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<p>This study focuses on the synthesis and characterization of vinylimidazolium-based ionic compounds with hydroxyl (–OH), carbonyl (–C(O)–), carboxyl (–COOH), and amino (–NH<sub>2</sub>) groups and halide anions of Cl<sup>−</sup>, Br<sup>−</sup>, and I<sup>−</sup>. These compounds were comprehensively characterized using <sup>1</sup>H and <sup>13</sup>C NMR, FTIR, MALDI-TOF mass&#xa0;spectrometry, and elemental analysis. Thermogravimetric analysis revealed excellent thermal stability up to 250&#xa0;°C. A combination of diverse functional groups such as hydrogen bond donors, nucleophilic moiety, and polymerizable vinyl group within a single molecule provides a unique multifunctional platform, enabling reasonable choice and the rational construction of advanced catalytic materials derived from such monomers. Their catalytic activity in chemical fixation of carbon dioxide (CO<sub>2</sub>) into cyclic carbonates was evaluated via cycloaddition reaction with epichlorohydrin, yielding chloropropylene carbonate and demonstrate their great catalytic potential in such reactions: most of compounds provided over 80% conversion with over 90% selectivity of main product using 2&#xa0;mol% of catalyst at 90&#xa0;°C and 1&#xa0;MPa within 2&#xa0;h, with average turn over freqency (TOF) value of 20&#xa0;h<sup>−1</sup>, demonstrating good performance for a metal-free catalyst. An impact of structural features—such as substituents and halide counterions—on catalytic performance was analyzed, alongside the effects of catalyst loading, temperature, pressure, and reaction time. The study establishes a strategic&#xa0;approach for designing polymeric catalysts through careful monomer selection. Novel compounds with well-defined properties can serve as key building blocks, enabling the development of functional materials for efficient CO<sub>2</sub> conversion into valuable products.</p>

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Multisite-Active Site Ionic Monomers for Catalytic CO2 Conversion: Synthesis and Comprehensive Characterization of Basic Units for Further Rational Design of Functional Materials

  • 期刊论文

  • 发表日期：

    2025年11月3日

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  • Anna A. Golovacheva,
  • Zakhar A. Markin,
  • Anastasiya I. Golovkina,
  • Artyom N. Markov,
  • Ivan D. Grishin,
  • Ksenia V. Otvagina,
  • Anna A. Zharkova,
  • Ibrahim S. M. Abufanar,
  • Ilya I. Vorobyov,
  • Andrey V. Vorotyntsev,
  • Anton N. Petukhov,
  • Olga V. Kazarina

摘要

This study focuses on the synthesis and characterization of vinylimidazolium-based ionic compounds with hydroxyl (–OH), carbonyl (–C(O)–), carboxyl (–COOH), and amino (–NH2) groups and halide anions of Cl−, Br−, and I−. These compounds were comprehensively characterized using 1H and 13C NMR, FTIR, MALDI-TOF mass spectrometry, and elemental analysis. Thermogravimetric analysis revealed excellent thermal stability up to 250 °C. A combination of diverse functional groups such as hydrogen bond donors, nucleophilic moiety, and polymerizable vinyl group within a single molecule provides a unique multifunctional platform, enabling reasonable choice and the rational construction of advanced catalytic materials derived from such monomers. Their catalytic activity in chemical fixation of carbon dioxide (CO2) into cyclic carbonates was evaluated via cycloaddition reaction with epichlorohydrin, yielding chloropropylene carbonate and demonstrate their great catalytic potential in such reactions: most of compounds provided over 80% conversion with over 90% selectivity of main product using 2 mol% of catalyst at 90 °C and 1 MPa within 2 h, with average turn over freqency (TOF) value of 20 h−1, demonstrating good performance for a metal-free catalyst. An impact of structural features—such as substituents and halide counterions—on catalytic performance was analyzed, alongside the effects of catalyst loading, temperature, pressure, and reaction time. The study establishes a strategic approach for designing polymeric catalysts through careful monomer selection. Novel compounds with well-defined properties can serve as key building blocks, enabling the development of functional materials for efficient CO2 conversion into valuable products.