Adsorbate-driven dynamic active sites in stannosilicate zeolites
Elucidating the nature of the active sites in heterogeneous catalysts is fundamental for understanding their reactivity and catalytic performances. Although stannosilicate zeolites have tremendous application potential for catalyzing biomass-related compounds in aqueous media, the detailed local str...
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| Format: | Article |
| Language: | English |
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KeAi Communications Co. Ltd.
2025-01-01
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| Series: | Fundamental Research |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2667325823000018 |
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| author | Xianfeng Yi Yao Xiao Changjiu Xia Fengqing Liu Yujia Liu Yu Hui Xin Yu Yucai Qin Wei Chen Zhiqiang Liu Lijuan Song Anmin Zheng |
| author_facet | Xianfeng Yi Yao Xiao Changjiu Xia Fengqing Liu Yujia Liu Yu Hui Xin Yu Yucai Qin Wei Chen Zhiqiang Liu Lijuan Song Anmin Zheng |
| author_sort | Xianfeng Yi |
| collection | DOAJ |
| description | Elucidating the nature of the active sites in heterogeneous catalysts is fundamental for understanding their reactivity and catalytic performances. Although stannosilicate zeolites have tremendous application potential for catalyzing biomass-related compounds in aqueous media, the detailed local structures and features of the real active sites and their possible structural variations under reaction conditions are poorly understood to date. In this study, a dynamic transformation of framework Sn−O−Si sites to Sn−OH/Si−OH pairs and subsequently a pseudo-Brønsted acid in stannosilicate zeolites upon molecular adsorption, which is analogous to various adsorbates/reactants under working conditions, was identified by solid-state nuclear magnetic resonance (NMR) spectroscopy for the first time, which challenges the widespread assumption that the active center structures remain rigid/stable during the catalytic process. These results provide new comprehensive insights for the fundamental understanding of the dynamic and flexible active centers and involved reaction mechanisms of novel zeolite catalysts with heterometal atoms, such as Sn, Ti, and Zr. |
| format | Article |
| id | doaj-art-5688930f8cbe4d899cd1ab62f1411061 |
| institution | Kabale University |
| issn | 2667-3258 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | KeAi Communications Co. Ltd. |
| record_format | Article |
| series | Fundamental Research |
| spelling | doaj-art-5688930f8cbe4d899cd1ab62f14110612025-01-29T05:02:30ZengKeAi Communications Co. Ltd.Fundamental Research2667-32582025-01-0151174182Adsorbate-driven dynamic active sites in stannosilicate zeolitesXianfeng Yi0Yao Xiao1Changjiu Xia2Fengqing Liu3Yujia Liu4Yu Hui5Xin Yu6Yucai Qin7Wei Chen8Zhiqiang Liu9Lijuan Song10Anmin Zheng11State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, ChinaKey Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaKey Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, ChinaKey Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, ChinaState Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China; Corresponding author.Elucidating the nature of the active sites in heterogeneous catalysts is fundamental for understanding their reactivity and catalytic performances. Although stannosilicate zeolites have tremendous application potential for catalyzing biomass-related compounds in aqueous media, the detailed local structures and features of the real active sites and their possible structural variations under reaction conditions are poorly understood to date. In this study, a dynamic transformation of framework Sn−O−Si sites to Sn−OH/Si−OH pairs and subsequently a pseudo-Brønsted acid in stannosilicate zeolites upon molecular adsorption, which is analogous to various adsorbates/reactants under working conditions, was identified by solid-state nuclear magnetic resonance (NMR) spectroscopy for the first time, which challenges the widespread assumption that the active center structures remain rigid/stable during the catalytic process. These results provide new comprehensive insights for the fundamental understanding of the dynamic and flexible active centers and involved reaction mechanisms of novel zeolite catalysts with heterometal atoms, such as Sn, Ti, and Zr.http://www.sciencedirect.com/science/article/pii/S2667325823000018Dynamic active sitesPseudo-Brønsted acidStannosilicate zeolitesReaction conditionsSolid-state NMR |
| spellingShingle | Xianfeng Yi Yao Xiao Changjiu Xia Fengqing Liu Yujia Liu Yu Hui Xin Yu Yucai Qin Wei Chen Zhiqiang Liu Lijuan Song Anmin Zheng Adsorbate-driven dynamic active sites in stannosilicate zeolites Fundamental Research Dynamic active sites Pseudo-Brønsted acid Stannosilicate zeolites Reaction conditions Solid-state NMR |
| title | Adsorbate-driven dynamic active sites in stannosilicate zeolites |
| title_full | Adsorbate-driven dynamic active sites in stannosilicate zeolites |
| title_fullStr | Adsorbate-driven dynamic active sites in stannosilicate zeolites |
| title_full_unstemmed | Adsorbate-driven dynamic active sites in stannosilicate zeolites |
| title_short | Adsorbate-driven dynamic active sites in stannosilicate zeolites |
| title_sort | adsorbate driven dynamic active sites in stannosilicate zeolites |
| topic | Dynamic active sites Pseudo-Brønsted acid Stannosilicate zeolites Reaction conditions Solid-state NMR |
| url | http://www.sciencedirect.com/science/article/pii/S2667325823000018 |
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