytic performance for this conversion is motivated by current drawbacks including: expensive noble metal catalysts, poor conversion, low selectivity, and fast decay of efficiency. The in situ visualization of complex catalysis at the atomic level is therefore a major advance in the rational framework upon building the future catalysts. Herein, the catalytic C-H bond activations of ethylbenzene on TiO2(110)-(1 × 1) were explored with high-resolution scanning tunneling microscopy and first-principles calculations. We report that the first C-H bond scission is a two-step process that can be triggered by either heat or ultraviolet light at 80 K, with near 100% selectivity of β-CH bond cleavage. This work provides fundamental understanding of C-H bonds cleavage of ethylbenzene on metal oxides, and it may promote the design of new catalysts for selective styrene production under mild conditions.

SCI ; EI

英语

NI期刊

其他

Strategic Priority Research Program of Chinese Academy of Science[XDB17000000] ; National Key Research and Development Program of the MOST of China[2016 YFA0200603] ; National Natural Science Foundation of China[91745115][21703074][21673236][21771134][21972083][21872099]

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

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

WOS:000592959100046

AMER CHEMICAL SOC

2-s2.0-85096456817

Scopus

1.School of Physics and Information Technology,Shaanxi Normal University,Xi'an,710062,China
2.Institute of Functional Nano and Soft Materials and Collaborative,Innovation Center of Suzhou Nano Science and Technology,Soochow University,Suzhou,215123,China
3.Institute for Advanced Study,Chengdu University,Chengdu,610106,China
4.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
5.School of Physics and Astronomy,University of Birmingham,Birmingham,B15 2TT,United Kingdom
6.School of Physics,Huazhong University of Science and Technology,Wuhan,430074,China
7.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
8.University of Chinese Academy of Sciences,Beijing,100049,China

Lin，Haiping,Wang，Zhijun,Wang，Haochen,et al. In Situ Observation of Stepwise C-H Bond Scission: Deciphering the Catalytic Selectivity of Ethylbenzene-to-Styrene Conversion on TiO2[J]. Journal of Physical Chemistry Letters,2020,11(22):9850-9855.

Lin，Haiping.,Wang，Zhijun.,Wang，Haochen.,Gao，Jianzhi.,Ding，Haoxuan.,...&Pan，Minghu.(2020).In Situ Observation of Stepwise C-H Bond Scission: Deciphering the Catalytic Selectivity of Ethylbenzene-to-Styrene Conversion on TiO2.Journal of Physical Chemistry Letters,11(22),9850-9855.

Lin，Haiping,et al."In Situ Observation of Stepwise C-H Bond Scission: Deciphering the Catalytic Selectivity of Ethylbenzene-to-Styrene Conversion on TiO2".Journal of Physical Chemistry Letters 11.22(2020):9850-9855.