Nitrogen-Rich Tetrazole–Amide-Functionalised Zn Metal–Organic Framework as Catalyst for Efficient Catalytic CO2 Cycloaddition with Epoxides

IF 3.8 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysts Pub Date : 2023-12-20 DOI:10.3390/catal14010006

Anup Paul, Ismayil M. Garazade, Anirban Karmakar, R. A. Khan, M. F. C. Guedes da Silva, Ana V M Nunes, A. Pombeiro

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引用次数: 0

Abstract

In this study, we report the design, synthesis, and catalytic application of the novel nitrogen-rich Zn(II) MOF [Zn2(μ3-1κN,2κN′,3κO-HL)2(DMF)2]n·nH2O (HL2− = 4-((4-(1H-tetrazol-5-yl)phenyl)carbamoyl)benzoate), denoted as ZnMOF, for the efficient conversion of carbon dioxide (CO2) to cyclic carbonates via cycloaddition with epoxides. It was synthesised from a tetrazole appended amide-functionalised pro-ligand (H3L) and Zn(NO3)2·6H2O under hydrothermal conditions. The synthesised material was characterised namely by elemental analysis, infrared spectroscopy, powder X-ray diffraction (PXRD), and single-crystal X-ray diffraction analyses. The catalytic potential of ZnMOF was investigated in the CO2 cycloaddition reaction with various epoxides, with conversions ranging from 17% to 99%. The catalyst retained its activity across multiple reaction cycles, demonstrating its stability and reusability. The influence of co-catalysts on the reaction was explored, with tetrabutylammonium bromide (TBABr) emerging as the most effective one. A plausible reaction mechanism is proposed.

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富氮四唑-酰胺官能化 Zn 金属有机框架作为催化剂高效催化 CO2 与环氧化物的环加成反应

在本研究中，我们报告了新型富氮 Zn(II) MOF [Zn2(μ3-1κN,2κN′、3κO-HL）2（DMF）2]n-nH2O（HL2- = 4-((4-(1H-四唑-5-基)苯基)氨基甲酰基)苯甲酸酯），简称 ZnMOF，用于通过与环氧化物的环加成将二氧化碳（CO2）高效转化为环碳酸盐。它是在水热条件下，由添加了酰胺功能化原配体（H3L）的四唑和 Zn(NO3)2-6H2O 合成的。合成材料的表征包括元素分析、红外光谱、粉末 X 射线衍射 (PXRD) 和单晶 X 射线衍射分析。在与各种环氧化物进行 CO2 环加成反应时，研究了 ZnMOF 的催化潜能，其转化率从 17% 到 99%。该催化剂在多个反应循环中均保持活性，证明了其稳定性和可重复使用性。研究还探讨了助催化剂对反应的影响，发现四丁基溴化铵（TBABr）是最有效的助催化剂。提出了一种合理的反应机制。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Catalysts CHEMISTRY, PHYSICAL-

CiteScore

6.80

自引率

7.70%

发文量

1330

审稿时长

3 months

期刊介绍： Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.