Abstract：
The current landscape of perfluoroalkyl substances (PFAS) extraction methodologies presents significant challenges, particularly for multiple PFAS with different carbon chain lengths. This study introduced an energy-driven strategic approach for screening deep eutectic solvents (DESs) to effectively remove a diverse range of PFAS, including perfluoroalkylcarboxylic acids (PFCAs), perfluoroalkanesulfonic acids (PFSAs), and perfluoroalkyl amides (FAAs), from contaminated environments (total 13 target compounds). Utilizing energy-based screening, we identified DES candidates with high affinity for a spectrum of PFAS compounds from 1234 potential starting materials of eutectic systems. Key findings revealed the superior removal efficiency of tributylphosphineoxide/2-methylpiperazine system, exceeding 99 % for various PFAS with different carbon chain lengths in real environmental water samples. Additionally, we elucidated the molecular interactions between DESs and PFAS through ab initio molecular dynamics (AIMD) simulations, providing valuable insights into the mechanisms governing the removal process. The mechanism of extraction involves hydrogen bond network topology and structural organization, with DESs capable of extracting PFAS while maintaining a weakly aggregated state of target molecules and minimizing the impact on the intrinsic structures of DES. The proposed system forms a dynamic, complementary, and flexible non-covalent interaction network structure with PFAS. The study advances the understanding of DES as a designable, effective, and sustainable alternative to conventional solvents for PFAS remediation, offering a significant contribution to environmental chemistry and green technology.
摘要：
全氟烷基物质（PFAS）提取方法的现状提出了重大挑战，特别是对于具有不同碳链长度的多个PFAS。这项研究引入了一种能源驱动的战略方法，用于筛选深共晶溶剂（DES），以有效地去除各种PFAS，包括全氟烷基羧酸（PFCA），全氟链烷磺酸（PFSA），和全氟烷基酰胺(FAA)，来自污染环境（共13种目标化合物）。利用基于能量的筛选，我们从共晶系统的1234种潜在起始材料中鉴定出对PFAS化合物光谱具有高亲和力的DES候选物。主要发现揭示了三丁基氧化膦/2-甲基哌嗪系统的优异去除效率，在实际环境水样中，具有不同碳链长度的各种PFAS超过99%。此外,我们通过从头算分子动力学（AIMD）模拟阐明了DES和PFAS之间的分子相互作用，为治理移除过程的机制提供有价值的见解。萃取机理涉及氢键网络拓扑和结构组织，DES能够提取PFAS，同时保持靶分子的弱聚集状态，并将对DES固有结构的影响降至最低。拟议的系统形成了一个动态的，互补,以及与PFAS的柔性非共价相互作用网络结构。这项研究推进了对DES作为可设计的理解，有效,以及用于PFAS修复的常规溶剂的可持续替代品，为环境化学和绿色技术做出重大贡献。
