Hydrochemical characteristics and pollution source apportionment of a karst underground river system in northern Guizhou
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摘要: 岩溶生态系统脆弱且复杂，有效提高岩溶区多种相似污染源并存的污染溯源的准确性，对保护岩溶地下水具有重要意义。通过分析现状条件下地下水化学特征，采用主要离子溯源、氮氧同位素及PMF模型方法识别污染主控因子，实现多源地下水污染精准解析和量化。结果表明，研究区地下水中K+、Na+、${\rm{HCO}}_3^{-}$、Cl−、TFe、Mn、TP、NH$_4^{+}$、${\rm{NO}}_3^{-}$-N含量超过背景值1.17~
4940 倍，部分地下水化学类型改变为SO4·HCO3—NH4·Ca·Mg型，表明区内地下水受到污染。通过主要离子溯源、氮氧同位素分析方法确定了地下水污染来源的种类，基于新污染物筛查的PMF模型对污染贡献进行了量化，上游酒企废水、农业面源污染贡献率分别为85.06%~96.07%、3.04%~13.74%；中下游酒企废水、农业面源、养殖废水污染贡献率分别为0.22%~0.68%、15.56%~48.13%、51.24%~84.22%。通过整合水化学分析、氮氧同位素分析、PMF模型、新污染物筛查技术，准确地识别了地下水污染来源，提高岩溶区多种相似污染源并存的污染溯源的准确性。Abstract:The karst ecosystem is fragile and complex. How to effectively improve the accuracy of pollution source identification when multiple similar pollution sources coexist in karst areas is of great significance for the protection of karst groundwater.Taking the groundwater pollution of a certain underground river in northern Guizhou, where multiple similar pollution sources such as agricultural non-point sources, domestic sewage, brewery sewage, and aquaculture wastewater coexist, as the research object, this study analyzes the hydrochemical characteristics of groundwater under current conditions, identifies the main pollution-controlling factors using methods including major ion source tracing, nitrogen and oxygen isotope analysis, and the PMF (Positive Matrix Factorization) model based on emerging pollutant screening, determines the contribution rates of pollution sources, and ultimately achieves accurate analysis and quantification of groundwater pollution under the condition of coexisting multiple similar pollution sources. Results show that: the contents of K+,Na+,${\rm{HCO}}_3^{-}$,Cl−,TFe (Total Iron), Mn (Manganese), TP (Total Phosphorus), NH$_4^{+}$ (Ammonium), and ${\rm{NO}}_3^{-}$-N (Nitrate Nitrogen) in the groundwater of the study area exceed the background values by 1.17 to 4940 times, and show a pattern where their contents in the wet season are higher than those in the dry season.Some of the groundwater chemical types have changed from the HCO3—Ca·Mg type to the SO4·HCO3—NH4·Ca·Mg type.In the wet season, the ions with a coefficient of variation (CV) greater than 100% include K+,Na+,${\rm{HCO}}_3^{-}$,Cl−, TFe, Mn, TP, NH$_4^{+}$ , and ${\rm{NO}}_3^{-}$-N. In the dry season, the ions with a CV greater than 100% are Mn, TP, NH$_4^{+}$, and ${\rm{NO}}_3^{-}$-N. The groundwater in the study area is contaminated by external source inputs, and the external input in the wet season is higher than that in the dry season, which is related to the leakage of potential pollution sources in the study area during the wet season of the sampling period.The main ion tracing based on changes in the molar concentration ratio of Cl− to ${\rm{NO}}_3^{-}$/Cl− in groundwater identified that the pollution at CK18 originated from the distiller's grains yard upstream. The nitrates in the groundwater outcrops at K57, K39, K61, S02, K001, K29, and S01 mainly came from agricultural planting areas.The nitrogen and oxygen isotope analysis method confirmed that the S01 spring point, DB01 surface water, and SL08 leakage point share the same source, with the pollution originating from the leakage of brewery wastewater from the sewage treatment plant.The pollution at leakage points SL01 and SL02, domestic sewage sampling point SH01, and spring points K29, K61, S02, K39, K57, and K001 originates from the leakage of stock solution from the chemical fertilizer production workshops YY05 and YY06.The PMF model based on emerging pollutant screening was used to quantify pollution contributions. In the upper reaches of the karst underground river system, the contribution rates of brewery wastewater and agricultural non-point sources were 85.06% to 96.07% and 3.04% to 13.74%, respectively; in the middle and lower reaches, the contribution rates of brewery wastewater, agricultural non-point sources, and aquaculture wastewater were 0.22% to 0.68%, 15.56% to 48.13%, and 51.24% to 84.22%, respectively.By integrating hydrochemical analysis, nitrogen and oxygen isotope analysis, the PMF model, and emerging pollutant screening technology, the sources of groundwater pollution were accurately identified. This has improved the accuracy of pollution source tracing when multiple similar pollution sources coexist in karst areas, providing a scientific basis for regional groundwater pollution control and management. -
图 1 研究区水文地质略图
1-纯碳酸盐岩含水岩组 2-碳酸盐岩与碎屑岩互层含水岩组 3-隔水层 4-地下河出口及编号 5-岩溶下降泉 6-岩溶竖井 7-地下河天窗 8-监测井 9-采样点 10-养殖场 11-等水位线及地下水流向 12-地下水系统界线 13-推测断层 14-向斜轴 15-地质界线及地层代号 16-岩层产状 17-河流及溪沟 18-潜在污染源边界
Figure 1. Simplified hydrogeological map of the study area
图 2 研究区水体改进型Piper三线图
Figure 2. Modified piper trilinear diagram of water bodies in the study area
图 3 研究区地下水Cl−与${\rm{NO}}_3^{-}$/Cl−摩尔浓度比值变化
Figure 3. Variation of the molar concentration ratio of Cl− and ${\rm{NO}}_3^{-}$/Cl− in groundwater of the study area
图 4 地下水与污水δ15 N-${\rm{NO}}_3^{-}$、δ18O-${\rm{NO}}_3^{-}$浓度箱线图
Figure 4. Boxplot of concentrations of δ15N-${\rm{NO}}_3^{-}$ and δ18O-${\rm{NO}}_3^{-}$ in groundwater and sewage
图 5 研究区水体δ15 N-${\rm{NO}}_3^{-}$与δ18O-${\rm{NO}}_3^{-}$分布
Figure 5. Distribution of δ15 N-${\rm{NO}}_3^{-}$andδ18O-${\rm{NO}}_3^{-}$in water bodies of the study area
图 6 研究区地下水各污染源贡献比例（PMF模型）
Figure 6. Contribution ratios of various pollution sources to groundwater in the study area (PMF model)
表 1 研究区地下水理化参数统计表
Table 1. Statistics of physicochemical parameters of groundwater in the study area
离子类别 季节 最大值/mg·L−1 最小值/mg·L−1 平均值/mg·L−1 标准差 变异系数/% 背景值/mg·L−1 地下水Ⅲ类限值 K+ 丰季 142.80 0.40 15.61 40.13 257.10 0.76-4.80 — 枯季 20.22 3.00 8.86 6.17 69.66 Na+ 丰季 56.30 3.50 10.56 14.56 137.90 2.76-7.20 200 枯季 19.41 5.22 10.34 5.19 50.13 Ca2+ 丰季 220.66 52.16 135.67 42.96 31.67 117.6-132.0 — 枯季 154.06 31.01 114.58 31.67 27.64 Mg2+ 丰季 48.33 7.30 24.97 15.81 63.33 6.48-21.30 — 枯季 32.60 19.14 24.30 3.99 16.43 ${\rm{HCO}}_3^{-}$ 丰季 2561.91 127.10 470.08 669.88 142.50 133.00-264.00 — 枯季 494.07 192.30 356.82 94.50 26.48 ${\rm{SO}}_4^{2-}$ 丰季 389.94 41.33 174.17 110.50 63.44 45.20-98.6 250 枯季 160.71 45.15 92.81 38.21 41.17 Cl− 丰季 120.77 7.28 26.89 30.37 112.94 8.10-13.20 — 枯季 27.74 8.10 18.20 7.10 39.07 TFe 丰季 8.89 0.05 0.88 2.53 287.46 0.05-0.08 0.3 枯季 1.05 0.05 0.35 0.34 98.77 Mn 丰季 3.56 0.01 0.82 1.02 262.99 0.005-0.02 0.1 枯季 2.83 0.01 0.76 0.87 114.22 TP 丰季 6.78 0.01 0.67 1.94 290.74 0.01 — 枯季 2.25 0.01 0.55 0.88 159.94 NH$_4^{+}$ 丰季 247.00 0.02 21.27 71.10 334.16 0.02-0.05 0.5 枯季 17.10 0.02 3.82 6.55 171.52 ${\rm{NO}}_3^{-}$−N 丰季 148.37 0.59 49.55 47.70 96.29 0.10-1.80 20 枯季 6.61 0.04 1.55 2.18 140.94 pH 丰季 8.09 7.29 7.81 0.27 3.49 7.6-8.1 6.5-8.5 枯季 7.88 7.10 7.39 0.24 3.21 注：pH值为无量纲. 
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表 2 研究区地下水样品新污染物的定量靶向筛查分析测试结果(ng·L−1)
Table 2. Analytical test results of quantitative targeted screening for emerging contaminants in groundwater samples of the study area (ng·L−1)
新污染物 化合物名称
（中文）采样点位 JD10 H507 K001-1 K001-2 K001-3 K501 K505 S003 S004-1 S004-2 S004-3 ZK4 抗生
素及
药物
类磺胺对甲氧嘧啶 N.D. 6587.2 5.1 8.1 35.8 755.8 477.0 263.6 397.2 591.7 514.9 N.D. 盐酸金霉素 N.D. 9984.2 N.D. N.D. N.D. 708.4 226.3 200.6 124.6 27.5 27.4 N.D. 氟尼辛 N.D. 158.9 N.D. N.D. N.D. 166.1 41.6 24.5 46.6 43.6 41.3 N.D. 磺胺氯哒嗪 N.D. 5355.6 N.D. N.D. 23.9 977.2 417.7 197.5 299.5 470.0 412.1 N.D. 腺苷 N.D. N.D. 332.6 136.4 105.3 309.0 110.5 111.0 254.9 19.8 44.8 N.D. 埃莫福汀B N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 盐酸差向金霉素 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 阿苯达唑亚砜 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 农药
类及
内分
泌干
扰物类啶虫脒 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 扑灭津- 2 -羟基 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 阿特拉通莠去通除草剂 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N,N-二乙基-3-甲基苯甲酰胺 N.D. 0.6 0.9 4.0 1.5 2.0 1.2 N.D. 1.3 1.5 1.0 1.8 扑灭通 N.D. N.D. N.D. N.D. N.D. 0.5 0.4 0.6 0.7 N.D. N.D. 0.6 阿特拉津 N.D. N.D. 1.8 2.9 3.0 21.5 11.6 4.6 9.4 8.7 8.4 6.2 酒
企
发
酵
污
水阿魏酸 25932.4 N.D. 1037.3 797.9 531.9 N.D. N.D. N.D. N.D. N.D. N.D. N.D. 水杨酸 1143.8 N.D. 95.3 79.4 61.1 N.D. N.D. N.D. N.D. N.D. N.D. N.D. 4-羟基-3-甲基苯甲酸 519.8 N.D. 52.0 47.3 39.4 N.D. N.D. N.D. N.D. N.D. N.D. N.D. 对羟基苯甲醛 1970.7 N.D. 115.9 82.8 63.7 N.D. N.D. N.D. N.D. N.D. N.D. N.D. 苜蓿素 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. 咖啡酸乙酯 N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D.
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