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Alkyl-chain-tuned hierarchically porous ionic polymers with ultrahigh surface area for CO2 adsorption and conversion

作者:Xuanbo Liu, Xiuli Yan, Shuangshuo Li, Zheng Zhu, Xionglei Wang, Jiajia Yang, Shenjun Qin, Tao Chang, Yongjing Hao · 发表于:Separation and Purification Technology · 年份:2025 · DOI:10.1016/j.seppur.2025.134673 · 被引用次数:3 · 研究领域:Carbon dioxide utilization in catalysis、Ionic liquids properties and applications、Carbon Dioxide Capture Technologies

ABSTRACT Porous ionic polymers (PIPs) featuring high specific surface area ( S BET ) and abundance of ionic active sites have emerged as advanced materials for synergistic CO 2 capture and conversion. In this study, a novel class of hydroamino-functionalized ionic polymers, designed as PHAIPs, was constructed through a one-pot three-component strategy integrating Friedel-Crafts alkylation, quaternization, and nucleophilic epoxide ring-opening reactions. The synthesis employed α , α’ -dibromo-p-xylene, N , N -dimethylethylene diamine and glycidyl-dimethyl-alkyl-ammonium bromide as modular building blocks, facilitating precise control over textural properties. Systematic structural optimization through alkyl chain length variation and reactant stoichiometric adjustments generated ionic polymers with tunable S BET up to 1731 m 2 ·g −1 and hierarchical pore architecture. The optimized PHAIP-C 16 exhibited a moderate CO 2 adsorption capacity of 2.45 mmol·g −1 and a CO 2 /N 2 selectivity factor of 71 at 1 bar, governed by a synergistic Langmuir and Freundlich adsorption mechanism with thermodynamically spontaneous and exothermic characteristics. Notably, the PHAIP-C 16-4/3/1.5 demonstrated particularly effectiveness in CO 2 cycloaddition reactions, achieving an excellent conversion yield of 95.5%. Mechanistic investigations revealed a dual-activation pathway, with bromide anion (Br − ) nucleophilically activated epoxides, while hydroamino groups function as hydrogen-bond donors to ...