4.7 Article

One-pot construction of nitrogen-rich polymeric ionic porous networks for effective CO2 capture and fixation

期刊

POLYMER CHEMISTRY
卷 13, 期 1, 页码 121-129

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1py01121a

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资金

  1. National Natural Science Foundation of China [51873232]
  2. Open Sharing Fund for the Large-scale Instruments and Equipment of Central South University [CSUZC201930, CSUZC201927]
  3. European Research Council (ERC) [NAPOLI-639720]
  4. Wallenberg Academy Fellow program from the Knut & Alice Wallenberg Foundation in Sweden [KAW 2017.0166]

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This study presents a strategy for facile construction of nitrogen-rich IPNs through one-pot base-mediated synthesis, showing efficient CO2 capture and catalysis of the cycloaddition reaction between CO2 and epoxides. This unique strategy of combining two coupling routes in one pot has potential applications in selective molecular separation and conversion.
Facile preparation of ionic porous networks (IPNs) with large and permanent porosity is highly desirable for CO2 capture and transformation but remains a challenge. Here we report a one-pot base-mediated construction of nitrogen-rich IPNs through a combination of nucleophilic substitution and quaternisation chemistry from H-imidazole. This strategy, as proven by the model reactions of 1H-imidazole or 1-methyl-1H-imidazole with cyanuric chloride, allows for fine regulation of porosity and physicochemical properties, leading to nitrogen-rich IPNs featuring abundant ionic units and radicals. The as-prepared networks, termed IPN-CSUs, efficiently capture CO2 (80.1 cc g(-1) at 273 K/1 bar) with an ideal CO2/N-2 selectivity of 139.7. They can also effectively catalyse the cycloaddition reaction between CO2 and epoxides with high yields of up to 99% under mild conditions (0.1 MPa, 298 K), suggesting their possible applications in the fields of both selective molecular separation and conversion. Unlike the previously known strategies generally involving single coupling chemistry, our strategy combining two coupling routes in one pot appears to be unique and potentially applicable to other building blocks.

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