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采用巯基化石墨烯/Fe-Mn 复合材料在固定床柱中从模拟地下水中高效去除汞:实验性能和数学建模。

Efficient removal of mercury from simulated groundwater using thiol-modified graphene oxide/Fe-Mn composite in fixed-bed columns: Experimental performance and mathematical modeling.

机构信息

Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, Guangzhou 511443, China.

Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, Guangzhou 511443, China.

出版信息

Sci Total Environ. 2020 Apr 20;714:136636. doi: 10.1016/j.scitotenv.2020.136636. Epub 2020 Jan 17.

DOI:10.1016/j.scitotenv.2020.136636
PMID:31991272
Abstract

Mercury contamination in groundwater has been considered as an environmental and public health issue all over the world. Yet, effective in situ remediation techniques have been lacking. A thiol-modified graphene oxide/Fe-Mn composite (SGO/Fe-Mn) was employed as a reactive sorbent of permeable reactive barrier (PRB) for in situ remediation of mercury contaminated groundwater using fixed-bed columns. Mercury existed as HgCl, Hg(OH), and HgClOH, and was mainly removed through surface complexation. The Brunauer-Emmett-Teller sorption isotherm model provided adequate fitting of the sorption isotherm data with a maximum monolayer sorption capacity of 112.03 ± 16.59 mg g. Breakthrough time, the time when 5% of initial Hg concentration is measured in the effluent, increased with the decrease of influent mercury concentration, pore velocity, dissolved oxygen (DO), and dissolved organic matter (DOM). The resultant column sorption capacity was enhanced at higher influent mercury concentration, lower groundwater pore velocity, lower DOM and DO. Moreover, when the SGO/Fe-Mn was thoroughly mixed with quartz sand in the column, the breakthrough time was increased and the resultant sorption capacity was improved compared to the case that SGO/Fe-Mn was packed between two layers of quartz sand. Mathematically, the Adams-Bohart model satisfactorily reproduced the initial behavior of mercury breakthrough curves (<40 pore volumes). Yan model adequately simulated the breakthrough curves. The results reveal the potential of SGO/Fe-Mn as an efficient PRB reactive material for in situ remediation of mercury in contaminated groundwater.

摘要

地下水汞污染已被认为是一个全球性的环境和公共健康问题。然而,有效的原位修复技术仍然缺乏。本研究采用巯基改性氧化石墨烯/Fe-Mn 复合材料(SGO/Fe-Mn)作为可渗透反应屏障(PRB)的反应性吸附剂,通过固定床柱原位修复受汞污染的地下水。汞主要以 HgCl、Hg(OH) 和 HgClOH 的形式存在,主要通过表面络合去除。Brunauer-Emmett-Teller 吸附等温线模型对吸附等温线数据进行了充分拟合,最大单层吸附容量为 112.03±16.59mg/g。穿透时间,即流出物中初始 Hg 浓度的 5%被测量的时间,随着进水汞浓度、孔速、溶解氧(DO)和溶解有机物(DOM)的降低而增加。在较高的进水汞浓度、较低的地下水孔速、较低的 DOM 和 DO 条件下,柱吸附容量得到增强。此外,当 SGO/Fe-Mn 在柱中与石英砂充分混合时,与 SGO/Fe-Mn 填充在两层石英砂之间的情况相比,穿透时间增加,吸附容量提高。从数学上看,Adams-Bohart 模型很好地再现了汞穿透曲线的初始行为(<40 个孔隙体积)。Yan 模型很好地模拟了穿透曲线。结果表明,SGO/Fe-Mn 作为一种有效的 PRB 反应性材料,具有原位修复受污染地下水中汞的潜力。

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