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利用非热等离子体与金属氧化物吸附耦合去除饮用水中低浓度正丁醇

Removal and Oxidation of Low Concentration -Butanol from Potable Water using Nonthermal Plasma Coupled with Metal Oxide Adsorption.

作者信息

Stere Cristina E, Delarmelina Maicon, Dlamini Mbongiseni W, Chansai Sarayute, Davies Philip R, Hutchings Graham J, Catlow C Richard A, Hardacre Christopher

机构信息

Department of Chemical Engineering, University of Manchester, Oxford Road, Manchester M13 9PL, U.K.

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, U.K.

出版信息

ACS ES T Eng. 2024 Aug 20;4(9):2121-2134. doi: 10.1021/acsestengg.4c00166. eCollection 2024 Sep 13.

Abstract

Taste and odor are crucial factors in evaluating the quality of drinking water for consumers. Geosmin is an example of a pollutant commonly found in potable water responsible for earthy and musty taste, and odor even at low concentrations. We have investigated the use of a hybrid two-step adsorption-mineralization process for low-level volatile organic compounds removal from potable water using dielectric barrier discharge over common metal oxides (MO). The system proposed is a proof of principle with -butanol (TBA) used as a model compound for geosmin removal/degradation during wastewater treatment when combined with an appropriate metal oxide adsorbent. Initial assessments of the adsorption properties of titania by density functional theory (DFT) calculations and experimental tests indicated that the adsorption of geosmin and TBA with water present results in only weak interactions between the sorbate and the metal oxide. In contrast, the DFT results show that alumina could be a suitable adsorbent for these tertiary alcohols and were reinforced by experimental studies. We find that while there is a competitive effect between the water and TBA adsorption from gaseous/liquid feed, the VOC can be removed, and the alumina will be regenerated by the reactive oxygen species (ROS) produced by a dielectric barrier discharge (DBD). The use of alumina in conjunction with NTP leads to efficient degradation of the adsorbate and the formation of oxygenated intermediates (formates, carbonates, and carboxylate-type species), which could then be mineralized for the regeneration of the adsorbent. A reaction mechanism has been proposed based on the infrared measurements and DFT calculations, while the removal of TBA with conventional heating is indicative of a gradual desorption process as a function of temperature rather than the destruction of the adsorbate. Furthermore, steady performance was observed after several adsorption-regeneration cycles, indicating no alteration of the adsorption properties of alumina during the NTP treatment and demonstrating the potential of the approach to be applied in the treatment of high throughput of water, without the challenges faced by the biocatalysts or formation of toxic byproducts.

摘要

味道和气味是评估饮用水对消费者质量的关键因素。土臭素是一种常见于饮用水中的污染物,即使在低浓度下也会导致泥土味和霉味以及气味。我们研究了使用混合两步吸附 - 矿化工艺,通过在普通金属氧化物(MO)上进行介质阻挡放电,从饮用水中去除低水平挥发性有机化合物。所提出的系统是一种原理验证,当与合适的金属氧化物吸附剂结合时,使用叔丁醇(TBA)作为废水处理过程中土臭素去除/降解的模型化合物。通过密度泛函理论(DFT)计算和实验测试对二氧化钛吸附性能的初步评估表明,在有水存在的情况下土臭素和TBA的吸附导致吸附质与金属氧化物之间只有微弱的相互作用。相比之下,DFT结果表明氧化铝可能是这些叔醇合适的吸附剂,并且实验研究进一步证实了这一点。我们发现,虽然从气态/液态进料中吸附水和TBA之间存在竞争效应,但挥发性有机化合物(VOC)可以被去除,并且氧化铝将通过介质阻挡放电(DBD)产生的活性氧物种(ROS)进行再生。将氧化铝与非热等离子体(NTP)结合使用可导致吸附质的有效降解并形成氧化中间体(甲酸盐、碳酸盐和羧酸盐类物质),然后这些中间体可以被矿化以实现吸附剂的再生。基于红外测量和DFT计算提出了一种反应机理,而用传统加热去除TBA表明这是一个随温度变化的逐渐解吸过程,而不是吸附质的破坏。此外,在几个吸附 - 再生循环后观察到稳定的性能,表明在NTP处理过程中氧化铝的吸附性能没有改变,并证明了该方法应用于处理高通量水的潜力,而不存在生物催化剂面临的挑战或有毒副产物的形成。

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