Water-Soluble Iron Porphyrins as Catalysts for Suppressing Chlorinated Disinfection Byproducts in Hypochlorite-Dependent Water Remediation.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2024-12-27 DOI:10.1002/cssc.202402171
Silène Engbers, Maja J Lind, Mathias L Skavenborg, Johannes E M N Klein, Frants R Lauritsen, Christine J McKenzie
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Abstract

We are facing a world-wide shortage of clean drinking water which will only be further exacerbated by climate change. The development of reliable and affordable methods for water remediation is thus of utmost importance. Chlorine (which forms active hypochlorites in solution) is the most commonly used disinfectant due to its reliability and low cost. One drawback is that it reacts with organic pollutants to generate toxic chlorinated byproducts. To mitigate chlorination in water remediation, we have investigated the use of catalytic amounts of charged water-soluble iron porphyrins. These are known to activate hypochlorite to generate high valent oxoiron species. We studied the depletion of the model micropollutant phenol and the accumulation of chlorinated disinfection byproducts under water remediation conditions, using iron porphyrins [(TMPyP)FeCl]Cl4 and (NH4)4[(TPPS)FeCl] as catalysts, by membrane inlet mass spectrometry. Despite bearing opposite charges on the meso-substituent, both iron porphyrins suppress the formation of chlorinated disinfection by-products equally well. To gain further insight, spectroscopic studies were performed. These showed the transient formation of Compound II, followed by either regeneration of the iron(III) porphyrin at low NaOCl concentrations, or total decomposition of the porphyrin complex at high NaOCl concentrations. Potential future directions for modifications of porphyrin-based catalysts are discussed.

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水溶性铁卟啉作为抑制次氯酸盐依赖水修复中氯化消毒副产物的催化剂。
我们正面临着世界范围内清洁饮用水的短缺,气候变化只会进一步加剧这种短缺。因此,开发可靠和负担得起的水修复方法至关重要。氯(在溶液中形成活性次氯酸盐)因其可靠性和低成本而成为最常用的消毒剂。缺点之一是它会与有机污染物发生反应,产生有毒的氯化副产物。为了减轻水修复中的氯化作用,我们研究了带电水溶性铁卟啉的催化用量。已知这些物质可以激活次氯酸盐,产生高价氧化铁。采用膜入口质谱法,以铁卟啉[(TMPyP)FeCl]Cl4和(NH4)4[(TPPS)FeCl]为催化剂,研究了水修复条件下模型微污染物苯酚的耗竭和氯化消毒副产物的积累。尽管在中取代基上带有相反的电荷,但两种铁卟啉都能很好地抑制氯化消毒副产物的形成。为了进一步了解,进行了光谱研究。这些结果表明,化合物II的形成是短暂的,随后是铁(III)卟啉在低NaOCl浓度下的再生,或在高NaOCl浓度下卟啉复合物的完全分解。讨论了卟啉基催化剂的潜在改性方向。
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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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