Chemical characteristics and evolutionary mechanism of hot spring water in Dabie Mountain area, Anhui Province
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摘要:研究目的
分析总结受构造控制的安徽大别山区温泉的水化学特征及其演化机制，有利于加深对独特地质背景下（造山带硅酸盐岩）水-岩相互作用的认识，同时可以为大别山区地热的勘探和合理开发利用提供科学依据。
研究方法在对研究区温泉水化学组分基本特征分析的基础上，综合利用Gibbs图、岩石风化图、离子比例系数、矿物稳定场图等方法对研究区温泉的水-岩相互作用进行研究。此外，还借助PHREEQC软件开展反向水文地球化学模拟工作，对地热水在循环过程中主要矿物的溶解及沉淀情况进行定量分析。
研究结果①大别山区5个温泉的水化学类型以SO4−Na型和SO4·HCO3−Na型水为主，均为中低温、弱碱性温泉；②研究区温泉中稀土元素表现出明显的Eu正异常，轻稀土元素相对富集，中稀土元素其次，重稀土元素相对缺乏；③研究区温泉水化学组分主要受岩石风化作用的影响。温泉中Na+主要来自硅酸盐矿物（如钠长石、钠蒙脱石等）的溶滤，Ca2+来源于碳酸盐矿物和石膏的溶滤；SO42−的含量主要受到石膏溶解的影响；HCO3−含量主要受硅酸盐和碳酸盐矿物溶解的影响。④模拟结果表明，雨水-地下热水路径上发生的水岩相互作用主要为钠长石、钙长石、萤石、石膏、黑云母和CO2的溶解，以及钠蒙脱石、方解石和白云石的沉淀，同时发生了Ca2+置换Na+的阳离子交替吸附作用。
结论雨水至地下热水路径属于地下水深循环，复杂的深部地层岩性及结构容易阻碍地下水径流，使地下水流速放缓，发生了充分的水-岩相互作用，完成了HCO3−Ca型雨水向SO4·HCO3−Na型和SO4−Na型弱碱性温泉的转化。
Abstract:ObjectiveThe analysis and summary of the hydrochemical characteristics and evolution mechanism of the tectonically controlled hot springs in Dabie Mountain area, Anhui Province, is conducive to deepen the understanding of water−rock interaction under the unique geological background (orogenic silicic rocks), and can provide scientific basis for geothermal exploration and rational development and utilization in Dabie Mountain area.
MethodsBased on the analysis of the basic characteristics of the chemical components of the hot spring in the study area, the water−rock interaction of the hot spring in the study area is studied by comprehensive use of Gibbs map, rock weathering map, ion ratio coefficient and mineral stability field map. In addition, the reverse hydrogeochemical simulation work was carried out with the help of PHREEQC software to quantitatively analyze the dissolution and precipitation of major minerals during the geothermal water cycle.
Results① The hydrochemical types of the five hot springs in Dabie Mountain are mainly SO4−Na and SO4·HCO3−Na, all of which are moderate−low temperature and weak alkaline hot springs; ② Eu values in hot springs in the study area show obvious positive anomalies, with light rare earth elements relatively abundant, medium rare earth elements second, and heavy rare earth elements relatively lacking; ③ The chemical composition of hot spring water in the study area is mainly affected by rock weathering. Na+ mainly comes from the leaching of silicate rocks (such as albite and sodium montmorillonite), and Ca2+ comes from the leaching of carbonate rocks and gypsum. The content of SO42− is mainly affected by the dissolution of gypsum. The content of HCO3− is mainly affected by the dissolution of silicate rocks and carbonate rocks. ④ The water−rock interaction on the path of rainwater−deep circulation underground hot water is the dissolution of albite, anorthite, fluorite, gypsum, biotite , and CO2, and the precipitation of sodium montmorillonite, calcite , and dolomite, and the cation alternating adsorption of Ca2+ replacing Na+ occurs.
ConclusionsThe path from rainwater to underground hot water belongs to the groundwater depth cycle. The complex lithology and structure of deep strata easily hinder groundwater runoff, slowing down groundwater velocity, and thus promote sufficient water−rock interaction in groundwater, completing the transformation of HCO3−Ca rainwater into SO4·HCO3−Na and SO4−Na weakly alkaline hot springs.
创新点（1）综合利用Gibbs图、岩石风化图、硅酸平衡图和离子比例系数等图解法，分析温泉深循环过程中发生的水-岩相互作用和主要的物质来源。（2）利用PHREEQC软件进行水化学模拟，对研究区经深循环形成的温泉的水-岩相互作用及水化学组分的迁移和富集进行定量分析。
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图 1 安徽大别山区地质略图（据徐树桐等，1992修改）
Ⅰ—江淮台隆和后继盆地；Ⅱ—北淮阳地槽褶皱带；Ⅲ—大别山中深变质杂岩带；Ⅲ1—罗田-岳西变质杂岩带；Ⅲ2—英山-潜山超高压变质岩带；Ⅲ3—宿松变质岩带和张八岭构造滑脱带；Ⅳ—前陆褶皱冲断带和磨拉斯盆地；Z-T1—卷入前陆褶皱冲断带的震旦系−下三叠统；Cm—石炭系梅山群；J3—晚侏罗世安山岩；γ—花岗岩；1—榴辉岩类；2—冲断带；3—走滑断层；4—地质界线；5—雨水样点及编号；6—温泉采样点及编号
Figure 1. Simplified geologic map of the Dabie Mountain area in Anhui
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图 2 安徽大别山区温泉Piper图
Figure 2. Piper map of hot springs in Dabie Mountain, Anhui Province
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图 3 研究区温泉轻、中、重稀土元素含量三角图
Figure 3. Triangle diagram of contents of light, medium and heavy rare earth elements in hot springs in the study area
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图 4 研究区温泉稀土元素配分模式图
Figure 4. Distribution pattern of rare earth elements in hot springs in the study area
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图 7 研究区温泉SiO2−Na+/H+(a)和SiO2−Ca2+/H+(b)系统矿物平衡体系图
Figure 7. Activity diagrams for SiO2−Na+/H+ (a) and SiO2−Ca2+/H+ (b)
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图 9 [(Ca2++Mg2+)−(SO42−+HCO3−)]−(Na+−Cl−)关系及氯碱指数
Figure 9. [(Ca2++Mg2+)−(SO42−+HCO3−)]−(Na+−Cl−) and chlor−alkali index
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图 10 主要矿物饱和指数与主要离子的比例关系图
Figure 10. The ratio of saturation index of major minerals to major ions
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图 11 安徽大别山区温泉成因模式示意剖面图（据李状等，2022）
1—花岗岩（表层风化）；2—大气降水入渗补给；3—示意性地下水流向；4—温泉；5—大地热流；6—破碎带
Figure 11. Schematic profile showing the formation of the hot springs in the Dabie Mountain area, Anhui Province
表 1 安徽大别山区温泉水化学组分
Table 1 Chemical composition of hot spring water in Dabie Mountain, Anhui Province
化学组分 单位 AH2 AH6 AH7 AH11 AH12 AHYS1 K+ mg/L 5 1.72 3.32 13.7 7.75 2.41 Na+ mg/L 113 55.2 100 321 294 0.96 Ca2+ mg/L 20.6 5.63 16.1 44.2 163 14.6 Mg2+ mg/L 1.31 0.03 0.03 0.03 0.03 0.37 Fe mg/L 0.19 0.06 0.03 0.05 0.06 0.05 HCO3− mg/L 94.8 50.2 19.5 58.7 9.48 43.4 CO32− mg/L 2.72 12.6 8.71 4.32 4.17 0 Cl− mg/L 4.61 6.24 4.03 48.9 49.3 0.76 SO42− mg/L 188 44.6 192 645 913 4.47 F− mg/L 5.56 3.38 6.5 8.02 3.86 0.1 NO3− mg/L 0.04 4.96 0.04 0.04 0.04 0.04 TDS mg/L 411 253 426 1172 1518 79 偏硅酸 mg/L 72.73 90.26 71.26 93.02 92.16 8.45 游离CO2 mg/L 0.66 0.09 总硬度 mg/L 56.83 14.06 40.2 110 407 37.96 Li μg/L 104 20.9 69.7 255 181 0.73 Sr μg/L 706 118 543 2238 5659 168 Zn μg/L 14.9 31.4 3.69 12.5 39.1 34.1 Ba μg/L 37.2 2.99 22.9 33.8 37.7 37.8 Cr μg/L 3.76 1.87 1.22 2.6 1.05 2.03 Mn μg/L 1.17 0.69 0.18 14.8 9.26 13.4 Ni μg/L 1.34 1.11 1.02 2.48 9.57 1.27 V μg/L 0.43 4.1 0.1 0.86 0.75 0.4 Eh mV −109 −80 −147 −152 −160 169 标高 m 80 408 120 40 100 408 T ℃ 46.3 51 40 61.3 64 30.6 pH 7.8 8.8 8.8 8 7.9 7.8 水化学类型 SO4·HCO3−Na SO4·HCO3−Na SO4−Na SO4−Na SO4−Na HCO3−Ca 
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表 2 矿物的溶解反应方程式
Table 2 Dissolution reaction equation of minerals
序号 矿物 反应式 1 钠长石 7NaAlSi3O8+6H++20H2O=3Na0.33Al2.33Si3.67O10(OH)2（钠蒙脱石）+6Na++10Si(OH)4 2 钙长石 CaAl2Si2O8+2H2CO3+H2O=Ca2++2HCO3−+Al2Si2O5(OH)4(高岭石) 3 钠蒙脱石 3Na0.33Al2.33Si3.67O10(OH)2+30H2O+6OH−=Na++7Al(OH)4−+11H4SiO4 4 石膏 CaSO4·2H2O=Ca2++2SO42− 5 方解石 CaCO3+H+=Ca2++HCO3− 6 白云石 CaMg(CO3)2+2H+=Ca2++Mg2++2HCO3− 7 萤石 CaF2=Ca2++2F− 8 黑云母 KMg3AlSi3O10(OH)2+6H++4H2O= K++3Mg2++Al(OH)4−+3H4SiO4 9 CO2 CO2(g)+H2O=H2CO3(aq)；H2CO3=H++HCO3− 10 Na+/Ca2+ Ca2++2NaX=2Na++CaX2 2Na++CaX2=2NaX+Ca2+
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表 3 可能矿物相在各路径上的溶解-沉淀量
Table 3 Dissolution-precipitation amount of possible mineral phases in each path
mmol/L 矿物相 分子式 路径Ⅰ 路径Ⅱ 路径Ⅲ AHYS1-AH2 AHYS1-AH6 AHYS1-AH7 钠长石 NaAlSi3O8 0.894 1.726 2.871 钙长石 CaAl2Si2O8 0.5924 1.371 3.007 钠蒙脱石 3Na0.33Al2.33Si3.67O10(OH)2 −0.9206 −1.91 −3.824 方解石 CaCO3 −0.3552 −1.729 −3.836 白云石 CaMg(CO3)2 −0.16 0.0389 −0.09606 萤石 CaF2 0.1438 0.0864 0.1686 石膏 CaSO4:2H2O 1.95 0.4875 1.974 黑云母 K(Mg,Fe)3AlSi3O10(F,OH)2 0.0663 −0.01764 0.027 CO2(g) CO2 1.595 1.937 3.514 Na+/Ca2+ 4.028 0.9418 2.347 注：正值表示溶解或Ca置换Na进入水中，负值表示沉淀或Na置换Ca进入水中；CO2(g)表示CO2以气体相参与水化学反应
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