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Research Article

Kinetics and mechanistic insights into the active sites of Au catalysts for selective propylene oxidation

Qianhong Wang§, Zhihua Zhang§, Keng Sang, Wenyao Chen( ), Gang Qian, Jing Zhang, Xinggui Zhou, Xuezhi Duan ( )
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

§ Qianhong Wang and Zhihua Zhang contributed equally to this work.

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Graphical Abstract

A kinetics strategy to identify the active sites of Au catalyst for the disentanglement of geometric and electronic effects on the selective oxidation of propylene to acrolein is provided. Acrolein is found likely to generate over Au (111) site via the hydrogen-assisted O2 activation to oxygenated species for its oxidizing propylene.

Abstract

Identification of the catalytically active sites emerges as the prerequisite for an atomic-level comprehensive understanding and further rational design of highly efficient catalysts. Here, we demonstrate a kinetics strategy to identify the active sites of Au catalyst for the disentanglement of geometric and electronic effects on the selective oxidation of propylene to acrolein. Both the Ti-containing titanium-silicalite-1 (TS-1) and Ti-free silicalite-1 (S-1) were employed as supports to immobilize Au catalysts, which were investigated by a combination of multiple characterization, kinetics analysis, and crystal structure modelling. The Au (111) sites are identified as the main active site for acrolein formation, while their electronic effects are highly relevant to the presence or absence of Ti. Moreover, propylene epoxide (PO) formation mainly involves the co-participation of Au and Ti sites, and the proximity between Au and Ti sites is found to have less influences on PO formation in a certain distance. In comparison, acrolein is very likely to generate over Au (111) sites via the hydrogen-assisted O2 activation to oxygenated species for its oxidizing propylene. The insights gained here could guide the design and preparation of Au catalysts for selective propylene oxidation.

Keywords

propylene oxidationAu catalystsactive sitegeometric and electronic effectsAu-Ti proximity

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Nano Research
Volume 16 Issue 5,
May 2023
Pages 6220-6227
DOI: 10.1007/s12274-022-5283-5
Cite this article:
Wang Q, Zhang Z, Sang K, et al. Kinetics and mechanistic insights into the active sites of Au catalysts for selective propylene oxidation. Nano Research, 2023, 16(5): 6220-6227. https://doi.org/10.1007/s12274-022-5283-5
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Received: 25 August 2022
Revised: 20 October 2022
Accepted: 31 October 2022
Published: 27 December 2022
© Tsinghua University Press 2022
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