巢湖、洞庭湖、鄱阳湖沉积物重金属污染及来源的Meta分析

李 贺,王书航,车霏霏,姜 霞,牛 勇

巢湖、洞庭湖、鄱阳湖沉积物重金属污染及来源的Meta分析

李 贺,王书航,车霏霏,姜 霞,牛 勇*

(中国环境科学研究院,湖泊水污染治理与生态修复技术国家工程实验室,国家环境保护湖泊污染控制重点实验室,北京 100012)

对2004～2021年关于巢湖、洞庭湖、鄱阳湖沉积物中重金属浓度的研究进行了分析,并对3个湖泊沉积物的重金属地质累积、潜在生态风险和毒性进行了蒙特卡洛分析,以清晰、客观、全面地描述3个湖泊沉积物的重金属污染情况.结果表明,3个湖泊均存在不同程度的Cu、Zn、Pb、Ni、Cr和Cd污染,总体污染程度上,鄱阳湖>洞庭湖>巢湖.地累积指数表明,Cd是3个湖泊中最主要的污染元素,巢湖沉积物中Cd处于偏中度污染水平占比为84.76%,洞庭湖沉积物中Cd处于偏重度污染水平占比为32.64%,鄱阳湖沉积物中Cd偏重度污染水平占比达到46.64%.巢湖、洞庭湖和鄱阳湖RI值中Cd元素为主要贡献者,占比分别为80.26%、91.04%和90.03%.巢湖整体处于中低风险,洞庭湖RI值高风险概率为60.74%;鄱阳湖重金属RI值高风险概率68.95%,生态风险高.毒性结果表明,三个湖泊沉积物毒性较高的是Pb和Cr,巢湖沉积物中的重金属毒性处于低度毒性水平,洞庭湖沉积物中度毒性水平的累积概率为69.03%,鄱阳湖中度毒性水平的累积概率为7.18%.巢湖、洞庭湖、鄱阳湖重金属污染情况各不相同,重金属大体上存在3～4个不同来源:工业源、交通源、农业源和自然源,巢湖交通源为主要影响,污染较轻;洞庭湖和鄱阳湖主要污染源为工业活动,污染较重.

巢湖；洞庭湖；鄱阳湖；重金属；污染评价

重金属是湖泊沉积物的主要污染物,具有致毒性、累积性、放大性等特征,严重威胁水生生物安全以及人类健康[1-2].作为水体底栖环境的主要固相介质,沉积物与上覆水体存在密切联系[3].沉积物还是水体中各种污染物的储存库,进入到水体的重金属会在各种作用下蓄积在沉积物中,但蓄积的重金属会在环境条件变化时再次释放出来,破坏上覆水体环境质量、危害水生生物[4-5].因此,研究沉积物中重金属含量变化是水体污染评价和调控的重要基础[6-8].

随着长江流域经济的快速发展,生态资源透支严重,环境污染问题日益凸显,长江流域湖泊也面临多种污染问题,尤其是长效污染物重金属的污染问题[9].国家长江保护修复攻坚战行动计划开始后,长江流域内巢湖、洞庭湖和鄱阳湖等湖泊重金属污染研究也在同步进行,已开展许多关于巢湖、洞庭湖和鄱阳湖沉积物中重金属含量调查,但在不同的研究中出现了不同的重金属含量水平.巢湖2020年沉积物重金属Cr含量是2018年研究中Cr含量的4倍[10-11];有研究表明巢湖底泥处于清洁状态,还有研究表明巢湖仍然存在偏重度的 Hg 污染和偏中度的 Cd 污染[12].洞庭湖沉积物中Cd含量调查也存在较大差异[13-15].在已经开展的很多鄱阳湖沉积物重金属研究中Cu 和 Cd 为主要污染元素,但在2017年的研究中Pb、Cr对总毒性的贡献较大[16-17],我们认为这种差异主要由于重金属在沉积物中浓度分布不均匀所致,空间部分的不均匀受到pH值、温度等多因素的影响[18],这种差异结论存在,不利于管理者对于湖泊沉积物重金属污染情况的了解,同时也增加了污染防治策略制定的难度,因此,需要更好的一种评价方式去描述湖泊沉积物的污染状态.

近年来,Meta分析逐步在环境污染现状分析中使用,主要用于弥补研究区域内长时间调查数据缺失问题,例如,使用Meta分析评估了长江三角洲农田表土重金属污染的时间趋势;还有研究人员整合了2450份出版物中的数据,绘制了中国农田土壤中重金属的空间分布图,还有对中国耕地As污染情况的分析[19-21].在缺乏监测数据的情况下,对已公布的数据开展Meta分析用于研究各种环境介质污染情况具有重要价值.目前,Meta分析还没有发展成一个系统的分析过程来进行环境污染评估,现在可用的方法通常是从相关出版物收集污染物数据并重新分析,以描述研究区域的污染状态.

因此,本文以长江中下游巢湖、洞庭湖和鄱阳湖沉积物重金属调查研究为基础,基于Meta分析的基本原理系统性分析沉积物重金属污染水平,并采用蒙特卡洛方法对重金属地累积特征和潜在生态风险状态展开不确定性分析[22],从而更加清晰、客观的呈现湖泊沉积物重金属污染水平、风险等级以及湖泊之间污染的差异.研究结果可为长江中下游湖泊重金属污染防治提供参考,研究方法可为世界其他湖泊污染状况诊断提供借鉴.

1 材料和方法

1.1 研究方法

1.1.1 Meta分析 Meta分析是一种统计方法,用于综合分析众多研究中的大量数据并整合结果,其本质是将多个研究结果中的子效应量进行综合评价,从而得到感兴趣的总效应量[23-24],其主要步骤是使用正式的方法进行文献检索、研究筛选(包括根据预定义标准对合格的研究进行批判性评估)、数据提取、编码和通常的统计分析,以及每个步骤的详细、透明的文档记录,在开展巢湖、洞庭湖和鄱阳湖沉积物重金属积累特征时遵循了Meta分析基本原理及步骤.

1.1.2 蒙特卡洛模拟 蒙特卡洛模拟法是以统计抽样理论为基础,利用随机数,经过对随机变量已有数据的统计进行抽样实验或随机模拟,以求得统计量的某个数字特征并将其作为待解决问题的数值解[22].在分析巢湖、洞庭湖和鄱阳湖沉积物重金属积累特征时,通过经典蒙特卡洛模拟方法来处理评价结果的不确定性,采用CrystalBall工具软件分别对地质累积指数(简称geo)、潜在生态风险指数(简称RI)和毒性(简称TU)进行了1000次模拟计算来反映3个湖泊重金属污染情况.

1.2 数据收集

本文通过中国知网(CNKI)和Web of Science收集了2002～2021年巢湖、洞庭湖和鄱阳湖沉积物中重金属的监测数据,在数据库中使用的搜索词是SU=(’巢湖‘+’洞庭湖‘+’鄱阳湖‘)*’沉积物‘*’重金属‘和ts=(chaohu lake) or ts=(dongting lake) or ts= (poyang lake) and ts=sediment and ts=(heavy metal),符合筛选条件的文章主要集中在2004～2021年.最后,如图所示,筛选获得了其中52份文献资料,370多份数据记录[7,11-17,25-68].首先,本文选择的文章种应包括巢湖、洞庭湖、鄱阳湖全湖表层沉积物(顶部5cm)的调查.其次,还应包括调查点的明确数量、重金属含量.在所有已收集的研究中,沉积物中重金属的总含量基本上通过单酸或混合酸消化进行分析,并采用了严格的质量控制和保证,图2为筛选文献中3个湖泊的采样点位置.

图1 文献筛选过程与结果

1.3 数据处理

1.3.1 样本数加权平均(SNWM)在实际调查中,调查点的数量越多,获得的浓度水平的代表性就越大.因此,本研究使用调查点的数量进行样本数加权平均.

式中:N是数据记录中的采样数,C是数据记录中的重金属浓度,是数据记录的数量.N和C是从原始研究中获得的.

1.3.2 地累积指数法 地累积指数法常被用于定量研究沉积物中重金属的污染程度,该方法能够直观反映外源重金属在沉积物中的富集程度[69].本研究将对全国重要湖泊重金属累积程度进行评估,具体计算过程如下:

式中:B为沉积岩(普通页岩)中该元素的地球化学背景值;C为元素在沉积物中的含量;为考虑各地岩石差异可能会引起背景值的变动而取的系数(一般取值为1.5);geo为地累积指数,依据地累积指数大小将重金属污染程度划分为5个等级,geo<0,清洁状态;05,严重污染.

1.3.3 潜在生态风险指数法 Hakanson提出的将重金属含量、生态、环境与毒理性综合的潜在生态风险指数法[70],既简单快速又标准地对生态风险进行了等级划分.具体计算公式如下:

表1 潜在生态危害与风险等级

1.3.4 毒性 毒性用于评估沉积物中重金属对水环境的影响[72],以使各种重金属引起的毒性正常化,从而比较它们的相对效应,定义为测定浓度(C)与可能效应水平值(PEL)(P)的比率[73-74].总毒性(STU)是TU的总和.

2 结果和讨论

2.1 数据统计分析

表2 文献信息和沉积物指导值统计描述

注:a:安徽省江淮流域土壤地球化学背景值,b: 洞庭湖区土壤地球化学背景值,c: 江西省Ｃ层土壤的各元素背景值.

表2显示了所选52篇论文(巢湖20篇、洞庭湖18篇、鄱阳湖14篇)中沉积物的重金属浓度统计结果.主要开展了3个湖泊的Cu、Zn、Pb、Ni、Cr、Cd重金属研究,巢湖、洞庭湖和鄱阳湖Cd 加权均值较高为0.43、3.18和1.24mg/kg,分别是其环境背景值的3.75、10.26、11.50倍,均高于南四湖[75](0.23mg/kg)、艾比湖[76](0.17mg/kg)和乌伦古湖[77](0.33mg/kg).洞庭湖除Cr加权均值外,其他元素的浓度略高于环境背景值,鄱阳湖Cr 加权均值为其环境背景值的1.24倍,巢湖Cr加权均值相对为环境背景值的1.23倍,但3个湖泊Cr元素加权均值也高于阳澄湖[78]和艾比湖,此外3个湖泊Cu、Zn、Pb、Ni加权均值也高于或接近其余4个湖泊.从变异系数来看,巢湖Pb、Cr和Cd的变异系数分别为46%、51%和44%,洞庭湖Zn和Cd的变异系数分别为39%和45%,鄱阳湖Zn、Cr和Cd的变异系数为66%、49%和66%,其他元素的变异系数为10%～37%.结果表明,3个湖泊Cr和Cd的浓度在空间上有很大差别,浓度水平存在很大的不确定性.

2.2 Igeo、RI和TU分析

2.2.1geo分析 根据已收集到的数据,对地累积指数进行1000次模拟计算,计算3个湖泊沉积物中6种重金属元素,得到各重金属元素的geo指数,如图3所示.3个湖泊Cdgeo最高,巢湖沉积物中Cd处于轻度污染水平和偏中度污染水平占比分别为15.24%、84.76%,洞庭湖沉积物中Cd处于中度污染水平占比为58.41%,处于偏重度污染水平占比为32.64%,鄱阳湖沉积物中Cd中度污染及以上水平占比达到89.31%;除Cd外,巢湖和洞庭湖沉积物Zn Igeo最高,巢湖处于偏中度污染水平占比为12.72%;洞庭湖处于轻度污染水平占比为55.30%,其余元素均处于清洁或轻度污染水平;鄱阳湖沉积物Nigeo最高,处于轻度污染水平达到83.55%,其余元素均处于清洁或轻度污染水平.3个湖泊地累积指数显示的污染程度而言,鄱阳湖>洞庭湖>巢湖.

2.2.2 RI分析 根据统计数据,对3个湖泊沉积物重金属潜在生态风险进行1000次模拟计算,计算3个湖泊沉积物中6种重金属元素,得到RI,如图4、5所示.巢湖、洞庭湖和鄱阳湖RI值中Cd元素为主要贡献者,占比分别为80.26%、91.04%和90.03%,贡献值最低为Zn元素,分别为1.69%、0.51%和0.55%.其余元素贡献占比1.59%～4.90%,贡献值偏低.图5表明,巢湖重金属RI低风险概率为47.49%,中风险为52.51%,巢湖整体处于中低风险;洞庭湖重金属RI中风险概率为39.26%,高风险概率为60.74%,洞庭湖生态风险较高,整体处于中高风险;鄱阳湖重金属RI低风险、中风险和高风险概率分别为3.74%,27.31%和68.95%,鄱阳湖生态风险也较高.总体来看,鄱阳湖生态风险最高,洞庭湖次之,巢湖生态风险最低.

2.2.3 TU分析 针对3个湖泊沉积物中重金属的毒性特征,进行了1000次模拟计算,统计结果如图6、7所示.图6显示了不同金属元素的毒性对总毒性贡献,巢湖沉积物中重金属的总毒性依次为Pb、Cr、Zn、Ni、Cu和Cd;洞庭湖沉积物中重金属总毒性最高为Pb,其次为Cr,最低为Cu;鄱阳湖中重金属总毒性最高也为Pb,3个湖泊中Pb和Cr总毒性较高,表明3个湖泊Pb和Cr元素毒性较高.图7显示了3个湖泊沉积物总毒性的风险分布特征,巢湖沉积物中的重金属毒性低度毒性水平的累积概率为100%,处于低毒性水平,风险较低;洞庭湖沉积物中的重金属毒性低度毒性水平的累积概为30.97%,中度毒性水平的累积概率为69.03%,整体处于中低度毒性水平;鄱阳湖沉积物中的重金属毒性低度毒性水平的累积概率为92.82%,中度毒性水平的累积概率为7.18%,整体处于低度毒性水平.3个湖泊毒性水平:洞庭湖>鄱阳湖>巢湖.

3 湖泊重金属污染来源分析

3.1 巢湖重金属污染来源分析

巢湖处于位于安徽省江淮丘陵与长江之间,是“引江济淮”工程重要的链接点,与安徽主要城市合肥、巢湖等相接,其周边人类活动频繁,重金属污染情况复杂,来源多样.根据2.3结果分析可知,巢湖表层沉积物Igeo和RI分析中,Cd污染风险最高,其次是Zn;表层沉积物重金属TU分析中,Pb毒性最高,其次是Cr.研究表明[10],巢湖流域产业结构与水污染程度联系十分紧密,如合肥市电力、热力的生产和供应业、食品制造、有色金属冶炼及压延加工业、文教体育用品制造业、家具制造业、农林牧渔业等造成巢湖表层沉积物重金属污染问题.其中 Cd污染原因可能是流域内电镀工业企业污水未进入污水处理厂,直接进入南淝河,最终汇入巢湖[11];其次巢湖周边农业区生产中商品有机肥、农药以及农家肥大量投入产生Cd 排放,围湖造田等不良耕作更加剧了这一过程[83],水溶性肥料的使用也会带来超标的 Cd、As[84].巢湖周边交通干道密布,汽车润滑油的使用及金属分解会带来大量 Zn[85],造成巢湖Zn污染;汽车制动过程的器械摩擦、设备磨损均会产生Pb、Cr[86-87],造成巢湖Pb、Cr污染.巢湖重金属来源主要包括自然源、农业源、交通源、工业源,其中交通源占主体,其次为自然源,工业源整体贡献较小,主要是因为周边城市城市化刚刚抵达巢湖湖滨,滨湖工业体系构建不完全,但周边基础设施建设已展开,路网纵横、交通繁忙,进而成为主要污染贡献源[11].巢湖整体处于受人类活动影响的初步阶段,污染较轻,但仍要开展重金属的预防工作.

3.2 洞庭湖重金属污染来源分析

洞庭湖位于湖南省东北部,长江中游荆江南岸,是我国第二大淡水湖,受人类活动的影响,已经明显分化为东、西、南的3个湖区[51],是长江至关重要且拥有调蓄作用的湖泊.2.3的结果表明洞庭湖表层沉积物中Cdgeo和RI指数最高,污染较重;TU分析中Pb、Cr占比较高.研究表明[53]洞庭湖重金属污染主要来自与“四水”流域的人类活动.Cd含量较高的原因是有色金属采矿与冶炼工业,大量富含重金属的工业废水排放有关[88-89],其次洞庭湖流域处于南方喀斯特地貌区域,碳酸盐岩风化成土的巨大的岩/土体积变化以及Cd的地球化学性质,很容易导致Cd的相对富集,并在地表径流等自然搬运过程进入湖泊,此外围湖造田造成的水土流失等也增加了Cd的入湖通量[90].Pb除来自岩石风化外,流域上游Pb-Zn矿床矿石、煤和柴油燃烧等人为源也占一定比例,大气沉降也越来越成为沉积物中活动Pb的重要潜在来源[91].Cr和Ni受自然因素影响较大,主要与岩石的自然风化和侵蚀有关;但在一定程度上也受到了人为活动的影响,可能与沿岸生活污水以及湖区周边畜禽养殖废水和农业径流有关[89].洞庭湖重金属污染主要受人为活动影响,其主要来源包括工业源、自然源、农业和生活污水源,洞庭湖重金属污染的空间特征与洞庭湖输入河流和周边城市的特征密切相关,尤其是湘江沿岸大量的有色金属采矿和冶炼和岳阳市化工企业的发展[45].洞庭湖重金属整体处于中重度污染.因此,要综合考虑整个流域,制定污染控制和管理战略,优化相应城市的产业结构,逐步恢复洞庭湖水生系统.

3.3 鄱阳湖重金属污染来源分析

鄱阳湖流域广阔,遍布江西全省,主要的河流有修水、赣江、抚河、信江和饶河,又由湖口与长江接壤,是长江中下游平原重要的湖泊之一[92].根据2.3结果可知,鄱阳湖表层沉积物中Cd Igeo指数和RI指数占比最高,TU分析同样是Pb、Cr占比较高.研究表明[93]“五河”输入是入湖污染负荷的主要来源,其占污染负荷总量的80%左右,乐安河(饶河南支)中、下游的德兴铜矿、信江中游的永平铜矿、信江流经贵溪市大型有色金属冶炼厂、抚河上游的铀矿、赣南有色金属采矿区等携带大量工业废水进入鄱阳湖.湖区东南部德兴矿区已探明铅锌矿有数百万吨,在铜矿、铅锌矿开采和冶炼过程中会释放出Pb、Hg、Zn、Cu、As和Cd进入环境[94];其次鄱阳湖周边为江西传统农业大县南昌县和余干县,大量农药化肥的施用导致了Cd等重金属残留于土壤,通过降水、地表径流带入湖泊河流[56],流域内水土流失严重,土壤中肥料极易随地表径流进入鄱阳湖,也导致面源污染负荷增加[93].鄱阳湖重金属污染主要来自与工业源,农业源和自然源,其有大量有色金属采矿和冶炼废水对湖泊重金属贡献最高,其次为农药化肥的使用,自然源也对其有一定影响[16].当前鄱阳湖存在较大的重金属污染风险,应减少采矿冶炼等工业活动产生的污染物,提高开采冶炼水平,保护鄱阳湖生态环境.

4 结论

4.1 3个湖泊沉积物均存在不同程度的Cu、Zn、Pb、Ni、Cr和Cd污染,总体污染程度上,鄱阳湖>洞庭湖>巢湖.三个湖泊Cd Igeo最高;除Cd外,巢湖和洞庭湖沉积物Zn Igeo最高,鄱阳湖沉积物Ni Igeo最高.

4.2 巢湖、洞庭湖和鄱阳湖RI值中Cd元素为主要贡献者,占比分别为80.26%、91.04%和90.03%.巢湖RI整体处于中低风险,洞庭湖、鄱阳湖RI值高风险概率分别为60.74%、68.59%,生态风险较高.

4.3 三个湖泊沉积物毒性较高的是Pb和Cr,巢湖沉积物中的重金属毒性处于低毒性水平,洞庭湖沉积物重金属毒性低度、中度毒性水平的累积概分别为30.97%、69.03%,整体处于中度毒性水平,鄱阳湖沉积物中的重金属毒性低度、中度毒性水平的累积概率为92.82%、7.18%,整体处于低度毒性水平.

4.4 巢湖、洞庭湖、鄱阳湖重金属污染情况各不相同,重金属大体上存在3～4个不同来源工业源、交通源、农业源和自然源,巢湖交通源为主要影响,整体污染轻,应开展预防工作;洞庭湖和鄱阳湖主要污染源为工业活动,包括有色金属采矿和冶炼,化工企业生产等,污染较重,应综合考虑流域情况,提高有色金属开采和冶炼技术,逐步恢复流域生态环境.

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Mate analysis of heavy metal pollution in sediments of Chaohu Lake, Dongting Lake and Poyang Lake.

LI He, WANG Shu- hang, CHE Fei-fei, JIANG Xia, NIU Yong*

(National Engineering Laboratory for Lake Pollution Control and Eeological Restoration, State Environment Protection Key Laboratory for Lake Pollution Control, Chinese Research Academy of Environmental Sciences, Beijing 100012, China)., 2023,43(2)：831～842

The study analyzed the heavy metal concentrations of Chaohu Lake,Dongting Lake and Poyang Lake sediment from 2004 to 2021, and conduct the Monte Carlo uncertainty analysis of geoaccumulation, potential ecological risk and toxicity heavy metal of the three lakes to objectively and comprehensively describe the contamination degree. The results showed that,the three lakes were polluted by Cu, Zn, Pb, Ni, Cr and Cd in different degrees and followed with the order: Poyang Lake > Dongting Lake > Chaohu Lake. The geoaccumulation indices showed that Cd is the dominant pollutant in all three lakes, and the probabilities were 84.76% for moderatesediment contamination, in Chaohu Lake, 32.64% for heavy sediment contamination in Dongting Lake and 46.64% for heavy sediment contamination in Poyang Lake respectively. Cd contribute most to the potential ecological risks index (RI), and its proportion in the Chaohu lake, Dongting lake and Poyang lake were 80.26%、91.04% and 90.03%, respectively. Chaohu lake were at low-moderate risk, Dongting lake take the 60.74% possibility of high risk and Poyang lake take 68.95% possibility of high risk. Toxicity unit evaluation results indicated that Pb and Cr were the main contributor of toxicity in three Lakes sediment. The toxicity of heavy metals was observed the low level in the Chaohu lake and Dongting lake, but the moderate leve in Poyang lake with a 69.03% cumulative probability. The heavy metals of surface sediments in Chaohu lake, Dongting lake and Poyang Lake mainly derived from industry, transportation, agriculture and natural sources. The heavy metal contaminatio of Chaohu Lake mainly came from transportation, while Dongting lake and Poyang Lake mainly came from industry.

Chaohu lake；Dongting lake；Poyang lake；heavy metal；pollution assessment

X524

A

1000-6923(2023)02-0831-12

李 贺(1998-),男,山东聊城人,中国环境科学研究院硕士研究生,主要研究方向为湖泊沉积物重金属.

2022-06-27

国家自然科学基金资助项目(41807494)

* 责任作者, 副研究员, niu.yong@craes.org.cn