4.6 Article

Framework-confined Sn in Si-beta stabilizing ultra-small Pt nanoclusters as direct propane dehydrogenation catalysts with high selectivity and stability

期刊

CATALYSIS SCIENCE & TECHNOLOGY
卷 9, 期 24, 页码 6993-7002

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy01907c

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资金

  1. National Natural Science Foundation of China [21421001, 21573115, 21875118]
  2. Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering [2017-K13]
  3. Ph.D. Candidate Research Innovation Fund of NKU School of Materials Science and Engineering

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Industrial propane dehydrogenation (PDH) catalysts generally suffer from low catalytic stability due to coke deposition and metal sintering. Herein, highly stable Pt/Sn-Si-beta catalysts for PDH were prepared by an improved post-synthesis strategy, which consists of dealumination of H-beta and subsequent metal impregnation. It is indicated that Sn species existing in tetrahedral coordination states were incorporated into the framework of dealuminated beta (Si-beta). Meanwhile, Pt species were highly dispersed in the form of ultra-small nanoclusters on Pt/Sn-Si-beta due to the strong interaction between Pt and Sn(iv) sites confined in the Si-beta framework. The prepared Pt/Sn-Si-beta catalysts show excellent catalytic performance for PDH, in which the propene formation rate was 2.3 mol g(Pt)(-1) h(-1) with a propene selectivity of >99% at 550 degrees C and the higher propene formation rate was 3.1 mol g(Pt)(-1) h(-1) at 600 degrees C. Moreover, the strong Pt-Sn interactions and the confinement effect of Sn in the Si-beta framework inhibit the coke and sintering of Pt clusters, thereby achieving good stability of dehydrogenation and regeneration with almost unchanged catalytic activity during four cycles at 550 degrees C.

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