在无催化剂和无溶剂条件下一步缩合合成二叔铵盐原离子液体，用于高效催化 CO2 环化反应

IF 5.3 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Liquids Pub Date : 2024-11-10 DOI:10.1016/j.molliq.2024.126423

Yuchen Hu , Ziyu Gao , Huidong Wang , Li Yang , Jiaxu Zhang , Jianmin Sun

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引用次数: 0

摘要

通过在 0 ℃ 下一步缩合合成了一种新型原生离子液体二叔丁基溴化铵离子液体（DTAB-IL），收率达 85%。在无助催化剂和溶剂的情况下，DTAB-IL 对 CO2 环加成反应也表现出有效的催化活性。催化反应条件优化为 90 ℃、4 h、1 MPa，碳酸丙烯酯的产率为 96%，选择性高达 99%。在最佳条件下，DTAB-IL 催化剂表现出良好的可回收性和对各种环氧化物的通用性。此外，还研究了温度对碳酸丙烯酯合成的影响和动力学调查。发现 DTAB-IL 催化 CO2 环加成反应的活化能为 43.93 kJ/mol，环氧丙烷的反应遵循一阶反应。二氧化碳和环氧化物的高效环加成反应归因于 DTAB-IL 中二叔铵对环氧化物和二氧化碳的活化作用以及溴阴离子对环氧化物开环作用。

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One-step condensation synthesis of di-tertiary ammonium salt protic ionic liquid for efficiently catalytic CO2 cycloaddition reaction under cocatalyst- and solvent-free conditions

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One-step condensation synthesis of di-tertiary ammonium salt protic ionic liquid for efficiently catalytic CO2 cycloaddition reaction under cocatalyst- and solvent-free conditions

A novel protic ionic liquid di-tertiary ammonium bromide ionic liquid (DTAB-IL) was synthesized by one-step condensation at 0 ℃ with 85 % yield. DTAB-IL also exhibited effective catalytic activity for CO₂ cycloaddition without cocatalyst and solvent. The catalytic reaction conditions were optimized to 90 ℃, 4 h, 1 MPa, and the yield of propylene carbonate was obtained 96 % with high selectivity 99 %. Under the optimal conditions, DTAB-IL catalyst exhibited good recyclability and universality to various epoxides. Furthermore, temperature influence and kinetic investigation for propylene carbonate synthesis were studied. The activation energy for DTAB-IL catalyzing CO₂ cycloaddition reaction was 43.93 kJ/mol, and the reaction was found to follow first-order for propylene oxide. Efficient cycloaddition reaction of CO₂ and epoxide was attributed to the activation of epoxide and CO₂ by di-tertiary ammonium and epoxide ring-opening by bromide anion in DTAB-IL.

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来源期刊

Journal of Molecular Liquids 化学-物理：原子、分子和化学物理

CiteScore

10.30

自引率

16.70%

发文量

2597

审稿时长

78 days

期刊介绍： The journal includes papers in the following areas: – Simple organic liquids and mixtures – Ionic liquids – Surfactant solutions (including micelles and vesicles) and liquid interfaces – Colloidal solutions and nanoparticles – Thermotropic and lyotropic liquid crystals – Ferrofluids – Water, aqueous solutions and other hydrogen-bonded liquids – Lubricants, polymer solutions and melts – Molten metals and salts – Phase transitions and critical phenomena in liquids and confined fluids – Self assembly in complex liquids.– Biomolecules in solution The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include: – Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.) – Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.) – Light scattering (Rayleigh, Brillouin, PCS, etc.) – Dielectric relaxation – X-ray and neutron scattering and diffraction. Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.