过渡金属辅酶催化降解全氟己磺酸的仿生体系优化

摘要
图/表
参考文献
相关文章 (8)

全文: PDF (734 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要优化了过渡金属辅酶仿生降解体系以实现直链(L-PFHxS)和支链全氟己磺酸(Br-PFHxS)的仿生降解和脱氟.结果表明,维生素B₁₂(VB₁₂)可同时仿生催化降解L-PFHxS和Br-PFHxS,辅助因子430(F430)仅可仿生降解Br-PFHxS,且降解效能远低于VB₁₂,而羟高铁血红素无法仿生降解PFHxS.VB₁₂和F430仿生降解PFHxS过程可采用指数衰减模型进行拟合,表明投加的PFHxS可分为两类,即可降解部分和不可降解部分.VB₁₂轴向配体可影响其仿生催化降解PFHxS效能,其中腺苷钴胺仿生催化PFHxS脱氟的效能最高.nZn⁰最适宜作为仿生降解体系的电子供体,在60℃和pH = 9.0的条件下PFHxS去除率和脱氟率分别高达57.1%±2.9%和8.19%±0.65%,且可降解PFHxS去除速率系数高达1.01d^-1.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	曾煜源
	陈铃心
	杨志敏
	刘淑坡
	周真明
	邹景
	李飞

关键词 ：全氟己磺酸, 过渡金属辅酶, 电子供体, 仿生降解, 脱氟

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

收稿日期: 2024-02-06

PACS:

X703

基金资助:国家自然科学基金资助项目(51878300);泉州市科技计划(2018C084R);华侨大学中青年教师科研提升计划(ZQN-YX602)

通讯作者: 李飞,教授,lfflxyz@hqu.edu.cn E-mail: lfflxyz@hqu.edu.cn

作者简介: 曾煜源(1999-),男,福建泉州人,华侨大学硕士研究生,主要研究方向为持久性有机污染物控制.214030580@qq.com.

引用本文:

曾煜源, 陈铃心, 杨志敏, 刘淑坡, 周真明, 邹景, 李飞. 过渡金属辅酶催化降解全氟己磺酸的仿生体系优化[J]. 中国环境科学, 2024, 44(10): 5576-5583. ZENG Yu-yuan, CHEN Ling-xin, YANG Zhi-min, LIU Shu-po, ZHOU Zhen-ming, ZOU Jing, LI Fei. Catalytic degradation of perfluorohexanesulfonate by transition-metal coenzymes: Optimization of the biomimetic systems. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(10): 5576-5583.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2024/V44/I10/5576

[1] Li D, Zhang J, Liu X, et al. Are PFBS, PFHxS, and 6:2FTSA more friendly to the soil environment compared to PFOS? A new insight based on ecotoxicity study in soil invertebrates (Eisenia fetida) [J]. Science of the Total Environment, 2023,904:166689.
[2] Nguyen M D, Sivaram A K, Megharaj M, et al. Investigation on removal of perfluorooctanoic acid (PFOA), perfluorooctane sulfonate (PFOS), perfluorohexane sulfonate (PFHxS) using water treatment sludge and biochar [J]. Chemosphere, 2023,338:139412.
[3] Lucas K, Gaines L G T, Paris Davila T, et al. Occupational exposure and serum levels of per- and polyfluoroalkyl substances (PFAS): A review [J]. American Journal of Industrial Medicine, 2023,66(5):379-392.
[4] Hallberg I, Persson S, Olovsson M, et al. Bovine oocyte exposure to perfluorohexane sulfonate (PFHxS) induces phenotypic, transcriptomic, and DNA methylation changes in resulting embryos in vitro [J]. Reproductive Toxicology, 2022,109:19-30.
[5] Yao W, Xu J, Tang W, et al. Developmental toxicity of perfluorohexane sulfonate at human relevant dose during pregnancy via disruption in placental lipid homeostasis [J]. Environment International, 2023,177:108014.
[6] Adyeni B S, Carlos U, Tatiana H M, et al. Perfluorohexane sulfonate (PFHxS) disturbs the estrous cycle, ovulation rate, oocyte cell communication and calcium homeostasis in mice [J]. Reproductive Biology, 2023,23(2):100768.
[7] Ulhaq Z S, Tse W K F. Perfluorohexanesulfonic acid (PFHxS) induces oxidative stress and causes developmental toxicities in zebrafish embryos [J]. Journal of Hazardous Materials, 2023,457:131722.
[8] Liu W, Wu J, He W, et al. A review on perfluoroalkyl acids studies: Environmental behaviors, toxic effects, and ecological and health risks [J]. Ecosystem health and sustainability, 2019,5(1):1-19.
[9] Zhong H, Liu W, Li N, et al. Assessment of perfluorohexane sulfonic acid (PFHxS)-related compounds degradation potential: Computational and experimental approaches [J]. Journal of Hazardous Materials, 2022,436:129240.
[10] Wang S, Yang Q, Chen F, et al. Photocatalytic degradation of perfluorooctanoic acid and perfluorooctane sulfonate in water: A critical review [J]. Chemical Engineering Journal, 2017,328:927-942.
[11] Ross I, Mcdonough J, Miles J, et al. A review of emerging technologies for remediation of PFASs [J]. Remediation Journal, 2018,28(2):101-126.
[12] Trojanowicz M, Bojanowska-Czajka A, Bartosiewicz I, et al. Advanced oxidation/reduction processes treatment for aqueous perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) — A review of recent advances [J]. Chemical Engineering Journal, 2018, 336:170-199.
[13] Cui J, Gao P, Deng Y. Destruction of per- and polyfluoroalkyl substances (PFAS) with advanced reduction processes (ARPs): A critical review [J]. Environmental Science & Technology, 2020,54(7): 3752-3766.
[14] Du Z, Deng S, Bei Y, et al. Adsorption behavior and mechanism of perfluorinated compounds on various adsorbents—A review [J]. Journal of Hazardous Materials, 2014,274:443-454.
[15] Grgas D, Petrina A, Atefanac T, et al. A review: Per- and polyfluoroalkyl substances—Biological degradation [J]. Toxics, 2023,11(5):446.
[16] 杨宁,李飞,杨志敏,等.维生素B₁₂催化纳米零价铁仿生降解全氟辛磺酸[J]. 中国环境科学, 2020,40(11):4770-4778. Yang N, Li F, Yang Z, et al. Biomimetic degradation of PFOS catalyzed by vitamin B₁₂using nanoscale zero-valent iron as reductants [J]. China Environmental Science, 2020,40(11):4770-4778.
[17] Glod G, Angst W, Holliger C, et al. Corrinoid-mediated reduction of tetrachloroethene, trichloroethene, and trichlorofluoroethene in homogeneous aqueous solution: Reaction kinetics and reaction mechanisms [J]. Environmental Science & Technology, 1997,31(1):253-260.
[18] Gantzer C J, Wackett L P. Reductive dechlorination catalyzed by bacterial transition-metal coenzymes [J]. Environmental Science and Technology, 1991,25(4):715-722.
[19] Assaf-Anld N, Hayes K F, M V T. Reductive dechlorination of carbon tetrachloride by cobalamin(II) in the presence of dithiothreitol: Mechanistic study, effect of redox potential and pH [J]. Environmental Science & Technology, 1994,28(2):246-252.
[20] Holliger C, Schraa G, Stupperich E, et al. Evidence for the involvement of corrinoids and factor F430in the reductive dechlorination of 1,2-dichloroethane by Methanosarcina barkeri [J]. Journal of bacteriology, 1992,174(13):4427-4434.
[21] Kim Y H, Carravay E R. Reductive dechlorination of PCE and TCE by vitamin B₁₂ and ZVMs [J]. Environmental Technology, 2002, 23(10):1135-1145.
[22] Park S, de Perre C, Lee L S. Alternate reductants with VB₁₂ to transform C8 and C6 perfluoroalkyl sulfonates: Limitations and insights into isomer-specific transformation rates, products and pathways [J]. Environmental Science & Technology, 2017,51(23):13869-13877.
[23] Ochoa-Herrera V, Sierra-Alvarez R, Somogyi A, et al. Reductive defluorination of perfluorooctane sulfonate [J]. Environmental Science & Technology, 2008,42(9):3260-3264.
[24] Li F, Yang N, Yang Z, et al. Biomimetic degradability of linear perfluorooctanesulfonate (L-PFOS): Degradation products and pathways [J]. Chemosphere, 2020,259:127502.
[25] Sun Z, Geng D, Zhang C, et al. Vitamin B₁₂ (Co^II) initiates the reductive defluorination of branched perfluorooctane sulfonate (br- PFOS) in the presence of sulfide [J]. Chemical Engineering Journal, 2021,423:130149.
[26] Sun J, Jennepalli S, Lee M, et al. Efficient reductive defluorination of branched PFOS by metal-porphyrin complexes [J]. Environmental Science & Technology, 2022,56(12):7830-7839.
[27] Lee Y, Chen Y, Chen M, et al. Reductive defluorination of perfluorooctanoic acid by titanium(III) citrate with vitamin B₁₂and copper nanoparticles [J]. Journal of Hazardous Materials, 2017,340:336-343.
[28] Liu J, Van Hoomissen D J, Liu T, et al. Reductive defluorination of branched per- and polyfluoroalkyl substances with cobalt complex catalysts [J]. Environmental Science & Technology Letters, 2018, 5(5):289-294.
[29] Schulz K, Silva M R, Klaper R. Distribution and effects of branched versus linear isomers of PFOA, PFOS, and PFHxS: A review of recent literature [J]. Science of the Total Environment, 2020,733:139186.
[30] Londhe K, Lee C, Mcdonough C A, et al. The need for testing isomer profiles of perfluoroalkyl substances to evaluate treatment processes [J]. Environmental Science & Technology, 2022,56(22):15207-15219.
[31] Ankel-Fuchs D, Jaenchen R, Gebhardt N A, et al. Functional relationship between protein-bound and free factor F430in Methanobacterium [J]. Archives of Microbiology, 1984,139:332-337.
[32] Torres F J, Ochoa-Herrera V, Blowers P, et al. Ab initio study of the structural, electronic, and thermodynamic properties of linear perfluorooctane sulfonate (PFOS) and its branched isomers [J]. Chemosphere, 2009,76(8):1143-1149.
[33] Van Hoomissen D J, Vyas S. Early events in the reductive dehalogenation of linear perfluoroalkyl substances [J]. Environmental Science & Technology Letters, 2019,6(6):365-371.
[34] Lexa D, Saveant J. The electrochemistry of vitamin B_I2 [J]. Account of Chemical Research, 1983,16(7):235-243.
[35] Shibata N, Sueyoshi Y, Higuchi Y, et al. Direct participation of a peripheral side chain of a corrin ring in coenzyme B₁₂ catalysis [J]. Angewandte Chemie, 2018,130(26):7956-7961.