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Complete Defluorination and Mineralization of Perfluorooctanoic Acid by a Mechanochemical Method Using Alumina and Persulfate
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2019-06-13 , DOI: 10.1021/acs.est.9b00486 Nan Wang 1 , Hanqing Lv 1 , Yuqi Zhou 1 , Lihua Zhu 1 , Yue Hu 2 , Tetsuro Majima 1 , Heqing Tang 2
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2019-06-13 , DOI: 10.1021/acs.est.9b00486 Nan Wang 1 , Hanqing Lv 1 , Yuqi Zhou 1 , Lihua Zhu 1 , Yue Hu 2 , Tetsuro Majima 1 , Heqing Tang 2
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Perfluorooctanoic acid (PFOA) is a persistent organic pollutant that has received concerns worldwide due to its extreme resistance to conventional degradation. A mechanochemical (MC) method was developed for complete degradation of PFOA by using alumina (Al2O3) and potassium persulfate (PS) as comilling agents. After ball milling for 2 h, the MC treatment using Al2O3 or PS caused conversion of PFOA to either 1-H-1-perfluoroheptene or dimers with a defluorination efficiency lower than 20%, but that using both Al2O3 and PS caused degradation of PFOA with a defluorination of 100% and a mineralization of 98%. This method also caused complete defluorination of other C3∼C6 homologues of PFOA. The complete defluorination of PFOA attributes to Al2O3 and PS led to the weakening of the C–F bond in PFOA and the generation of hydroxyl radical (•OH), respectively. During the MC degradation, Al2O3 strongly anchors PFOA through COO––Al coordination and in situ formed from Lewis-base interaction and PS through hydrogen bond. Meanwhile, mechanical effects induce the homolytic cleavage of PS to produce SO4•–, which reacts with OH group of Al2O3 to generate •OH. The degradation of PFOA is initiated by decarboxylation as a result of weakened C–COO– due to Al3+ coordination. The subsequent addition of •OH, elimination of HF, and reaction with water induce the stepwise removal of all carboxyl groups and F atoms as CO2 and F–, respectively. Thus, complete defluorination and mineralization are achieved.
中文翻译：
使用氧化铝和过硫酸盐的机械化学方法将全氟辛酸完全脱氟和矿化
全氟辛酸（PFOA）是一种持久性有机污染物，由于其对常规降解的极强抵抗力而受到全世界的关注。通过使用氧化铝（Al 2 O 3）和过硫酸钾（PS）作为混合剂，开发了一种机械化学（MC）方法来完全降解PFOA 。球磨2小时后，使用Al 2 O 3或PS进行MC处理会导致PFOA转化为1-H-1-全氟庚烯或二聚体，其脱氟效率低于20％，但同时使用Al 2 O 3和PS导致PFOA降解，脱氟率为100％，矿化度为98％。该方法还导致PFOA的其他C3-C6同系物完全脱氟。PFOA的完全脱氟归因于Al 2 O 3和PS分别导致PFOA中的CF键减弱和羟基自由基（•OH）的产生。在MC降解期间，Al 2 O 3通过COO – –Al配位牢固地固定了PFOA，并通过路易斯碱相互作用和PS通过氢键原位形成。同时，机械作用引起PS的均质裂解，生成SO 4 •–，与Al 2 O 3的OH基反应生成•OH。PFOA的降解是由于C–COO减弱（由于Al 3+配位作用）而由脱羧作用引发的。随后加入•OH，消除HF并与水反应，导致逐步除去所有羧基和F原子，分别为CO 2和F –。因此，实现了完全的脱氟和矿化。
更新日期：2019-06-13
中文翻译：
使用氧化铝和过硫酸盐的机械化学方法将全氟辛酸完全脱氟和矿化
全氟辛酸（PFOA）是一种持久性有机污染物，由于其对常规降解的极强抵抗力而受到全世界的关注。通过使用氧化铝（Al 2 O 3）和过硫酸钾（PS）作为混合剂，开发了一种机械化学（MC）方法来完全降解PFOA 。球磨2小时后，使用Al 2 O 3或PS进行MC处理会导致PFOA转化为1-H-1-全氟庚烯或二聚体，其脱氟效率低于20％，但同时使用Al 2 O 3和PS导致PFOA降解，脱氟率为100％，矿化度为98％。该方法还导致PFOA的其他C3-C6同系物完全脱氟。PFOA的完全脱氟归因于Al 2 O 3和PS分别导致PFOA中的CF键减弱和羟基自由基（•OH）的产生。在MC降解期间，Al 2 O 3通过COO – –Al配位牢固地固定了PFOA，并通过路易斯碱相互作用和PS通过氢键原位形成。同时，机械作用引起PS的均质裂解，生成SO 4 •–，与Al 2 O 3的OH基反应生成•OH。PFOA的降解是由于C–COO减弱（由于Al 3+配位作用）而由脱羧作用引发的。随后加入•OH，消除HF并与水反应，导致逐步除去所有羧基和F原子，分别为CO 2和F –。因此，实现了完全的脱氟和矿化。
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