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宋波, 刘畅, 陈同斌. 广西土壤和沉积物砷含量及污染分布特征.自然资源学报,2017 32(4): 654-668
SONG Bo, LIU Chang, CHEN Tong-bin. Contents and Pollution Distribution Characteristics of Arsenic in Soils and Sediments in Guangxi Zhuang Autonomous Region. Journal of Natural Resources, 2017 32(4): 654-668  
doi: 10.11849/zrzyxb.20160508
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广西土壤和沉积物砷含量及污染分布特征
宋波1a,1b, 刘畅1a, 陈同斌1a,2,*
1. 桂林理工大学 a. 环境科学与工程学院,b. 广西环境污染控制理论与技术重点实验室,广西 桂林 541004
2. 中国科学院地理科学与资源研究所,北京100101

第一作者简介：宋波（1972- ）,男,教授,博士,研究方向为区域环境调查与风险评估、污染土壤修复。E-mail:songbo@glut.edu.cn

*通信作者简介：陈同斌（1963- ）,男,研究员,博士生导师,研究方向为植物修复、废弃物资源化利用、区域土壤环境质量与风险评估。E-mail:chentb@igsnrr.ac.cn

收稿日期: 2016-05-17
基金: 国家自然科学基金项目（41261082）; 广西自然科学基金项目（2013GXNSFEA053002）; 广西高等学校高水平创新团队及卓越学者计划项目（002401013001）; “八桂学者”建设工程专项经费
摘要

广西素有“有色金属之乡”美誉,土壤重金属污染问题较为突出。通过总结1989年以来相关文献,探讨了广西土壤和沉积物中砷含量及污染分布特征。3 045个和477个土壤和沉积物有效样点的统计分析表明,广西砷污染土壤主要分布于桂西北地区,尤其是刁江及金城江流域;矿业活动显著影响土壤砷积累,从其均值看：工矿区非农用土壤（140.5 mg/kg）>工矿区农用土壤（80.68 mg/kg）>非工矿区农用土壤（19.11 mg/kg）>城区土壤（18.35 mg/kg）,重度砷污染农用地样本均来自南丹;工矿区河流沉积物砷含量（283.5 mg/kg）远高于非工矿区,主要受影响区分布在刁江及大环江流域。为了控制环境风险,建议开展主要水系沉积物砷污染详查,加强南丹及周边区域污染防控和污染土壤修复。

关键词: 砷; 污染评价; 土壤; 沉积物; 广西
中图分类号:X53 文献标志码:A 文章编号:1000-3037(2017)04-0654-15
Contents and Pollution Distribution Characteristics of Arsenic in Soils and Sediments in Guangxi Zhuang Autonomous Region
SONG Bo1a,1b, LIU Chang1a, CHEN Tong-bin2,*
1. a. College of Environmental Science and Engineering, b. Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, China
2. Institute of Geographic Sciences and Natural Resources Research, CAS, Beijing 100101, China
Fund:National Natural Science Fondation of China, No.41261082; Guangxi Natural Science Foundation Program, No.2013GXNSFEA053002; High Level Innovation Team and Outstanding Scholar Program of Guangxi, No.002401013001; Special Funds for Construction Projects of Bagui Scholars
Abstract

Guangxi was known as “the hometown of nonferrous metals”, and the problem of heavy metal pollution in soil was very prominent. Based on the published papers about arsenic(As) in Guangxi since 1989 and our previous work in Guilin, Nandan and Huanjiang, this study explored the concentration and pollution distribution of As in soils and sediments in Guangxi. Totally, 3 045 soil samples and 477 sediment samples were collected. Results showed that: 1) In Guangxi, the As polluted soil mainly distributed in the northwest of Guangxi, especially in the Diaojiang and Jinchengjiang River basins. 2) Mining activity affected the accumulation of As in soil significantly. The soils with concentrations of As from high to low in order were non-agricultural soil in industrial and mining areas (140.5 mg/kg), agricultural soil in industrial and mining areas (80.68 mg/kg), agricultural soil in non-industrial and mining areas (19.11 mg/kg) and urban soil (18.35 mg/kg). Compared with the standard of soil environment quality in China (GB15618-1995), 89.4%, 69.0%, 18.7% and 12.1% of the above four types of soil samples exceeded the standard limit. The most seriously polluted samples in agricultural soil were all in Nandan. 3) The accumulation of As in marine sediments (8.76 mg/kg) and river sediments in non-industrial and mining areas (16.11 mg/kg) were not remarkable. As for river sediments, the pollution levels of As in industrial and mining areas (283.5 mg/kg) were much higher than those in non-industrial and mining areas. The affected areas mainly distributed in the Diaojiang and Dahuanjiang basins. In order to control the environmental risk, it is recommended to carry out the survey of As pollution in the surface sediments of the main river systems in Guangxi, especially in the river of Diaojiang, Dahuanjiang and Jinchengjiang, and the pollution in Nandan areas should be controlled and prevented and the contaminated soil should be repaired.

Key words: arsenic; pollution assessment; soil; sediment; Guangxi

在生物毒性显著的几种主要重金属及类金属元素中, 砷表现出其特殊的性质。在自然界中, 砷大多以硫化物的形式伴生于铜、铅、锌、锡、镍、金与钴矿中[1], 或与铁、铝、锰的氧化物和氢氧化物、粘土矿物、磷酸盐和碳酸盐矿物结合[2]。因此, 矿业活动常会引发环境砷污染问题。此外, 燃煤、木材处理过程中砷的释放及含砷化学品（除草剂、杀虫剂、防腐剂和肥料等）在环境中的长期积累也是造成砷污染与砷危害的重要原因[3, 4, 5]。事实上, 砷在生物体、空气、水体、土壤、沉积物中无处不在[6], 它是一种强有力的环境污染物和人类致癌物, 尤其是在水介质中[7]。土壤砷污染不仅影响土壤肥力、作物产量和品质, 且会通过食物链的生物放大作用对人体健康产生威胁。土壤中的砷可进入水体, 特别是雨季会加速表层土壤细粒中砷的迁移率[8], 从而影响地下水与地表水质量。姜勇等人研究发现, 污水灌溉使得农用土壤中的砷含量在2 a内达到了中国土壤环境质量Ⅲ 级标准规定的最大容量限制值[9]。

中国是世界上砷的高浓度聚集地之一, 砷污染问题及其对当地居民的健康威胁备受世界各国关注。广西是我国砷采出量最多的省区, 亦是我国砷潜在污染风险最大的地区[1]。

2000— 2009年, 广西砷中毒人数累计超过1 000人, 多因饮用含砷污染水源引起[10]。典型的喀斯特岩溶地貌使得母岩碳酸盐岩在成土过程中发生淋溶, 重金属易富集, 土壤中砷背景偏高。广西砷污染历史遗留问题突出, 现有工矿企业污染源集中且排放量大, 特别是河池地区, 大部分冶炼区周边土壤污染严重[11]。在总结前人研究的基础上, 本文通过ArcGIS描述了广西土壤和沉积物砷含量及污染分布特征。

1 材料与方法
1.1 研究区概况

广西地处云贵高原与东南沿海丘陵、平原的过渡带, 亚热带季风气候区, 雨量充沛, 地势由西北向东南倾斜, 地形破碎, 山地丘陵为主, 岩溶广布, 岸线曲折, 河流众多, 年径流量大。广西土壤成土因素复杂, 土壤类型多样, 以红壤、赤红壤为主。该区位于环太平洋成矿带西部, 有色金属、锰及非金属矿等都极丰富。从公开的文献资料中, 收集到土壤和沉积物有效样点数分别为3 045和477个（图1）。

图1 广西有色金属矿及土壤、沉积物、水体样点分布Fig. 1 Distribution of nonferrous metal ores and sampling sites of soil, sediment and water in Guangxi

1.2 研究方法

1.2.1 土壤砷污染评价

根据样本来源, 分非工矿区和工矿区进行讨论。对于工矿区土壤, 又分为非农用土壤、工矿区农用土壤; 对非工矿区土壤, 分城区土壤和农用土壤两种类型, 对工矿区非农用土壤、工矿区农用土壤、城区土壤采用《土壤环境质量标准》（GB15618— 1995）Ⅲ 级标准作为评价标准, 非工矿区农用土壤采用Ⅱ 级标准。计算公式如下：

P=CS（1）

式中：P为砷污染指数; C为样品砷实测值（mg/kg）; S为砷限量标准值（mg/kg）。分级标准：P≤ 1, 非污染; 1< P≤ 2, 轻微污染; 2< P≤ 3, 轻度污染; 3< P≤ 5, 中度污染; P> 5, 重度污染。

1.2.2 沉积物砷污染评价

对海洋沉积物, 以《海洋沉积物质量（GB 18668— 2002）》中一类标准为限量值, 采用单因子污染指数评价（式1）。对河流沉积物, 采用地累积指数法进行污染评价（式2）。

Igeo=log2CkB（2）

式中：C为研究区域沉积物砷含量的实测值; B为砷背景值（本研究采用桂林市、环江县及南丹县土壤背景值[12]）; k用于校正区域背景值差异（一般取常数1.5, 无量纲）。分级标准：Igeo≤ 0, 无污染; 0< Igeo≤ 1, 轻微污染; 1< Igeo≤ 2, 轻度污染; 2< Igeo≤ 3; 中度污染; 3< Igeo≤ 4 偏重污染; 4< Igeo≤ 5, 重污染; Igeo> 5 高度污染。

2 结果与分析
2.1 广西土壤砷含量特征

按照土地利用方式及其所在区域, 将土壤分工矿区非农用土壤、工矿区农用土壤、城区土壤、非工矿区农用土壤和自然土壤五类（表1）。对表1中55个有效样本平均值进行分析, 广西土壤砷含量范围、中值、均值、标准差、几何均值、几何标准差分别为5.28~1 490 mg/kg、29.2 mg/kg、120 mg/kg、281 mg/kg、38.9 mg/kg和1.67。工矿区非农用土壤、工矿区农用土壤、城区土壤、非工矿区农用土壤砷含量经对数转换后均符合正态分布, 有效样点数分别为142、733、113、2 057个, 算术均值分别为283.2、218.6、20.86、22.98 mg/kg, 几何均值分别为140.5、80.68、18.35、19.11 mg/kg。通过几何均值比较, 广西土壤砷含量表现为工矿区土壤> 非工矿区土壤, 其中工矿区非农用土壤> 工矿区农用土壤> 非工矿区农用土壤> 城区土壤。样本及样点超标率呈现相同的规律特征。

表1 广西部分土壤环境As含量状况 Table 1 Concentration of As in some soil situations in Guangxi

对于工矿区土壤, 非农用土壤（P=3.51）及农用土壤（P=2.01）分别遭受了中度污染与轻度污染。农用土壤重度污染样本均来自南丹, 占整个工矿区农用土壤样本的23.8%, 中度、轻度、轻微污染样本分别占工矿区农田土壤样本的14.3%、4.8%、19.1%。由图1不难发现, 南丹集中分布着大中规模砷矿、硫铁矿（伴生砷）、锑— 多金属矿、锡— 多金属矿及铅锌矿等[48, 49], 矿业活动显著影响土壤砷积累。对于非工矿区土壤, 城区土壤与农用土壤砷含量相差不大, 且均未超出土壤环境质量Ⅱ 级标准。

表2 广西不同类型土壤砷含量特征 Table 2 Characteristics of As in different types of soil in Guangxi
2.2 广西沉积物砷含量特征

广西境内河流众多, 主要有南盘江、西江、贺江、红水河、左江、右江, 柳江、黔江、郁江、浔江、桂江、漓江等, 分属4大水系。西江流域作为广西最大的一支水系, 贯穿广西, 流经广东后抵达珠江三角洲; 南部诸河流注入北部湾。广西北部湾位于我国南海西北部。现有对沉积物的研究, 可分为河流沉积物和海洋沉积物（表3）。

表3 广西沉积物采样环境及As含量状况 Table 3 Sampling environment of sediments and the concentrations of As in Guangxi

广西工矿区河流沉积物、非工矿区河流沉积物、海洋沉积物砷含量经对数转换后均符合正态分布, 研究区内有效样点数分别为106、28、345个, 算术均值分别为2 660、16.71、9.05 mg/kg, 几何均值分别为283.5、16.11、8.76 mg/kg（表4）。通过几何均值比较, 广西工矿区沉积物砷含量远高于非工矿区, 其中工矿区河流沉积物> 非工矿区河流沉积物> 海洋沉积物。与广西土壤砷背景值[15]、工业化前全球沉积物重金属最高背景值[70]及中国水系沉积物平均值[71]相比, 工矿区河流沉积物砷超标倍数分别为28、18、31, 整体污染态势严峻。

表4 广西不同类型沉积物As含量特征 Table 4 Concentrations of As in different types of sediments in Guangxi
2.3 广西土壤和沉积物砷污染空间分布

运用ArcGIS分别绘制土壤样本及样点、沉积物样点砷污染特征空间分布图（图2）。由图2可知, 现有对土壤砷的研究集中分布在南丹矿区、大环江流域、金城江区、百色市、都安县、桂林各县市及南宁市, 对沉积物砷的研究主要集中于漓江、大环江、刁江流域及北部湾近海海域。

就土壤样本均值而言, 中度— 重度污染样本集中分布于刁江流域上游、金城江流域及金秀县三角乡; 无污染样本主要分布于大环江流域、桂北及桂西南地区。

对比土壤样本砷高值污染特征, 中度— 重度污染高值样本集中分布于刁江、大环江及金城江流域。桂北、桂西南地区及贵港市出现了局部砷污染高值, 主要呈轻度— 轻微污染。

对比土壤样点污染特征不难发现, 重度污染样点集中分布于刁江及金城江流域, 且尽管桂林地区及都安县样本总体处于无污染状态, 个别样点仍呈现不同程度污染特征, 特别是都安县土壤流域性砷污染特征明显, 重度污染样点集中分布于刁江流域。

由图2(d)可知, 广西海洋沉积物并未受砷污染困扰。河流沉积物砷重度污染样本集中分布于刁江流域上游, 大环江沉积物主要受轻微— 轻度砷污染, 漓江沉积物处于清洁状态。

3 讨论与展望

众所周知, 广西是中国十大重点有色金属产区之一, 砷保有储量一度居全国首位。广西砷矿主要分有色金属伴生砷矿和以毒砂/雄黄为主矿的砷矿两类。前者见于南丹、钟山、靖西等地, 以大中型矿床为主, 矿业活动密集, 砷矿利用较小而多弃于尾矿; 后者分布于宾阳、河池等地, 均为中小型矿床, 多用于炼制砒霜[48, 72]。据研究, 广西锡-多金属、锑-多金属及铅锌矿矿床中常有大量砷伴生, 它们多分布于刁江流域上中游及大环江流域上游, 如南丹县大厂矿床、河池市五圩矿床及环江县北山矿床, 其中南丹县大厂矿田已有一千余年的开采历史, 是世界上公认最大的锡多金属矿田之一, 伴生砷含量大, 锡探明储量116.3万t, 砷矿石储量与之相当, 约113.7万t, 但砷矿并没有得到很好的利用, 尾矿中砷品味达到国家砷矿床工业品味指标[73, 74, 75]。1992年底, 大厂矿田年产锡已达 6 509 t, 采选矿石能力8 050 t/d, 年冶炼能力1万余t [73]。近年来, 广西建矿开采活动不断加剧, 全区矿山累计占用及破坏土地面积高达2万多hm2, 但矿产资源综合利用率低, 尾矿渣综合利用率不足16%, 尾矿渣的堆放不仅侵占土地且易造成水土污染, 长期氧化中的含砷尾矿易使砷在酸水中释放, 进入自然水系和农田, 危及人体健康[76, 77]。长期的矿业活动、尾矿渣的无序堆放、尾矿库的溃坝及人为与自然因素的相互作用, 使得南丹部分地区成为土壤与沉积物砷污染的重灾区。从图2不难看出, 与其它地方相比, 南丹土壤与沉积物中砷污染问题突出。

图2 广西土壤样本及样点、沉积物样点砷污染特征空间分布Fig. 2 Distribution of As contamination in soils and sediments of Guangxi

就土壤背景值而言, 广西土壤砷背景值在全国30个省、市及自治区（未包括香港、澳门、台湾和重庆）中排名第四位, 含量值略低于湖南省土壤砷背景值, 分别为全国土壤砷背景值及世界土壤砷[15]平均含量的1.5和2.2倍, 其中广西南丹县及环江县土壤砷背景值约为广西土壤砷背景值的1.6和1.5倍。南丹及环江土壤本身砷含量值偏高, 加之频繁的矿业活动, 使得矿区周边土壤砷含量显著增加。特别是南丹大厂和车河镇土壤与沉积物存在不同程度的砷污染问题, 当地居民的生活与生存条件受到挑战。随着时间的推移, 南丹县局部区域土壤砷含量有增加的风险, 而且即使在矿山关闭后, 大范围的环境污染仍会持续。南丹有色金属矿业经济区, 作为广西六大矿业经济区之一, 包含大厂、芒场、五圩三个矿田, 矿点总数超过200处, 根据规划, 它们仍将为广西经济发展服务, 而矿业活动与当地环境污染问题在很长一段时间内都会成为人们关注的焦点[77]。

从现有文献看, 以下几点问题值得思考：1）矿区土壤污染问题相比其他地区应最先提上日程。大量研究表明, 采矿作业易造成当地土壤砷含量升高, 土壤酸化, 地表水与地下水砷污染, 亦对当地居民健康状况构成了较大的威胁[78, 79, 80, 81, 82, 83]; 2）建议开展主要水系沉积物砷污染详查。沉积物是一个危险信号, 它既是上游环境释放出来的重金属的汇, 也是水体重金属的源, 尤其在受到人为扰动的情况下, 会对下游居民的饮用水安全构成威胁, 还会影响水系水生生物的生存环境, 且污染一旦发生后的破坏性大、影响深远; 3）污染区大气颗粒物砷含量需引起足够重视。张新英等对南丹矿区环境中重金属的分析表明, 该地区土壤污染的主要途径为大气颗粒物的沉降[22]。殷汉琴等人认为, 大气沉降对土壤及蔬菜砷的富集有不同程度的贡献作用[84, 85, 86]。大气沉降输入土壤中的重金属含量为工矿区> 城区[87]。相对于土壤、水体、生物体等主要运输途径, 大气颗粒污染物在运输非挥发性污染物中具有更大的潜力, 由于空气团并不局限于一个明显的地形边界, 也不存在妨碍污染物运输的障碍, 这加快了污染物的运输速度, 污染范围更加广泛[88]。

4 结论

广西土壤砷含量总体并未超过土壤环境质量Ⅲ 级标准（40 mg/kg）, 但刁江及金城江流域局部砷污染程度较高。广西工矿区土壤砷含量显著高于非工矿区土壤, 特别是南丹地区显示出比其他地方更高的砷污染特征, 重度砷污染农用土壤均来自南丹。广西海洋沉积物及非工矿区河流沉积物无明显砷积累, 沉积物砷偏重— 高度污染样本集中分布于刁江及金城江流域, 大环江流域沉积物受轻微砷污染。考虑到刁江大环江上游频繁的矿业活动及尾矿库溃坝事故, 尽管矿业活动影响区土壤砷背景值普遍较高, 但采矿活动引发的环境污染更为突出。为了控制环境风险, 建议加强南丹及周边区域污染防控和污染土壤修复, 并开展主要水系沉积物砷污染详查。

The authors have declared that no competing interests exist.

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