Pollution Characteristics of Toxic and Harmful Elements and Its Environmental Impact in Water Co-Produced from Coalbed Methane Wells in the CBM Development Block in Western Guizhou
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摘要: 由于含煤地层不同程度地富集氟、砷、镉、铬、汞和锑等多种有毒有害元素，煤层气开发过程中的大量产出水会对表生生态环境构成严重威胁.对贵州西部某煤层气开发区块产出水的水化学特征进行了系统研究，结果表明：与地下水质量标准（GB/T 14848-2017）Ⅲ类水质相比，研究区煤层气产出水中Ba和Hg严重超标，平均含量分别达到10 621.6 μg/L和16.5 μg/L.较强的硫酸盐还原作用导致地层水中硫酸盐被耗尽，含Ba碳酸盐矿物的溶解进而造成产出水表现出明显的Ba异常.Hg主要来源于含煤地层中的硫化物，而硫化物和碳酸盐矿物的溶解是Cr、Mo、Cd和Sb四种元素的主要来源；较高浓度的Mo与离子交换反应有关，并可能以铁锰氧化物和氢氧化物、硫代钼酸盐和钼的金属硫化物等形式存在；Al的氢氧化物吸附态是产出水中Cr、Mo、Mn、Cd、Sb、Cd、Cu、Pb和Ba的主要赋存形态；Ni主要来源于煤有机质的矿化.水质评价结果显示，研究区煤层气产出水的污染状况极为严重；其中，Hg在SH9煤层气井中超标27倍，而Ba在SH8煤层气井中超标23倍.Abstract: Coal seams are often enriched in various toxic and harmful elements such as F, As, Cd, Cr, Ni, Pb, Hg and Sb, so the ecosystem might be faced with serious environmental threats when the co-produced water is brought to the surface in the production of coalbed methane (CBM). In this paper, we present a systematic water chemistry study of co-produced water from Songhe coalbed methane development block in western Guizhou Province. The results show that, compared to Class Ⅲ of Groundwater Quality Standard (GB/T 14848-2017), Ba and Hg in co-produced water in the study area exceeded the standard seriously, and the average concentrations were 10 621.6 μg/L and 16.5 μg/L, respectively. The Ba anomaly in co-produced water was attributed to the dissolution of Ba-bearing carbonates and the depletion of sulfate induced by sulfate reduction, and Hg was from sulfide minerals. The sources for Cr, Mo, Cd and Sb were sulfides and carbonates in coal seams. The high content of Mo is associated with ion exchange reactions under high salinity, and molybdate and metallic sulfides are the main forms for Mo. Under weak alkaline conditions, the hydroxide adsorption state of Al is the main occurrence form of Cr, Mo, Mn, Cd, Sb, Cd, Cu, Pb and Ba in the co-produced water. The sources of Ni were obviously different from those of other elements, and it most likely came from the mineralization of coal organic matters. The results of water quality evaluation showed that the pollution of the water coproduced from coalbed methane wells in the study area is very serious, which is mainly due to the serious overstandard of Hg and Ba. In SH9, mercury is 27 times the legal limits and that is 23 times for barium in SH8.
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图 2 研究区煤层气产出水重金属组分聚类分析图
Fig. 2. Pearson cluster analysis diagram for different heavy metals in co-produced water in the study area
图 3 研究区煤层气产出水Ba2+含量与Na+、Sr2+、Cl-和TDS的关系
Fig. 3. The relationships between Ba2+ and Na+, Sr2+, Cl- and TDS
图 4 研究区煤层气产出水重金属污染程度
Fig. 4. The pollution degree of different heavy metals in co-produced water in the study area
表 1 研究区煤层气产出水重金属含量
Table 1. The trace elements contents in coalbed methane co-produced water in the study area
采样点 pH Eh As
(μg/L)Cd
(μg/L)Cr
(μg/L)Pb
(μg/L)Hg
(μg/L)Al
(μg/L)Fe
(μg/L)Mn
(μg/L)Cu
(μg/L)Zn
(μg/L)Sb
(μg/L)Ba
(μg/L)Be
(μg/L)Mo
(μg/L)Ni
(μg/L)SH1 7.13 -85 0.5 0.0 0.3 1.5 5.4 32.1 2 831.9 244.6 0.4 33.3 8.3 9 068.3 0.1 9.2 0.6 SH2 7.71 -133 0.7 0.2 0.1 1.4 22.7 45.5 60.0 67.9 0.0 18.5 4.7 6 283.7 0.0 11.7 0.0 SH3 7.71 -127 1.6 0.1 0.1 1.4 21.3 28.7 64.6 20.4 0.0 112.6 4.1 9 090.7 0.1 8.7 9.9 SH4 7.89 68 1.1 0.1 0.4 3.7 18.0 42.1 59.5 36.2 0.0 51.4 3.0 6 635.0 0.0 6.9 10.8 SH5 8.27 33 0.9 0.1 2.2 4.9 8.2 112.7 104.5 47.8 0.3 118.6 2.7 9 303.3 0.0 12.4 6.6 SH6 8.22 16 1.3 0.1 2.3 3.7 7.1 51.6 652.5 170.2 0.2 476.3 2.2 13 679.5 0.0 17.2 0.7 SH7 8.21 39 1.3 1.1 126.4 9.3 14.1 267.5 144.2 185.2 3.4 110.1 12.4 14 786.0 0.3 633.4 1.2 SH8 8.25 -76 1.4 2.0 247.7 10.6 24.8 274.6 115.6 286.8 1.2 101.1 21.4 16 224.8 0.1 1 318.4 1.3 SH9 8.48 -99 1.0 2.4 247.0 3.8 27.4 231.4 95.1 232.4 1.3 244.7 20.8 10 523.3 0.0 1 367.7 1.0 平均值 7.99 -40 1.1 0.7 69.6 4.5 16.5 120.7 458.7 143.5 0.7 140.7 8.8 10 621.6 0.0 376.2 3.6 地下水质量Ⅲ类水质标准GB/T 14848-2017 6.5~8.5 10 5 50 10 1 200 300 100 1 000 1 000 5 700 2 70 20 
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表 2 研究区煤层气产出水重金属相关关系
Table 2. Correlation matrix of different trace elements in coalbed methane co-produced water in the study area
pH Be Al Cr Mn Fe Ni Cu Zn As Mo Cd Sb Ba Hg Pb pH 1.00 Be 0.03 1.00 Al 0.67 0.52 1.00 Cr 0.60 0.24 0.90 1.00 Mn 0.14 0.27 0.62 0.71 1.00 Fe -0.71 0.02 -0.34 -0.27 0.41 1.00 Ni -0.08 -0.19 -0.39 -0.40 -0.74 -0.32 1.00 Cu 0.41 0.84 0.83 0.60 0.52 -0.12 -0.43 1.00 Zn 0.52 -0.19 0.05 0.10 0.21 -0.10 -0.24 0.00 1.00 As 0.48 0.35 0.35 0.31 -0.05 -0.58 0.33 0.24 0.34 1.00 Mo 0.59 0.21 0.89 1.00 0.70 -0.27 -0.40 0.58 0.11 0.30 1.00 Cd 0.61 0.20 0.88 0.99 0.68 -0.29 -0.41 0.59 0.12 0.28 1.00 1.00 Sb 0.40 0.27 0.85 0.97 0.79 -0.08 -0.47 0.58 -0.03 0.18 0.97 0.96 1.00 Ba 0.51 0.53 0.73 0.62 0.69 -0.07 -0.44 0.64 0.45 0.55 0.60 0.55 0.56 1.00 Hg 0.32 -0.08 0.40 0.61 0.04 -0.61 0.04 0.08 -0.21 0.34 0.62 0.64 0.58 -0.02 1.00 Pb 0.59 0.57 0.86 0.67 0.49 -0.33 -0.22 0.73 0.03 0.45 0.64 0.60 0.59 0.82 0.15 1.00
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表 3 研究区煤层气产出水重金属水质评价结果
Table 3. Evaluation results of heavy metal quality of coalbed methane co-produced water in the study area
样品编号 单因子评价法相对污染程度值 内梅罗指数法 As Cd Cr Pb Hg Al Fe Mn Cu Zn Sb Ba Be Mo Ni S值 评价结果 SH1 0.05 0.01 0.01 0.15 5.40 0.16 9.44 2.45 0.00 0.03 1.66 12.95 0.03 0.13 0.03 9.29 极差 SH2 0.07 0.04 0.00 0.14 22.65 0.23 0.20 0.68 0.00 0.02 0.95 8.98 0.00 0.17 0.00 16.10 极差 SH3 0.16 0.01 0.00 0.14 21.25 0.14 0.22 0.20 0.00 0.11 0.82 12.99 0.03 0.12 0.50 15.13 极差 SH4 0.11 0.01 0.01 0.37 18.00 0.21 0.20 0.36 0.00 0.05 0.60 9.48 0.00 0.10 0.54 12.81 极差 SH5 0.09 0.02 0.04 0.49 8.20 0.56 0.35 0.48 0.00 0.12 0.54 13.29 0.00 0.18 0.33 9.47 极差 SH6 0.13 0.02 0.05 0.37 7.13 0.26 2.18 1.70 0.00 0.48 0.45 19.54 0.00 0.25 0.04 13.90 极差 SH7 0.13 0.22 2.53 0.93 14.11 1.34 0.48 1.85 0.00 0.11 2.47 21.12 0.13 9.05 0.06 15.16 极差 SH8 0.14 0.40 4.95 1.06 24.79 1.37 0.39 2.87 0.00 0.10 4.28 23.18 0.03 18.83 0.07 17.96 极差 SH9 0.10 0.48 4.94 0.38 27.38 1.16 0.32 2.32 0.00 0.24 4.17 15.03 0.00 19.54 0.05 19.69 极差
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表 4 不同国际机构最大可接受风险和可忽略水平
Table 4. Maximum acceptable risk and negligible levels for different international institutions
机构 最大可接受（a-1） 可忽略水平（a-1） 国际辐射防护委员会 5×10-5 国际原子能机构 5×10-7 美国环境保护局 1×10-4 瑞典环保局 1×10-6 英国皇家协会 1×10-6 1×10-7 荷兰建设环保局 1×10-6 1×10-8 注：据林曼利等（2014）.
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表 5 饮水途径化学致癌物质和化学非致癌物的健康危害风险值(a-1)
Table 5. Risk levels for health hazards (a-1) of chemical carcinogens and chemical noncarcinogens in co-produced water in the study area
样品编号 致癌污染物 非致癌污染物 As Cd Cr Pb Hg Al Fe Mn Cu Zn Sb Ba Be Mo Ni SH1 3.60×10-6 8.65×10-8 5.35×10-6 5.28×10-10 8.80×10-9 3.14×10-8 4.61×10-9 2.60×10-9 4.66×10-12 5.42×10-11 1.01×10-8 2.22×10-8 1.38×10-11 9.04×10-10 1.57×10-11 SH2 4.94×10-6 5.84×10-7 1.13×10-6 4.90×10-10 3.69×10-8 4.45×10-8 9.78×10-11 7.22×10-10 2.15×10-13 3.02×10-11 5.79×10-9 1.54×10-8 - 1.15×10-9 - SH3 1.17×10-5 2.21×10-7 2.99×10-6 4.93×10-10 3.46×10-8 2.80×10-8 1.05×10-10 2.17×10-10 - 1.83×10-10 4.99×10-9 2.22×10-8 1.47×10-11 8.55×10-10 2.43×10-10 SH4 7.90×10-6 1.86×10-7 8.78×10-6 1.30×10-9 2.93×10-8 4.11×10-8 9.70×10-11 3.85×10-10 1.07×10-14 8.37×10-11 3.66×10-9 1.62×10-8 - 6.70×10-10 2.65×10-10 SH5 6.34×10-6 2.46×10-7 4.39×10-5 1.69×10-9 1.34×10-8 1.10×10-8 1.70×10-10 5.08×10-10 3.09×10-12 1.93×10-10 3.29×10-9 2.27×10-8 - 1.21×10-9 1.61×10-10 SH6 9.27×10-6 3.00×10-7 4.53×10-5 1.29×10-9 1.16×10-8 5.05×10-8 1.06×10-9 1.81×10-9 2.07×10-12 7.76×10-10 2.73×10-9 3.34×10-8 - 1.68×10-9 1.75×10-11 SH7 9.87×10-6 3.35×10-6 2.31×10-3 3.24×10-9 2.30×10-8 2.62×10-7 2.35×10-10 1.97×10-9 4.10×10-11 1.79×10-10 1.51×10-8 3.61×10-8 6.17×10-11 6.19×10-8 2.84×10-11 SH8 1.02×10-5 5.96×10-6 4.14×10-3 3.69×10-9 4.04×10-8 2.69×10-7 1.88×10-10 3.05×10-9 1.43×10-11 1.65×10-10 2.62×10-8 3.97×10-8 1.54×10-11 1.29×10-7 3.23×10-11 SH9 7.61×10-6 7.13×10-6 4.14×10-3 1.32×10-9 4.46×10-8 2.26×10-7 1.55×10-10 2.47×10-9 1.55×10-11 3.99×10-10 2.55×10-8 2.57×10-8 - 1.34×10-7 2.33×10-11 平均值 7.94×10-6 2.01×10-6 1.20×10-3 1.56×10-9 2.709×10-8 1.18×10-7 7.47×10-10 1.52×10-9 8.99×10-12 2.29×10-10 1.08×10-8 2.60×10-8 1.17×10-11 3.69×10-8 8.72×10-11
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