A phenyl-rich β-cyclodextrin porous crosslinked polymer for efficient removal of aromatic pollutants: Insight into adsorption performance and mechanism
A phenyl-rich β-cyclodextrin porous crosslinked polymer for efficient removal of aromatic pollutants: Insight into adsorption performance and mechanism
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一种富含苯基的β-环糊精多孔交联聚合物，可有效去除芳香族污染物：深入了解吸附性能和机制
DOI：
10.1016/j.cej.2020.124020
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发表时间：
2020-05-01
影响因子：
15.1
通讯作者：
Ji, Hongbing
中科院分区：
文献类型：
--
作者：
Huang, Qiuyuan;Chai, Kungang;Ji, Hongbing
在此，一种具有高苯基含量和稳定孔隙结构的富含苯基的β - 环糊精多孔交联聚合物（PCD - PCP）被用于去除水中的芳香族污染物。PCD - PCP是通过苄基化β - 环糊精与交联剂4,4'-二（氯甲基）-1,1'-联苯进行高效的傅 - 克烷基化反应获得的。我们已经证明，通过控制交联度，可以调节所得材料的纳米结构、多孔特性和苯基含量，进而控制吸附能力。令人印象深刻的是，具有高交联密度的PCD - PCP(H)在去除污染水中的有机物方面表现出显著的吸附能力和良好的可回收性。以2,4,6 - 三氯苯酚和双酚A作为模型吸附质，吸附过程均很好地符合准二级动力学模型和弗罗因德利希模型，并且热力学研究证实吸附是一个自发的放热过程。PCD - PCP(H)能够在较宽的pH值和离子强度范围以及循环过程中保持较高的吸附能力。此外，对实验和理论计算结果的综合分析表明，π - π相互作用和主 - 客相互作用可能共同促进吸附过程，这为开发用于吸附芳香族分子的先进β - 环糊精基吸附剂提供了新的见解。
Herein, a phenyl-rich beta-cyclodextrin porous crosslinked polymer (PCD-PCP) with high phenyl content and consistent pore structure was used to remove the aromatic pollutants from water. The PCD-PCP was obtained through the efficient Friedel-Crafts alkylation of benzylated beta-cyclodextrin with the crosslinker 4,4'-bis(chloromethyl)-1,1'-biphenyl. We have demonstrated that by controlling the crosslinking degree, the nanostructure, porous features and phenyl contents of the resulting materials can be tuned, in turn allowing the control of the adsorption capacities. Impressively, PCD-PCP(H) with high crosslinking density exhibited a notable sorption ability and good recyclability for removal of organics from contaminated water. Using 2,4,6-trichlorophenyl and bisphenol A as model adsorbates, the adsorption processes both fitted well the pseudo-second-order model and the Freundlich model, and thermodynamic studies certified that the adsorption was a spontaneous and exothermic process. PCD-PCP(H) was able to maintain high adsorption capacity in wide pH and ionic strength ranges as well as in recycling process. Furthermore, the comprehensive analysis of experimental and theoretical calculations results suggested that the pi-pi interactions and host-guest interactions may jointly promote the uptake process, providing new insights into the development of advanced beta-cyclodextrin based adsorbents for aromatic molecule adsorption.