CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst
The production of light olefins from the hydrogenation of CO2 is an efficient way to utilize CO2, where the surface oxygen vacancy in metal oxide plays an important role in CO2 adsorption and activation. Here, the Ga-Zr metal oxides were prepared by hydrolysis of urea at different temperatures and c...
| Autores: | , , , , , , , , |
|---|---|
| Tipo de documento: | artigo |
| Estado: | Versión aceptada para publicación |
| Data de publicação: | 2024 |
| País: | España |
| Recursos: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositório: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/389705 |
| Acesso em linha: | http://hdl.handle.net/10261/389705 https://api.elsevier.com/content/abstract/scopus_id/85204430464 |
| Access Level: | Acesso embargado |
| Palavra-chave: | CO hydrogenation 2 Urea hydrolysis temperature Oxygen vacancy Light olefins Ga-Zr metal oxide http://metadata.un.org/sdg/13 Take urgent action to combat climate change and its impacts CO2 hydrogenation light olefins oxygen vacancy urea hydrolysis temperature |
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CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalystWang, QianXing, MingqinWang, LipingGong, ZhiyuanNawaz, Muhammad AsifBlay-Roger, RubénRamírez-Reina, TomásLi, ZhongMeng, FanhuiCO hydrogenation 2Urea hydrolysis temperatureOxygen vacancyLight olefinsGa-Zr metal oxidehttp://metadata.un.org/sdg/13Take urgent action to combat climate change and its impactsCO2 hydrogenationGa-Zr metal oxidelight olefinsoxygen vacancyurea hydrolysis temperatureThe production of light olefins from the hydrogenation of CO2 is an efficient way to utilize CO2, where the surface oxygen vacancy in metal oxide plays an important role in CO2 adsorption and activation. Here, the Ga-Zr metal oxides were prepared by hydrolysis of urea at different temperatures and combined with SAPO-34 to prepare the bifunctional catalyst for CO2 hydrogenation to light olefins. The surface oxygen vacancy content of Ga-Zr oxide increases with increasing urea hydrolysis temperature, and a high CO2 conversion of 26.4% and C2=–C4= hydrocarbon selectivity of 87.2% were obtained by a well-matched amount of desorbed CO2 and H2. Using the CO2 and H2/HCOOH/CH3OH as probe molecules, the in-situ DRIFT spectra reveal that the CO2 could be activated on surface oxygen vacancy and converted to CO3* and HCO3* species, which were further hydrogenated to HCOO* and CH3O* species. While the by-product CO mainly originates from the decomposition of HCOO* and the presence of SAPO-34 converts CH3O* to C2=–C4=. The current study illustrates that boosting the surface oxygen vacancy in defected surfaces of metal oxide and providing a matching H2 dissociation ability is the key to improve the performance of CO2 hydrogenation to light olefins.This work was supported by National Natural Science Foundation of China (22479106) and Natural Science Foundation of Shanxi Province (202103021224073).Peer reviewedElsevierNational Natural Science Foundation of ChinaNatural Science Foundation of Shaanxi ProvinceWang, Qian [0009-0002-2534-059X]Xing, Mingqin [0009-0008-7247-8093]Wang, Liping [0009-0003-8454-6384]Nawaz, Muhammad Asif [0000-0003-3234-031X]Blay-Roger, Rubén [0000-0002-3085-8134]Ramirez-Reina, Tomás [0000-0001-9693-5107]Li, Zhong [0000-0001-6087-6854]Meng, Fanhui [0000-0003-0998-5179]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/10261/389705https://api.elsevier.com/content/abstract/scopus_id/85204430464reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttps://doi.org/10.1016/j.mcat.2024.114567Síinfo:eu-repo/semantics/embargoedAccessoai:digital.csic.es:10261/3897052026-05-22T06:33:51Z |
| dc.title.none.fl_str_mv |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| title |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| spellingShingle |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst Wang, Qian CO hydrogenation 2 Urea hydrolysis temperature Oxygen vacancy Light olefins Ga-Zr metal oxide http://metadata.un.org/sdg/13 Take urgent action to combat climate change and its impacts CO2 hydrogenation Ga-Zr metal oxide light olefins oxygen vacancy urea hydrolysis temperature |
| title_short |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| title_full |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| title_fullStr |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| title_full_unstemmed |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| title_sort |
CO<inf>2</inf> hydrogenation to light olefins over highly active and selective Ga-Zr/SAPO-34 bifunctional catalyst |
| dc.creator.none.fl_str_mv |
Wang, Qian Xing, Mingqin Wang, Liping Gong, Zhiyuan Nawaz, Muhammad Asif Blay-Roger, Rubén Ramírez-Reina, Tomás Li, Zhong Meng, Fanhui |
| author |
Wang, Qian |
| author_facet |
Wang, Qian Xing, Mingqin Wang, Liping Gong, Zhiyuan Nawaz, Muhammad Asif Blay-Roger, Rubén Ramírez-Reina, Tomás Li, Zhong Meng, Fanhui |
| author_role |
author |
| author2 |
Xing, Mingqin Wang, Liping Gong, Zhiyuan Nawaz, Muhammad Asif Blay-Roger, Rubén Ramírez-Reina, Tomás Li, Zhong Meng, Fanhui |
| author2_role |
author author author author author author author author |
| dc.contributor.none.fl_str_mv |
National Natural Science Foundation of China Natural Science Foundation of Shaanxi Province Wang, Qian [0009-0002-2534-059X] Xing, Mingqin [0009-0008-7247-8093] Wang, Liping [0009-0003-8454-6384] Nawaz, Muhammad Asif [0000-0003-3234-031X] Blay-Roger, Rubén [0000-0002-3085-8134] Ramirez-Reina, Tomás [0000-0001-9693-5107] Li, Zhong [0000-0001-6087-6854] Meng, Fanhui [0000-0003-0998-5179] Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72] |
| dc.subject.none.fl_str_mv |
CO hydrogenation 2 Urea hydrolysis temperature Oxygen vacancy Light olefins Ga-Zr metal oxide http://metadata.un.org/sdg/13 Take urgent action to combat climate change and its impacts CO2 hydrogenation Ga-Zr metal oxide light olefins oxygen vacancy urea hydrolysis temperature |
| topic |
CO hydrogenation 2 Urea hydrolysis temperature Oxygen vacancy Light olefins Ga-Zr metal oxide http://metadata.un.org/sdg/13 Take urgent action to combat climate change and its impacts CO2 hydrogenation Ga-Zr metal oxide light olefins oxygen vacancy urea hydrolysis temperature |
| description |
The production of light olefins from the hydrogenation of CO2 is an efficient way to utilize CO2, where the surface oxygen vacancy in metal oxide plays an important role in CO2 adsorption and activation. Here, the Ga-Zr metal oxides were prepared by hydrolysis of urea at different temperatures and combined with SAPO-34 to prepare the bifunctional catalyst for CO2 hydrogenation to light olefins. The surface oxygen vacancy content of Ga-Zr oxide increases with increasing urea hydrolysis temperature, and a high CO2 conversion of 26.4% and C2=–C4= hydrocarbon selectivity of 87.2% were obtained by a well-matched amount of desorbed CO2 and H2. Using the CO2 and H2/HCOOH/CH3OH as probe molecules, the in-situ DRIFT spectra reveal that the CO2 could be activated on surface oxygen vacancy and converted to CO3* and HCO3* species, which were further hydrogenated to HCOO* and CH3O* species. While the by-product CO mainly originates from the decomposition of HCOO* and the presence of SAPO-34 converts CH3O* to C2=–C4=. The current study illustrates that boosting the surface oxygen vacancy in defected surfaces of metal oxide and providing a matching H2 dissociation ability is the key to improve the performance of CO2 hydrogenation to light olefins. |
| 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/10261/389705 https://api.elsevier.com/content/abstract/scopus_id/85204430464 |
| url |
http://hdl.handle.net/10261/389705 https://api.elsevier.com/content/abstract/scopus_id/85204430464 |
| dc.language.none.fl_str_mv |
Inglés |
| language_invalid_str_mv |
Inglés |
| dc.relation.none.fl_str_mv |
https://doi.org/10.1016/j.mcat.2024.114567 Sí |
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info:eu-repo/semantics/embargoedAccess |
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embargoedAccess |
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aplication/pdf |
| dc.publisher.none.fl_str_mv |
Elsevier |
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Elsevier |
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reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC instname:Consejo Superior de Investigaciones Científicas (CSIC) |
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Consejo Superior de Investigaciones Científicas (CSIC) |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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1869407680310804480 |
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15,81155 |