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Rationalizing the role of the anion in CO2 capture and conversion using imidazolium-based ionic liquid modified mesoporous silica

机译:使用基于咪唑鎓的离子液体改性的介孔二氧化硅合理化阴离子在CO2捕获和转化中的作用

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摘要

Covalently supported ionic liquids in mesoporous materials were prepared by grafting 1-methyl-3-(3-trimethoxysylilpropyl)imidazolium chloride in MCM-41. Subsequently, the [Cl-] anion was changed to [BF4-], [PF6-] or [Tf2N-]. These materials that present an advantageous combination of the properties of mesoporous solid materials and ionic liquids were evaluated for CO2 sorption as well as catalysts for CO2 conversion into cyclic carbonate using propylene oxide. The material with the [Cl-] anion had the best performance for both CO2 sorption and conversion. A CO2 sorption of 11 w/w% on the adsorbent was achieved and the cycloaddition reaction exhibited a conversion of 67% with 82% selectivity with the catalyst remaining active after 5 cycles, proving that the same sorbent/catalyst setup can be used for both CO2 capture and conversion. Based on the experimental data and electronic-structure numerical simulations, we have hypothesized two major reasons why chloride out performs other anions when adsorbed on MCM-41 unlike unsupported ionic liquids.
机译:通过在MCM-41中嫁接1-甲基-3-(3-三甲氧基金丙基)咪唑鎓氯化物制备中孔材料中共价支持的离子液体。随后,将[Cl-]阴离子改变为[BF4-],[PF6-]或[TF2N-]。呈现介孔固体材料和离子液体性质的有利组合的这些材料被评价CO 2吸附以及CO 2转化成使用环氧丙烷的环碳酸酯的催化剂。具有[Cl-]阴离子的材料具有CO2吸附和转化的最佳性能。实现了吸附剂上11w / w%的CO 2吸附,环加成反应表现出67%的转化率,在5个循环后剩余活性活性的催化剂的选择性为82%的选择性,证明可以使用相同的吸附剂/催化剂设置二氧化碳捕获和转换。基于实验数据和电子结构数值模拟,我们假设氯化氯在与不受支持的离子液体上吸附时,氯化物在MCM-41上进行其他阴离子进行两大原因。

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  • 来源
    《RSC Advances》 |2015年第79期|共8页
  • 作者单位

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Programa Posgard Engn &

    Tecnol Mat PGETEMA Porto Alegre RS Brazil;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Programa Posgard Engn &

    Tecnol Mat PGETEMA Porto Alegre RS Brazil;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Fac Quim FAQUI Porto Alegre RS Brazil;

    Univ Aveiro Dept Quim CICECO P-3800 Aveiro Portugal;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Fac Quim FAQUI Porto Alegre RS Brazil;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Programa Posgard Engn &

    Tecnol Mat PGETEMA Porto Alegre RS Brazil;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Programa Posgard Engn &

    Tecnol Mat PGETEMA Porto Alegre RS Brazil;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Fac Quim FAQUI Porto Alegre RS Brazil;

    Univ Fed Sao Paulo Inst Ciencia &

    Tecnol BR-12231280 Sao Jose Dos Campos SP Brazil;

    UCIBIO REQUIMTE Dept Quim Fac Ciencias &

    Tecnol P-2829516 Caparica Portugal;

    Pontificia Univ Catolica Rio Grande do Sul PUCRS Programa Posgard Engn &

    Tecnol Mat PGETEMA Porto Alegre RS Brazil;

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  • 正文语种 eng
  • 中图分类 化学;
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