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A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)

The preparation of 2-Oxazolidinones using CO(2) offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag(4) catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH-) an...

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Autores principales: Li, Lin, Lv, Ying, Sheng, Hongting, Du, Yonglei, Li, Haifeng, Yun, Yapei, Zhang, Ziyi, Yu, Haizhu, Zhu, Manzhou
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10620197/
https://www.ncbi.nlm.nih.gov/pubmed/37914680
http://dx.doi.org/10.1038/s41467-023-42723-3
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author Li, Lin
Lv, Ying
Sheng, Hongting
Du, Yonglei
Li, Haifeng
Yun, Yapei
Zhang, Ziyi
Yu, Haizhu
Zhu, Manzhou
author_facet Li, Lin
Lv, Ying
Sheng, Hongting
Du, Yonglei
Li, Haifeng
Yun, Yapei
Zhang, Ziyi
Yu, Haizhu
Zhu, Manzhou
author_sort Li, Lin
collection PubMed
description The preparation of 2-Oxazolidinones using CO(2) offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag(4) catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH-) and realizes the cyclization of propargylamine with CO(2) under mild conditions. As expected, the Turnover Number (TON) and Turnover Frequency (TOF) values of the Ag(4) nanocluster (NC) are higher than most of reported catalysts. The Ag(4)* NC intermediates are isolated and confirmed their structures by Electrospray ionization (ESI) and (1)H Nuclear Magnetic Resonance ((1)H NMR). Additionally, the key role of multiple Ag atoms revealed the feasibility and importance of low-nuclear catalysts at the atomic level, confirming the reaction pathways that are inaccessible to the Ag single-atom catalyst and Ag(2) NC. Importantly, the nanocomposite achieves multiple recoveries and gram scale product acquisition. These results provide guidance for the design of more efficient and targeted catalytic materials.
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spelling pubmed-106201972023-11-03 A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2) Li, Lin Lv, Ying Sheng, Hongting Du, Yonglei Li, Haifeng Yun, Yapei Zhang, Ziyi Yu, Haizhu Zhu, Manzhou Nat Commun Article The preparation of 2-Oxazolidinones using CO(2) offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag(4) catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH-) and realizes the cyclization of propargylamine with CO(2) under mild conditions. As expected, the Turnover Number (TON) and Turnover Frequency (TOF) values of the Ag(4) nanocluster (NC) are higher than most of reported catalysts. The Ag(4)* NC intermediates are isolated and confirmed their structures by Electrospray ionization (ESI) and (1)H Nuclear Magnetic Resonance ((1)H NMR). Additionally, the key role of multiple Ag atoms revealed the feasibility and importance of low-nuclear catalysts at the atomic level, confirming the reaction pathways that are inaccessible to the Ag single-atom catalyst and Ag(2) NC. Importantly, the nanocomposite achieves multiple recoveries and gram scale product acquisition. These results provide guidance for the design of more efficient and targeted catalytic materials. Nature Publishing Group UK 2023-11-01 /pmc/articles/PMC10620197/ /pubmed/37914680 http://dx.doi.org/10.1038/s41467-023-42723-3 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 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
Li, Lin
Lv, Ying
Sheng, Hongting
Du, Yonglei
Li, Haifeng
Yun, Yapei
Zhang, Ziyi
Yu, Haizhu
Zhu, Manzhou
A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title_full A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title_fullStr A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title_full_unstemmed A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title_short A low-nuclear Ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with CO(2)
title_sort low-nuclear ag(4) nanocluster as a customized catalyst for the cyclization of propargylamine with co(2)
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10620197/
https://www.ncbi.nlm.nih.gov/pubmed/37914680
http://dx.doi.org/10.1038/s41467-023-42723-3
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