College of Chemistry and Chemical Engineering, Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources , Central South University , Changsha 410083 , China.
ACS Appl Mater Interfaces. 2018 Oct 24;10(42):36002-36009. doi: 10.1021/acsami.8b13417. Epub 2018 Oct 15.
Building novel frameworks as sorbents remains a highly significant target for key environmental issues such as CO or SO emissions from coal-fired power plants. Here, we report the construction and tunable pore structure as well as gas adsorption properties of hierarchically porous covalent triazine-based frameworks (CTF-CSUs) functionalized by appended carboxylic acid/sodium carboxylate groups. The densely integrated functionalities on the pore walls bestow strong affinity to the as-made networks toward guest acid gases, in spite of their moderate Brunauer-Emmett-Teller surface areas. With abundant microporosity and integrated carboxylic acid groups, our frameworks deliver strong affinity toward CO with considerably high enthalpy (up to 44.6 kJ/mol) at low loadings. Moreover, the sodium carboxylate-anchored framework (termed as CTF-CSU41) shows an exceptionally high uptake of SO up to 6.7 mmol g (42.9 wt %) even under a low SO partial pressure of 0.15 bar (298 K), representing the highest value for a scrubbing material reported to date. Significantly, such pore engineering could pave the way to broad applications of porous organic polymers.
构建新型吸附剂框架仍然是解决关键环境问题的一个非常重要的目标,如燃煤电厂的 CO 或 SO 排放。在这里,我们报告了由附加的羧酸/羧酸根官能团功能化的分级多孔共价三嗪基框架(CTF-CSU)的构建和可调孔结构以及气体吸附性能。尽管其比表面积适中,但孔壁上密集集成的功能赋予了对制得的网络的客体酸性气体的强亲和力。由于具有丰富的微孔和整合的羧酸基团,我们的框架对 CO 具有很强的亲和力,在低负载下具有相当高的焓(高达 44.6 kJ/mol)。此外,用钠离子羧酸根锚定的框架(称为 CTF-CSU41)在 SO 分压低至 0.15 巴(298 K)的情况下,对 SO 的吸收量高达 6.7 mmol g(42.9 wt%),这是迄今为止报道的吸收材料的最高值。值得注意的是,这种孔工程为多孔有机聚合物的广泛应用铺平了道路。