白洋淀和长江中游短链氯化石蜡的分布特征

发布时间：2018-08-16 11:04

【摘要】：短链氯化石蜡(SCCPs)是一类组成复杂,具有远距离迁移、环境持久性、生物蓄积性和一定的生物毒性,已被列入《关于持久性有机污染物的斯德哥尔摩公约》受控名单。我国是氯化石蜡生产和使用最多的国家,且尚未限制SCCPs的生产。短链氯化石蜡(short-chain chlorinated paraffins,SCCPs)是碳链长度为10-13,氯原子取代数为1-13个的正构烷烃衍生物。工业上短链氯化石蜡是由氯气与正构烷烃反应合成,因此生产出的短链氯化石蜡是由数以万计的同系物和同分异构体组成的混合物,氯代程度通常为30%~70%(以质量计算)。目前文献多采用气相色谱负化学源质谱法进行环境中短链氯化石蜡的测定,发现环境中短链氯化石蜡普遍存在。本文首先对SCCPs商业标准品的组成进行了测定分析,结果表明:氯含量63%C10-13 SCCPs标准品中,氯代的C10、C11、C12、C13的百分组成分别为10.1%、33.8%、33.1%、23%;Chloroparaffin C10 65.02%Cl中主要以7氯代和8氯代化合物为主,分别占34%和38%;Chloroparaffin C11 65.25%Cl主要以8氯代和9氯代化合物为主,分别占40%和32%;Chloroparaffin C1269.98%Cl中主要以9氯代和10氯代化合物为主,分别占37%和35%;Chloroparaffin C1365.18%Cl中主要以9氯代化合物为主,占50%左右。对我国白洋淀水和沉积物中的短链氯化石蜡进行分析研究结果表明:白洋淀水中SCCPs浓度范围为1562.8~56 305.9 ng/L,平均值为7223ng/L,中值为3168.9ng/L;沉积物中SCCPs的浓度范围在1270~254203ng/g(干重)之间,平均值为24454ng/g,中值为3458ng/g。经分析白洋淀水和沉积物中短链氯化石蜡的污染趋势基本一致。总的来说,白洋淀15个采样点的水和沉积物均有SCCPs的检出,检出率为100%,主要以碳链C10和C11的六氯和七氯的SCCPs为主要同类物。主成分分析结果表明:白洋淀沉积物中主要以C10H15Cl7、C10H15Cl7、C12H13Cl9、C13H14Cl8、C11H16Cl6、C12H16Cl6、C13H16Cl6为污染特征。和国内外相比白洋淀污染水平较高。长江流域是我国经济发展水平和城镇化水平较高的地区之一,随着经济的发展,大量的生活污水和工业废水排入长江,污染日趋严重,所以本文采集了长江中游的水和沉积物,并进行了SCCPs的污染特征研究。所有的采样点均有短链氯化石蜡检出,检出率为100%。测的水中SCCPs浓度范围在1131~65640ng/L之间,平均浓度为18989ng/L,中值为14691ng/L。沉积物浓度范围在251.9-397600.4ng/g(干重)之间,平均浓度为54512ng/g,中值浓度为2363.7ng/g。长江中上游的污染水平要低于长江中下游的污染水平,其中长江14、长江15、长江21以及长江5中的短链氯化石蜡含量较高,主要以链长C10和C13的六氯的SCCPs为主要同类物。沉积物的中值粒径和SCCPs的污染水平没有相关性;沉积物中有机质SCCPs的浓度呈正相关。过滤膜中短链氯化石蜡的浓度范围在1868ng/L~513335.9ng/L之间,平均值为64219ng/L,中值为8211ng/L。与国外相比污染水平较高。长江中游主成分主要来自六氯和十氯代的短链氯化石蜡。
[Abstract]:Short chain chlorinated paraffins (SCCPs) are a class of complex SCCPs with long distance transport, environmental persistence, bioaccumulation and certain biotoxicity, which have been included in the Stockholm Convention on persistent Organic pollutants (pops) controlled list. The production and use of chlorinated paraffin is the most in China, and the production of SCCPs has not been restricted. Short chain chlorinated paraffins (short-chain chlorinated paraffins SCCPs) are n-alkane derivatives with carbon chain length of 10-13 and chlorine atom substitution number of 1-13. Industrial SCCPs are synthesized by the reaction of chlorine gas with n-alkanes, so the SCCPs produced are a mixture of tens of thousands of homologues and isomers, and the chlorination degree is usually 30% (by mass). At present, gas chromatography negative chemical source mass spectrometry is used to determine SCCPs in the environment, and it is found that SCCPs are ubiquitous in the environment. In this paper, the composition of SCCPs commercial standard was determined and analyzed. The results showed that in the 630-13 SCCPs standard of chlorine content, the percentage composition of chlorinated C10C11C11C12C13 was 10.1% and 33.833.833.1%, respectively. In the 65.02%Cl of Chloroparaffin C10, it was mainly composed of 7 chlorinated compounds and 8 chlorinated compounds. Chloroparaffin C11 65.25%Cl was mainly composed of 8 chlorinated compounds and 9 chlorinated compounds, 40% and 32% Chloroparaffin C1269.98%Cl were mainly 9 chlorinated compounds and 10 chlorinated compounds, respectively, and 37% and 35% Chloroparaffin C1365.18%Cl were mainly 9 chlorinated compounds, accounting for 50% or so. The results of analysis of SCCPs in Baiyangdian water and sediments in China show that the concentration of SCCPs in Baiyangdian water is in the range of 1562.8N 56 305.9 ng / L, the average value is 7223 ng / L, the median is 3168.9 ng / L, and the concentration of SCCPs in sediments is in the range of 1270~254203ng/g (dry weight). The average is 24454 ng / g, and the median is 3458 ng / g. The pollution trend of SCCPs in Baiyangdian water and sediment was basically consistent. In general, SCCPs was detected in water and sediment of 15 sampling sites in Baiyangdian, and the detection rate was 100. The main congeners were hexachloro and SCCPs of carbon chain C10 and C11 and heptachlor. The results of principal component analysis show that the main pollution characteristics in Baiyangdian sediments are C10H15Cl7, C10H15Cl7, C12H13Cl9, C13H14Cl8, C11H16Cl6, C12H16Cl6, C13H16Cl6. Compared with the domestic and foreign Baiyangdian pollution level is higher. The Yangtze River Valley is one of the areas with high level of economic development and urbanization. With the development of economy, a large amount of domestic sewage and industrial wastewater are discharged into the Yangtze River, and the pollution is becoming more and more serious. So, this paper collected the water and sediment from the middle reaches of the Yangtze River. The pollution characteristics of SCCPs were studied. SCCPs were detected in all sampling sites and the detection rate was 100%. The range of SCCPs concentration in water is between 1131~65640ng/L and the average concentration is 18989ng / L and the median is 14691ng / L. The sediment concentration is in the range of 251.9-397600.4ng/g (dry weight), the average concentration is 54512ng / g, the median concentration is 2363.7ng / g. The pollution level in the upper and middle reaches of the Yangtze River is lower than that in the middle and lower reaches of the Yangtze River. The SCCPs in the Yangtze River 14, Yangtze River 15, Changjiang 21 and Yangtze River 5 are higher, with the SCCPs of chain length C10 and C13 as the main congeners. There was no correlation between the median particle size of sediment and the pollution level of SCCPs, but there was a positive correlation between the concentration of SCCPs in organic matter and the concentration of SCCPs in sediment. The concentration of SCCPs in the filtration membrane was in the range of 1868ng/L~513335.9ng/L, with an average of 64219ng / L and a median value of 8211ng / L. Compared with foreign countries, the level of pollution is higher. The main components in the middle reaches of the Yangtze River mainly come from HCH and chlordated short chain chlorinated paraffins (SCCPs).
【学位授予单位】：河北师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X592

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