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饮用水及水源中的纳米银:稳定性及其对消毒副产物形成的影响

Nano-silver in drinking water and drinking water sources: stability and influences on disinfection by-product formation.

作者信息

Tugulea A-M, Bérubé D, Giddings M, Lemieux F, Hnatiw J, Priem J, Avramescu M-L

机构信息

Health Canada, Ottawa, Canada,

出版信息

Environ Sci Pollut Res Int. 2014 Oct;21(20):11823-31. doi: 10.1007/s11356-014-2508-5. Epub 2014 Jan 24.

DOI:10.1007/s11356-014-2508-5
PMID:24458938
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC4177100/
Abstract

Nano-silver is increasingly used in consumer products from washing machines and refrigerators to devices marketed for the disinfection of drinking water or recreational water. The nano-silver in these products may be released, ending up in surface water bodies which may be used as drinking water sources. Little information is available about the stability of the nano-silver in sources of drinking water, its fate during drinking water disinfection processes, and its interaction with disinfection agents and disinfection by-products (DBPs). This study aims to investigate the stability of nano-silver in drinking water sources and in the finished drinking water when chlorine and chloramines are used for disinfection and to observe changes in the composition of DBPs formed when nano-silver is present in the source water. A dispersion of nano-silver particles (10 nm; PVP-coated) was used to spike untreated Ottawa River water, treated Ottawa River water, organic-free water, and a groundwater at concentrations of 5 mg/L. The diluted dispersions were kept under stirred and non-stirred conditions for up to 9 months and analyzed weekly using UV absorption to assess the stability of the nano-silver particles. In a separate experiment, Ottawa River water containing nano-silver particles (at 0.1 and 1 mg/L concentration, respectively) was disinfected by adding sodium hypochlorite (a chlorinating agent) in sufficient amounts to maintain a free chlorine residual of approximately 0.4 mg/L after 24 h. The disinfected drinking water was then quenched with ascorbic acid and analyzed for 34 neutral DBPs (trihalomethanes, haloacetonitriles, haloacetaldehydes, 1,1 dichloro-2-propanone, 1,1,1 trichloro-2-propanone, chloropicrin, and cyanogen chloride). The results were compared to the profile of DBPs obtained under the same conditions in the absence of nano-silver and in the presence of an equivalent concentration of Ag(+) ions (as AgNO3). The stability of the nano-silver dispersions in untreated Ottawa River water, with a dissolved organic carbon concentration of 6 mg/L, was significantly higher than the stability of the nano-silver dispersions in distilled, organic-free water. Nano-silver particles suspended in the groundwater agglomerated and were quickly and quantitatively removed from the solution. Our data confirm previous observations that natural dissolved organic matter stabilizes nano-silver particles, while the high-ionic strength of groundwater appears to favor their agglomeration and precipitation. As expected, nano-silver was not stable in Ottawa River water through the chlorination process, but survived for many days when added to the Ottawa River water after treatment with chlorine or chloramines. Stirring appeared to have minimal effect on nano-silver stability in untreated and treated Ottawa River water. The profile of DBPs formed in the presence of nAg differed significantly from the profile of DBPs formed in the absence of nAg only at the 1 mg/L nAg concentration. The differences observed consisted mainly in reduced formation of some brominated DBPs and a small increase in the formation of cyanogen chloride. The reduced formation of brominated congeners may be explained by the decrease in available bromide due to the presence of Ag(+) ions. It should be noted that a concentration of 1 mg/L is significantly higher than nAg concentrations that would be expected to be present in surface waters, but these results could be significant for the disinfection of some wastewaters with comparably high nano-silver concentrations.

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/c09ab3c5ad1a/11356_2014_2508_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/6cb35b2f64e3/11356_2014_2508_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/fcd9995387dc/11356_2014_2508_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/e43d8e8e856e/11356_2014_2508_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/ef56661256bf/11356_2014_2508_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/fe19f005d881/11356_2014_2508_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/ccd5622aa4a1/11356_2014_2508_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/f168cf9a6f4e/11356_2014_2508_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/c09ab3c5ad1a/11356_2014_2508_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/6cb35b2f64e3/11356_2014_2508_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/fcd9995387dc/11356_2014_2508_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/e43d8e8e856e/11356_2014_2508_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/ef56661256bf/11356_2014_2508_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/fe19f005d881/11356_2014_2508_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/ccd5622aa4a1/11356_2014_2508_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/f168cf9a6f4e/11356_2014_2508_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3fe/4177100/c09ab3c5ad1a/11356_2014_2508_Fig8_HTML.jpg
摘要

纳米银越来越多地用于从洗衣机、冰箱到用于饮用水或娱乐用水消毒的设备等消费产品中。这些产品中的纳米银可能会释放出来,最终进入可能用作饮用水源的地表水体。关于纳米银在饮用水源中的稳定性、其在饮用水消毒过程中的去向以及它与消毒剂和消毒副产物(DBPs)的相互作用,目前所知甚少。本研究旨在调查当使用氯和氯胺进行消毒时,纳米银在饮用水源和成品饮用水中的稳定性,并观察当水源水中存在纳米银时形成的消毒副产物组成的变化。使用纳米银颗粒(10纳米;聚乙烯吡咯烷酮包覆)的分散液,以5毫克/升的浓度加入未处理的渥太华河水、处理过的渥太华河水、无有机物水和地下水中。稀释后的分散液分别在搅拌和不搅拌条件下保存长达9个月,并每周使用紫外吸收进行分析,以评估纳米银颗粒的稳定性。在另一个实验中,通过加入足量的次氯酸钠(一种氯化剂)对含有纳米银颗粒(浓度分别为0.1毫克/升和1毫克/升)的渥太华河水进行消毒,以使24小时后游离氯残留量维持在约0.4毫克/升。然后用抗坏血酸淬灭消毒后的饮用水,并分析其中34种中性消毒副产物(三卤甲烷、卤乙腈、卤代醛、1,1-二氯-2-丙酮、1,1,1-三氯-2-丙酮、氯化苦和氯化氰)。将结果与在相同条件下不存在纳米银以及存在等量浓度的银离子(以硝酸银形式)时获得的消毒副产物谱进行比较。在溶解有机碳浓度为6毫克/升的未处理渥太华河水中,纳米银分散液的稳定性显著高于蒸馏的无有机物水中纳米银分散液的稳定性。悬浮在地下水中的纳米银颗粒会凝聚,并迅速且定量地从溶液中去除。我们的数据证实了之前的观察结果,即天然溶解有机物会使纳米银颗粒稳定,而地下水的高离子强度似乎有利于它们的凝聚和沉淀。正如预期的那样,纳米银在渥太华河水中经过氯化过程不稳定,但在经过氯或氯胺处理后的渥太华河水中添加时能存活许多天。搅拌对未处理和处理后的渥太华河水中纳米银稳定性的影响似乎最小。仅在1毫克/升纳米银浓度下,存在纳米银时形成的消毒副产物谱与不存在纳米银时形成的消毒副产物谱有显著差异。观察到的差异主要在于一些溴化消毒副产物的形成减少以及氯化氰的形成略有增加。溴化同系物形成减少可能是由于银离子的存在导致可用溴化物减少。应当指出,1毫克/升的浓度显著高于预期在地表水中存在的纳米银浓度,但这些结果对于某些纳米银浓度较高的废水消毒可能具有重要意义。

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