Yu Hao, Zhang Peng, Song Dongbao, Chen Hao, Huang Peng, Rončević Srđan D, Sun Hongwen
MOE Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
Tianjin Engineering Center of Environmental Diagnosis and Contamination Remediation, Nankai University, Tianjin 300350, China.
Environ Sci Technol. 2025 Aug 5;59(30):16034-16045. doi: 10.1021/acs.est.5c06248. Epub 2025 Jul 21.
The global concern of per- and polyfluoroalkyl substance (PFAS) contamination has gradually shifted from long- to ultrashort- and short-chain PFAS, but the widely used pyrogenic carbons (PCs) are almost ineffective at removing such hydrophilic pollutants. Herein, a polypyrrole (PPy) nanostructured coating strategy was proposed to modify PCs (PPy@P-BC) for rapid and efficient removal of ultrashort- and short-chain PFAS from water. Static batch tests revealed that the sorption rate constant and sorption capacity of PFAS (C2-C6) on PPy@P-BC are at least 38 times and 5 times greater than those on undecorated PCs and benchmark materials of granular activated carbon, respectively, and their sorption equilibrium time is within 300 s. The outstanding sorption performance of PPy@P-BC is maintained in dynamic column tests (>3120 bed volumes) and different types of real water contaminated by 36 PFAS, including 11 previously identified emerging PFAS (removal >95.3%). PPy@P-BC also exhibited excellent regeneration and reusability. The following dual-drive mechanisms for PFAS removal were identified based on experimental results and density functional theory (DFT) calculations: (i) electrostatic attraction between amino functional groups (especially -NH-) on the nanostructured PPy coating and anionic PFAS and (ii) pore filling facilitated by the well-preserved porous structure via construction of the nanostructured coating. Overall, these results provide a promising solution to address the ultrashort- and short-chain PFAS crisis.
全球对全氟和多氟烷基物质(PFAS)污染的关注已逐渐从长链PFAS转向超短链和短链PFAS,但广泛使用的热解碳(PCs)在去除这类亲水性污染物方面几乎无效。在此,提出了一种聚吡咯(PPy)纳米结构涂层策略来修饰PCs(PPy@P-BC),以快速高效地从水中去除超短链和短链PFAS。静态批量试验表明,PFAS(C2-C6)在PPy@P-BC上的吸附速率常数和吸附容量分别比未修饰的PCs和颗粒活性炭基准材料至少高38倍和5倍,且其吸附平衡时间在300秒内。PPy@P-BC在动态柱试验(>3120床体积)和36种PFAS污染的不同类型实际水体(包括11种先前鉴定出的新兴PFAS,去除率>95.3%)中均保持出色的吸附性能。PPy@P-BC还表现出优异的再生性和可重复使用性。基于实验结果和密度泛函理论(DFT)计算,确定了以下PFAS去除的双重驱动机制:(i)纳米结构PPy涂层上的氨基官能团(特别是-NH-)与阴离子PFAS之间的静电吸引;(ii)通过构建纳米结构涂层而得以保留的多孔结构促进的孔隙填充。总体而言,这些结果为解决超短链和短链PFAS危机提供了一个有前景的解决方案。