A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2
Abstract The preparation of 2-Oxazolidinones using CO2 offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag4 catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH...
| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-42723-3 |
| _version_ | 1797636842489643008 |
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| author | Lin Li Ying Lv Hongting Sheng Yonglei Du Haifeng Li Yapei Yun Ziyi Zhang Haizhu Yu Manzhou Zhu |
| author_facet | Lin Li Ying Lv Hongting Sheng Yonglei Du Haifeng Li Yapei Yun Ziyi Zhang Haizhu Yu Manzhou Zhu |
| author_sort | Lin Li |
| collection | DOAJ |
| description | Abstract The preparation of 2-Oxazolidinones using CO2 offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag4 catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH-) and realizes the cyclization of propargylamine with CO2 under mild conditions. As expected, the Turnover Number (TON) and Turnover Frequency (TOF) values of the Ag4 nanocluster (NC) are higher than most of reported catalysts. The Ag4* NC intermediates are isolated and confirmed their structures by Electrospray ionization (ESI) and 1H Nuclear Magnetic Resonance (1H 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 Ag2 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. |
| first_indexed | 2024-03-11T12:39:58Z |
| format | Article |
| id | doaj.art-c86220f4f23b4b719d7a6fe315326e42 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-11T12:39:58Z |
| publishDate | 2023-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-c86220f4f23b4b719d7a6fe315326e422023-11-05T12:22:59ZengNature PortfolioNature Communications2041-17232023-11-011411710.1038/s41467-023-42723-3A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2Lin Li0Ying Lv1Hongting Sheng2Yonglei Du3Haifeng Li4Yapei Yun5Ziyi Zhang6Haizhu Yu7Manzhou Zhu8Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityDepartment of Chemistry and Centre for Atomic Engineering of Advanced Materials, Anhui UniversityAbstract The preparation of 2-Oxazolidinones using CO2 offers opportunities for green chemistry, but multi-site activation is difficult for most catalysts. Here, A low-nuclear Ag4 catalytic system is successfully customized, which solves the simultaneous activation of acetylene (-C≡C) and amino (-NH-) and realizes the cyclization of propargylamine with CO2 under mild conditions. As expected, the Turnover Number (TON) and Turnover Frequency (TOF) values of the Ag4 nanocluster (NC) are higher than most of reported catalysts. The Ag4* NC intermediates are isolated and confirmed their structures by Electrospray ionization (ESI) and 1H Nuclear Magnetic Resonance (1H 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 Ag2 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.https://doi.org/10.1038/s41467-023-42723-3 |
| spellingShingle | Lin Li Ying Lv Hongting Sheng Yonglei Du Haifeng Li Yapei Yun Ziyi Zhang Haizhu Yu Manzhou Zhu A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 Nature Communications |
| title | A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 |
| title_full | A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 |
| title_fullStr | A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 |
| title_full_unstemmed | A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 |
| title_short | A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2 |
| title_sort | low nuclear ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with co2 |
| url | https://doi.org/10.1038/s41467-023-42723-3 |
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