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Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation
Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalys...
Autores principales: | , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10162968/ https://www.ncbi.nlm.nih.gov/pubmed/37147403 http://dx.doi.org/10.1038/s41467-023-38361-4 |
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author | Chen, Xiaowen Qin, Xuetao Jiao, Yueyue Peng, Mi Diao, Jiangyong Ren, Pengju Li, Chengyu Xiao, Dequan Wen, Xiaodong Jiang, Zheng Wang, Ning Cai, Xiangbin Liu, Hongyang Ma, Ding |
author_facet | Chen, Xiaowen Qin, Xuetao Jiao, Yueyue Peng, Mi Diao, Jiangyong Ren, Pengju Li, Chengyu Xiao, Dequan Wen, Xiaodong Jiang, Zheng Wang, Ning Cai, Xiangbin Liu, Hongyang Ma, Ding |
author_sort | Chen, Xiaowen |
collection | PubMed |
description | Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalyst as the bridge between homogeneous and heterogeneous catalysis, which displays an outstanding catalytic performance for n-butane dehydrogenation, with a remarkable n-butane reaction rate (8.8 mol·g(Ir)(−1)·h(−1)) and high butene selectivity (95.6%) at low temperature (450 °C). Significantly, we correlate the BDH activity with the Ir species from nanoscale to sub-nanoscale, to reveal the nature of structure-dependence of catalyst. Moreover, we compare Ir single atoms with Pt single atoms and Pd single atoms for in-depth understanding the nature of metal-dependence at the atomic level. From experimental and theoretical calculations results, the isolated Ir site is suitable for both reactant adsorption/activation and product desorption. Its remarkable dehydrogenation capacity and moderate adsorption behavior are the key to the outstanding catalytic activity and selectivity. |
format | Online Article Text |
id | pubmed-10162968 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-101629682023-05-07 Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation Chen, Xiaowen Qin, Xuetao Jiao, Yueyue Peng, Mi Diao, Jiangyong Ren, Pengju Li, Chengyu Xiao, Dequan Wen, Xiaodong Jiang, Zheng Wang, Ning Cai, Xiangbin Liu, Hongyang Ma, Ding Nat Commun Article Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalyst as the bridge between homogeneous and heterogeneous catalysis, which displays an outstanding catalytic performance for n-butane dehydrogenation, with a remarkable n-butane reaction rate (8.8 mol·g(Ir)(−1)·h(−1)) and high butene selectivity (95.6%) at low temperature (450 °C). Significantly, we correlate the BDH activity with the Ir species from nanoscale to sub-nanoscale, to reveal the nature of structure-dependence of catalyst. Moreover, we compare Ir single atoms with Pt single atoms and Pd single atoms for in-depth understanding the nature of metal-dependence at the atomic level. From experimental and theoretical calculations results, the isolated Ir site is suitable for both reactant adsorption/activation and product desorption. Its remarkable dehydrogenation capacity and moderate adsorption behavior are the key to the outstanding catalytic activity and selectivity. Nature Publishing Group UK 2023-05-05 /pmc/articles/PMC10162968/ /pubmed/37147403 http://dx.doi.org/10.1038/s41467-023-38361-4 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 Chen, Xiaowen Qin, Xuetao Jiao, Yueyue Peng, Mi Diao, Jiangyong Ren, Pengju Li, Chengyu Xiao, Dequan Wen, Xiaodong Jiang, Zheng Wang, Ning Cai, Xiangbin Liu, Hongyang Ma, Ding Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title | Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title_full | Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title_fullStr | Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title_full_unstemmed | Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title_short | Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation |
title_sort | structure-dependence and metal-dependence on atomically dispersed ir catalysts for efficient n-butane dehydrogenation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10162968/ https://www.ncbi.nlm.nih.gov/pubmed/37147403 http://dx.doi.org/10.1038/s41467-023-38361-4 |
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