深共晶溶剂官能化 ZIF-67:将二氧化碳化学固定为环状碳酸盐的新型双功能异相催化剂

IF 5.5 3区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of the Taiwan Institute of Chemical Engineers Pub Date : 2024-08-08 DOI:10.1016/j.jtice.2024.105687
Reza Khalifeh, Maryam Rajabzadeh, Fahimeh Rezaei
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引用次数: 0

摘要

CO 是主要的温室气体之一,会导致全球变暖和一系列严重的环境问题。催化 CO 化学转化为高附加值产品是极具吸引力的方法之一。通过在 ZIF-67 表面加入氯化胆碱和基于硫代氨基脲的深共晶溶剂,成功合成了一种新型沸石咪唑酸框架(ZIF-67),命名为 ChTSC@ZIF-67。利用粉末 XRD、TGA、zeta 电位、扫描电镜和 BET 表面积测量分析了该材料的纹理和物理特性。在不同的实验条件下,研究了 ChTSC@ZIF-67 作为催化剂,在没有助催化剂或溶剂的情况下将环氧化物和二氧化碳转化为环碳酸盐的情况。在最佳条件下(3 毫克催化剂、4.0 巴 CO 压力、80 °C、3 小时反应时间),可生产出多种环碳酸盐,且产率和选择性极佳。ZIF-67 中的活性位点与深共晶溶剂之间的协同效应可能是催化活性高的主要原因。此外,该催化剂在超过六个循环后仍能保持其异质性,产率也没有大幅下降。
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Deep eutectic solvent-functionalized ZIF-67: A novel bifunctional heterogeneous catalyst for chemical fixation of CO2 into cyclic carbonates

Background

CO2 is one of the dominant greenhouse gases that causes global warming and a series of serious environmental problems. The catalytic chemical conversion of CO2 into value-added products is one of the attractive approaches.

Methods

A novel zeolitic imidazolate framework (ZIF-67) has been successfully synthesized by incorporating choline chloride and thiosemicarbazide-based deep eutectic solvent onto the surface of ZIF-67, denoted as ChTSC@ZIF-67. The material's textural and physical characteristics were analyzed using powder XRD, TGA, zeta potential, SEM, and BET surface area measurements.

Significant Findings

The utilization of ChTSC@ZIF-67 as a catalyst for the conversion of epoxides and carbon dioxide into cyclic carbonates, in the absence of a co-catalyst or solvent, was investigated under various experimental conditions. Optimum conditions (3 mg catalyst, 4.0 bar CO2 pressure, 80 °C, and 3 h reaction time) led to the production of diverse cyclic carbonates with excellent yield and selectivity. The synergistic effect between the active site in ZIF-67 and the deep eutectic solvent may be the main reason for the high catalytic activity. Furthermore, the catalyst retains its heterogeneous nature for more than six cycles, exhibiting no substantial decline in yield.

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来源期刊
CiteScore
9.10
自引率
14.00%
发文量
362
审稿时长
35 days
期刊介绍: Journal of the Taiwan Institute of Chemical Engineers (formerly known as Journal of the Chinese Institute of Chemical Engineers) publishes original works, from fundamental principles to practical applications, in the broad field of chemical engineering with special focus on three aspects: Chemical and Biomolecular Science and Technology, Energy and Environmental Science and Technology, and Materials Science and Technology. Authors should choose for their manuscript an appropriate aspect section and a few related classifications when submitting to the journal online.
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