Evolution and Enabling Capabilities of Spatially Resolved Techniques for the Characterization of Heterogeneously Catalyzed Reactions

Kevin Morgan; Jamal Touitou; Jae Soon Choi; Ciarán Coney; Christopher Hardacre; Josh A. Pihl; Cristina E. Stere; Mi Young Kim; Caomhán Stewart; Alexandre Goguet; William P. Partridge

doi:10.1021/acscatal.5b02602

Evolution and Enabling Capabilities of Spatially Resolved Techniques for the Characterization of Heterogeneously Catalyzed Reactions

Kevin Morgan, Jamal Touitou, Jae Soon Choi, Ciarán Coney, Christopher Hardacre, Josh A. Pihl, Cristina E. Stere, Mi Young Kim, Caomhán Stewart, Alexandre Goguet, William P. Partridge

Research output: Contribution to journal › Article › peer-review

65 Scopus citations

Abstract

The development and optimization of catalysts and catalytic processes requires knowledge of reaction kinetics and mechanisms. In traditional catalyst kinetic characterization, the gas composition is known at the inlet, and the exit flow is measured to determine changes in concentration. As such, the progression of the chemistry within the catalyst is not known. Technological advances in electromagnetic and physical probes have made visualizing the evolution of the chemistry within catalyst samples a reality, as part of a methodology commonly known as spatial resolution. Herein, we discuss and evaluate the development of spatially resolved techniques, including the evolutions and achievements of this growing area of catalytic research. The impact of such techniques is discussed in terms of the invasiveness of physical probes on catalytic systems, as well as how experimentally obtained spatial profiles can be used in conjunction with kinetic modeling. Furthermore, some aims and aspirations for further evolution of spatially resolved techniques are considered.

Original language	English
Pages (from-to)	1356-1381
Number of pages	26
Journal	ACS Catalysis
Volume	6
Issue number	2
DOIs	https://doi.org/10.1021/acscatal.5b02602
State	Published - Feb 5 2016

Funding

The authors of Queen''s University Belfast wish to thank EPSRC UK for funding under the First Grant Scheme (AG; EP/F026390/1), and the CASTech (EP/G02152X/1) and UK Catalysis Hub (EP/K014714/1) projects. Funding of studentships by EPSRC UK and Johnson Matthey under a CASE award (CC), and the Department of Employment and Learning NI (CS) are also acknowledged. W.P.P. thanks Professors William Epling, Michael Harold, Raimund Horn, Petr Kocǐ ,́ and Louise Olsson, as well as Neal Currier and Melanie DeBusk for helpful discussions. ORNL''s research and contributions were sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office, with Gurpreet Singh, Ken Howden, and Leo Breton as the Program Managers. The authors also wish to express gratitude to graphic artist Colby A. Earles of ORNL for the enhancement of the cover art design.

Funders	Funder number
Department of Employment and Learning NI
Louise Olsson
Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office
U.S. Department of Energy
Oak Ridge National Laboratory
Center for Advanced Systems and Engineering, Syracuse University
Engineering and Physical Sciences Research Council	EP/F026390/1, EP/G02152X/1, EP/K014714/1, EP/K014706/1, EP/K014854/1
UK Catalysis Hub

Keywords

catalyst characterization
electromagnetic probes
monoliths
packed beds
physical probes
spatial resolution

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10.1021/acscatal.5b02602

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title = "Evolution and Enabling Capabilities of Spatially Resolved Techniques for the Characterization of Heterogeneously Catalyzed Reactions",

abstract = "The development and optimization of catalysts and catalytic processes requires knowledge of reaction kinetics and mechanisms. In traditional catalyst kinetic characterization, the gas composition is known at the inlet, and the exit flow is measured to determine changes in concentration. As such, the progression of the chemistry within the catalyst is not known. Technological advances in electromagnetic and physical probes have made visualizing the evolution of the chemistry within catalyst samples a reality, as part of a methodology commonly known as spatial resolution. Herein, we discuss and evaluate the development of spatially resolved techniques, including the evolutions and achievements of this growing area of catalytic research. The impact of such techniques is discussed in terms of the invasiveness of physical probes on catalytic systems, as well as how experimentally obtained spatial profiles can be used in conjunction with kinetic modeling. Furthermore, some aims and aspirations for further evolution of spatially resolved techniques are considered.",

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AU - Hardacre, Christopher

AU - Pihl, Josh A.

AU - Stere, Cristina E.

AU - Kim, Mi Young

AU - Stewart, Caomhán

AU - Goguet, Alexandre

AU - Partridge, William P.

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Evolution and Enabling Capabilities of Spatially Resolved Techniques for the Characterization of Heterogeneously Catalyzed Reactions

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Keywords

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