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纳米零价铁催化过硫酸盐耦合羟基对PNP的协同降解作用

Synergistic degradation of PNP coupling HO with persulfate catalyzed by nano zero valent iron.

作者信息

Du Jiangkun, Wang Yang, Xu Tiantian, Zheng Han, Bao Jianguo

机构信息

School of Environmental Studies, China University of Geosciences Wuhan 430074 People's Republic of China

Hubei Provincial Key Laboratory of Mining Area Environmental Pollution Control and Remediation, Hubei Polytechnic University Huangshi People's Republic of China.

出版信息

RSC Adv. 2019 Jun 28;9(35):20323-20331. doi: 10.1039/c9ra02901j. eCollection 2019 Jun 25.

DOI:10.1039/c9ra02901j
PMID:35514697
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9065542/
Abstract

HO and persulfate (PDS) activated by iron are attracting much attention due to their strong oxidation capacity for the effective degradation of organic pollutants. However, they face problems such as requiring an acidic reaction pH and difficulty of Fe regeneration. In this study, the simultaneous activation of HO and persulfate by nanoscaled zero valent iron (nZVI) was investigated for the degradation of -nitrophenol (PNP). The nZVI/HO/PDS oxidation system exhibited significantly higher reactivity toward PNP degradation than the systems with a single oxidant. A synergistic effect was explored between HO and PDS during nZVI-mediated activation, and the molar ratio of HO/PDS was a key parameter in optimizing the performance of PNP degradation. The nZVI/HO/PDS system could function well in a wide pH range, and even 95% PNP was removed at an initial pH 10, thus markedly alleviating the pH limitations of Fenton-like processes. Both hydroxyl radicals and sulfate radicals could be identified during HO/PDS activation, in which H produced during PDS decomposition promoted HO activation. The increase of oxidant concentration could significantly enhance the PNP degradation, while the presence of HCO and HPO exerted great inhibition. Furthermore, five degradation intermediates of PNP were detected and its degradation pathways in the nZVI/HO/PDS system were presented. This study reveals that the simultaneous activation of HO and PDS by nZVI is a promising advanced oxidation tool as an alternative to typical Fenton processes for recalcitrant pollutant removal.

摘要

铁激活的羟基自由基(HO)和过硫酸盐(PDS)因其对有机污染物的有效降解具有强大的氧化能力而备受关注。然而,它们面临诸如需要酸性反应pH值以及铁再生困难等问题。在本研究中,研究了纳米零价铁(nZVI)同时激活HO和过硫酸盐以降解对硝基苯酚(PNP)的情况。nZVI/HO/PDS氧化体系对PNP降解的反应活性明显高于单一氧化剂体系。在nZVI介导的激活过程中,探讨了HO和PDS之间的协同效应,HO/PDS的摩尔比是优化PNP降解性能的关键参数。nZVI/HO/PDS体系可以在较宽的pH范围内良好运行,甚至在初始pH值为10时能去除95%的PNP,从而显著缓解了类芬顿过程的pH限制。在HO/PDS激活过程中可以识别出羟基自由基和硫酸根自由基,其中PDS分解过程中产生的H促进了HO的激活。氧化剂浓度的增加可以显著提高PNP的降解,而HCO和HPO的存在则产生了很大的抑制作用。此外,检测到了PNP的五种降解中间体,并给出了其在nZVI/HO/PDS体系中的降解途径。本研究表明,nZVI同时激活HO和PDS是一种有前景的高级氧化工具,可作为典型芬顿过程去除难降解污染物的替代方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/0da793819a36/c9ra02901j-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/bc92b890faa3/c9ra02901j-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/d01071395a36/c9ra02901j-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/2fc4aae4a358/c9ra02901j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/26c2a5841069/c9ra02901j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/f94283198571/c9ra02901j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/8569b7523af4/c9ra02901j-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/86f491b4a165/c9ra02901j-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/152cad3c3728/c9ra02901j-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/0da793819a36/c9ra02901j-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/bc92b890faa3/c9ra02901j-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/d01071395a36/c9ra02901j-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/2fc4aae4a358/c9ra02901j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/26c2a5841069/c9ra02901j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/f94283198571/c9ra02901j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/8569b7523af4/c9ra02901j-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/86f491b4a165/c9ra02901j-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/152cad3c3728/c9ra02901j-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/941a/9065542/0da793819a36/c9ra02901j-f9.jpg

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