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Integration of metalloporphyrin into cationic covalent triazine frameworks for the synergistically enhanced chemical fixation of CO2

机译:金属卟啉为阳离子的集成共价三嗪框架的表现为协同作用增强的化学固定二氧化碳

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摘要

The design and preparation of porous catalysts with multiple catalytically active sites for synergistically catalytic conversion of CO2 still remains a challenge. Herein, cobalt porphyrin as a Lewis acidic active site was introduced in imidazolium-functionalized cationic covalent triazine frameworks (denoted as Co-PCCTFs) via copolymerization of cobalt 5,10,15,20-tetrakis(4-cyanophenyl)porphyrin (Co-TPPCN) and 1,3-bis(4-cyanophenyl) imidazolium chloride ([BCIM]Cl). The obtained bifunctional Co-PCCTFs with positively charged imidazolium groups have high BET surface areas and show sufficient CO2 adsorption uptakes. The nucleophilic halide anions of the imidazolium parts and the cobalt porphyrin Lewis acid sites were positioned in close proximity so that the Co-PCCTFs could synergistically activate substrates and intermediates. Compared with ICTF-400 free of Co2+ that was obtained from [BCIM]Cl, Co-PCCTF5 exhibited enhanced activity for the cycloaddition of CO2 to epoxides to produce cyclic carbonates without a cocatalyst under mild conditions. Moreover, Co-PCCTF5 is sufficiently stable so that it could be reused more than 5 times without loss of catalytic activity. This work provides a new approach for the design and preparation of efficient multifunctional catalysts with multiple sites for synergistic catalysis.
机译:的设计和制备多孔催化剂与多个催化地活跃的站点协同催化转化二氧化碳仍然是一个挑战。介绍了路易斯酸性活性部位imidazolium-functionalized阳离子共价三嗪框架(表示Co-PCCTFs)通过共聚的钴(Co-TPPCN)和1,3 -二(4-cyanophenyl) imidazolium氯化([BCIM] Cl)。与带正电的imidazolium Co-PCCTFs组织高赌注表面区域和显示足够的二氧化碳吸附吸收。亲核imidazolium卤化物离子零件和钴卟啉路易斯酸的网站被放置在靠近,这样吗实现协同Co-PCCTFs可以激活基质和中间体。ictf - 400的二氧化碳+免费获得[BCIM] Cl, Co-PCCTF5表现出增强的活动二氧化碳与环氧化合物的环加成作用没有助催化剂生产循环碳酸盐在温和的条件下。足够稳定,以便它可以被再利用超过5次没有催化的损失活动。的设计和制备高效多功能催化剂与多个站点协同催化作用。

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