Deep Insight of the Mechanism for Nitrate-Promoted PFASs Defluorination in UV/Sulfite ARP: Activation of the Decarboxylation–Hydroxylation–Elimination–Hydrolysis Degradation Pathway DOI

Zhuoran Feng,

Yili Fu, Jiahui Li

и другие.

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

The UV/sulfite advanced reduction process (ARP) holds promise for the removal of per- and polyfluoroalkyl substances (PFASs) by a hydrated electron (eaq-)-induced H/F exchange under anoxic conditions. Traditionally, presence coexisting nitrate in water has always been regarded as major inhibitory factor PFASs defluorination. However, this study observed an unexpected promotive effect on defluorination, challenging previous phenomenon. Notably, addition 100 μM resulted remarkable 54% enhancement PFOA A novel mechanism was discovered that nitrate-derived reactive nitrogen species (RNS) activated decarboxylation-hydroxylation-elimination-hydrolysis (DHEH) process, important degradation pathway ARP. Induced eaq-, PFAS molecule first became perfluorinated radical then transformed into unstable alcohol reacting with water. Due to high reactivity driven unpaired electrons RNS, molecules were destabilized H-O bond stretched from 0.98 1.04 Å. This effectively enhanced spontaneity reaction between consequently made whole DHEH more thermodynamic favorable (ΔG, -23.53 → -376.28 kJ/mol). Such breaks through view directly reacts eaq- affect defluorination ARP systems. finding offers innovative perspective optimizing strategically regulating levels bodies.

Язык: Английский

Deep Insight of the Mechanism for Nitrate-Promoted PFASs Defluorination in UV/Sulfite ARP: Activation of the Decarboxylation–Hydroxylation–Elimination–Hydrolysis Degradation Pathway DOI

Zhuoran Feng,

Yili Fu, Jiahui Li

и другие.

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

The UV/sulfite advanced reduction process (ARP) holds promise for the removal of per- and polyfluoroalkyl substances (PFASs) by a hydrated electron (eaq-)-induced H/F exchange under anoxic conditions. Traditionally, presence coexisting nitrate in water has always been regarded as major inhibitory factor PFASs defluorination. However, this study observed an unexpected promotive effect on defluorination, challenging previous phenomenon. Notably, addition 100 μM resulted remarkable 54% enhancement PFOA A novel mechanism was discovered that nitrate-derived reactive nitrogen species (RNS) activated decarboxylation-hydroxylation-elimination-hydrolysis (DHEH) process, important degradation pathway ARP. Induced eaq-, PFAS molecule first became perfluorinated radical then transformed into unstable alcohol reacting with water. Due to high reactivity driven unpaired electrons RNS, molecules were destabilized H-O bond stretched from 0.98 1.04 Å. This effectively enhanced spontaneity reaction between consequently made whole DHEH more thermodynamic favorable (ΔG, -23.53 → -376.28 kJ/mol). Such breaks through view directly reacts eaq- affect defluorination ARP systems. finding offers innovative perspective optimizing strategically regulating levels bodies.

Язык: Английский

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