煤矸石堆场地下水污染特征及成因研究

赵子千; 沙浩群; 黄赳; 何小松; 潘琦; 柳榭阳

doi:10.12153/j.issn.1674-991X.20221129

煤矸石堆场地下水污染特征及成因研究

doi: 10.12153/j.issn.1674-991X.20221129

1.
国家环境保护地下水污染模拟与控制重点实验室, 中国环境科学研究院
2.
中国矿业大学环境与测绘学院

基金项目: 国家重点研发计划项目(2020YFC1806503)

详细信息

作者简介:
赵子千（1998—），男，硕士研究生，研究方向为地下水污染修复，2316335361@qq.com

通讯作者:
何小松（1982—），男，研究员，博士，主要从事固体废物处理处置与地下水污染控制研究，hxss82@126.com

中图分类号: X523
计量
- 文章访问数: 394
- HTML全文浏览量: 136
- PDF下载量: 76
- 被引次数: 0
出版历程
- 收稿日期: 2022-11-11
- 录用日期: 2023-05-21
- 修回日期: 2023-04-11
- 网络出版日期: 2023-09-20

Study on the characteristics and causes of groundwater pollution in coal gangue dumps

1.
State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Sciences
2.
School of Environment and Spatial Informatics, China University of Mining and Technology

摘要

摘要:
选择山西太原典型矿矸石堆场，采集自燃程度不同的煤矸石及其周边受污染地下水，测定其中重金属、无机盐和有机物组成与浓度，并基于统计学分析探究地下水污染来源。结果显示：矸石浸提液和堆场下山腰自流出的地下水，重金属Cd、Pb、As、Zn未污染，但Cr和Ni达到轻度污染；浸提液SO₄ ²⁻、Fe、Mn浓度较高，SO₄ ²⁻浓度高达5 982 mg/L，Fe浓度超过GB/T 14848—93《地下水质量标准》Ⅳ类标准限值1 081倍、Mn超标19倍。污染源解析显示，矸石堆场自流出的地下水Na⁺、K⁺、Cl⁻、NO₃ ⁻主要来自土壤和含水层介质，但SO₄ ²⁻、Fe、Mn、Cd、Zn、As、Cr、Ni主要来源于矸石浸出；不同的煤矸石污染浸出能力表现为正在自燃的矸石>自燃完全的矸石>新鲜矸石。矸石的自燃过程会强化污染物的释放，在矸石渗滤液迁移过程中，重金属污染快速衰减，但SO₄ ²⁻、Ni、Mn仍具有一定的风险，超过GB/T 14848—93Ⅳ类标准。
- 矸石山 /
- 渗滤液 /
- 地下水 /
- 重金属 /
- 硫酸盐
Abstract:
The stock of coal gangue in China is large, and it still increases rapidly, posing a high risk on the environment. However, the effect of the self-ignition degree of coal gangue on the release of leachates pollutant is unclear, and the information on the natural attenuation of these leachate pollutants is limited. The coal gangue with different self-ignition degrees and the contaminated groundwater were collected from a typical coal gangue dump site in Taiyuan City, Shanxi Province. The composition and concentration of heavy metals, inorganic salts and organic compounds in coal gangue and groundwater were investigated, and the sources of groundwater pollution were explored based on statistical analysis. The results showed that the gangue extracts and groundwater flowing from the mountainside below the gangue dump were not contaminated by Cd, Pb, As, and Zn, though they had been lightly polluted by Cr and Ni. The concentrations of SO₄ ²⁻, Fe, and Mn were high in the extracts, with SO₄ ²⁻ concentration of 5 982 mg/L and Fe and Mn concentrations of 1 081 and 19 times higher than the groundwater Ⅳ quality standard specified in Quality Standard for Ground (GB/T 14848-93), respectively. According to the pollution source analysis, it could be obtained that Na⁺, K⁺, Cl⁻ and NO₃ ⁻ in groundwater near the gangue dump sites mainly originated from soil and aquifer medium, while SO₄ ²⁻, Fe, Mn, Cd, Zn, As, Cr, and Ni were mainly released from gangue leaching. The pollution release of the coal gangue with different self-ignition degrees was as follows: burning gangue > burned gangue > fresh gangue. The self-ignition of coal gangue contributed to the release of pollution. Natural attenuation of heavy metal significantly occurred during the migration process of gangue leachates. However, the concentration of SO₄ ²⁻, Ni, and Mn still had certain risks, exceeding Class Ⅳ groundwater standard specified in GB/T 14848-93.
- coal gangue /
- leachate /
- groundwater /
- heavy metal /
- sulphate sulfate

HTML全文

图 1 污染点位布设示意

Figure 1. Schematic diagram of location layout of pollution points

下载: 全尺寸图片幻灯片

图 2 矸石浸提液与地下水中碱与碱土金属浓度分布

Figure 2. Distribution of alkali and alkaline earth metals in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 3 矸石浸提液与地下水中无机阴离子分布

Figure 3. Distribution of inorganic anions in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 4 矸石浸提液与地下水中重金属元素分布

注：黑色虚线为GB/T 14848—93 Ⅳ类标准。全文同。

Figure 4. Distribution of heavy metal elements in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 5 矸石浸提液与地下水中特征污染物分布

Figure 5. Distribution of characteristic pollutants in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 6 矸石浸提液与地下水中有机物组成特征

Figure 6. Composition characteristics of organic matter in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 7 矸石浸提液与地下水中有机物的三维荧光光谱

Figure 7. Three-dimensional fluorescence spectra of organic matter in gangue extract and groundwater

下载: 全尺寸图片幻灯片

图 8 不同污染物的相关性分析

注：*、**分别表示在0.1、0.05水平相关性显著。

Figure 8. Correlation analysis of different pollutants

下载: 全尺寸图片幻灯片

图 9 矸石浸提液与地下水样品的主成分分析

Figure 9. Principal component analysis of gangue extract and groundwater samples

下载: 全尺寸图片幻灯片

表 1 矸石浸提液与地下水中污染物不同组分载荷

Table 1. Different component loads of pollutants in gangue extract and groundwater

指标	主成分1	主成分2	主成分3	主成分4
Na⁺	−0.302	0.928	−0.051	−0.036
K⁺	−0.136	0.913	0.048	−0.177
Ca²⁺	0.391	0.546	0.669	−0.190
Mg²⁺	0.230	0.597	0.596	−0.422
SO₄ ²⁻	0.907	0.217	0.351	−0.047
Cl⁻	−0.411	0.511	−0.290	−0.505
NO³⁻	−0.430	−0.051	−0.113	−0.643
HCO₃ ⁻	0.392	0.480	0.225	0.548
Mn	0.865	0.315	0.345	0.147
Fe	0.972	−0.047	0.057	0.041
Zn	0.943	−0.131	0.214	0.060
pH	−0.431	0.386	−0.743	−0.301
Cr	0.974	−0.104	0.190	−0.013
Ni	0.888	−0.194	0.399	−0.036
As	0.985	−0.124	0.112	0.020
Cd	0.862	−0.213	0.451	−0.038
Pb	−0.167	−0.331	0.104	0.848
COD	0.684	0.634	0.226	0.183
FI	−0.213	−0.062	−0.142	0.939
HIX	−0.381	−0.129	−0.875	−0.180

下载: 导出CSV

参考文献(45)

[1]	何振嘉.矸石山对生态环境的影响及对策研究[J]. 煤炭技术,2020,39(3):37-38. HE Z J. Study on influence of waste rock hill on ecological environment and countermeasures[J]. Coal Technology,2020,39(3):37-38.
[2]	张保留, 王健, 吕连宏, 等.对资源型城市能源转型的思考: 以太原市为例[J]. 环境工程技术学报,2021,11(1):181-186. ZHANG B L, WANG J, LÜ L H, et al. Thoughts on energy transformation of resource-based cities: taking Taiyuan City as an example[J]. Journal of Environmental Engineering Technology,2021,11(1):181-186.
[3]	李红霞. 清水河流域煤矿区重金属的表生环境特征及潜在修复途径[D]. 北京: 北京科技大学, 2020.
[4]	周楠, 姚依南, 宋卫剑, 等.煤矿矸石处理技术现状与展望[J]. 采矿与安全工程学报,2020,37(1):136-146. ZHOU N, YAO Y N, SONG W J, et al. Present situation and prospect of coal gangue treatment technology[J]. Journal of Mining & Safety Engineering,2020,37(1):136-146.
[5]	NÁDUDVARI Á, KOZIELSKA B, ABRAMOWICZ A, et al. Heavy metal- and organic-matter pollution due to self-heating coal-waste dumps in the Upper Silesian Coal Basin (Poland)[J]. Journal of Hazardous Materials,2021,412:125244. doi: 10.1016/j.jhazmat.2021.125244
[6]	NAIDU G, RYU S, THIRUVENKATACHARI R, et al. A critical review on remediation, reuse, and resource recovery from acid mine drainage[J]. Environmental Pollution,2019,247:1110-1124. doi: 10.1016/j.envpol.2019.01.085
[7]	DAI S F, REN D Y, CHOU C L, et al. Geochemistry of trace elements in Chinese coals: a review of abundances, genetic types, impacts on human health, and industrial utilization[J]. International Journal of Coal Geology,2012,94:3-21. doi: 10.1016/j.coal.2011.02.003
[8]	徐双喜, 张众志, 杜晓惠, 等.京津冀及周边民用散煤燃烧控制对北京市PM_2.5的影响[J]. 环境科学研究,2021,34(12):2876-2886. XU S X, ZHANG Z Z, DU X H, et al. Impact of residential coal combustion control in Beijing-Tianjin-Hebei and surrounding region on PM_2.5 in Beijing[J]. Research of Environmental Sciences,2021,34(12):2876-2886.
[9]	姜华, 李艳萍, 高健.双碳背景下煤基产业绿色低碳转型之路[J]. 环境工程技术学报,2022,12(5):1580-1583. JIANG H, LI Y P, GAO J. The road of green and low-carbon transformation of coal-based industry under carbon peak and carbon neutrality background[J]. Journal of Environmental Engineering Technology,2022,12(5):1580-1583.
[10]	梁宏伟.煤矸石堆放地周边地下水环境污染特性及评价[J]. 江西煤炭科技,2019(4):79-83. LIANG H W. Polluting properties and evaluation of groundwater environment around gangue stocking area[J]. Jiangxi Coal Science & Technology,2019(4):79-83.
[11]	XIONG Q, YANG J S, XIONG H G. Analysis of leaching and soaking experiments on coal gangues as A roadbed filling material[J]. Journal of Changsha University of Science & Technology,2008,5:93-97.
[12]	郑刘根, 丁帅帅, 刘丛丛, 等.不同类型煤矸石中环境敏感性微量元素淋滤特性[J]. 中南大学学报(自然科学版),2016,47(2):703-710. ZHENG L G, DING S S, LIU C C, et al. Leaching characteristics of environmentally sensitive trace elements in different types of coal gangue[J]. Journal of Central South University (Science and Technology),2016,47(2):703-710.
[13]	谢宏全, 张光灿.煤矸石山对生态环境的影响及治理对策[J]. 北京工业职业技术学院学报,2002,1(3):27-30. XIE H Q, ZHANG G C. Ecological environment effects and administering countermeasures of coalmine tips[J]. Journal of Beijing Vocational & Technical Institute of Industry,2002,1(3):27-30.
[14]	WANG X W, ZHONG N N, HU D M, et al. Polycyclic aromatic hydrocarbon (PAHs) pollutants in groundwater from coal gangue stack area: characteristics and origin[J]. Water Science and Technology: a Journal of the International Association on Water Pollution Research,2009,59(5):1043-1051. doi: 10.2166/wst.2009.050
[15]	RIGOL A, MATEU J, GONZÁLEZ-NÚÑEZ R, et al. pH_stat vs. single extraction tests to evaluate heavy metals and arsenic leachability in environmental samples[J]. Analytica Chimica Acta,2009,632(1):69-79. doi: 10.1016/j.aca.2008.10.066
[16]	李宛霖. 煤矸石多金属提取过程及固化机理研究[D]. 昆明: 昆明理工大学, 2019.
[17]	ZHOU C C, LIU G J, WU D, et al. Mobility behavior and environmental implications of trace elements associated with coal gangue: a case study at the Huainan Coalfield in China[J]. Chemosphere,2014,95:193-199. doi: 10.1016/j.chemosphere.2013.08.065
[18]	RIBEIRO J, FERREIRA Da SILVA E, LI Z, et al. Petrographic, mineralogical and geochemical characterization of the Serrinha coal waste pile (Douro Coalfield, Portugal) and the potential environmental impacts on soil, sediments and surface waters[J]. International Journal of Coal Geology,2010,83(4):456-466. doi: 10.1016/j.coal.2010.06.006
[19]	ZHOU C C, LIU G J, WU S C, et al. The environmental characteristics of usage of coal gangue in bricking-making: a case study at Huainan, China[J]. Chemosphere,2014,95:274-280. doi: 10.1016/j.chemosphere.2013.09.004
[20]	SMOŁKA-DANIELOWSKA D. Heavy metals in fly ash from a coal-fired power station in Poland[J]. Polish Journal of Environmental Studies,2006,15(6):943-946.
[21]	BISWAS A, HENDRY M J, ESSILFIE-DUGHAN J. Geochemistry of arsenic in low sulfide-high carbonate coal waste rock, Elk Valley, British Columbia, Canada[J]. Science of the Total Environment,2017,579:396-408. doi: 10.1016/j.scitotenv.2016.11.084
[22]	KRUSZEWSKI Ł. Secondary sulphate minerals from Bhanine Valley coals (South Lebanon): a crystallochemical and geochemical study[J]. Geological Quarterly,2019,63:65-87.
[23]	ESSILFIE-DUGHAN J, HENDRY M J, DYNES J J, et al. Geochemical and mineralogical characterization of sulfur and iron in coal waste rock, Elk Valley, British Columbia, Canada[J]. Science of the Total Environment,2017,586:753-769. doi: 10.1016/j.scitotenv.2017.02.053
[24]	LEE P K, KANG M J, CHOI S H, et al. Sulfide oxidation and the natural attenuation of arsenic and trace metals in the waste rocks of the abandoned Seobo tungsten mine, Korea[J]. Applied Geochemistry,2005,20(9):1687-1703. doi: 10.1016/j.apgeochem.2005.04.017
[25]	VRIENS B, SEIGNEUR N, MAYER K U, et al. Scale dependence of effective geochemical rates in weathering mine waste rock[J]. Journal of Contaminant Hydrology,2020,234:103699. doi: 10.1016/j.jconhyd.2020.103699
[26]	HUGUET A, VACHER L, RELEXANS S, et al. Properties of fluorescent dissolved organic matter in the Gironde Estuary[J]. Organic Geochemistry,2009,40(6):706-719. doi: 10.1016/j.orggeochem.2009.03.002
[27]	RILEY K W, FRENCH D H, FARRELL O P, et al. Modes of occurrence of trace and minor elements in some Australian coals[J]. International Journal of Coal Geology,2012,94:214-224. doi: 10.1016/j.coal.2011.06.011
[28]	SEREDIN V V, FINKELMAN R B. Metalliferous coals: a review of the main genetic and geochemical types[J]. International Journal of Coal Geology,2008,76(4):253-289. doi: 10.1016/j.coal.2008.07.016
[29]	DAI S F, SEREDIN V V, WARD C R, et al. Composition and modes of occurrence of minerals and elements in coal combustion products derived from high-Ge coals[J]. International Journal of Coal Geology,2014,121:79-97. doi: 10.1016/j.coal.2013.11.004
[30]	KŘÍBEK B, SÝKOROVÁ I, VESELOVSKÝ F, et al. Trace element geochemistry of self-burning and weathering of a mineralized coal waste dump: the Novátor Mine, Czech Republic[J]. International Journal of Coal Geology,2017,173:158-175. doi: 10.1016/j.coal.2017.03.002
[31]	PANG L S K, WILSON M A. Nanotubes from coal[J]. Energy & Fuels,1993,7(3):436-437.
[32]	陈飞. 地表水环境质量标准中有机物荧光特性及应急处理[D]. 杭州: 浙江工业大学, 2016.
[33]	ACHTEN C, HOFMANN T. Native polycyclic aromatic hydrocarbons (PAH) in coals: a hardly recognized source of environmental contamination[J]. Science of the Total Environment,2009,407(8):2461-2473. doi: 10.1016/j.scitotenv.2008.12.008
[34]	曹津津. 生物碱类化合物荧光性质与分子结构的关系及分析方法研究[D]. 石家庄: 河北师范大学, 2019.
[35]	尹丹丹, 吴静, 谢超波, 等.同分异构体菲与蒽三维荧光特征的比较[J]. 光谱学与光谱分析,2013,33(12):3263-3268. doi: 10.3964/j.issn.1000-0593(2013)12-3263-06 YIN D D, WU J, XIE C B, et al. Comparison of three-dimensional fluorescence characteristics of two isomers: phenanthrene and anthrancene[J]. Spectroscopy and Spectral Analysis,2013,33(12):3263-3268. doi: 10.3964/j.issn.1000-0593(2013)12-3263-06
[36]	李庆霞, 刘亚轩, 陈卫明, 等.荧光光谱法分析油气化探样品中的芳烃[J]. 岩矿测试,2014,33(4):561-569. doi: 10.3969/j.issn.0254-5357.2014.04.018 LI Q X, LIU Y X, CHEN W M, et al. Analysis of aromatic hydrocarbons in oil and gas geochemical exploration samples by fluorescence spectrometry[J]. Rock and Mineral Analysis,2014,33(4):561-569. doi: 10.3969/j.issn.0254-5357.2014.04.018
[37]	RIBEIRO J, SILVA T, FILHO J G M, et al. Polycyclic aromatic hydrocarbons (PAHs) in burning and non-burning coal waste piles[J]. Journal of Hazardous Materials,2012,199/200:105-110. doi: 10.1016/j.jhazmat.2011.10.076
[38]	GRAEDEL T E, HAWKINS D T, CLAXTON L D. Atmospheric chemical compounds: sources, occurrence, and bioassay[M]. Orlando: Academic Press, 1986
[39]	SILVA L F O, IZQUIERDO M, QUEROL X, et al. Leaching of potential hazardous elements of coal cleaning rejects[J]. Environmental Monitoring and Assessment,2011,175(1):109-126.
[40]	SWAINE D J. Trace elements in coal and their dispersal during combustion[J]. Fuel Processing Technology,1994,39(1/2/3):121-137.
[41]	FINKELMAN R B. Modes of occurrence of environmentally-sensitive trace elements in coal[M]//Environmental aspects of trace elements in coal. Dordrecht: Springer, 1995: 24-50.
[42]	RIBEIRO J, Da SILVA E F, FLORES D. Burning of coal waste piles from Douro Coalfield (Portugal): petrological, geochemical and mineralogical characterization[J]. International Journal of Coal Geology,2010,81(4):359-372. doi: 10.1016/j.coal.2009.10.005
[43]	VASSILEV S V, VASSILEVA C G. Geochemistry of coals, coal ashes and combustion wastes from coal-fired power stations[J]. Fuel Processing Technology,1997,51(1/2):19-45.
[44]	ZHAO Y C, ZHANG J Y, SUN J M, et al. Mineralogy, chemical composition, and microstructure of ferrospheres in fly ashes from coal combustion[J]. Energy & Fuels,2006,20(4):1490-1497.
[45]	GLUSKOTER H J, LINDAHL P C. Cadmium: mode of occurrence in Illinois coals[J]. Science,1973,181(4096):264-266. ⊕ doi: 10.1126/science.181.4096.264