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Selective oxidation of pharmaceuticals and suppression of perchlorate formation during electrolysis of fresh human urine
Water Research ( IF 11.4 ) Pub Date : 2021-04-08 , DOI: 10.1016/j.watres.2021.117106
James A. Clark , Yuhang Yang , Nathanael C. Ramos , Hugh W. Hillhouse

Urine comprises only a small (~1%) volumetric fraction of municipal wastewater, but represents a dominant source of pharmaceuticals, many of which may pass through conventional wastewater treatment and pose risks to aquatic ecosystems. Point-source treatment of source-separated urine presents a unique opportunity to degrade pharmaceuticals before dilution with wastewater, and electrochemical advanced oxidation processes are one increasingly investigated option. However, they often lead to the formation of oxidation byproducts including chlorate, perchlorate at very high concentrations. Here, we show that the high urea content of fresh human urine suppresses the formation of oxychlorides by inhibiting formation of HOCl/OCl during electrolysis, while still enabling pharmaceutical degradation due to the slow rate of urea oxidation by OH. This results in improved performance compared to equivalent treatment of hydrolyzed aged urine. This electrochemical oxidation scheme is shown to degrade the model contaminants cyclophosphamide and sulfamethoxazole with surface-area-to-volume-normalized pseudo-first-order rate constants greater than 0.08 cm/min in authentic fresh human urine. It results in ~100 × decrease in pharmaceutical concentrations in 2 h while generating ~1000 × lower oxychloride byproduct concentrations in synthetic fresh urine than synthetic hydrolyzed aged urine matrixes. Importantly, this proof-of-principle shows that simple and safe electrochemical methods can be used for point-source-remediation of pharmaceuticals in fresh human urine (before storage and hydrolysis), without formation of significant oxychloride byproducts.



中文翻译:

药物的选择性氧化和抑制新鲜尿液电解过程中高氯酸盐的形成

尿液仅占市政废水的一小部分(〜1%),但代表了主要的药物来源,其中许多药物可能会通过常规废水处理,并对水生生态系统构成风险。源头分离尿液的点源处理为在废水稀释之前降解药物提供了独特的机会,电化学高级氧化工艺已成为越来越多的研究选择。然而,它们经常导致形成氧化副产物,包括非常高浓度的氯酸盐,高氯酸盐。在这里,我们表明,鲜人尿的高尿素含量通过抑制次氯酸形成/ OCL的氯氧化抑制的形成-在电解过程中,由于尿素氧化的缓慢速度而使药物降解哦。与水解的老化尿液的同等处理相比,这可以提高性能。该电化学氧化方案显示出可以在真实的新鲜人类尿液中以大于0.08 cm / min的表面积对体积归一化的伪一级速率常数降解模型污染物环磷酰胺和磺胺甲恶唑。与合成水解的老化尿液基质相比,合成新鲜尿液中的药物浓度在2小时内降低了约100倍,而氯氧化副产物的浓度降低了约1000倍。重要的是,该原理证明表明,简单安全的电化学方法可用于新鲜人尿液中药物的点源修复(在储存和水解之前),而不会形成明显的氯氧化物副产物。

更新日期:2021-04-30
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