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Multi-Length Scale 5D Diffraction Imaging of Ni–Pd/CeO2–ZrO2/Al2O3 Catalyst During Partial Oxidation of Methane Full article

Journal Journal of Materials Chemistry A, Materials for Energy and Sustainability
ISSN: 2050-7488 , E-ISSN: 2050-7496
Output data Year: 2021, Volume: 9, Number: 18, Pages: 11331-11346 Pages count : 16 DOI: 10.1039/d1ta01464a
Tags Ni-BASED CATALYSTS; FISCHER-TROPSCH SYNTHESIS; SYNTHESIS GAS; COKE FORMATION; COMPUTED-TOMOGRAPHY; HYDROGEN-PRODUCTION; SYNGAS PRODUCTION; PHYSICOCHEMICAL PROPERTIES; Ni/CeO2-Al2O3 CATALYSTS; SUPPORT COMPOSITION
Authors Matras Dorota 1,2,8,9 , Vamvakeros Antonis 3,4,5 , Jacques Simon D.M. 3 , di Michiel Marco 4 , Middelkoop Vesna 6 , Ismagilov Ilyas Z. 7 , Matus Ekaterina V. 7 , Kuznetsov Vadim V. 7 , Cernik Robert J. 1 , Beale Andrew M. 2,3,5
Affiliations
1 School of Materials, University of Manchester, Manchester, Lancashire M13 9PL, UK
2 Research Complex at Harwell, Harwell Science and Innovation Campus, Rutherford Appleton Laboratory, Didcot, Oxon, UK
3 Finden Limited, Merchant House, 5 East St Helen Street, Abingdon, UK
4 ESRF- The European Synchrotron, Grenoble, France
5 Department of Chemistry, University College London, 20 Gordon Street, London, UK
6 Flemish Institute for Technological Research, VITO NV, Boeretang 200, 2400 Mol, Belgium
7 Boreskov Institute of Catalysis SB RAS, Pr. Akademika Lavrentieva 5, 630090 Novosibirsk, Russia
8 The Faraday Institution, Quad One, Harwell Science and Innovation Campus
9 Diamond Light Source, Harwell Science and Innovation Campus, Didcot

Funding (3)

1 European Commission 679933 H2020-SPIRE-2015 MEMERE
2 Engineering and Physical Sciences Research Council EP/R026815/1
3 Engineering and Physical Sciences Research Council EP/S016481/1

Abstract: A 5D diffraction imaging experiment (with 3D spatial, 1D time/imposed operating conditions and 1D scattering signal) was performed with a Ni–Pd/CeO2–ZrO2/Al2O3 catalyst. The catalyst was investigated during both activation and partial oxidation of methane (POX). The spatio-temporal resolved diffraction data allowed us to obtain unprecedented insight into the behaviour and fate of the various metal and metal oxide species and how this is affected by the heterogeneity across catalyst particles. We show firstly, how Pd promotion although facilitating Ni reduction, over time leads to formation of unstable Ni–Pd metallic alloy, rendering the impact of Pd beyond the initial reduction less important. Furthermore, in the core of the particles, where the metallic Ni is primarily supported on Al2O3, poor resistance towards coke deposition was observed. We identified that this preceded via the formation of an active yet metastable interstitial solid solution of Ni–C and led to the exclusive formation of graphitic carbon, the only polymorph of coke observed. In contrast, at the outermost part of the catalyst particle, where Ni is predominantly supported on CeO2–ZrO2, the graphite formation was mitigated but sintering of Ni crystallites was more severe.
Cite: Matras D. , Vamvakeros A. , Jacques S.D.M. , di Michiel M. , Middelkoop V. , Ismagilov I.Z. , Matus E.V. , Kuznetsov V.V. , Cernik R.J. , Beale A.M.
Multi-Length Scale 5D Diffraction Imaging of Ni–Pd/CeO2–ZrO2/Al2O3 Catalyst During Partial Oxidation of Methane
Journal of Materials Chemistry A, Materials for Energy and Sustainability. 2021. V.9. N18. P.11331-11346. DOI: 10.1039/d1ta01464a WOS Scopus РИНЦ AN OpenAlex
Files: Full text from publisher
Dates:
Submitted: Feb 18, 2021
Accepted: Apr 21, 2021
Published online: Apr 22, 2021
Published print: May 14, 2021
Identifiers:
Web of science: WOS:000644940300001
Scopus: 2-s2.0-85105757734
Elibrary: 46091924
Chemical Abstracts: 2021:930746
OpenAlex: W3157500250
Citing:
DB Citing
Web of science 13
Scopus 14
Elibrary 14
OpenAlex 16
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