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Nanosecond Transient Absorption of Hydrated Electrons and Reduction of Linear Perfluoroalkyl Acids and Sulfonates
Environmental Science & Technology Letters ( IF 8.9 ) Pub Date : 2021-06-08 , DOI: 10.1021/acs.estlett.1c00383
William A. Maza 1 , Vanessa M. Breslin 2 , Jeffrey C. Owrutsky 1 , Bradford B. Pate 1 , Albert Epshteyn 1
Affiliation  

We report the rate constants (kq) and activation energies (Ea) associated with the initial reduction of linear perfluoroalkyl carboxylates (PFxA, x = the number of carbons present in the surfactant) and perfluoroalkyl sulfonates (PFxS) by the hydrated electron (eaq) as measured using temperature-dependent transient absorption spectroscopy. The reduction of PFxA and PFxS by eaq displays a negligible dependence on the number of carbons present in the surfactant and occurs with an apparent kq on the order of 108 to 109 M–1 s–1 with the kq corresponding to PFxA reduction being on average two times smaller than those for PFxS. There are no significant differences in the Ea associated with PFxA or PFxS reduction; the magnitude of Ea (∼11 kJ mol–1) is consistent with the reduction of PFxA and PFxS being a diffusion controlled process. These results are discussed within the framework of recent theoretical and experimental work on the degradation of PFxA and PFxS.

中文翻译:

水合电子的纳秒瞬态吸收和线性全氟烷基酸和磺酸盐的还原

我们报告了与线性全氟烷基羧酸盐(PFxA,x = 表面活性剂中存在的碳数)和全氟烷基磺酸盐(PFxS)的初始还原相关的速率常数(k q)和活化能(E a)通过水合电子( e aq ) 使用温度相关瞬态吸收光谱法测量。PFxA和PFxS的通过e还原水溶液-存在于表面活性剂显示对碳原子数可忽略的依赖和与表观发生ķ q 10的数量级上8到10 9中号-1小号-1k q对应于 PFxA 的减少平均是 PFxS 减少的两倍。与 PFxA 或 PFxS 减少相关的E a没有显着差异;的幅度Ë一个(〜11千焦摩尔-1)是具有PFxA和PFxS是扩散控制的过程的降低是一致的。这些结果在最近关于 PFxA 和 PFxS 降解的理论和实验工作的框架内进行了讨论。
更新日期:2021-07-13
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