Construction of heterogeneous frustrated lewis pairs based on covalent organic frameworks stabilized boron cations and investigation of cycloaddition reaction performance

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering Pub Date : 2024-09-16 DOI:10.1016/j.jece.2024.114137

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引用次数: 0

Abstract

Frustrated Lewis Pairs (FLPs) catalysts have been widely designed and synthesized in current chemistry, with the key being the selection of boron-based Lewis acids. Among novel boron-based Lewis acids, boron cations with higher Lewis acidity caused by cationic charge have been proven to have special reactivity. However, the current boron cations have only been used to construct homogeneous FLPs, which would be difficult to meet the industrial process demand for FLPs catalysts, possibly due to the lack of suitable stabilizers. In this paper, we propose a strategy to construct heterogeneous FLPs using covalent organic frameworks (COFs) stabilized boron cations as Lewis acid. Firstly, heterogeneous Lewis acid COFs@[B(C₆F₅)₂]⁺[Al₂Cl₇]^- was prepared by stabilizing boron cations with CN bonds in COFs, followed by introducing ^tBu₃P to construct heterogeneous FLPs COFs@[B(C₆F₅)₂]⁺[Al₂Cl₇]^-/^tBu₃P. Meanwhile, these FLPs catalysts exhibited excellent catalytic and cyclic performance in the preparation of cyclic carbonates by CO₂ addition from epoxy compounds.

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基于共价有机框架稳定硼阳离子的异质失谐路易斯对的构建及环化反应性能研究

受挫路易斯对（FLPs）催化剂在当前的化学研究中得到了广泛的设计和合成，其关键在于硼基路易斯酸的选择。在新型硼基路易斯酸中，由阳离子电荷引起的路易斯酸度较高的硼阳离子已被证明具有特殊的反应活性。然而，可能由于缺乏合适的稳定剂，目前的硼阳离子只能用于构建均相的 FLPs，难以满足工业过程对 FLPs 催化剂的需求。在本文中，我们提出了一种利用共价有机框架（COFs）稳定硼阳离子作为路易斯酸来构建异质 FLPs 的策略。首先，通过在 COFs 中用 CN 键稳定硼阳离子，然后引入 tBu3P，制备出异质路易斯酸 COFs@[B(C6F5)2]+[Al2Cl7]-，从而构建出异质 FLPs COFs@[B(C6F5)2]+[Al2Cl7]-/tBu3P。同时，这些 FLPs 催化剂在利用环氧化合物的 CO2 加成法制备环状碳酸盐时表现出优异的催化性能和循环性能。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Environmental Chemical Engineering Environmental Science-Pollution

CiteScore

11.40

自引率

6.50%

发文量

2017

审稿时长

27 days

期刊介绍： The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.