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Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts
The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack...
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Published in: | Applied catalysis. B, Environmental Environmental, 2024-03, Vol.342, p.123368, Article 123368 |
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container_title | Applied catalysis. B, Environmental |
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creator | Tang, Tian Ye, Lyumeng Chen, Yanrong Xue, Jingyu Shen, Xiaoqiang Chen, Jinfei Quarcoo, Fiona Hammond Rac, Vladislav Rakić, Vesna Li, Xinbao Du, Xuesen |
description | The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures.
[Display omitted]
•A new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism was provided for CO oxidation.•The continuous operation of the M−vK mechanism on the surface of CuOx/CeO2 catalysts exhibited oxidant-dependent properties.•The spatial effect of double oxygen vacancies (Ov) promotes the sustained and dynamic activation of O2. |
doi_str_mv | 10.1016/j.apcatb.2023.123368 |
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[Display omitted]
•A new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism was provided for CO oxidation.•The continuous operation of the M−vK mechanism on the surface of CuOx/CeO2 catalysts exhibited oxidant-dependent properties.•The spatial effect of double oxygen vacancies (Ov) promotes the sustained and dynamic activation of O2.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2023.123368</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>CO oxidation ; Copper−ceria interface ; DFT+U ; Mars-van Krevelen (M−vK)</subject><ispartof>Applied catalysis. B, Environmental, 2024-03, Vol.342, p.123368, Article 123368</ispartof><rights>2023 Elsevier B.V.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c306t-4db6785c31c9878b625534c7b6fba710f50debc949ca92aa50f9d472ec4283e73</citedby><cites>FETCH-LOGICAL-c306t-4db6785c31c9878b625534c7b6fba710f50debc949ca92aa50f9d472ec4283e73</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Tang, Tian</creatorcontrib><creatorcontrib>Ye, Lyumeng</creatorcontrib><creatorcontrib>Chen, Yanrong</creatorcontrib><creatorcontrib>Xue, Jingyu</creatorcontrib><creatorcontrib>Shen, Xiaoqiang</creatorcontrib><creatorcontrib>Chen, Jinfei</creatorcontrib><creatorcontrib>Quarcoo, Fiona Hammond</creatorcontrib><creatorcontrib>Rac, Vladislav</creatorcontrib><creatorcontrib>Rakić, Vesna</creatorcontrib><creatorcontrib>Li, Xinbao</creatorcontrib><creatorcontrib>Du, Xuesen</creatorcontrib><title>Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts</title><title>Applied catalysis. B, Environmental</title><description>The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures.
[Display omitted]
•A new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism was provided for CO oxidation.•The continuous operation of the M−vK mechanism on the surface of CuOx/CeO2 catalysts exhibited oxidant-dependent properties.•The spatial effect of double oxygen vacancies (Ov) promotes the sustained and dynamic activation of O2.</description><subject>CO oxidation</subject><subject>Copper−ceria interface</subject><subject>DFT+U</subject><subject>Mars-van Krevelen (M−vK)</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNp9kLtOwzAUhi0EEqXwBgweYXDwJRdnQULhqrbqArPlOCfUVZtEtonoGzDziDwJicLMdP7hfL9-fQhdMhoxytKbbaQ7o0MZccpFxLgQqTxCMyYzQYSU4hjNaM5TIkQmTtGZ91tKh08uZ2h_b3vbvGPbhBaHDYwBXK0NkD1UVgeo8Eo7T3rd4IWDHnbQ4KvVz9d3v7jGZqOdNgNhfbAGtzUuPtafxH90XetGtoA1x8M2vTv44M_RSa13Hi7-7hy9PT68Fs9kuX56Ke6WxAiaBhJXZZrJxAhmcpnJMuVJImKTlWld6ozROqEVlCaPc6NzrnVC67yKMw4m5lJAJuYonnqNa713UKvO2b12B8WoGpWprZqUqVGZmpQN2O2EwbCtt-CUNxYaM4hwYIKqWvt_wS8JuHhV</recordid><startdate>202403</startdate><enddate>202403</enddate><creator>Tang, Tian</creator><creator>Ye, Lyumeng</creator><creator>Chen, Yanrong</creator><creator>Xue, Jingyu</creator><creator>Shen, Xiaoqiang</creator><creator>Chen, Jinfei</creator><creator>Quarcoo, Fiona Hammond</creator><creator>Rac, Vladislav</creator><creator>Rakić, Vesna</creator><creator>Li, Xinbao</creator><creator>Du, Xuesen</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>202403</creationdate><title>Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts</title><author>Tang, Tian ; Ye, Lyumeng ; Chen, Yanrong ; Xue, Jingyu ; Shen, Xiaoqiang ; Chen, Jinfei ; Quarcoo, Fiona Hammond ; Rac, Vladislav ; Rakić, Vesna ; Li, Xinbao ; Du, Xuesen</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c306t-4db6785c31c9878b625534c7b6fba710f50debc949ca92aa50f9d472ec4283e73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>CO oxidation</topic><topic>Copper−ceria interface</topic><topic>DFT+U</topic><topic>Mars-van Krevelen (M−vK)</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Tang, Tian</creatorcontrib><creatorcontrib>Ye, Lyumeng</creatorcontrib><creatorcontrib>Chen, Yanrong</creatorcontrib><creatorcontrib>Xue, Jingyu</creatorcontrib><creatorcontrib>Shen, Xiaoqiang</creatorcontrib><creatorcontrib>Chen, Jinfei</creatorcontrib><creatorcontrib>Quarcoo, Fiona Hammond</creatorcontrib><creatorcontrib>Rac, Vladislav</creatorcontrib><creatorcontrib>Rakić, Vesna</creatorcontrib><creatorcontrib>Li, Xinbao</creatorcontrib><creatorcontrib>Du, Xuesen</creatorcontrib><collection>CrossRef</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Tang, Tian</au><au>Ye, Lyumeng</au><au>Chen, Yanrong</au><au>Xue, Jingyu</au><au>Shen, Xiaoqiang</au><au>Chen, Jinfei</au><au>Quarcoo, Fiona Hammond</au><au>Rac, Vladislav</au><au>Rakić, Vesna</au><au>Li, Xinbao</au><au>Du, Xuesen</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2024-03</date><risdate>2024</risdate><volume>342</volume><spage>123368</spage><pages>123368-</pages><artnum>123368</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures.
[Display omitted]
•A new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism was provided for CO oxidation.•The continuous operation of the M−vK mechanism on the surface of CuOx/CeO2 catalysts exhibited oxidant-dependent properties.•The spatial effect of double oxygen vacancies (Ov) promotes the sustained and dynamic activation of O2.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2023.123368</doi></addata></record> |
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subjects | CO oxidation Copper−ceria interface DFT+U Mars-van Krevelen (M−vK) |
title | Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts |
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