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1.北华航天工业学院材料工程学院 廊坊 065000
2.(2.河北省热防护材料重点实验室 廊坊 065000) (中国矿业大学
3.安全工程学院
4.材料与物理学院 徐州 221116
Huan Xu, E-mail: hihuan@cumt.edu.cn
Received:16 April 2025,
Accepted:09 June 2025,
Published Online:14 July 2025,
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李冬至, 刘巧宾, 张嘉龙, 董方, 孙艳荣, 汪少振, 张生辉, 徐欢. 可循环固碳聚合物制备及其同步捕集颗粒物机理研究. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25102
Li, D. Z.; Liu, Q. B.; Zhang, J. L.; Dong, F.; Sun, Y. R.; Wang, S. Z.; Zhang, S. H.; Xu, H. Preparation and mechanistic investigation of recyclable carbon-fixing polymers with simultaneous interception of particulate matter. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25102
李冬至, 刘巧宾, 张嘉龙, 董方, 孙艳荣, 汪少振, 张生辉, 徐欢. 可循环固碳聚合物制备及其同步捕集颗粒物机理研究. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25102 DOI: CSTR: 32057.14.GFZXB.2025.7438.
Li, D. Z.; Liu, Q. B.; Zhang, J. L.; Dong, F.; Sun, Y. R.; Wang, S. Z.; Zhang, S. H.; Xu, H. Preparation and mechanistic investigation of recyclable carbon-fixing polymers with simultaneous interception of particulate matter. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25102 DOI: CSTR: 32057.14.GFZXB.2025.7438.
尽管整体式吸附材料因操作简便、吸附热效应低和再生性能优异而在烟气CO
2
与PM捕集领域备受关注,但其吸附容量与再生性能间的“权衡”效应以及粉末加工成型造成的高气体渗透阻力,严重制约了工业应用前景. 本研究通过调整系列反应功能基摩尔比,巧妙地将酰基官能团定向引入聚合物分子框架,成功制备出具有分级多孔结构与丰富吸附位点的整体式固碳聚合物(A-CMPs),实现对PM与CO
2
的高效循环吸附分离. 该材料的微观结构呈现由随机排列编织的中空纳米管构成的三维网络特征,可有效增强单位体积气流的分散与传质,分级多孔结构则为客体分子提供了充足的存储空间与结合位点. 通过连续共价键构建的高度离域
π
-
π
共轭多孔骨架赋予材料优异的结构稳定性,使其在高湿环境中仍能保持分子构型与捕获性能的完整性,并支持PM/CO
2
的多次循环再生. 得益于骨架内开放氧原子构建的高极性微环境及微孔/介孔比例,A-CMPs展现出46.6 cm
3
·g
-1
的CO
2
吸附容量,且循环使用后吸附性能保持稳定. 因此,开发兼具高性能与可循环的整体式聚合物材料,对满足工业实际应用需求具有重要价值.
Monolithic adsorbent materials have garnered significant attention for flue gas carbon dioxide (CO
2
) and particulate matter (PM) capture because of their operational simplicity
low adsorption heat effects
and superior regeneration capabilities. However
the intrinsic "t
rade-off" between adsorption capacity and cyclic regeneration performance
coupled with the high gas permeation resistance induced by powder processing
severely restricts their industrial applicability. In this study
we strategically incorporated acyl functional groups into a polymeric molecular framework through precise regulation of the reaction functional basis
successfully synthesizing monolithic carbon-fixing polymers (A-CMPs) with hierarchical porous architectures and multiple active sites for efficient cyclic PM/CO
2
adsorption separation. The material exhibits a unique three-dimensional network microstructure composed of randomly interwoven hollow nanotubes
which effectively enhances gas dispersion and mass transfer per unit volume
whereas the hierarchical porosity provides ample storage space and adsorption sites for guest molecules. The highly delocalized
π-π
conjugated porous framework constructed through continuous covalent bonds confers exceptional structural stability
enabling the preservation of molecular integrity and capture performance under high humidity
along with sustained PM/CO
2
capture-regeneration cycling. Thanks to the highly polar microenvironment constructed by open oxygen atoms in the skeleton and the microporous/mesoporous ratio
the A-CMPs exhibited a CO
2
adsorption capacity of 46.6 cm
3
·g
-1
and the adsorption performance remained stable after recycling. Therefore
the development of monolithic polymeric materials with high performance and recyclability is of great value for meeting the demands of industrial applications.
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