Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol

The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high met...

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Autores principales: Zhang, Hailong, Han, Peijie, Wu, Danfeng, Du, Congcong, Zhao, Jiafei, Zhang, Kelvin H. L., Lin, Jingdong, Wan, Shaolong, Huang, Jianyu, Wang, Shuai, Xiong, Haifeng, Wang, Yong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Article
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10673993/
https://www.ncbi.nlm.nih.gov/pubmed/38001068
http://dx.doi.org/10.1038/s41467-023-43508-4
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author Zhang, Hailong
Han, Peijie
Wu, Danfeng
Du, Congcong
Zhao, Jiafei
Zhang, Kelvin H. L.
Lin, Jingdong
Wan, Shaolong
Huang, Jianyu
Wang, Shuai
Xiong, Haifeng
Wang, Yong
author_facet Zhang, Hailong
Han, Peijie
Wu, Danfeng
Du, Congcong
Zhao, Jiafei
Zhang, Kelvin H. L.
Lin, Jingdong
Wan, Shaolong
Huang, Jianyu
Wang, Shuai
Xiong, Haifeng
Wang, Yong
author_sort Zhang, Hailong
collection PubMed
description The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu−1 h−1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement.
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spelling pubmed-106739932023-11-24 Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol Zhang, Hailong Han, Peijie Wu, Danfeng Du, Congcong Zhao, Jiafei Zhang, Kelvin H. L. Lin, Jingdong Wan, Shaolong Huang, Jianyu Wang, Shuai Xiong, Haifeng Wang, Yong Nat Commun Article The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu−1 h−1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement. Nature Publishing Group UK 2023-11-24 /pmc/articles/PMC10673993/ /pubmed/38001068 http://dx.doi.org/10.1038/s41467-023-43508-4 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Zhang, Hailong
Han, Peijie
Wu, Danfeng
Du, Congcong
Zhao, Jiafei
Zhang, Kelvin H. L.
Lin, Jingdong
Wan, Shaolong
Huang, Jianyu
Wang, Shuai
Xiong, Haifeng
Wang, Yong
Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title_full Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title_fullStr Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title_full_unstemmed Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title_short Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol
title_sort confined cu-oh single sites in ssz-13 zeolite for the direct oxidation of methane to methanol
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10673993/
https://www.ncbi.nlm.nih.gov/pubmed/38001068
http://dx.doi.org/10.1038/s41467-023-43508-4
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