A New Aluminum Porphyrin-Based Porous Hyper-Cross-Linked Polymer Modified by Imidazolium Salts for Cooperative Conversion of CO2 into Cyclic Carbonates under Mild Conditions

IF 3.8 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Kechi Chen, Yu Chen, Zixuan Zhang, Rongchang Luo
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Abstract

Metalloporphyrin-based porous organic polymers that behave as advanced biomimetic nanoreactors have drawn continuous attention for heterogeneous CO2 cycloaddition conversion in the past decades. However, the use of homogeneous onium salts, usually acting as nucleophilic cocatalysts, may increase the cost of product purification and cause additional environmental problems. In this contribution, a new aluminum porphyrin-based porous hyper-cross-linked polymer modified by imidazolium salts (denoted as Im@Al-HCP) has been successfully constructed for the first time. The two-step process of hyper-cross-linking reaction combined with postsynthetic modification endows the catalyst with a large surface area (about 213 m2·g–1), good CO2 adsorption capacity (up to 1.45 mmol·g–1), and highly dispersed cooperative active sites. Accordingly, bifunctional Im@Al-HCP exhibits an outstanding catalytic activity, good recyclability, and broad substrate generality without cocatalysts and solvents under mild conditions. In particular, a high turnover frequency (TOF) value of up to 5000 h–1 can be acquired, which far exceeds that of most reported heterogeneous catalysts under identical conditions. In addition, the as-made heterogeneous catalyst can be recycled for at least six times without an obvious loss in catalytic activity. This work not only bring some inspirations for the construction of multifunctional catalysts but also provides great potential for industrial applications of CO2 cycloadditions.

Abstract Image

一种新型咪唑盐改性卟啉铝基多孔超交联聚合物在温和条件下协同将CO2转化为环状碳酸盐
基于金属卟啉的多孔有机聚合物作为先进的仿生纳米反应器,在CO2非均相环加成转化方面受到了广泛的关注。然而,使用均相铵盐,通常作为亲核助催化剂,可能会增加产品纯化的成本,并造成额外的环境问题。本文首次成功构建了咪唑盐修饰的新型卟啉铝基多孔超交联聚合物(表示为Im@Al-HCP)。通过两步超交联反应与合成后改性相结合,催化剂具有较大的比表面积(约213 m2·g-1)、良好的CO2吸附能力(可达1.45 mmol·g-1)和高度分散的协同活性位点。因此,双功能Im@Al-HCP在温和的条件下表现出出色的催化活性,良好的可回收性和广泛的底物通用性,无需助催化剂和溶剂。特别是,在相同条件下,可以获得高达5000 h-1的高周转频率(TOF)值,远远超过大多数报道的多相催化剂。此外,制备的多相催化剂可循环使用至少6次,且催化活性无明显损失。本研究不仅为构建多功能催化剂提供了一些启示,而且为CO2环加成的工业应用提供了巨大的潜力。
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
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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