Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene

Shen Zhao, Yuanyuan Li, Deyu Liu, Jing Liu, Yao Min Liu, Dmitri N. Zakharov, Qiyuan Wu, Alexander Orlov, Andrew A. Gewirth, Eric A. Stach, Ralph G. Nuzzo, Anatoly I. Frenkel

Research output: Contribution to journalArticle

Abstract

In this work we describe a multimodal exploration of the atomic structure and chemical state of silica-supported palladium nanocluster catalysts during the hydrogenation of ethylene in operando conditions that variously transform the metallic phases between hydride and carbide speciations. The work exploits a microreactor that allows combined multiprobe investigations by high-resolution transmission electron microscopy (HR-TEM), X-ray absorption fine structure (XAFS), and microbeam IR (μ-IR) analyses on the catalyst under operando conditions. The work specifically explores the reaction processes that mediate the interconversion of hydride and carbide phases of the Pd clusters in consequence to changes made in the composition of the gas-phase reactant feeds, their stability against coarsening, the reversibility of structural/compositional transformations, and the role that oligomeric/waxy byproducts (here forming under hydrogen-limited reactant compositions) might play in modifying activity. The results provide new insights into structural features of the chemistry/mechanisms of Pd catalysis during the selective hydrogenation of acetylene in ethylene - a process simplified here in the use of binary ethylene/hydrogen mixtures. These explorations, performed in operando conditions, provide new understandings of structure-activity relationships for Pd catalysis in regimes that actively transmute important attributes of electronic and atomic structures. (Chemical Equation Presented).

Original languageEnglish (US)
Pages (from-to)18962-18972
Number of pages11
JournalJournal of Physical Chemistry C
Volume121
Issue number34
DOIs
StatePublished - Aug 31 2017

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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  • Cite this

    Zhao, S., Li, Y., Liu, D., Liu, J., Liu, Y. M., Zakharov, D. N., Wu, Q., Orlov, A., Gewirth, A. A., Stach, E. A., Nuzzo, R. G., & Frenkel, A. I. (2017). Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene. Journal of Physical Chemistry C, 121(34), 18962-18972. https://doi.org/10.1021/acs.jpcc.7b06270