A Pt-cluster-based heterogeneous catalyst for homogeneous catalytic reactions: X-ray absorption spectroscopy and reaction kinetic studies of their activity and stability against leaching

Yimin Li, Jack Hung Chang Liu, Cole A. Witham, Wenyu Huang, Matthew A. Marcus, Sirine C. Fakra, Pinar Alayoglu, Zhongwei Zhu, Christopher M. Thompson, Arpana Arjun, Kihong Lee, Elad Gross, F. Dean Toste*, Gabor A. Somorjai

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

89 Scopus citations

Abstract

The design and development of metal-cluster-based heterogeneous catalysts with high activity, selectivity, and stability under solution-phase reaction conditions will enable their applications as recyclable catalysts in large-scale fine chemicals production. To achieve these required catalytic properties, a heterogeneous catalyst must contain specific catalytically active species in high concentration, and the active species must be stabilized on a solid catalyst support under solution-phase reaction conditions. These requirements pose a great challenge for catalysis research to design metal-cluster-based catalysts for solution-phase catalytic processes. Here, we focus on a silica-supported, polymer-encapsulated Pt catalyst for an electrophilic hydroalkoxylation reaction in toluene, which exhibits superior selectivity and stability against leaching under mild reaction conditions. We unveil the key factors leading to the observed superior catalytic performance by combining X-ray absorption spectroscopy (XAS) and reaction kinetic studies. On the basis of the mechanistic understandings obtained in this work, we also provide useful guidelines for designing metal-cluster-based catalyst for a broader range of reactions in the solution phase.

Original languageAmerican English
Pages (from-to)13527-13533
Number of pages7
JournalJournal of the American Chemical Society
Volume133
Issue number34
DOIs
StatePublished - 31 Aug 2011
Externally publishedYes

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