Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, 330063, PR China; National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang, 330063, PR China.
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, 330063, PR China; National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang, 330063, PR China.
Environ Res. 2022 Aug;211:113007. doi: 10.1016/j.envres.2022.113007. Epub 2022 Feb 26.
The maximum targeted capture silver from contaminated water is urgently necessary for sustainable development. Herein, the perfluorination conjugated microporous polymer adsorbent (F-CMP) has been fabricated by Sonogashira-Hagihara coupling reaction and employed to remove Ag(I) ions. Characterizations of NMR, XPS and FT-IR indicate the successful synthesis of F-CMP adsorbent. The influence factors of F-CMP on Ag(I) adsorption behavior are studied, and the adsorption capacity of Ag(I) reaches 251.3 mg/g. The experimental results of isothermal adsorption and kinetic adsorption are consistent with the Freundlich model and pseudo-second-order isothermal adsorption model, which follows a multilayer adsorption behavior on the uniform surface of the adsorbent, and the chemical adsorption becomes the main rate-limiting step. Combined with DFT calculation, the adsorption mechanism of Ag(I) by F-CMP is elucidated. The peaks shift of sp before and after adsorption is larger than that of F1s, suggesting that the -CC- on the F-CMP becomes the dominant chelation site of Ag(I). Furthermore, F-CMP exhibits specific adsorption for Ag(I) in polymetallic complex water, with the maximum selectivity coefficient of 31.5. Our study may provide a new possibility of perfluorinated CMPs for effective capture of Ag(I) ions to address environmental issues.
从受污染的水中最大限度地靶向捕获银对于可持续发展是非常必要的。本文通过 Sonogashira-Hagihara 偶联反应制备了全氟化共轭微孔聚合物吸附剂（F-CMP），并将其用于去除 Ag(I)离子。NMR、XPS 和 FT-IR 的表征表明成功合成了 F-CMP 吸附剂。研究了 F-CMP 对 Ag(I)吸附行为的影响因素，Ag(I)的吸附容量达到 251.3mg/g。等温吸附和动力学吸附的实验结果与 Freundlich 模型和拟二级等温吸附模型一致，表明吸附剂表面均匀，Ag(I)的吸附行为遵循多层吸附，化学吸附成为主要的速率限制步骤。结合 DFT 计算，阐明了 F-CMP 吸附 Ag(I)的机制。吸附前后 sp 峰的位移大于 F1s 的位移，表明 F-CMP 上的 -CC-成为 Ag(I)的主要螯合位点。此外，F-CMP 在多金属络合水中对 Ag(I)表现出特殊的吸附作用，最大选择性系数为 31.5。我们的研究为有效捕获 Ag(I)离子以解决环境问题提供了全氟化 CMPs 的新可能性。
