Scholarlink

<p>A covalently co-networked poly(vinylmethyldimethoxysilane)/polyvinylpyrrolidone (PVMDMS@PVP) aerogel scaffold enables in-situ growth of UiO-66-NH<sub>2</sub> and grafting of 1-methylacetamido-3-methylimidazolium bromide ([MAmim]Br), forming a monolithic catalyst for integrated carbon dioxide (CO<sub>2</sub>) capture and cycloaddition reaction. Tuning PVP content (5–20 wt %) during sol–gel synthesis yields a hierarchically porous network (&gt; 1,000 m<sup>2</sup>·g<sup>–1</sup>) that resists collapse under solvothermal conditions. Solvothermal crystallization within the network produces uniformly dispersed UiO-66-NH<sub>2</sub> (~ 34 wt %) without pore blockage, and ionic liqud (IL) grafting introduces dual sites for CO<sub>2</sub> adsorption and epoxide activation. The composite achieves 2.8 mmol g<sup>–1</sup> CO<sub>2</sub> uptake at 25&#xa0;°C and promotes solvent- and co-catalyst-free cycloaddition of allyl glycidyl ether (AGE) at 120&#xa0;°C, 0.6&#xa0;MPa CO<sub>2</sub> to &gt; 99% conversion and selectivity with 0.151&#xa0;mol % catalyst loading. Ten consecutive adsorption–desorption and reaction cycles retain &gt; 97% of activity and structural integrity. An apparent activation energy of 37.5&#xa0;kJ mol<sup>–1</sup> (vs. 47.8&#xa0;kJ·mol<sup>–1</sup> for UiO-66-NH<sub>2</sub>-IL) highlights accelerated kinetics. Exceptional water tolerance and multi-cycle stability underscore its potential as a scalable platform for practical CO<sub>2</sub> valorization.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Boosted mass transfer and water tolerance in CO2 cycloaddition via hierarchically porous PVMDMS@PVP aerogel containing in-situ grown UiO-66-NH2

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年1月22日

查看全文
  • Kyung Hoon Min,
  • Byeongseok Kim,
  • Hyung-Ho Park,
  • Sung-Hyeon Baeck,
  • Sang Eun Shim

摘要

A covalently co-networked poly(vinylmethyldimethoxysilane)/polyvinylpyrrolidone (PVMDMS@PVP) aerogel scaffold enables in-situ growth of UiO-66-NH2 and grafting of 1-methylacetamido-3-methylimidazolium bromide ([MAmim]Br), forming a monolithic catalyst for integrated carbon dioxide (CO2) capture and cycloaddition reaction. Tuning PVP content (5–20 wt %) during sol–gel synthesis yields a hierarchically porous network (> 1,000 m2·g–1) that resists collapse under solvothermal conditions. Solvothermal crystallization within the network produces uniformly dispersed UiO-66-NH2 (~ 34 wt %) without pore blockage, and ionic liqud (IL) grafting introduces dual sites for CO2 adsorption and epoxide activation. The composite achieves 2.8 mmol g–1 CO2 uptake at 25 °C and promotes solvent- and co-catalyst-free cycloaddition of allyl glycidyl ether (AGE) at 120 °C, 0.6 MPa CO2 to > 99% conversion and selectivity with 0.151 mol % catalyst loading. Ten consecutive adsorption–desorption and reaction cycles retain > 97% of activity and structural integrity. An apparent activation energy of 37.5 kJ mol–1 (vs. 47.8 kJ·mol–1 for UiO-66-NH2-IL) highlights accelerated kinetics. Exceptional water tolerance and multi-cycle stability underscore its potential as a scalable platform for practical CO2 valorization.