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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
Journal of the American Chemical Society (2011)
  • Yimin Li, University of California - Berkeley
  • Jack Hung Chang Liu, University of California - Berkeley
  • Cole A. Witham, University of California - Berkeley
  • Wenyu Huang, University of California - Berkeley
  • Matthew A. Marcus, University of California - Berkeley
  • Sirine C. Fakra, University of California - Berkeley
  • Pinar Alayoglu, University of California - Berkeley
  • Zhongwei Zhu, University of California - Berkeley
  • Christopher M. Thompson, University of California - Berkeley
  • Arpana Arjun, University of California - Berkeley
  • Kihong Lee, University of California - Berkeley
  • Elad Gross, University of California - Berkeley
  • F. Dean Toste, University of California - Berkeley
  • Gabor A. Somorjai, University of California - Berkeley
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.

Publication Date
2011
Publisher Statement
Reprinted (adapted) with permission from J. Am. Chem. Soc., 2011, 133 (34), pp 13527–13533. Copyright 2011 American Chemical Society.
Citation Information
Yimin Li, Jack Hung Chang Liu, Cole A. Witham, Wenyu Huang, et al.. "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" Journal of the American Chemical Society Vol. 133 Iss. 34 (2011)
Available at: http://works.bepress.com/wenyu_huang/7/