Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins

Supplementary data associated with this article can be found in the online version at doi:10.1016/j.cattod.2024.114661.

Detalles Bibliográficos
Autores: Meng, Fanhui, Gong, Zhiyuan, Wang, Qian, Xing, Mingqin, Nawaz, Muhammad Asif, Qiao, Zhipeng, Jing, Jieying, Li, Wenying, Li, Zhong
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/389707
Acceso en línea:http://hdl.handle.net/10261/389707
https://api.elsevier.com/content/abstract/scopus_id/85189025752
Access Level:acceso embargado
Palabra clave:CO2 conversion
GaZr oxide
Light olefin
Oxygen vacancy
ZrO2 crystal phase
http://metadata.un.org/sdg/13
Take urgent action to combat climate change and its impacts
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spelling Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefinsMeng, FanhuiGong, ZhiyuanWang, QianXing, MingqinNawaz, Muhammad AsifQiao, ZhipengJing, JieyingLi, WenyingLi, ZhongCO2 conversionGaZr oxideLight olefinOxygen vacancyZrO2 crystal phasehttp://metadata.un.org/sdg/13Take urgent action to combat climate change and its impactsSupplementary data associated with this article can be found in the online version at doi:10.1016/j.cattod.2024.114661.A bifunctional catalyst, comprising GaZr oxide and SAPO-34 zeolite, manifests enhanced catalytic activity in CO2 hydrogenation to light olefins; nonetheless, the comprehensive analysis of the pivotal role played by the underlying structure of ZrO2 in Ga-Zr oxide has not been investigated. Herein, different crystalline structures of ZrO2 were prepared by the co-precipitation method and adopted as a support to deposit Ga to obtain ZrO2 with different ratios of monoclinic ZrO2 (m-ZrO2) to tetragonal ZrO2 (t-ZrO2) in GaZr oxides for CO2 hydrogenation to light olefins. Various characterizations demonstrated that the interface between Ga and the mixed phase of (m-t) ZrO2 produces more oxygen vacancies which favors the adsorption and activation of CO2, and the larger specific surface area and stronger H2 adsorption and dissociation capacity promote CO2 conversion. Interestingly, the GaZr oxide with high m-ZrO2 content exhibits superior catalytic activity than the GaZr oxide with high content of t-ZrO2. The highest light olefins yield (9.0%) and selectivity (77.9%) (CO free) with 27.9% CO2 conversion was achieved. In-situ DRIFT spectra further elaborated that the GaZr oxides with different ZrO2 crystalline phases follow the same reaction pathway to hydrogenate CO2 first to HCOO* and then to CH3O* on GaZr oxide surface. While compared with sole ZrO2, the introduction of Ga significantly promotes the hydrogenation of HCOO* to CH3O*, acting as a crucial reaction intermediate that subsequently diffuses into SAPO-34 pores to enhance the desired light olefins selectivity.This work was supported by the National Key R&D Program of China (2022YFE0208400) and the Natural Science Foundation of Shanxi Province (202103021224073).Peer reviewedElsevier BVNational Key Research and Development Program (China)Natural Science Foundation of Shanxi ProvinceMeng, Fanhui [0000-0003-0998-5179]Gong, Zhiyuan [0000-0003-4916-5730]#NODATA#Xing, Mingqin [0009-0008-7247-8093]Nawaz, Muhammad Asif [0000-0003-3234-031X]Qiao, Zhipeng [0009-0002-4466-6317]Jing, Jieying [0000-0002-5004-8411]Li, Wenying [0000-0001-9765-6089]Li, Zhong [0000-0001-6087-6854]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionaplication/pdfhttp://hdl.handle.net/10261/389707https://api.elsevier.com/content/abstract/scopus_id/85189025752reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttps://doi.org/10.1016/j.cattod.2024.114661Síinfo:eu-repo/semantics/embargoedAccessoai:digital.csic.es:10261/3897072026-05-22T06:33:51Z
dc.title.none.fl_str_mv Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
title Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
spellingShingle Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
Meng, Fanhui
CO2 conversion
GaZr oxide
Light olefin
Oxygen vacancy
ZrO2 crystal phase
http://metadata.un.org/sdg/13
Take urgent action to combat climate change and its impacts
title_short Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
title_full Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
title_fullStr Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
title_full_unstemmed Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
title_sort Effects of ZrO<inf>2</inf> crystalline phase on oxygen vacancy of GaZr oxides and their properties for CO<inf>2</inf> hydrogenation to light olefins
dc.creator.none.fl_str_mv Meng, Fanhui
Gong, Zhiyuan
Wang, Qian
Xing, Mingqin
Nawaz, Muhammad Asif
Qiao, Zhipeng
Jing, Jieying
Li, Wenying
Li, Zhong
author Meng, Fanhui
author_facet Meng, Fanhui
Gong, Zhiyuan
Wang, Qian
Xing, Mingqin
Nawaz, Muhammad Asif
Qiao, Zhipeng
Jing, Jieying
Li, Wenying
Li, Zhong
author_role author
author2 Gong, Zhiyuan
Wang, Qian
Xing, Mingqin
Nawaz, Muhammad Asif
Qiao, Zhipeng
Jing, Jieying
Li, Wenying
Li, Zhong
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv National Key Research and Development Program (China)
Natural Science Foundation of Shanxi Province
Meng, Fanhui [0000-0003-0998-5179]
Gong, Zhiyuan [0000-0003-4916-5730]
#NODATA#
Xing, Mingqin [0009-0008-7247-8093]
Nawaz, Muhammad Asif [0000-0003-3234-031X]
Qiao, Zhipeng [0009-0002-4466-6317]
Jing, Jieying [0000-0002-5004-8411]
Li, Wenying [0000-0001-9765-6089]
Li, Zhong [0000-0001-6087-6854]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv CO2 conversion
GaZr oxide
Light olefin
Oxygen vacancy
ZrO2 crystal phase
http://metadata.un.org/sdg/13
Take urgent action to combat climate change and its impacts
topic CO2 conversion
GaZr oxide
Light olefin
Oxygen vacancy
ZrO2 crystal phase
http://metadata.un.org/sdg/13
Take urgent action to combat climate change and its impacts
description Supplementary data associated with this article can be found in the online version at doi:10.1016/j.cattod.2024.114661.
publishDate 2024
dc.date.none.fl_str_mv 2024
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/389707
https://api.elsevier.com/content/abstract/scopus_id/85189025752
url http://hdl.handle.net/10261/389707
https://api.elsevier.com/content/abstract/scopus_id/85189025752
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv https://doi.org/10.1016/j.cattod.2024.114661
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/embargoedAccess
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv aplication/pdf
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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