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

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

doi:10.1021/acs.jpcc.7b06270

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

Journal Article · Mon Aug 07 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b06270· OSTI ID:1395943

Zhao, Shen ^[1]; Li, Yuanyuan ^[2]; Liu, Deyu ^[3]; Liu, Jing ^[2]; Liu, Yao-Min ^[3]; Zakharov, Dmitri N. ^[4]; Wu, Qiyuan ^[2]; Orlov, Alexander ^[2];

^[3];

^[4]; Nuzzo, Ralph G. ^[3];

^[5]

Univ. of Illinois, Urbana, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States)
Univ. of Illinois, Urbana, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

In this paper 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. Finally, 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.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); BNL Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: SC0012704; FG02-03ER15476

OSTI ID:: 1395943

Report Number(s):: BNL-114361-2017-JA

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 34; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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