Luo Xiaoyan, Liu Yibang, Li Mingxing, Ling Renhui, Ye Ling, Cao Xuegong, Wang Congmin
Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Key Laboratory of Molecular Designing and Green Conversions (Fujian Province University), College of Materials Science and Engineering, Huaqiao University Xiamen 361021 P.R. China
Department of Chemistry, Center of Chemistry for Frontier Technologies, Zhejiang University Hangzhou 310027 P. R. China
RSC Adv. 2023 Oct 2;13(41):28729-28735. doi: 10.1039/d3ra05346f. eCollection 2023 Sep 26.
Carboxylic acid-modified materials are a common means of achieving efficient NH adsorption. In this study, we report that improved NH adsorption capacity and easier desorption can be achieved through the introduction of substances containing Lewis basic groups into carboxylic acid-modified materials. Easily synthesized mesoporous acid-base hybrid polymers were constructed with polymers rich in carboxylic acid and Lewis base moieties through cooperative hydrogen bonding interactions (CHBs). The hybrid polymer PAA-P4VP presented higher NH capacity (18.2 mmol g at 298 K and 1 bar NH pressure) than PAA (6.0 mmol g) through the acid-base reaction and the assistance from CHBs with NH, while the NH desorption from PAA-P4VP was easier for the reformation of CHBs. Based on the introduction of CHBs, a series of mesoporous acid-base hybrid polymers was synthesized with NH adsorption capacity of 15.8-19.3 mmol g and high selectivity of NH over CO ( = 25.4-56.3) and N ( = 254-1068), and the possible co-existing gases, such as SO, had a lower effect on NH uptake by hybrid polymers. Overall, the hybrid polymers present efficient NH adsorption owing to the abundant acidic moieties and CHBs, while the concomitant Lewis bases promote NH desorption.
羧酸改性材料是实现高效氨吸附的常用手段。在本研究中，我们报道了通过将含路易斯碱性基团的物质引入羧酸改性材料中，可以提高氨吸附容量并使脱附更容易。通过协同氢键相互作用（CHBs），用富含羧酸和路易斯碱部分的聚合物构建了易于合成的介孔酸碱杂化聚合物。杂化聚合物PAA-P4VP通过酸碱反应以及与氨的CHBs辅助，在298 K和1 bar氨压力下表现出比PAA（6.0 mmol/g）更高的氨容量（18.2 mmol/g），而对于PAA-P4VP，由于CHBs的重新形成，氨脱附更容易。基于CHBs的引入，合成了一系列介孔酸碱杂化聚合物，其氨吸附容量为15.8 - 19.3 mmol/g，对氨的选择性高于一氧化碳（α = 25.4 - 56.3）和氮气（α = 254 - 1068），并且可能共存的气体如二氧化硫对杂化聚合物氨吸附的影响较小。总体而言，由于丰富的酸性部分和CHBs，杂化聚合物表现出高效的氨吸附，而伴随的路易斯碱促进了氨的脱附。
