含氟缺陷共价三嗪框架高效吸附水中全氟-2,5-二甲基-3,6-二氧杂庚酸的特性和机理

张芝诚; 李芮; 肖国涛; 李德燕; 张明潮; 朱东海; 王维

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (11) : 6091-6100.

水污染与控制

含氟缺陷共价三嗪框架高效吸附水中全氟-2,5-二甲基-3,6-二氧杂庚酸的特性和机理

张芝诚^1,2, 李芮², 肖国涛^1,2, 李德燕¹, 张明潮¹, 朱东海¹, 王维^1,2

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Efficient adsorption behavior and mechanism of C7HFPO-TA in water by fluorinated defective covalent triazine frameworks

ZHANG Zhi-cheng^1,2, LI Rui², XIAO Guo-tao^1,2, LI De-yan¹, ZHANG Ming-chao¹, ZHU Dong-hai¹, WANG Wei^1,2

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摘要

本研究设计并成功制备了含氟缺陷共价三嗪框架(CTFs),相较于原始CTFs,含氟缺陷CTFs吸附量提升了55%,并比较了不同粒径CTFs的吸附效果,相较于CTF-F595 (154.403mg/g), CTF-F10 (246.421mg/g)提升了59%.结果表明,吸附剂粒径的减小不仅能显著提升吸附剂对于吸附质的饱和吸附量,而且可以极快地提升吸附剂对于吸附质的吸附速率.研究发现,在pH=2时, CTF-F10对C7HFPO-TA的去除率(89.55%)显著高于pH=6 (50.15%)和pH=10 (26.35%).而NaCl和FA对CTF-F10吸附C7HFPO-TA效果的影响大致相同,两者的存在使去除率下降了约20%.DFT计算结果表明,含氟缺陷CTFs对C7HFPO-TA的吸附以静电作用和亲氟作用为主.吸附再生实验证明粉末态CTFs具有良好的再生性能和循环使用性能.本研究为设计含氟缺陷CTFs吸附水中PFAS提供了新的思路,并创新性比较CTFs不同粒径对C7HFPO-TA吸附性能的影响,为水环境中PFAS的削减和去除提供了科学技术指导.

Abstract

In this study, fluorine-defective covalent triazine frameworks (CTFs) were designed and synthesized to improve adsorption performance for per-and polyfluoroalkyl substances (PFAS). Compared with pristine CTFs, the fluorine-defective CTFs exhibited a 55% increase in adsorption capacity. A systematic evaluation of different particle sizes revealed that CTF-F10 (246.421mg/g) achieved a 59% higher capacity than CTF-F595 (154.403mg/g). These results demonstrate that reducing the adsorbent particle size not only substantially increases the equilibrium adsorption capacity, but also accelerates the adsorption rate. At pH 2, CTF-F10 achieved a C7HFPO-TA removal efficiency of 89.55%, significantly higher than that at pH 6 (50.15%) and pH 10 (26.35%). The presence of NaCl or fulvic acid (FA) reduced removal efficiency by about 20%. DFT calculations indicated that the adsorption of C7HFPO-TA onto fluorine-defective CTFs is primarily governed by electrostatic and fluorophilic interactions. Regeneration experiments also excellent recyclability and reusability of powdered CTFs. This work establishes a novel design strategy for fluorine-defective CTFs for PFAS removal from water and provides a first comparative evaluation of the particle size effects on C7HFPO-TA adsorption, providing scientific and technical guidance for mitigating PFAS contamination in aquatic environments.

导出引用

张芝诚, 李芮, 肖国涛, 李德燕, 张明潮, 朱东海, 王维. 含氟缺陷共价三嗪框架高效吸附水中全氟-2,5-二甲基-3,6-二氧杂庚酸的特性和机理[J]. 中国环境科学. 2025, 45(11): 6091-6100

ZHANG Zhi-cheng, LI Rui, XIAO Guo-tao, LI De-yan, ZHANG Ming-chao, ZHU Dong-hai, WANG Wei. Efficient adsorption behavior and mechanism of C7HFPO-TA in water by fluorinated defective covalent triazine frameworks[J]. China Environmental Science. 2025, 45(11): 6091-6100

中图分类号： X703

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