过渡金属辅酶催化降解全氟己磺酸的仿生体系优化

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Abstract Biomimetic systems containing transition-metal coenzymes as catalyst have been optimized for simultaneous degradation and defluorination of both linear- (L-PFHxS) and branched-perfluorohexanesulfonate (Br-PFHxS). Vitamin B₁₂ (VB₁₂) catalyzed the reductive degradation and defluorination of both L-PFHxS and Br-PFHxS, whereas hematin did not. For cofactor 430 (F430), biomimetic degradation and defluorination was only found for Br-PFOS but not for L-PFHxS. However, the removal rate and defluorination rate of technical PFHxS catalyzed by VB₁₂ were both much higher than that catalyzed by F430. Biomimetic degradation of technical PFHxS catalyzed by VB₁₂as well as F430 could well be described by a first-order exponential decay model, indicating that the spiked PFHxS could initially distribute between two completely separate pools with independent degradability, i.e. non-degradable and degradable fractions. The axial ligands of VB₁₂ could impact their catalytic defluorination of PFHxS, and the highest defluorination rate was achieved by adenosylcobalamin. Nanoscale zero-valent zinc (nZn⁰) is the best electron-donor for the biomimetic system under the experimental conditions. At 60℃ and pH = 9.0, the removal rate and defluorination rate of technical PFHxS were as high as 57.1%±2.9% and 8.19%±0.65%, respectively, with cyanocobalamin as biomimetic catalyst and nZn⁰as electron-donor, and then the degradable fraction accounted for about 54.6% and its depletion rate was 1.01d^-1.

Key words： PFHxS transition-metal coenzymes electron-donors biomimetic degradation defluorination

Received: 06 February 2024

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X703

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	ZENG Yu-yuan
	CHEN Ling-xin
	YANG Zhi-min
	LIU Shu-po
	ZHOU Zhen-ming
	ZOU Jing
	LI Fei

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ZENG Yu-yuan,CHEN Ling-xin,YANG Zhi-min等. Catalytic degradation of perfluorohexanesulfonate by transition-metal coenzymes: Optimization of the biomimetic systems[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(10): 5576-5583.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I10/5576

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