由离子交联剂和布朗斯梯酸构建的超交联离子聚合物在常压下催化低浓度二氧化碳与环氧化物的环化反应

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL
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引用次数: 0

摘要

在温和条件下捕获低浓度二氧化碳并将其转化为高附加值产品仍然是一项重大挑战。在这项工作中,使用超交联离子聚合物(IMPy-HIP 或 BPy-HIP)作为催化剂,通过咪唑基离子链接剂与 1、1′-萘基-2,2′-二基磷酸氢酯(BNDHP,一种勃朗斯特酸,强氢键供体)之间的一锅弗里德尔-卡夫烷基化反应制备而成。带有强氢键位点(ArPO3OH)、活性阳离子(咪唑鎓)和亲核反离子(Cl-)的 HIPs 在低浓度 CO2- 环氧化物环加成中表现出极高的催化效率和稳定的可循环性。实验结果与 DFT 理论计算相结合发现,该催化剂的高性能归功于勃朗斯特德酸位点(P-OH)、碱性吡啶 N 和离子位点的协同作用。此外,该催化剂还具有出色的结构稳定性和底物通用性,而且可以通过离心轻松分离,重复使用五次而不会明显降低催化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Hypercrosslinked ionic polymers constructed by ionic cross-linkers and Bronsted acid for catalytic cycloaddition of low-concentration CO2 with epoxide under atmospheric pressure

Hypercrosslinked ionic polymers constructed by ionic cross-linkers and Bronsted acid for catalytic cycloaddition of low-concentration CO2 with epoxide under atmospheric pressure
The capture and conversion of low-concentration CO2 into high value-added products under mild conditions remains a major challenge. In this work, an additive/metal/solvent-free catalytic transformation between epoxides and low-concentration CO2 under atmospheric conditions is achieved by using hypercrosslinked ionic polymers (IMPy-HIP or BPy-HIP) as catalysts prepared by an one-pot Friedel–Crafts alkylation between an imidazolium-based ionic linker and 1, 1′-binaphthyl-2, 2′-diyl hydrogenphosphate (BNDHP, a Bronsted acid, strong hydrogen bond donor). The HIPs bearing a strong hydrogen bonding site (ArPO3OH), active cations (imidazolium) and nucleophilic counterion (Cl) demonstrate highly catalytic efficiency and stable recyclability for low-concentration CO2-epoxide cycloaddition. The experiment results combining with DFT theoretical calculations reveal that the high performance of this catalyst attributes to the cooperation of the Bronsted acid site (P-OH), basic pyridine N and ionic site. In addition, the catalyst shows excellent structural stability and substrate universality, and it can be easily separated by centrifugation and reused for five runs without significant decrease in catalytic performance.
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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