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芬顿预处理减轻垃圾渗滤液膜浓缩液处理过程中的膜蒸馏结垢:性能和机制。

Fenton pretreatment to mitigate membrane distillation fouling during treatment of landfill leachate membrane concentrate: Performance and mechanism.

机构信息

State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China.

State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

Water Res. 2023 Oct 1;244:120517. doi: 10.1016/j.watres.2023.120517. Epub 2023 Aug 23.

Abstract

Membrane distillation (MD) is regarded as a promising technology for treatment of landfill leachate membrane concentrate (LLMC) due to its merits of low cost and high rejection of non-volatile components. However, the high concentration of pollutants in the wastewater will cause severe membrane fouling, resulting in costly cleaning and maintenance. In this study, Fenton pretreatment was applied to alleviate membrane fouling during MD treatment of LLMC. Compared to rapid flux decline of 88.2% at concentration factor (CF) of 3 for raw LLMC, MD flux only decreased by 17.4% at CF = 6 for treating acidic Fenton effluent without subsequent pH adjustment (Fe and HO concentration were 600 mg/L and 1457 mg/L, respectively). The pH neutralization of Fenton effluent or merely acidification of LLMC could not achieve such excellent fouling mitigation. It was concluded that both oxidation and acidification were critical and the collaboration mechanism was revealed to explain low membrane fouling. Firstly, Fenton oxidation removed organic contaminants, reduced the hydrophobicity of organic substances and increased the percentage of carboxylic group within LLMC. Thus, hydrophobic (HP) attraction was weakened but multivalent cation bridging became dominant fouling mechanism for neutral Fenton effluent. Then, acidification weakened multivalent cation bridging by inhibiting the deprotonation of carboxylic group, further mitigating membrane fouling. However, acidification of LLMC caused more severe organic fouling due to decrease in electrostatic (EL) repulsion. In addition to low membrane fouling, satisfactory total organic carbon (TOC) rejection rate of 96.23% was achieved during combined Fenton-MD process. This study demonstrated that Fenton pretreatment without pH neutralization could effectively alleviate MD fouling and elucidated the synergistic mechanism between oxidation and acidification for fouling mitigation.

摘要

膜蒸馏(MD)因其低成本和高截留非挥发性成分的优点,被认为是处理垃圾渗滤液膜浓缩液(LLMC)的一种很有前途的技术。然而,废水中污染物的高浓度会导致严重的膜污染,从而导致昂贵的清洗和维护。在本研究中,芬顿预处理被应用于缓解 MD 处理 LLMC 过程中的膜污染。与未经后续 pH 调整的原始 LLMC 在浓缩因子(CF)为 3 时快速通量下降 88.2%相比,处理酸性芬顿废水(Fe 和 HO 浓度分别为 600 mg/L 和 1457 mg/L)时 MD 通量仅在 CF = 6 时下降了 17.4%。芬顿废水的 pH 中和或 LLMC 的单纯酸化都不能达到如此优异的防污效果。研究结果表明,氧化和酸化都很关键,并揭示了协同作用机制来解释低膜污染。首先,芬顿氧化去除了有机污染物,降低了有机物质的疏水性,增加了 LLMC 中羧酸基团的比例。因此,疏水性(HP)吸引力减弱,但多价阳离子桥接成为中性芬顿废水的主要污染机制。然后,酸化通过抑制羧酸基团的去质子化来减弱多价阳离子桥接,进一步减轻膜污染。然而,由于羧酸基团的去质子化减少,LLMC 的酸化会导致更严重的有机污染,从而进一步加重膜污染。此外,在芬顿-MD 联合工艺中,还实现了令人满意的总有机碳(TOC)去除率 96.23%。本研究表明,无需 pH 中和的芬顿预处理可以有效地缓解 MD 污染,并阐明了氧化和酸化之间协同减轻污染的机制。

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