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Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane

[Image: see text] Boron-based catalysts for oxidative dehydrogenation of propane (ODHP) have displayed excellent olefin selectivity. However, the drawback of deboronation leading to catalyst deactivation limited their scalable applications. Hereby, a series of mesoporous B-MCM-41 (BM-x, B/Si = 0.015...

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Autores principales: Liu, Qingying, Wang, Jiang, Liu, Zhenxing, Zhao, Ruisheng, Xu, Aiju, Jia, Meilin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8793070/
https://www.ncbi.nlm.nih.gov/pubmed/35097303
http://dx.doi.org/10.1021/acsomega.1c06504
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author Liu, Qingying
Wang, Jiang
Liu, Zhenxing
Zhao, Ruisheng
Xu, Aiju
Jia, Meilin
author_facet Liu, Qingying
Wang, Jiang
Liu, Zhenxing
Zhao, Ruisheng
Xu, Aiju
Jia, Meilin
author_sort Liu, Qingying
collection PubMed
description [Image: see text] Boron-based catalysts for oxidative dehydrogenation of propane (ODHP) have displayed excellent olefin selectivity. However, the drawback of deboronation leading to catalyst deactivation limited their scalable applications. Hereby, a series of mesoporous B-MCM-41 (BM-x, B/Si = 0.015–0.147) catalysts for ODHP were prepared by a simple hydrothermal synthesis method. It was found that propane conversion was increased and the initial reaction temperature was reduced with an increase of boron content, and the optimal values appeared on BM-2.0 (B/Si = 0.062), while olefins’ (ethylene and propylene) selectivity was maintained at ca. 70–80%. Most importantly, BM-1.0 (B/Si = 0.048) exhibited favorable activity, stability, and water tolerance after washing treatment or long-time operation (e.g., propane conversion of ca. 15% and overall olefin selectivity of ca. 80% at 550 °C) because its high structural stability prevented boron leaches. These features were identified by X-ray diffraction (XRD), N(2) physisorption, inductively coupled plasma-mass spectrometry (ICP-MS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and solid-state magic-angle-spinning nuclear magnetic resonance (MAS NMR) spectroscopy studies. The tri-coordinated B–OH species incorporated into the mesoporous silica framework are considered to be the active sites for ODHP.
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spelling pubmed-87930702022-01-28 Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane Liu, Qingying Wang, Jiang Liu, Zhenxing Zhao, Ruisheng Xu, Aiju Jia, Meilin ACS Omega [Image: see text] Boron-based catalysts for oxidative dehydrogenation of propane (ODHP) have displayed excellent olefin selectivity. However, the drawback of deboronation leading to catalyst deactivation limited their scalable applications. Hereby, a series of mesoporous B-MCM-41 (BM-x, B/Si = 0.015–0.147) catalysts for ODHP were prepared by a simple hydrothermal synthesis method. It was found that propane conversion was increased and the initial reaction temperature was reduced with an increase of boron content, and the optimal values appeared on BM-2.0 (B/Si = 0.062), while olefins’ (ethylene and propylene) selectivity was maintained at ca. 70–80%. Most importantly, BM-1.0 (B/Si = 0.048) exhibited favorable activity, stability, and water tolerance after washing treatment or long-time operation (e.g., propane conversion of ca. 15% and overall olefin selectivity of ca. 80% at 550 °C) because its high structural stability prevented boron leaches. These features were identified by X-ray diffraction (XRD), N(2) physisorption, inductively coupled plasma-mass spectrometry (ICP-MS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and solid-state magic-angle-spinning nuclear magnetic resonance (MAS NMR) spectroscopy studies. The tri-coordinated B–OH species incorporated into the mesoporous silica framework are considered to be the active sites for ODHP. American Chemical Society 2022-01-13 /pmc/articles/PMC8793070/ /pubmed/35097303 http://dx.doi.org/10.1021/acsomega.1c06504 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Liu, Qingying
Wang, Jiang
Liu, Zhenxing
Zhao, Ruisheng
Xu, Aiju
Jia, Meilin
Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title_full Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title_fullStr Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title_full_unstemmed Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title_short Water-Tolerant Boron-Substituted MCM-41 for Oxidative Dehydrogenation of Propane
title_sort water-tolerant boron-substituted mcm-41 for oxidative dehydrogenation of propane
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8793070/
https://www.ncbi.nlm.nih.gov/pubmed/35097303
http://dx.doi.org/10.1021/acsomega.1c06504
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