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Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions

Oxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion...

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Autores principales: Liu, Zhankai, Liu, Ziyi, Fan, Jie, Lu, Wen-Duo, Wu, Fan, Gao, Bin, Sheng, Jian, Qiu, Bin, Wang, Dongqi, Lu, An-Hui
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814760/
https://www.ncbi.nlm.nih.gov/pubmed/36604430
http://dx.doi.org/10.1038/s41467-022-35776-3
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author Liu, Zhankai
Liu, Ziyi
Fan, Jie
Lu, Wen-Duo
Wu, Fan
Gao, Bin
Sheng, Jian
Qiu, Bin
Wang, Dongqi
Lu, An-Hui
author_facet Liu, Zhankai
Liu, Ziyi
Fan, Jie
Lu, Wen-Duo
Wu, Fan
Gao, Bin
Sheng, Jian
Qiu, Bin
Wang, Dongqi
Lu, An-Hui
author_sort Liu, Zhankai
collection PubMed
description Oxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion over BN by interacting with hydroperoxyl and alkoxyl radicals and generating reactive species which promote oxidation of alkane and olefin formation, through feeding a mixture of alkane and olefin and DFT calculations. The isotope tracer studies reveal the cleavage of C-C bond in propylene when co-existing with propane, directly evidencing the deep-oxidation of olefins occur in the ODH reaction over BN. Furthermore, enhancing the activation of ethane by the in-situ formed olefins from propane is successfully realized at lower temperature by co-feeding alkane mixture strategy. This work unveils the realistic ODH reaction pathway over BN and provides an insight into efficiently producing olefins.
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spelling pubmed-98147602023-01-06 Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions Liu, Zhankai Liu, Ziyi Fan, Jie Lu, Wen-Duo Wu, Fan Gao, Bin Sheng, Jian Qiu, Bin Wang, Dongqi Lu, An-Hui Nat Commun Article Oxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion over BN by interacting with hydroperoxyl and alkoxyl radicals and generating reactive species which promote oxidation of alkane and olefin formation, through feeding a mixture of alkane and olefin and DFT calculations. The isotope tracer studies reveal the cleavage of C-C bond in propylene when co-existing with propane, directly evidencing the deep-oxidation of olefins occur in the ODH reaction over BN. Furthermore, enhancing the activation of ethane by the in-situ formed olefins from propane is successfully realized at lower temperature by co-feeding alkane mixture strategy. This work unveils the realistic ODH reaction pathway over BN and provides an insight into efficiently producing olefins. Nature Publishing Group UK 2023-01-05 /pmc/articles/PMC9814760/ /pubmed/36604430 http://dx.doi.org/10.1038/s41467-022-35776-3 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
Liu, Zhankai
Liu, Ziyi
Fan, Jie
Lu, Wen-Duo
Wu, Fan
Gao, Bin
Sheng, Jian
Qiu, Bin
Wang, Dongqi
Lu, An-Hui
Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title_full Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title_fullStr Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title_full_unstemmed Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title_short Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
title_sort auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814760/
https://www.ncbi.nlm.nih.gov/pubmed/36604430
http://dx.doi.org/10.1038/s41467-022-35776-3
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