Functionalization of ionic liquids for heterogeneous catalysis in CO2 conversion: Cycloaddition of epoxides and hydrogenation

IF 5.2 2区化学 Q1 CHEMISTRY, APPLIED

Catalysis Today Pub Date : 2024-10-02 DOI:10.1016/j.cattod.2024.115087

Aline Scaramuzza Aquino , Ismael dos Santos Belmonte , Cristiano Favero , Cristiane Xavier da Silva Campos , Anderson Joel Schwanke , Anne Gabriella Dias Santos , Michèle Oberson de Souza , Katia Bernardo Gusmão

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Abstract

The mitigation of environmental impacts caused by greenhouse gas emissions has become increasingly urgent, and the use of CO₂ as a primary carbon source is an alternative in chemical transformations, including the synthesis of organic carbonates, formic acid, or methanol. This work aims to synthesize ionic liquids from the imidazolium cation family to be used in the cycloaddition of CO₂ with ILs anchored in SiO₂-clay heterostructure, MCM-41 and KIT-6 mesoporous materials, as well as the hydrogenation of CO₂ with ILs added to ruthenium complexes, i.e., two catalytic systems. The most satisfactory result for CO₂ cycloaddition (TON _PC = 226) was obtained using the IL (MeO)₃Sipmim.Cl anchored in SiO₂-clay heterostructure (0.16 mol%) as the catalyst and ZnBr₂ (0.04 mol%) as the co-catalyst. The hydrogenation was conducted with the IL (edaO)₃Sipmim.Cl and the ruthenium complex Ru-PNN were not successful, but with co-catalyst PEHA, formic acid/formamide was produced (TON _Form = 552). The unique catalytic system that showed activity for forming methanol was the commercial Ru-MACHO, Ru-C₂₉H₃₀ClNOP₂, (TON _MeOH = 3.3). These results highlight the potential of ruthenium-based complexes and supported ionic liquids as active systems in CO₂ conversion.

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离子液体功能化用于二氧化碳转化的异相催化：环氧化物的环加成和氢化

减轻温室气体排放对环境的影响已变得日益紧迫，而使用二氧化碳作为主要碳源是化学转化（包括合成有机碳酸盐、甲酸或甲醇）的一种替代方法。这项工作旨在合成咪唑阳离子家族的离子液体，用于二氧化碳与锚定在二氧化硅-粘土异质结构、MCM-41 和 KIT-6 介孔材料中的离子液体的环加成反应，以及二氧化碳与添加到钌配合物中的离子液体的氢化反应，即两种催化体系。使用锚定在 SiO2-clay 异质结构中的 IL (MeO)3Sipmim.Cl （0.16 摩尔%）作为催化剂，ZnBr2（0.04 摩尔%）作为助催化剂，获得了最令人满意的 CO2 环加成结果（TON PC = 226）。使用 IL (edaO)3Sipmim.Cl 和钌络合物 Ru-PNN 进行氢化并不成功，但使用助催化剂 PEHA 则生成了甲酸/甲酰胺（TON Form = 552）。在生成甲醇方面显示出活性的独特催化体系是商用 Ru-MACHO，即 Ru-C29H30ClNOP2（TON MeOH = 3.3）。这些结果凸显了钌基配合物和支撑离子液体作为二氧化碳转化活性体系的潜力。

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

Catalysis Today 化学-工程：化工

CiteScore

11.50

自引率

3.80%

发文量

573

审稿时长

2.9 months

期刊介绍： Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.