避免令人遗憾的替代：新功能组的引入能否将 PFAS 从顽固性转变为反应性？,Environmental Science & Technology

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避免令人遗憾的替代：新功能组的引入能否将 PFAS 从顽固性转变为反应性？
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-10-25 , DOI: 10.1021/acs.est.3c06232
Andrew P Folkerson ₁ , Stephanie R Schneider ₁ , Jonathan P D Abbatt ₁ , Scott A Mabury ₁

Affiliation

全氟烷基物质和多氟烷基物质 (PFAS) 存在于一系列商业和消费品中。由于其化学稳定性，这些化学品通常是高性能表面活性剂或不粘/防水涂层；然而，这种稳定性导致某些 PFAS 具有环境持久性。为了促进降解，新的含氟表面活性剂结构单元（F ₇ C ₃ –O–CHF-CF ₂ –S-CH ₂ –CH ₂ –OH (FESOH)、F ₃ C–O–CHF-CF ₂ –S-CH ₂ – CH ₂ –OH (MeFESOH)、F ₇ C ₃ –O–CHF-CF ₂ –O–CH ₂ –CH ₂ –OH (ProFdiEOH)、F ₇ C ₃ –O–CHF-CF ₂ –CH ₂ –OH ( ProFEOH) 和 F ₃ C–O–CHF-CF ₂ –O–CH ₂ –CH ₂ –OH (MeFdiEOH)) 已通过醚、硫醚和多氟化碳等杂原子键进行系统开发。在大气室中监测室温、气相 OH 氧化速率常数和这些化学品的产物，以研究它们在大气中的命运。使用碘化物试剂离子并通过离线 UPLC-MS/MS 使用在线高分辨率化学电离质谱 (CIMS) 进行分析。硫醚同系物 FESOH 和 MeFESOH 的最大速率常数为k _FESOH = 2.82 (±0.33) 和k _MeFESOH = 2.17 (±0.17)（分别为 ×10 ^–12 cm ³分子^–1 s ^–1）。观察到第一代、第二代和第三代 OH 氧化产物随时间的变化，同时产物定量产生了超短全氟丙酸 (PFPrA) 和短聚氟醚酸物质作为 FESOH 和 ProFdiEOH 的最终产物。有证据表明 MeFESOH 已完全矿化，展示了潜在的良性化学结构。

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Avoiding Regrettable Replacements: Can the Introduction of Novel Functional Groups Move PFAS from Recalcitrant to Reactive?

Per- and polyfluoroalkyl substances (PFASs) are present in a range of commercial and consumer products. These chemicals are often high-performance surfactants or nonstick/water-repellant coatings due to their chemical stability; however, this stability leads to select PFAS being environmentally persistent. To facilitate degradation, new fluorosurfactant building blocks (F₇C₃–O–CHF-CF₂–S-CH₂–CH₂–OH (FESOH), F₃C–O–CHF-CF₂–S-CH₂–CH₂–OH (MeFESOH), F₇C₃–O–CHF-CF₂–O–CH₂–CH₂–OH (ProFdiEOH), F₇C₃–O–CHF-CF₂–CH₂–OH (ProFEOH), and F₃C–O–CHF-CF₂–O–CH₂–CH₂–OH (MeFdiEOH)) have been systematically developed with heteroatom linkages such as ethers, thioethers, and polyfluorinated carbons. The room temperature, gas-phase OH oxidation rate constants, and products of these chemicals were monitored in an atmospheric chamber to investigate their fate in the atmosphere. Analysis was performed using online high-resolution chemical ionization mass spectrometry (CIMS) using the iodide reagent ion and via offline UPLC-MS/MS. FESOH and MeFESOH, the thioether congeners, were observed to have the largest rate constants of k_FESOH = 2.82 (±0.33) and k_MeFESOH = 2.17 (±0.17) (×10^–12 cm³ molecules^–1 s^–1, respectively). First-, second-, and third-generation products of OH oxidation were observed as a function of time, while product quantification yielded ultrashort perfluoropropionic acid (PFPrA) and short polyfluoroether acid species as the terminal products for FESOH and ProFdiEOH. There was evidence for MeFESOH being fully mineralized, demonstrating the potential benign chemical architecture.

更新日期：2023-10-25

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