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Superhydrophobic Phosphonium Modified Robust 3D Covalent Organic Framework for Preferential Trapping of Charge Dispersed Oxoanionic Pollutants
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-07-18 , DOI: 10.1002/adfm.202205222 Yue Wang 1 , Jianhui Lan 2 , Xiaofan Yang 2 , Shouchao Zhong 1 , Liyong Yuan 2 , Jiuqiang Li 1 , Jing Peng 1 , Zhifang Chai 2 , John K. Gibson 3 , Maolin Zhai 1 , Weiqun Shi 2
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-07-18 , DOI: 10.1002/adfm.202205222 Yue Wang 1 , Jianhui Lan 2 , Xiaofan Yang 2 , Shouchao Zhong 1 , Liyong Yuan 2 , Jiuqiang Li 1 , Jing Peng 1 , Zhifang Chai 2 , John K. Gibson 3 , Maolin Zhai 1 , Weiqun Shi 2
Affiliation
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Charge dispersed and less hydrophilic anionic pollutants are often difficult to be preferentially captured by common cationic framework materials. A gamma radiation modification approach is employed to anchor a superhydrophobic phosphonium-containing coating on a robust crystalline 3D covalent organic framework (COF). By regulating the surface hydrophobicity, the prepared 3DCOF-g-VBPPh3Cl is endowed with a strong affinity for charge dispersed and less hydrophilic oxoanions, such as MnO4−, TcO4− and ReO4−, to surmount the Hofmeister bias, which much favors remediation of oxoanionic pollutants in complex aqueous systems. Batch and column experiments with 3DCOF-g-VBPPh3Cl in both tap water and simulated groundwater are performed, and rapid sequestration is achieved with removal efficacy up to 99.995%, record-high distribution coefficient of 1.0 × 108 mL g−1, and desirable priority over competing anions such as Cl−, SO42−, HCO3−, and NO3−, confirming promise for remediation of charge dispersed anionic pollutants. Theoretical calculations reveal a mechanism of preferential capture based on electrostatic and dispersion interaction between charge dispersed anions and 3DCOF-g-VBPPh3Cl that effectively competes with solvation of the aqueous anions.
中文翻译：
用于优先捕获电荷分散的含氧阴离子污染物的超疏水磷鎓改性稳健 3D 共价有机框架
电荷分散且亲水性较低的阴离子污染物通常难以被常见的阳离子骨架材料优先捕获。采用伽马辐射改性方法将超疏水含鏻涂层锚定在坚固的结晶 3D 共价有机框架 (COF) 上。通过调节表面疏水性，制备的 3DCOF- g -VBPPh 3 Cl 赋予了对电荷分散和亲水性较低的含氧阴离子如 MnO 4 -、TcO 4 -和 ReO 4 -的强亲和力，以克服 Hofmeister 偏压，即非常有利于修复复杂水系统中的含氧阴离子污染物。使用 3DCOF-g-VBPPh 进行批量和色谱柱实验对自来水和模拟地下水中的3 Cl 进行了分析，实现了快速螯合，去除效率高达 99.995%，分配系数达到创纪录的 1.0 × 10 8 mL g -1，并且优先于竞争阴离子如 Cl -、SO 4 2-、HCO 3 -和 NO 3 -，证实了修复电荷分散阴离子污染物的前景。理论计算揭示了基于电荷分散阴离子和 3DCOF-g-VBPPh 3 Cl之间的静电和分散相互作用的优先捕获机制，该机制有效地与水性阴离子的溶剂化竞争。
更新日期：2022-07-18
中文翻译：
用于优先捕获电荷分散的含氧阴离子污染物的超疏水磷鎓改性稳健 3D 共价有机框架
电荷分散且亲水性较低的阴离子污染物通常难以被常见的阳离子骨架材料优先捕获。采用伽马辐射改性方法将超疏水含鏻涂层锚定在坚固的结晶 3D 共价有机框架 (COF) 上。通过调节表面疏水性，制备的 3DCOF- g -VBPPh 3 Cl 赋予了对电荷分散和亲水性较低的含氧阴离子如 MnO 4 -、TcO 4 -和 ReO 4 -的强亲和力，以克服 Hofmeister 偏压，即非常有利于修复复杂水系统中的含氧阴离子污染物。使用 3DCOF-g-VBPPh 进行批量和色谱柱实验对自来水和模拟地下水中的3 Cl 进行了分析，实现了快速螯合，去除效率高达 99.995%，分配系数达到创纪录的 1.0 × 10 8 mL g -1，并且优先于竞争阴离子如 Cl -、SO 4 2-、HCO 3 -和 NO 3 -，证实了修复电荷分散阴离子污染物的前景。理论计算揭示了基于电荷分散阴离子和 3DCOF-g-VBPPh 3 Cl之间的静电和分散相互作用的优先捕获机制，该机制有效地与水性阴离子的溶剂化竞争。
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