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Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation

Highly dispersed metal sites on the surface of silica, achieved from immobilization of metal precursor within hydroxyl groups, has gained increasing attention in the field of heterogeneous catalyst. However, the special role of adsorbed water derived by hydroxyl groups on the silica is generally ign...

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Autores principales: Huang, Zijun, He, Dedong, Deng, Weihua, Jin, Guowu, Li, Ke, Luo, Yongming
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9823098/
https://www.ncbi.nlm.nih.gov/pubmed/36609564
http://dx.doi.org/10.1038/s41467-022-35698-0
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author Huang, Zijun
He, Dedong
Deng, Weihua
Jin, Guowu
Li, Ke
Luo, Yongming
author_facet Huang, Zijun
He, Dedong
Deng, Weihua
Jin, Guowu
Li, Ke
Luo, Yongming
author_sort Huang, Zijun
collection PubMed
description Highly dispersed metal sites on the surface of silica, achieved from immobilization of metal precursor within hydroxyl groups, has gained increasing attention in the field of heterogeneous catalyst. However, the special role of adsorbed water derived by hydroxyl groups on the silica is generally ignored. Herein, a new understanding of adsorbed water on the formation of highly dispersed tetrahedral Co(II) (T(d)-cobalt(II)) sites is illustrated. It is indicated that sufficient adsorbed water induces the transformation of precursor of Co(NO(3))(2) into intermediate of [Co(H(2)O)(6)](2+). Subsequently, [Co(H(2)O)(6)](2+) makes the highly dispersed T(d)-cobalt(II) sites to be available during direct H(2)-reduction process. A systematic characterization and DFT calculation prove the existence of the adsorbed water and the importance of the intermediate of [Co(H(2)O)(6)](2+), respectively. The as-synthesized catalyst is attempted to the propane dehydrogenation, which shows better reactivity when compared with other reported Co based catalysts.
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spelling pubmed-98230982023-01-08 Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation Huang, Zijun He, Dedong Deng, Weihua Jin, Guowu Li, Ke Luo, Yongming Nat Commun Article Highly dispersed metal sites on the surface of silica, achieved from immobilization of metal precursor within hydroxyl groups, has gained increasing attention in the field of heterogeneous catalyst. However, the special role of adsorbed water derived by hydroxyl groups on the silica is generally ignored. Herein, a new understanding of adsorbed water on the formation of highly dispersed tetrahedral Co(II) (T(d)-cobalt(II)) sites is illustrated. It is indicated that sufficient adsorbed water induces the transformation of precursor of Co(NO(3))(2) into intermediate of [Co(H(2)O)(6)](2+). Subsequently, [Co(H(2)O)(6)](2+) makes the highly dispersed T(d)-cobalt(II) sites to be available during direct H(2)-reduction process. A systematic characterization and DFT calculation prove the existence of the adsorbed water and the importance of the intermediate of [Co(H(2)O)(6)](2+), respectively. The as-synthesized catalyst is attempted to the propane dehydrogenation, which shows better reactivity when compared with other reported Co based catalysts. Nature Publishing Group UK 2023-01-06 /pmc/articles/PMC9823098/ /pubmed/36609564 http://dx.doi.org/10.1038/s41467-022-35698-0 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Huang, Zijun
He, Dedong
Deng, Weihua
Jin, Guowu
Li, Ke
Luo, Yongming
Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title_full Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title_fullStr Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title_full_unstemmed Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title_short Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation
title_sort illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(ii) for propane dehydrogenation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9823098/
https://www.ncbi.nlm.nih.gov/pubmed/36609564
http://dx.doi.org/10.1038/s41467-022-35698-0
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