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用于炔丙胺与一氧化碳高效环化反应的咪唑功能化UiO-66封装钯纳米颗粒

Imidazolium-Functionalized UiO-66 Encapsulating Palladium Nanoparticles for Efficient Cyclization of Propargylamine and CO.

作者信息

Tao Zekun, Chen Jie, Zhang Qinggang, Qi Qi, Wu Xiyue, Zhang Shiyong, Qu Hongen, Liu Yuling, Zhou Zhonggao

机构信息

College of Chemistry and Chemical Engineering, Analysis and Testing Center, Key Laboratory of Jiangxi University for Functional Materials Chemistry, Jiangxi Province Key Laboratory of Synthetic Pharmaceutical Chemistry, Gannan Normal University, Ganzhou, 341000, PR China.

School of Resources and Civil Engineering, Gannan University of Science and Technology, Ganzhou, 341000, PR China.

出版信息

Chem Asian J. 2025 Jun;20(12):e202500150. doi: 10.1002/asia.202500150. Epub 2025 Apr 16.

Abstract

Highly efficient and stable catalysts for carbon dioxide (CO) capture and conversion into value-added chemicals are critically needed. In this study, postmodification of UiO-66-MeIm with iodomethane via N-alkylation results in a roughened octahedral structure, yielding (I)BisMe-Im-UiO-66. A series of palladium nanoparticles (UiO-66-Pd-NPs) were subsequently synthesized through an ion exchange strategy with NaPdCl, followed by chemical reduction with NaBH. Comprehensive characterization of UiO-66-Pd-NPs was conducted using multiple analytical techniques, revealing PdNPs with an average size of 6.634 ± 1.510 nm. The catalyst demonstrated exceptional efficiency in the cyclization of CO and propargylamine, achieving a yield of 100% in DMSO under mild conditions and ambient pressure with NaOAc as a weak base. No significant deactivation of catalytic performance was observed after the catalyst was reused three times. The synergistic effect of the imidazolium moiety and PdNPs facilitates the activation of both CO and propargylamines, enabling the formation of 2-oxazolidinones.

摘要

迫切需要高效且稳定的用于捕获二氧化碳(CO)并将其转化为增值化学品的催化剂。在本研究中,通过N-烷基化用碘甲烷对UiO-66-MeIm进行后修饰,得到了粗糙的八面体结构,即(I)双甲基咪唑-UiO-66。随后通过与NaPdCl进行离子交换策略,接着用NaBH进行化学还原,合成了一系列钯纳米颗粒(UiO-66-Pd-NPs)。使用多种分析技术对UiO-66-Pd-NPs进行了全面表征,结果显示钯纳米颗粒的平均尺寸为6.634±1.510纳米。该催化剂在CO与炔丙胺的环化反应中表现出卓越的效率,在温和条件和常压下,以醋酸钠作为弱碱,在二甲基亚砜中实现了100%的产率。该催化剂重复使用三次后,催化性能未出现明显失活。咪唑鎓部分与钯纳米颗粒的协同效应促进了CO和炔丙胺的活化,从而能够形成2-恶唑烷酮。

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