开发新的高锰酸盐/亚氯酸盐水净化工艺。

IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2024-09-17 Epub Date: 2024-09-01 DOI:10.1021/acs.est.4c02257
Liping Luo, Min Zheng, Erdeng Du, Jingquan Wang, Xiaohong Guan, Hongguang Guo
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摘要

开发对目标污染物具有强选择性、对水基质具有低敏感性的新技术仍具有挑战性。在这里,我们介绍了一种新策略,即在 pH 值为 4.8 时使用亚氯酸盐作为 Mn(VII)的活化剂,将污染物对 Mn(VII)的惰性反应转变为强反应。这为引发水污染反应开辟了一条新路。我们以磺胺甲噁唑(SMX)为典型污染物,提出了电子跨氢键转移(TEHB)和活性锰氧化的耦合途径。结果表明,在氢键转移途径中,最初是通过亚氯酸盐与 SMX 的氨基结合形成氢键复合物 SMX-ClO2-*;这种复合物对锰(VII)具有更强的还原能力。然后,氢键络合物 SMX-ClO2-* 中的亚氯酸盐可与锰(VII)络合。因此,形成了一个新的反应中心(SMX-ClO2--Mn(VII)*),启动了氢键间的电子转移和 SMX 的初步降解。随后,生成的 Mn(V)-ClO2-/Mn(III) 参与了 Mn(VII) 的还原过程。这一过程显示出与 pH 值相关的降解,当 pH 值从 4.8 升至 7 时,去除率从 80% 到接近停滞。结合 pKa 分析表明,污染物的主要形式对于锰(VII)/亚氯酸盐工艺去除污染物的效率至关重要。水基质的影响被证明几乎没有不利甚至有利的影响。这项研究引入了一种新的 Mn(VII)协同策略和一种新的反应模式,重点是降低污染物的还原电位,而不是提高氧化剂的氧化电位,因此对多种污染物的去除效果令人满意。
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Development of a New Permanganate/Chlorite Process for Water Decontamination.

Development of new technologies with strong selectivity for target pollutants and low sensitivity toward a water matrix remains challenging. Herein, we introduced a novel strategy that used chlorite as an activator for Mn(VII) at pH 4.8, turning the inert reactivity of the pollutants toward Mn(VII) into a strong reactivity. This paved a new way for triggering reactions in water decontamination. By utilizing sulfamethoxazole (SMX) as a typical pollutant, we proposed coupled pathways involving electron transfer across hydrogen bonds (TEHB) and oxidation by reactive manganese species. The results indicated that a hydrogen bonding complex, SMX-ClO2-*, formed through chlorite binding the amino group of SMX initially in the TEHB route; such a complex exhibited a stronger reduction capability toward Mn(VII). Chlorite, in the hydrogen bonding complex SMX-ClO2-*, can then complex with Mn(VII). Consequently, a new reactive center (SMX-ClO2--Mn(VII)*) was formed, initiating the transfer of electrons across hydrogen bonds and the preliminary degradation of SMX. This is followed by the involvement of the generated Mn(V)-ClO2-/Mn(III) in the reduction process of Mn(VII). Such a process showed pH-dependent degradation, with a removal ratio ranging from 80% to near-stagnation as pH increased from 4.8 to 7. Combining with pKa analysis showed that the predominant forms of contaminants were crucial for the removal efficiency of pollutants by the Mn(VII)/chlorite process. The impact of the water matrix was demonstrated to have few adverse or even beneficial effects. With satisfactory performance against numerous contaminants, this study introduced a novel Mn(VII) synergistic strategy, and a new reactivity pattern focused on reducing the reduction potential of the contaminant, as opposed to increasing the oxidation potential of oxidants.

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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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