Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene
Abstract
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.
- Authors:
-
[3];
[4];
[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)
- Publication Date:
- Research Org.:
- Univ. of Illinois at Urbana-Champaign, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); BNL Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1395943
- Report Number(s):
- BNL-114361-2017-JA
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704; FG02-03ER15476
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 34; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
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., and Frenkel, Anatoly I. Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b06270.
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. Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene. United States. https://doi.org/10.1021/acs.jpcc.7b06270
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., and Frenkel, Anatoly I. Mon .
"Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene". United States. https://doi.org/10.1021/acs.jpcc.7b06270. https://www.osti.gov/servlets/purl/1395943.
@article{osti_1395943,
title = {Multimodal Study of the Speciations and Activities of Supported Pd Catalysts During the Hydrogenation of Ethylene},
author = {Zhao, Shen and Li, Yuanyuan and Liu, Deyu and Liu, Jing and Liu, Yao-Min and Zakharov, Dmitri N. and Wu, Qiyuan and Orlov, Alexander and Gewirth, Andrew A. and Stach, Eric A. and Nuzzo, Ralph G. and Frenkel, Anatoly I.},
abstractNote = {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.},
doi = {10.1021/acs.jpcc.7b06270},
journal = {Journal of Physical Chemistry. C},
number = 34,
volume = 121,
place = {United States},
year = {Mon Aug 07 00:00:00 EDT 2017},
month = {Mon Aug 07 00:00:00 EDT 2017}
}
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