饮用水氯化消毒副产物污染控制技术及健康风险评价的研究
摘要
自1974年首次发现氯消毒副产物DBPs氯仿以来,人们非常关注由此带来的致畸、致癌、致突变等慢性毒性对人类健康的危害,世界各国开展了有关DBPs检测分析、处理、以及风险研究的工作,以预测区域饮用水消毒副产物的人体健康影响。饮用水消毒副产物的区域研究是环境安全领域的热点问题之一。
本文研究了饮用水氯消毒副产物的来源及种类、氯消毒副产物的鉴定及分析技术、净化控制技术以及健康风险,重点探讨THMs和HAAs的安全控制技术和健康风险评价技术。针对钱塘江流域的饮用水安全问题,调查分析了衢县航埠(江山港)、衢州龙游(衢江)、兰溪游埠(衢江)、兰溪市区(兰江)、淳安威坪(新安江)、建德梅城(新安江)、桐庐横村(分水江)、富阳(富春江)、萧山义桥(浦阳江)、萧山章正(钱塘江)、萧山闻堰(钱塘江)、杭州九溪(钱塘江)、杭州南星桥(钱塘江)等13个水厂的THMs (CHC13、CHCl2Br、CHClBr2)和HAAs (MBAA、DCAA、BCAA、TCAA)氯消毒副产物的存在水平,研制了安全的活性炭-壳聚糖净水吸附剂,研究吸附净化CDBPs技术,在细胞水平上深入探讨了MBAA、DCAA、TCAA、BCAA、BDCM、DBCM和.CHCl3等7种DBPs的细胞凋亡毒理效应,初步评价了钱塘江流域饮用水致癌的潜在健康风险。研究结果如下：
(1)钱塘江流域饮用水中氯消毒副产物处于相对低含量水平,各江水质的饮用水厂出水氯消毒副产物总体水平和DBPs中类存在差异。钱塘江流域15个水厂检测出13个加氯消毒剂的水厂的消毒副产物远低于国家饮用水标准,83.3%的水厂饮用水中HAAs含量大于THMs;冬季水厂出水HAAs和THMs平均浓度分别是5.87μg/L和3.34μg/L, HAAs浓度范围为0.44-13.72μg/L、THMs为0.21～15.23μg/L,其中CHCl3是THMs最普遍存在的物质,MBAA和TCAA是HAAs中普遍存在的物质；兰江段兰溪市水厂氯消毒副产物总浓度水平最高,其次为衢江段龙游、富春江段富阳、浦阳江段义桥、钱塘江段南星桥。
(2)钱塘江源水中有机物主要是小分子量的溶解性有机物和大分子量的苯衍生物。钱塘江流域源水中DOC主要分布在分子量<2K Da,占全部分布比例的52.2%；其次是分子量5K Da-10KDa之间占18.9%。UV-254在>100K Da区间,占全部分布比例的97.9%。THMFP的主要分布区间为<2K Da,而HAAFP则以2-5K Da分子量物质为主。
(3)自制了安全的DBPs净化壳聚糖-活性炭吸附剂。吸附剂产品直径为1-1.5mm、比表面积为303.8 m2/g、具有较大的孔容的颗粒型壳聚糖一活性炭吸附剂,该技术已于2005年获得中国发明专利。吸附剂对THMs弱极性物质具有较高吸附效率,对CHCl3和CHBrCl2的去除率可以达到79.67%和87.66%,吸附平衡时间为3小时,符合Freundrich吸附等温式,pH值和温度对净化效率的影响较小。
(4) THMs和HAAs能诱导细胞凋亡。七种消毒副产物在O.1μg/-10μg/L的范围内,诱导2小时,均能明显地引起鲫鱼淋巴细胞发生凋亡；低剂量(0.1μg/L,2h)诱导实验表明,低氯代的MBAA、BCAA和DBCM诱导组产生明显的早期细胞凋亡细胞形态学特征。分子结构中含有2-3个氯原子的DCAA、TCAA、BCAA、CHC13和BDCM诱导组产生明显的晚期细胞凋亡细胞形态学特征；流式细胞仪的定量测定结果表明七种消毒副产物引起细胞凋亡的能力为TCAA> CHC13>BDCM>DCAA>DBCM>BCAA>MBAA.
(5)钱塘江流域饮用水氯消毒副产物THMs的暴露健康风险低。钱塘江流域THMs平均癌风险为3.59×10-5,富阳地区THMs暴露癌风险最高达1.48×10-4,CHClBr2是引起THMs癌风险的最主要致癌因子,癌风险贡献率达60%以上；钱塘江流域饮用水THMs的非致癌性风险评价结果表明,流域危险指数平均危险指数为6.99×10-8,最高与最低地区分别为兰溪(2.33×10-7)和章正(1.08×10-8)。
With the public health triumph of the 20th century in chemical disinfection of water for dramatic decreasing in waterborne diseases, chronic exposure to a very large number of chlorinated disinfection byproducts(CDBPs),which formed through reaction of the chlorine disinfectant with naturally occurring inorganic and organic material in the source water. The health effects and risk of DBPs have been focused in the range of world.
This thesis provides an overview of CDBPs research on pollution control and risk assessment. The purpose is to address concerns related to CDBPs pollution control technology and health risk from levels of CDBPs in drinking water to impossible control technology to exposure within Qiantangjiang watershed in Zhejiang province, China.. Seven types of CDBPs were studied including THMs (CHC13, CHCl2Br and CHClBr2) and HAAs (MBAA, DCAA, BCAA and TCAA) in thirteen drinking water plants, located in Jiangshan Harbor, Qu River, Lan River, Xinan River, Fenshui River, Fuchun River, Puyang River in the watershed. The research results are showed as follows:
(1) The levels of CDBPs in 13 drinking water plants with chlorine disinfectants of the watershed were relatively low, and there were significant differences between total CDBPs levels and CDBPs type.the levels of HAAs were higher than THMs at 83.3% of drinking water plants; the average levels of HAAs and THMs in the finished water were 5.87μ.g/L and 3.34μg/L, respectively in winter; the levels of HAAs were between 0.44 and 13.72μg/L and the levels of THMs were between 0.21 and 15.23μg/L; CHC13 was the most detected THMs, and MBAA and TCAA were the most detected HAAs; the total CDBPs levels in Lanxi of Lan River were the highest, and secondly in Longyou of Qu River, Fuyang of Fuchun River, Duanyiqiao of Puyang River and Nanxingqiao of Qiantang River.
(2) The dissolved small molecular weight organic compounds and big molecular weight aromatic substance were the main organic compounds in the source water of Qiantang River. The dissolved organic carbons (DOC) in the source water of Qiantang River were mainly distributed lower than 2K Dalton molecular weights, which the proportion was 52.2%; secondly, the proportion of the molecular weights distributed between 5K and 10K Dalton was 18.9%; according to the UV-254 detection the proportion of the molecular weights that were>100K Dalton was 97.9%. The molecular weights of THMFP were mainly below 2K Dalton, but the molecular weights of HAAFP were between 2K and 5K Dalton.
(3) A kind of safety activated carbon-chitosan water-cleaning adsorbent was modified. The diameter of the adsorbent was 1 to 1.5 mm, and the specific surface area was 303.8 m2/g. This adsorbent had very high cleaning efficiency for THMs, and the efficiencies for CHC13 and CHBrCl2 were 79.67% and 87.66%, respectively; the adsorption equilibrium time was only three hours; both pH and temperature have little influence on the cleaning efficiency. This modified technology has obtained the Chinese invention patent in 2005.
(4) Both THMs and HAAs can induce apoptosis. All the seven CDBPs can induce obvious apoptosis on crucian carp(Carassius auratus) lymphocytes in vitro for two hours at the exposed levels of 0.1μg/L and 10μ.g/L. The low exposed level (0.1μg/L) induction experiments showed that typical morphological characteristics of early apoptosis could be found after the induction by MBAA, BCAA and DBCM which were low chlorine substituted compounds, however typical morphological characteristics of later apoptosis could be observed after the induction by TCAA, BCAA, CHCl3 and BDCM which have 2-3 chlorine atoms in the molecular structures. According to the quantitative determination by flow cytometry, the apoptosis induction abilities of all the seven CDBPs were TCAA>CHCl3>BDCM>DCAA>DBCM>BCAA>MBAA.
(5) The exposure health risk of THMs in the watershed of Qiantang River was low. The average cancer risk of THMs in the watershed was 3.59×10-5, but the cancer risk of THMs in Fuyang area was up to 1.48×10-4. Among all the THMs, CHClBr2 was the main carcinogenic factor with the cancer contribution efficiency of over 60%. The non-cancer risk assessment results also showed that the average risk index in the watershed was 6.99×10-8, and Lanxi and Zhangzheng were the highest with the risk index of 2.33×10-8 and 1.08×10-8, respectively.
本文研究了饮用水氯消毒副产物的来源及种类、氯消毒副产物的鉴定及分析技术、净化控制技术以及健康风险,重点探讨THMs和HAAs的安全控制技术和健康风险评价技术。针对钱塘江流域的饮用水安全问题,调查分析了衢县航埠(江山港)、衢州龙游(衢江)、兰溪游埠(衢江)、兰溪市区(兰江)、淳安威坪(新安江)、建德梅城(新安江)、桐庐横村(分水江)、富阳(富春江)、萧山义桥(浦阳江)、萧山章正(钱塘江)、萧山闻堰(钱塘江)、杭州九溪(钱塘江)、杭州南星桥(钱塘江)等13个水厂的THMs (CHC13、CHCl2Br、CHClBr2)和HAAs (MBAA、DCAA、BCAA、TCAA)氯消毒副产物的存在水平,研制了安全的活性炭-壳聚糖净水吸附剂,研究吸附净化CDBPs技术,在细胞水平上深入探讨了MBAA、DCAA、TCAA、BCAA、BDCM、DBCM和.CHCl3等7种DBPs的细胞凋亡毒理效应,初步评价了钱塘江流域饮用水致癌的潜在健康风险。研究结果如下：
(1)钱塘江流域饮用水中氯消毒副产物处于相对低含量水平,各江水质的饮用水厂出水氯消毒副产物总体水平和DBPs中类存在差异。钱塘江流域15个水厂检测出13个加氯消毒剂的水厂的消毒副产物远低于国家饮用水标准,83.3%的水厂饮用水中HAAs含量大于THMs;冬季水厂出水HAAs和THMs平均浓度分别是5.87μg/L和3.34μg/L, HAAs浓度范围为0.44-13.72μg/L、THMs为0.21～15.23μg/L,其中CHCl3是THMs最普遍存在的物质,MBAA和TCAA是HAAs中普遍存在的物质；兰江段兰溪市水厂氯消毒副产物总浓度水平最高,其次为衢江段龙游、富春江段富阳、浦阳江段义桥、钱塘江段南星桥。
(2)钱塘江源水中有机物主要是小分子量的溶解性有机物和大分子量的苯衍生物。钱塘江流域源水中DOC主要分布在分子量<2K Da,占全部分布比例的52.2%；其次是分子量5K Da-10KDa之间占18.9%。UV-254在>100K Da区间,占全部分布比例的97.9%。THMFP的主要分布区间为<2K Da,而HAAFP则以2-5K Da分子量物质为主。
(3)自制了安全的DBPs净化壳聚糖-活性炭吸附剂。吸附剂产品直径为1-1.5mm、比表面积为303.8 m2/g、具有较大的孔容的颗粒型壳聚糖一活性炭吸附剂,该技术已于2005年获得中国发明专利。吸附剂对THMs弱极性物质具有较高吸附效率,对CHCl3和CHBrCl2的去除率可以达到79.67%和87.66%,吸附平衡时间为3小时,符合Freundrich吸附等温式,pH值和温度对净化效率的影响较小。
(4) THMs和HAAs能诱导细胞凋亡。七种消毒副产物在O.1μg/-10μg/L的范围内,诱导2小时,均能明显地引起鲫鱼淋巴细胞发生凋亡；低剂量(0.1μg/L,2h)诱导实验表明,低氯代的MBAA、BCAA和DBCM诱导组产生明显的早期细胞凋亡细胞形态学特征。分子结构中含有2-3个氯原子的DCAA、TCAA、BCAA、CHC13和BDCM诱导组产生明显的晚期细胞凋亡细胞形态学特征；流式细胞仪的定量测定结果表明七种消毒副产物引起细胞凋亡的能力为TCAA> CHC13>BDCM>DCAA>DBCM>BCAA>MBAA.
(5)钱塘江流域饮用水氯消毒副产物THMs的暴露健康风险低。钱塘江流域THMs平均癌风险为3.59×10-5,富阳地区THMs暴露癌风险最高达1.48×10-4,CHClBr2是引起THMs癌风险的最主要致癌因子,癌风险贡献率达60%以上；钱塘江流域饮用水THMs的非致癌性风险评价结果表明,流域危险指数平均危险指数为6.99×10-8,最高与最低地区分别为兰溪(2.33×10-7)和章正(1.08×10-8)。
With the public health triumph of the 20th century in chemical disinfection of water for dramatic decreasing in waterborne diseases, chronic exposure to a very large number of chlorinated disinfection byproducts(CDBPs),which formed through reaction of the chlorine disinfectant with naturally occurring inorganic and organic material in the source water. The health effects and risk of DBPs have been focused in the range of world.
This thesis provides an overview of CDBPs research on pollution control and risk assessment. The purpose is to address concerns related to CDBPs pollution control technology and health risk from levels of CDBPs in drinking water to impossible control technology to exposure within Qiantangjiang watershed in Zhejiang province, China.. Seven types of CDBPs were studied including THMs (CHC13, CHCl2Br and CHClBr2) and HAAs (MBAA, DCAA, BCAA and TCAA) in thirteen drinking water plants, located in Jiangshan Harbor, Qu River, Lan River, Xinan River, Fenshui River, Fuchun River, Puyang River in the watershed. The research results are showed as follows:
(1) The levels of CDBPs in 13 drinking water plants with chlorine disinfectants of the watershed were relatively low, and there were significant differences between total CDBPs levels and CDBPs type.the levels of HAAs were higher than THMs at 83.3% of drinking water plants; the average levels of HAAs and THMs in the finished water were 5.87μ.g/L and 3.34μg/L, respectively in winter; the levels of HAAs were between 0.44 and 13.72μg/L and the levels of THMs were between 0.21 and 15.23μg/L; CHC13 was the most detected THMs, and MBAA and TCAA were the most detected HAAs; the total CDBPs levels in Lanxi of Lan River were the highest, and secondly in Longyou of Qu River, Fuyang of Fuchun River, Duanyiqiao of Puyang River and Nanxingqiao of Qiantang River.
(2) The dissolved small molecular weight organic compounds and big molecular weight aromatic substance were the main organic compounds in the source water of Qiantang River. The dissolved organic carbons (DOC) in the source water of Qiantang River were mainly distributed lower than 2K Dalton molecular weights, which the proportion was 52.2%; secondly, the proportion of the molecular weights distributed between 5K and 10K Dalton was 18.9%; according to the UV-254 detection the proportion of the molecular weights that were>100K Dalton was 97.9%. The molecular weights of THMFP were mainly below 2K Dalton, but the molecular weights of HAAFP were between 2K and 5K Dalton.
(3) A kind of safety activated carbon-chitosan water-cleaning adsorbent was modified. The diameter of the adsorbent was 1 to 1.5 mm, and the specific surface area was 303.8 m2/g. This adsorbent had very high cleaning efficiency for THMs, and the efficiencies for CHC13 and CHBrCl2 were 79.67% and 87.66%, respectively; the adsorption equilibrium time was only three hours; both pH and temperature have little influence on the cleaning efficiency. This modified technology has obtained the Chinese invention patent in 2005.
(4) Both THMs and HAAs can induce apoptosis. All the seven CDBPs can induce obvious apoptosis on crucian carp(Carassius auratus) lymphocytes in vitro for two hours at the exposed levels of 0.1μg/L and 10μ.g/L. The low exposed level (0.1μg/L) induction experiments showed that typical morphological characteristics of early apoptosis could be found after the induction by MBAA, BCAA and DBCM which were low chlorine substituted compounds, however typical morphological characteristics of later apoptosis could be observed after the induction by TCAA, BCAA, CHCl3 and BDCM which have 2-3 chlorine atoms in the molecular structures. According to the quantitative determination by flow cytometry, the apoptosis induction abilities of all the seven CDBPs were TCAA>CHCl3>BDCM>DCAA>DBCM>BCAA>MBAA.
(5) The exposure health risk of THMs in the watershed of Qiantang River was low. The average cancer risk of THMs in the watershed was 3.59×10-5, but the cancer risk of THMs in Fuyang area was up to 1.48×10-4. Among all the THMs, CHClBr2 was the main carcinogenic factor with the cancer contribution efficiency of over 60%. The non-cancer risk assessment results also showed that the average risk index in the watershed was 6.99×10-8, and Lanxi and Zhangzheng were the highest with the risk index of 2.33×10-8 and 1.08×10-8, respectively.
引文
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