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Efficient Reductive Defluorination of Branched PFOS by Metal–Porphyrin Complexes
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-06-02 , DOI: 10.1021/acs.est.1c08254 Jun Sun 1 , Sreenu Jennepalli 2 , Matthew Lee 3 , Adele Jones 3 , Denis M O'Carroll 3 , Michael J Manefield 3 , Mohan Bhadbhade 4 , Björn Åkermark 5 , Biswanath Das 5 , Naresh Kumar 1
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-06-02 , DOI: 10.1021/acs.est.1c08254 Jun Sun 1 , Sreenu Jennepalli 2 , Matthew Lee 3 , Adele Jones 3 , Denis M O'Carroll 3 , Michael J Manefield 3 , Mohan Bhadbhade 4 , Björn Åkermark 5 , Biswanath Das 5 , Naresh Kumar 1
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Vitamin B12 (VB12) has been reported to degrade PFOS in the presence of TiIII citrate at 70 °C. Porphyrin-based catalysts have emerged as VB12 analogues and have been successfully used in various fields of research due to their interesting structural and electronic properties. However, there is inadequate information on the use of these porphyrin-based metal complexes in the defluorination of PFOS. We have therefore explored a series of porphyrin-based metal complexes for the degradation of PFOS. CoII–5,10,15,20-tetraphenyl-21H,23H-porphyrin (CoII–TPP), CoII–5,10,15,20-tetrakis(4-methoxyphenyl)-21H,23H-porphyrin (CoII–M-TPP), and CoIII–M-TPP exhibited efficient reductive defluorination of the branched PFOS. Within 5–8 h, these compounds achieved the same level of PFOS defluorination as VB12 achieved in 7–10 days. For branched isomers, the specific removal rate of the CoII–TPP–TiIII citrate system is 64–105 times higher than that for VB12–TiIII citrate. Moreover, the CoII–TPP–TiIII citrate system displayed efficient (51%) defluorination for the branched PFOS (br-PFOS) in 1 day even at room temperature (25 °C). The effects of the iron and cobalt metal centers, reaction pH, and several reductants (NaBH4, nanosized zerovalent zinc (nZn0), and TiIII citrate) were systematically investigated. Based on the analysis of the products and previously published reports, a new possible defluorination pathway of branched PFOS is also proposed.
中文翻译：
金属-卟啉配合物对支链全氟辛烷磺酸的高效还原脱氟
据报道，维生素 B 12 (VB 12 )在 70 °C 的柠檬酸钛III存在下可降解 PFOS。基于卟啉的催化剂已作为 VB 12类似物出现，并且由于其有趣的结构和电子特性而已成功用于各个研究领域。然而，关于在全氟辛烷磺酸脱氟中使用这些卟啉基金属配合物的信息不足。因此，我们探索了一系列基于卟啉的金属配合物来降解 PFOS。Co II –5,10,15,20-四苯基-21 H ,23 H-卟啉 (Co II –TPP), Co II –5,10,15,20-四(4-甲氧基苯基)-21H ,23 H-卟啉 (Co II –M-TPP) 和 Co III –M-TPP 表现出对支链 PFOS 的有效还原脱氟。在 5-8 小时内，这些化合物的 PFOS 脱氟水平与 VB 12在 7-10 天内达到的水平相同。对于支链异构体，Co II -TPP-Ti III柠檬酸盐体系的比去除率是 VB 12 -Ti III柠檬酸盐的 64-105 倍。此外，Co II –TPP–Ti III即使在室温 (25 °C) 下，柠檬酸盐系统也能在 1 天内对支链 PFOS (br-PFOS) 进行有效的 (51%) 脱氟。系统地研究了铁和钴金属中心、反应 pH 值和几种还原剂（NaBH 4、纳米级零价锌 (nZn 0 ) 和 Ti III柠檬酸盐）的影响。基于对产品的分析和先前发表的报告，还提出了一种可能的支链 PFOS 新的脱氟途径。
更新日期：2022-06-02
中文翻译：
金属-卟啉配合物对支链全氟辛烷磺酸的高效还原脱氟
据报道，维生素 B 12 (VB 12 )在 70 °C 的柠檬酸钛III存在下可降解 PFOS。基于卟啉的催化剂已作为 VB 12类似物出现，并且由于其有趣的结构和电子特性而已成功用于各个研究领域。然而，关于在全氟辛烷磺酸脱氟中使用这些卟啉基金属配合物的信息不足。因此，我们探索了一系列基于卟啉的金属配合物来降解 PFOS。Co II –5,10,15,20-四苯基-21 H ,23 H-卟啉 (Co II –TPP), Co II –5,10,15,20-四(4-甲氧基苯基)-21H ,23 H-卟啉 (Co II –M-TPP) 和 Co III –M-TPP 表现出对支链 PFOS 的有效还原脱氟。在 5-8 小时内，这些化合物的 PFOS 脱氟水平与 VB 12在 7-10 天内达到的水平相同。对于支链异构体，Co II -TPP-Ti III柠檬酸盐体系的比去除率是 VB 12 -Ti III柠檬酸盐的 64-105 倍。此外，Co II –TPP–Ti III即使在室温 (25 °C) 下，柠檬酸盐系统也能在 1 天内对支链 PFOS (br-PFOS) 进行有效的 (51%) 脱氟。系统地研究了铁和钴金属中心、反应 pH 值和几种还原剂（NaBH 4、纳米级零价锌 (nZn 0 ) 和 Ti III柠檬酸盐）的影响。基于对产品的分析和先前发表的报告，还提出了一种可能的支链 PFOS 新的脱氟途径。
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