A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2

作者：Lin Li, Ying Lv, Hongting Sheng, Yonglei Du, Haifeng Li, Yapei Yun, Ziyi Zhang, Haizhu Yu, Manzhou Zhu · 发表于：Nature Communications · 年份：2023 · DOI：10.1038/s41467-023-42723-3 · 被引用次数：56 · 研究领域：Carbon dioxide utilization in catalysis、Nanocluster Synthesis and Applications、Machine Learning in Materials Science

Abstract 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.