Study on water quality criteria, ecological risk and adverse outcome pathway of lindane in freshwater environment
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摘要:
为多角度评估我国淡水水体中林丹生态风险，按照HJ 831—2022《淡水生物水质基准推导技术指南》方法推导，获得林丹短期和长期淡水水质基准值分别为6.15和0.12 μg/L，再依据林丹基准值对我国主要淡水水体中林丹生态风险进行评价。结果显示，我国长江流域的太湖以及岷江、黄河、海河和大辽河河口等水体林丹生态风险处于高风险水平。目前生态风险评价的毒性效应终点仍为一般毒性效应终点（MATC、EC10、EC20、NOEC、LOEC、EC50和LC50等），而有害结局路径（AOP）从基因、细胞、组织及器官水平对污染物毒性效应的因果关系进行定性和定量，可为未来精细化生态风险评价提供科学依据。因此，基于林丹淡水生物毒性研究的文献计量学分析结果，按照经济合作与发展组织（OECD）指导原则，从生物毒性机制的角度构建了肝损伤、生殖损伤和神经损伤3条有害结局路径。
Abstract:In order to evaluate the ecological risk of lindane in freshwater bodies of China, the short-term and long-term freshwater quality criteria values were derived according to the method of Technical Guideline for Deriving Water Quality Criteria for Freshwater Organisms (HJ 831-2022). The derived short-term and long-term freshwater quality criteria values were 6.15 and 0.12 μg/L, respectively. According to the water quality criteria, the ecological risk of lindane in major freshwater bodies of China was assessed and the results showed that the ecological risk of lindane was at high risk level in Taihu Lake and the Minjiang River of Yangtze River basin, the Yellow River, the Haihe River and the Daliao River estuary. At present, the toxic effect endpoints of ecological risk assessment are still the general toxic effects (MATC, EC10, EC20, NOEC, LOEC, EC50, LC50, etc.), while the adverse outcome pathway (AOP) can qualitatively and quantitatively analyze the causal relation between the pollutants and their toxic effects from the levels of genes, cells, tissues and organs, which can provide a scientific basis for future refined ecological risk assessment. Thus, based on the results of the bibliometric analysis on the toxicity of lindane to freshwater organisms, three adverse outcome pathways of liver injury, reproductive injury and nerve injury were constructed according to the guidelines of the Organization for Economic Co-operation and Development (OECD).
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Key words:
- lindane /
- water quality criteria /
- ecosystem risk /
- adverse outcome pathway /
- freshwater environment
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图 4 林丹水生生物的有害结局路径
Figure 4. Lindane adverse outcome pathways of freshwater aquatic organism
表 1 毒性数据和文献检索
Table 1. Toxicity data and literature retrieval scheme
数据库名称 检索时间 检索式 急性毒性 慢性毒性 ECOTOX 数据库覆盖年限截至
2022年12月31日化合物名称：lindane
暴露介质：freshwater
毒性效应测试终点：EC50或LC50化合物名称：lindane
暴露介质：freshwater
毒性效应测试终点：NOEC或LOEC或MATC或EC10或EC20或EC50或LC50CNKI、万方数据知识
服务平台、维普中文科技期刊数据库数据库覆盖年限截至
2022年12月31日题名：林丹
主题：毒性
期刊来源类别：中文核心期刊题名：林丹
主题：毒性或NOEC或LOEC或MATC或EC10或EC20或EC50或LC50
期刊来源类别：中文核心期刊WoS 数据库覆盖年限截至
2022年12月31日题名：lindane
主题：toxicity或EC50或LC50题名：lindane
主题：toxicity或NOEC或LOEC或MATC或EC10或EC20或EC50或LC50
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表 2 数据筛选方法
Table 2. Data filtering method
筛选类型 筛选原则 受试物 明确受试物准确名称及CAS号，纯度一般大于95% 受试物种 反映中国淡水生物区系特征，野生物种应鉴定准确，剔除外来入侵物种，剔除单细胞动物和微生物（微藻除外） 试验设计 试验设计应依据国家或国际标准毒性测试方法，急性毒性试验浓度间隔系数一般不超过2.2，慢性毒性试验浓度间隔系数一般不超过3.2 暴露条件 试验暴露条件应符合标准毒性测试方法，受试物实测浓度毒性数据>理论浓度毒性数据，流水式暴露毒性数据>半静态暴露毒性数据>静态暴露毒性数据；急性毒性数据的动物暴露时间为轮虫24 h左右、溞类和摇蚊48 h左右、其他物种96 h左右，植物适宜的暴露时间为96 h左右；慢性毒性数据轮虫大于等于48 h、其他动物大于等于21 d或覆盖1个敏感生命阶段，植物适宜的暴露时间为大于等于21 d或至少跨越1个世代 离群值判断 当同一物种的同一毒性终点试验数据之间相差10倍以上时，结合专业判断剔除离群值，当无法判断离群值时，弃用全部相关数据 数据优先性判断 效应指标：急性毒性数据通常为LC50或EC50，不区分优先性；慢性毒性数据的优先性为MATC>EC20>EC10=
NOEC>LOEC>EC50>LC50。生命阶段：相对敏感生命阶段毒性数据>相对不敏感生命阶段毒性数据；全生命周期数据>部分生命周期数据>单一生命阶段数据
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表 3 最少毒性数据需求
Table 3. Minimal toxicity data requirements for water quality criteria derivation
类别 数据需求 营养级 至少涵盖包括生产者、初级消费者和次级消费者在内的3个不同营养级 物种和生物类群 至少包括10个物种且涵盖以下生物类群：1种硬骨鱼纲鲤科鱼，1种硬骨鱼纲非鲤科鱼，1种浮游动物，1种非鱼类的底栖动物（如贝类、底栖甲壳类等），1种两栖类或与上述动物分属于不同门的其他水生动物，1种浮游植物或水生维管束植物 污染物毒性特点 推导杀虫剂的基准应包括水生昆虫的毒性数据
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表 4 同效应急性值及累积频率
Table 4. Acute value for the same effect and cumulative frequency
序号 拉丁名 物种名 数据类型 AVE/（μg/L） lg AVE R f FR/% 1 Chaoborus sp. 幽蚊 存活类 3.30 0.52 1 1 2.38 2 Gammarus fasciatus 淡水钩虾 存活类 10.32 1.01 2 1 4.76 3 Gammarus pulex 蚤状钩虾 存活类 16.09 1.21 3 1 7.14 4 Salmo trutta 褐鳟 存活类 23.63 1.37 4 1 9.52 5 Oncorhynchus mykiss 虹鳟 存活类 27.21 1.43 5 1 11.90 6 Micropterus salmoides 大口黑鲈 存活类 32.00 1.51 6 1 14.29 7 Perca flavescens 黄金鲈 存活类 39.55 1.60 7 1 16.67 8 Oncorhynchus tshawytscha 大鳞大马哈鱼 存活类 40.00 1.60 8 1 19.05 9 Salvelinus fontinalis 溪红点鲑 存活类 44.30 1.65 9 1 21.43 10 Ictalurus punctatus 斑点叉尾鮰 存活类 46.43 1.67 10 1 23.81 11 Cloeon sp. 二翅蜉 存活类 50.00 1.70 11 1 26.19 12 Lepomis macrochirus 蓝鳃太阳鱼 存活类 55.53 1.74 12 1 28.57 13 Ameiurus melas 黑鮰 存活类 64.00 1.81 13 1 30.95 14 Gobio gobio 鮈 存活类 73.50 1.87 14 1 33.33 15 Pimephales promelas 黑头软口鲦 存活类 75.04 1.88 15 1 35.71 16 Lepomis cyanellus 绿太阳鱼 存活类 76.22 1.88 16 1 38.10 17 Lepomis microlophus 小冠太阳鱼 存活类 83.00 1.92 17 1 40.48 18 Gammarus lacustris 湖泊钩虾 存活类 88.00 1.94 18 1 42.86 19 Channa punctata 翠鳢 存活类 106.55 2.03 19 1 45.24 20 Danio rerio 斑马鱼 存活类 114.59 2.06 20 1 47.62 21 Heteropneustes fossilis 囊鳃鲇 存活类 125.00 2.10 21 1 50.00 22 Carassius auratus 鲫 存活类 127.87 2.11 22 1 52.38 23 Cyprinus carpio 鲤 存活类 134.16 2.13 23 1 54.76 24 Paracheirodon axelrodi 霓虹脂鲤 存活类 140.00 2.15 24 1 57.14 25 Chironomus tentans 伸展双叶摇蚊 存活类 207.00 2.32 25 1 59.52 26 Poecilia reticulata 孔雀鱼 存活类 222.89 2.35 26 1 61.90 27 Anabas testudineus 龟壳攀鲈 存活类 240.30 2.38 27 1 64.29 28 Lepidocephalichthys thermalis 温泉鳞头鳅 存活类 280.00 2.45 28 1 66.67 29 Microcystis aeruginosa 铜绿微囊藻 生长类 442.00 2.65 29 1 69.05 30 Daphnia pulex 蚤状溞 生长类 460.00 2.66 30 1 71.43 31 Daphnia magna 大型溞 生长类 516.00 2.71 31 1 73.81 32 Chlorella vulgaris 普通小球藻 生长类 524.00 2.72 32 1 76.19 33 Anguilla anguilla 鳗鲡 存活类 538.05 2.73 33 1 78.57 34 Simocephalus serrulatus 锯顶低额溞 生长类 676.46 2.83 34 1 80.95 35 Desmodesmus subspicatus 近具棘链带藻 生长类 2 500.00 3.40 35 1 83.33 36 Scenedesmus abundans 多棘栅藻 生长类 2 500.00 3.40 36 1 85.71 37 Pseudacris triseriata 三锯拟蝗蛙 存活类 2 650.00 3.42 37 1 88.10 38 Lampetra tridentata 七鳃鳗 存活类 2 680.00 3.43 38 1 90.48 39 Lymnaea stagnalis 静水椎实螺 存活类 3 300.00 3.52 39 1 92.86 40 Cyclotella meneghiniana 梅尼小环藻 生长类 11 849.00 4.07 40 1 95.24 41 Brachionus calyciflorus 萼花臂尾轮虫 存活类 22500000.00 7.35 41 1 97.62
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表 5 同效应慢性值及累积频率
Table 5. Chronic value for the same effect and cumulative frequency
序号 拉丁名 物种名 数据类型 CVE/（μg/L） lg CVE R f FR/% 1 Algae 绿藻 生长类 1.57 0.20 1 1 9.09 2 Chironomus tentans 伸展双叶摇蚊 生长类 2.20 0.34 2 1 18.18 3 Gammarus fasciatus 淡水钩虾 生长类 4.30 0.63 3 1 27.27 4 Danio rerio 斑马鱼 生长类 5.85 0.77 4 1 36.36 5 Salvelinus fontinalis 溪红点鲑 生长类 8.80 0.94 5 1 45.45 6 Pimephales promelas 黑头软口鲦 生长类 9.10 0.96 6 1 54.55 7 Lepomis macrochirus 蓝鳃太阳鱼 生长类 9.10 0.96 7 1 63.64 8 Brachionus angularis 角突臂尾轮虫 生长类 12.00 1.08 8 1 72.73 9 Daphnia magna 大型溞 生长类 72.19 1.86 9 1 81.82 10 Rana temporaria 林蛙 生长类 58 000.00 4.76 10 1 90.91
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表 6 我国七大流域部分水体林丹赋存情况
Table 6. Occurrence of lindane in seven basins of China
流域 年份 地点 林丹浓度/(ng/L) 数据来源 流域 年份 地点 林丹浓度/(ng/L) 数据来源 长江流域 2002 岷江(核心) 530~2 400 文献[11] 松辽河流域 1998 西泉眼水库 >1.9 文献[27] 2008 松花江 0.17~80 文献[23] 2003 太湖 ND~36 000 文献[12] 2008 辽河 0.17~120 文献[23] 2005 钱塘江 ND~170 文献[13] 2009 大辽河河口 8.5~970 文献[28] 2009 三峡水库 0.055~0.35 文献[14] 2013 条子河 0.80~1.08 文献[29] 2013 洪湖 0.23~2.7 文献[15] 淮海河
流域2004 海河 43~2 100 文献[30] 2011 淮河湖 0.47~1.9 文献[31] 2013 嵊州市浅层地下水 ND~34.32 文献[16] 2011 微山湖 34.40~195.90 文献[32] 2008 淮河 0.17~98 文献[24] 2014 长江 0.17~70 文献[11] 东南沿海
诸河流域2002 九龙江(核心) 4~25 文献[11] 2015 巢湖 14.01~44.01 文献[17] 2005 胶州港 ND~7.1 文献[22] 2016 汉江 ND~2.11 文献[18] 2011 千岛湖 ND~44.40 文献[33] 2021 安徽淮南市 583.45~797.62 文献[19] 2011 桂林地下河 1.25~7.36 文献[34] 2012 晋江 3~5.8 文献[35] 黄河流域 2003 官厅水库 ND~120 文献[20] 珠江流域 1998 厦门港 0.3~3.5 文献[36] 2005 莱州港 ND~0.95 文献[21] 1999 大亚湾 8.5~970 文献[37] 2007 天津大沽河 5.00~38.10 文献[22] 2008 珠江 0.17~48 文献[24] 2008 黄河 0.17~860 文献[23] 2009 珠江三角洲 2.4~5.1 文献[38] 2011 白洋淀 3.13~10.60 文献[24] 2015 贵州百花湖猫跳河 3 800 文献[39] 2011 南四湖 19.60~26.30 文献[25] 2015 贵州贵化取水口 2 700 文献[39] 2016 北京地表水 2.11~2.82 文献[26] 2015 南宁朝阳溪 <1 文献[40] 注：ND为未检出。
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表 8 淡水水体林丹生态风险评价比较
Table 8. Comparison of ecological risk assessment of lindane in freshwater water at home and abroad
水体 基准值 暴露浓度（MEC） 风险评价结果 哈萨克斯坦锡尔河[57] 据文献报道的浮游动物、浮游植物、软体动物、
昆虫和鱼类5种水生生物的林丹毒性数据确定的PNEC0.014~0.240 μg/L 生态风险极高（≤100） 恒河地表水[58] 根据US EPA ECOTOX毒性数据库中的藻类、
水生无脊椎动物和鱼类3个物种的毒性数据确定的PNEC0.004~4.346 μg/L 中等风险 伊朗塔拉尔河、巴博尔
鲁德河、哈拉兹河[59]生态毒理学水平评估标准（EAC） 0~12 ng/L 生态风险低（>1） 沙颍河[60] 文献中获得的PNEC为1 ng/L 1.8~9.3 ng/L 生态风险极高（≤9.33） 扬州城区古运河[55] 0.05 μg/L 132.03 ng/L 生态风险高（2.64） 巢湖[55] 0.05 μg/L — 中等风险（1.10×10−1） 乌江[55] 0.05 μg/L — 中等风险（1.04×10−1） 白洋淀[55] 0.05 μg/L — 中等风险（4.80×10−1） 会仙湿地[55] 0.05 μg/L — 中等风险（6.20×10−1）
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