Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction

Although Cu/ZnO-based catalysts have been long used for the hydrogenation of CO2 to methanol, open questions still remain regarding the role and the dynamic nature of the active sites formed at the metal-oxide interface. Here, we apply high-pressure operando spectroscopy methods to well-defined Cu a...

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Authors: Jiménez Divins, Nuria|||0000-0001-6010-5419, Kordus, David, Timoshenko, Janis, Sinev, Ilya, Zegkinoglou, Ioannis, Bergmann, Arno, Chee, See Wee, Widrinna, Simon, Karslioglu, Osman, Mistry, Hemma, Lopez Luna, Mauricio, Zhong, Jian Qiang, Hoffman, Adam S., Anibal Boscoboinik, Jorge, Heggen, Marc, Dunin-Borkowski, Rafal E., Roldan Cuenya, Beatriz
Format: article
Publication Date:2021
Country:España
Institution:Universitat Politècnica de Catalunya (UPC)
Repository:UPCommons. Portal del coneixement obert de la UPC
Language:English
OAI Identifier:oai:upcommons.upc.edu:2117/393924
Online Access:https://hdl.handle.net/2117/393924
https://dx.doi.org/10.1038/s41467-021-21604-7
Access Level:Open access
Keyword:Catalysts
Global warming
Catalitzadors
Escalfament global
Àrees temàtiques de la UPC::Enginyeria química
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spelling Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reactionJiménez Divins, Nuria|||0000-0001-6010-5419Kordus, DavidTimoshenko, JanisSinev, IlyaZegkinoglou, IoannisBergmann, ArnoChee, See WeeWidrinna, SimonKarslioglu, OsmanMistry, HemmaLopez Luna, MauricioZhong, Jian QiangHoffman, Adam S.Anibal Boscoboinik, JorgeHeggen, MarcDunin-Borkowski, Rafal E.Roldan Cuenya, BeatrizCatalystsGlobal warmingCatalitzadorsEscalfament globalÀrees temàtiques de la UPC::Enginyeria químicaAlthough Cu/ZnO-based catalysts have been long used for the hydrogenation of CO2 to methanol, open questions still remain regarding the role and the dynamic nature of the active sites formed at the metal-oxide interface. Here, we apply high-pressure operando spectroscopy methods to well-defined Cu and Cu0.7Zn0.3 nanoparticles supported on ZnO/Al2O3, ¿-Al2O3 and SiO2 to correlate their structure, composition and catalytic performance. We obtain similar activity and methanol selectivity for Cu/ZnO/Al2O3 and CuZn/SiO2, but the methanol yield decreases with time on stream for the latter sample. Operando X-ray absorption spectroscopy data reveal the formation of reduced Zn species coexisting with ZnO on CuZn/SiO2. Near-ambient pressure X-ray photoelectron spectroscopy shows Zn surface segregation and the formation of a ZnO-rich shell on CuZn/SiO2. In this work we demonstrate the beneficial effect of Zn, even in diluted form, and highlight the influence of the oxide support and the Cu-Zn interface in the reactivity.This work was funded by the European Research Council under grant ERC-OPERANDOCAT (ERC-725915) and the Forschungsgemeinschaft (DFG) under Germany’s Excellence Strategy—EXC 2008 – 390540038—UniSysCat and EXC 1069 - RESOLV. The majority of the XAS work was performed at Stanford Synchrotron Radiation Lightsource (beamline 2–2) of SLAC National Accelerator Laboratory, supported by the Office of Basic Energy Sciences of the US Department of Energy (DOE) under Contract No. DE-AC02-76SF00515 and by Co-ACCESS (Chemical Sciences, Geosciences, and Biosciences Division). Additional studies were carried out at the National Synchrotron Light Source II (NSLS-II, IOS and QAS beamlines) of Brookhaven National Laboratory supported by DOE under Contract No. DE-SC0012704. We also acknowledge MAX IV Laboratory (Sweden) for access to the Beamline HIPPIE and Andrey Shavorskiy for his assistance during the NAP-XPS measurements. Max IV is funded by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. We further thank Olaf Timpe, Stephanie Kühl, and Frank Girgsdies (FHI) for the ICP and some of the XRD measurements and Alba Titze Alonso (RUB) for her assistance with sample preparation.Peer Reviewed20212021-03-0420232023-09-22journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/393924https://dx.doi.org/10.1038/s41467-021-21604-7reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3939242026-05-27T15:37:01Z
dc.title.none.fl_str_mv Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
title Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
spellingShingle Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
Jiménez Divins, Nuria|||0000-0001-6010-5419
Catalysts
Global warming
Catalitzadors
Escalfament global
Àrees temàtiques de la UPC::Enginyeria química
title_short Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
title_full Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
title_fullStr Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
title_full_unstemmed Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
title_sort Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
dc.creator.none.fl_str_mv Jiménez Divins, Nuria|||0000-0001-6010-5419
Kordus, David
Timoshenko, Janis
Sinev, Ilya
Zegkinoglou, Ioannis
Bergmann, Arno
Chee, See Wee
Widrinna, Simon
Karslioglu, Osman
Mistry, Hemma
Lopez Luna, Mauricio
Zhong, Jian Qiang
Hoffman, Adam S.
Anibal Boscoboinik, Jorge
Heggen, Marc
Dunin-Borkowski, Rafal E.
Roldan Cuenya, Beatriz
author Jiménez Divins, Nuria|||0000-0001-6010-5419
author_facet Jiménez Divins, Nuria|||0000-0001-6010-5419
Kordus, David
Timoshenko, Janis
Sinev, Ilya
Zegkinoglou, Ioannis
Bergmann, Arno
Chee, See Wee
Widrinna, Simon
Karslioglu, Osman
Mistry, Hemma
Lopez Luna, Mauricio
Zhong, Jian Qiang
Hoffman, Adam S.
Anibal Boscoboinik, Jorge
Heggen, Marc
Dunin-Borkowski, Rafal E.
Roldan Cuenya, Beatriz
author_role author
author2 Kordus, David
Timoshenko, Janis
Sinev, Ilya
Zegkinoglou, Ioannis
Bergmann, Arno
Chee, See Wee
Widrinna, Simon
Karslioglu, Osman
Mistry, Hemma
Lopez Luna, Mauricio
Zhong, Jian Qiang
Hoffman, Adam S.
Anibal Boscoboinik, Jorge
Heggen, Marc
Dunin-Borkowski, Rafal E.
Roldan Cuenya, Beatriz
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Catalysts
Global warming
Catalitzadors
Escalfament global
Àrees temàtiques de la UPC::Enginyeria química
topic Catalysts
Global warming
Catalitzadors
Escalfament global
Àrees temàtiques de la UPC::Enginyeria química
description Although Cu/ZnO-based catalysts have been long used for the hydrogenation of CO2 to methanol, open questions still remain regarding the role and the dynamic nature of the active sites formed at the metal-oxide interface. Here, we apply high-pressure operando spectroscopy methods to well-defined Cu and Cu0.7Zn0.3 nanoparticles supported on ZnO/Al2O3, ¿-Al2O3 and SiO2 to correlate their structure, composition and catalytic performance. We obtain similar activity and methanol selectivity for Cu/ZnO/Al2O3 and CuZn/SiO2, but the methanol yield decreases with time on stream for the latter sample. Operando X-ray absorption spectroscopy data reveal the formation of reduced Zn species coexisting with ZnO on CuZn/SiO2. Near-ambient pressure X-ray photoelectron spectroscopy shows Zn surface segregation and the formation of a ZnO-rich shell on CuZn/SiO2. In this work we demonstrate the beneficial effect of Zn, even in diluted form, and highlight the influence of the oxide support and the Cu-Zn interface in the reactivity.
publishDate 2021
dc.date.none.fl_str_mv 2021
2021-03-04
2023
2023-09-22
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/393924
https://dx.doi.org/10.1038/s41467-021-21604-7
url https://hdl.handle.net/2117/393924
https://dx.doi.org/10.1038/s41467-021-21604-7
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
collection UPCommons. Portal del coneixement obert de la UPC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300719

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