The Morphological Distribution and Geochemical Genesis of Antimony in Typical High-Temperature Hot Springs
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摘要: 锑为典型有害元素，地热成因锑是天然水环境中溶解态锑的重要来源，富锑热泉排泄的负面环境效应不容忽视.本文在藏南和滇西选择典型地热区，分析了热泉中锑的形态分布及其地球化学成因.总体上，研究区排泄的地热水具有远高于天然水环境背景值的锑含量，最高可达2 128.7 μg/L.水文地球化学计算表明热泉中锑的主要存在形态为锑酸盐和亚锑酸盐，但部分热泉样品中硫代锑占总锑百分比可高达35%.硫化物浓度、S（-Ⅱ）/Sb摩尔比，以及砷锑之间的竞争巯基化作用是影响热泉中硫代锑含量的关键因素.在本研究所涉及地热系统中，西藏玛旁雍错曲色涌巴、门士、莫落江为岩浆热源型地热系统，其地热水中锑源自高温条件下热储围岩淋滤和作为热源的岩浆房所释出流体的输入，西藏曲卓木、朗久与云南邦腊掌则属于非岩浆热源型地热系统，其热泉中的锑主要来源于地热水‒围岩矿物相互作用.Abstract: Antimony is a typical harmful element, and the negative environmental effects of antimony-rich hot springs discharge can not be neglected since geothermal genesis of antimony is an important source of antimony in the natural water environments. In this paper, the morphological distribution of antimony in hot springs and its geochemical genesis were analyzed in selected typical geothermal areas in southern Tibet and western Yunnan. In general, the antimony of geothermal water discharged from the study area can be up to 2 128.7 μg/L, which is much higher than the background values in the natural water environments. Hydrogeochemical calculations indicate that the main forms of antimony present in the hot springs are antimonate and antimonite, however, the percentage of thioantimony in some hot spring samples can be as high as 35% of the total antimony. Sulfide concentration, S(-Ⅱ)/Sb molar ratio, and competitive thiolation between arsenic and antimony are the key factors affecting the content of thioantimony in hot springs. Among the geothermal systems involved in this study, the Tibetan MapamYumco, Moincer, and Moluojiang are magma-heat geothermal systems, and the antimony in the geothermal water originates from the input of fluids released from the hot storage surrounding rocks leaching and magma house as the heat source under high temperature conditions, while the Tibetan Quzuomu, Langjiu and Yunnan Banglazhang are non-magma-heat geothermal systems, and the main source of antimony in their thermal springs is geothermal water-peripheral rock mineral interaction.
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Key words:
- hot springs /
- antimony /
- thioantimony /
- water‐rock interactions /
- magmatic fluid input /
- geochemistry
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图 1 采样区域分布(据Guo et al., 2019修改)
Fig. 1. Distribution of sampling areas (modified from Guo et al., 2019)
图 2 西藏热泉（a）与邦腊掌热泉（b）S(-Ⅱ)/Sb摩尔占比
Fig. 2. S(-Ⅱ)/Sb molar ratio of Tibet (a) and Banglazhang hot springs (b)
图 5 玛旁雍错与门士热泉样品中锑‒砷（a）、锑‒氯（b）、锑‒硼（c）、锑‒铷（d）、锑‒锂（e）、锑‒铯（f）散点图
Fig. 5. Scatter plots of antimony-arsenic (a), antimony-chlorine (b), antimony-boron (c), antimony-rubidium (d), antimony- lithium (e), antimony-cesium (f) in samples from MapamYumco and Moincer hot springs
表 1 热泉水文地球化学特征
Table 1. Hydrogeochemical characteristics of hot springs
样品编号 地热区 T (℃) pH EC (μs/cm) Sb (μg/L) H2S (mg/L) As (μg/L) LJ01 朗久 78.0 7.84 2 992 78.9 0.09 5 510 LJ02 朗久 65.0 8.36 3 037 65.1 0.01 5 690 LJ03 朗久 69.9 8.08 2 926 72.5 0.03 5 480 LJ04 朗久 63.0 7.94 3 239 57.0 0.03 4 860 LJ05 朗久 84.4 8.13 3 259 64.7 0.05 5 510 LJ06 朗久 82.0 8.41 3 116 60.6 0.06 5 890 LJ07 朗久 83.2 8.34 3 142 55.1 0.06 5 310 QSYB01 玛旁雍错曲色涌巴 85.0 8.51 1 715 301.3 0.34 360 QSYB02 玛旁雍错曲色涌巴 88.4 8.53 1 766 336.1 0.22 460 QSYB03 玛旁雍错曲色涌巴 84.0 8.32 2 077 240.1 0.66 410 QSYB04 玛旁雍错曲色涌巴 76.0 9.20 1 760 207.8 0.21 400 QSYB05 玛旁雍错曲色涌巴 75.0 8.94 1 818 191.2 0.39 410 QSYB06 玛旁雍错曲色涌巴 70.0 8.92 1 848 310.6 0.35 450 QSYB07 玛旁雍错曲色涌巴 70.0 8.90 1 828 330.2 0.43 420 QSYB08 玛旁雍错曲色涌巴 66.0 8.96 1 804 335.7 0.56 420 QSYB09 玛旁雍错曲色涌巴 65.0 8.96 1 818 331.1 0.74 440 QSYB10 玛旁雍错曲色涌巴 90.0 9.13 1 845 349.3 0.22 460 QSYB11 玛旁雍错曲色涌巴 84.0 9.09 1 796 272.7 0.40 460 QSYB12 玛旁雍错曲色涌巴 84.0 2.40 3 014 134.2 0.05 210 MS01 门士 71.2 7.50 1 482 18.8 0.08 170 MS01-1 门士 69.0 8.05 1 414 18.7 0.03 90 MS01-2 门士 67.5 7.88 1 491 18.1 0.02 100 MS01-3 门士 64.1 8.01 1 460 16.6 0.04 100 MS01-4 门士 60.5 7.95 1 431 15.3 0.02 20 MS02 门士 71.7 7.69 1 461 50.5 0.02 70 MS03 门士 72.5 7.72 1 452 98.0 0.04 90 MLJ01 莫落江 83.3 7.30 6 453 1 164.5 0.10 20 750 MLJ02 莫落江 82.0 7.80 5 590 2 157.6 0.03 17 030 MLJ03 莫落江 79.0 8.21 6 225 584.1 0.05 18 940 MLJ04 莫落江 87.0 8.33 5 870 2 128.7 0.01 14 770 MLJ05 莫落江 87.0 8.48 5 447 1 996.2 0.11 13 940 MLJ06 莫落江 85.0 8.19 5 468 885.5 0.26 13 390 QZM01 曲卓木 70.0 6.95 1 995 168.6 0.02 40.0 QZM02 曲卓木 65.0 6.53 1 670 8.60 0.02 50.0 QZM03 曲卓木 69.0 7.16 1 970 163.9 0.02 80.0 QZM04 曲卓木 72.0 6.87 2 037 11.5 0.02 60.0 QZM05 曲卓木 67.0 7.17 2 057 207.5 0.02 60.0 QZM06 曲卓木 62.0 6.98 2 085 19.2 0.01 50.0 QZM07 曲卓木 58.0 7.29 2 082 230.1 0.01 50.0 QZM08 曲卓木 54.0 7.60 2 054 15.2 0.01 60.0 QZM09 曲卓木 74.0 6.73 2 101 10.9 0.01 60.0 QZM10 曲卓木 71.0 8.26 1 071 9.82 0.02 80.0 LL00 邦腊掌 91.0 8.36 1 080 8.31 8.00 168.8 LL01 邦腊掌 75.0 7.97 1 054 9.22 5.30 183.8 LL02 邦腊掌 87.0 8.45 1 045 8.53 8.80 174.9 LL03 邦腊掌 88.0 9.13 1 075 9.49 8.20 191.4 LL04 邦腊掌 63.0 8.25 1 000 6.99 1.00 139.0 LL05 邦腊掌 84.5 8.58 1 053 8.73 3.60 138.2 LL06 邦腊掌 57.5 8.73 938 7.43 8.40 112.8 LL07 邦腊掌 94.0 9.23 1 057 9.13 13.60 170.0 LL08 邦腊掌 76.0 9.67 981 7.23 2.90 165.4 
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表 2 水中不同锑形态的化学热力学数据
Table 2. Chemical thermodynamic data of various tungsten species in water
名称 化学式 反应式 平衡
常数焓变
(kJ/mol)数据来源 Tetrathioantimonate Sb2S42‒ 2Sb(OH)3+4HS‒+2H+=Sb2S42‒+6H2O 49.39 ‒321.78 University of Waterloo-
minteqv4uw.datAntimonate SbO3‒ Sb(OH)6‒=SbO3‒+3H2O 2.93 -- SbO2+ Sb(OH)6‒+2H+=SbO2++4H2O 2.39 -- Sb(OH)6‒ Sb2O5+7H2O=2Sb(OH)6‒+2H+ ‒27.82 -- Antimonite Sb(OH)3 Sb(OH)6‒+2e‒+3H+=Sb(OH)3+3H2O 24.31 -- Sb(OH)4‒ Sb(OH)3+H2O=Sb(OH)4‒+H+ 12.04 69.85 Sb(OH)2+ Sb(OH)3+H+=Sb(OH)2++H2O 1.39 -- HSbO2 Sb(OH)3=HSbO2+H2O ‒0.01 ‒0.13 SbO2‒ Sb(OH)3=SbO2‒+H2O+H+ ‒11.80 70.186 6 SbO+ Sb(OH)3+H+=SbO++2H2O 0.92 8.242 5 SbOF Sb(OH)3+F‒+H+=SbOF+2H2O 6.19 -- Sb(OH)2F Sb(OH)3+F‒+H+=Sb(OH)2F+H2O 6.19 --
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表 3 热泉样品中锑的形态分布模拟结果
Table 3. Simulation results of the morphological distribution of antimony in hot spring samples
样品编号 Sb Sb(Ⅲ) Sb(Ⅴ) Sb2S42- （mol/L） （mol/L） (%) （mol/L） (%) （mol/L） (%) LJ01 6.52E-07 6.48E-07 99.76 1.57E-09 0.24 9.22E-29 0 LJ02 5.38E-07 6.22E-08 11.61 4.74E-07 88.39 5.32E-32 0 LJ03 5.99E-07 1.24E-07 20.79 4.73E-07 79.21 1.20E-30 0 LJ04 4.71E-07 1.42E-07 30.19 3.28E-07 69.81 1.14E-29 0 LJ05 5.35E-07 9.41E-08 17.67 4.38E-07 82.33 8.32E-32 0 LJ06 5.01E-07 4.12E-08 8.26 4.58E-07 91.74 1.98E-31 0 LJ07 4.55E-07 4.72E-08 10.41 4.06E-07 89.59 1.97E-31 0 QSYB01 2.49E-06 2.48E-06 99.99 1.46E-10 0.01 5.17E-15 0 QSYB02 2.78E-06 2.77E-06 100 1.69E-11 0 1.31E-17 0 QSYB03 1.98E-06 1.98E-06 100 1.07E-11 0 1.96E-12 0 QSYB04 1.72E-06 1.71E-06 99.78 3.75E-09 0.22 1.07E-18 0 QSYB05 1.58E-06 1.57E-06 99.91 1.41E-09 0.09 1.28E-15 0 QSYB06 2.57E-06 2.55E-06 99.93 1.69E-09 0.07 1.60E-14 0 QSYB07 2.73E-06 2.71E-06 99.92 2.17E-09 0.08 1.19E-13 0 QSYB08 2.77E-06 2.76E-06 99.87 3.69E-09 0.13 1.89E-12 0 QSYB09 2.74E-06 2.72E-06 99.85 4.00E-09 0.15 1.28E-11 0 QSYB10 2.89E-06 2.87E-06 99.96 1.19E-09 0.04 1.21E-20 0 QSYB11 2.25E-06 2.24E-06 100 2.81E-11 0 7.76E-18 0 QSYB12 1.11E-06 1.10E-06 100 1.19E-11 0 4.71E-32 0 MS01 1.55E-07 1.54E-07 99.88 1.89E-10 0.12 3.83E-16 0 MS01-1 1.55E-07 3.76E-08 24.43 1.16E-07 75.57 3.17E-22 0 MS01-2 1.49E-07 5.12E-08 34.37 9.77E-08 65.63 2.70E-24 0 MS01-3 1.37E-07 3.45E-08 25.27 1.02E-07 74.73 4.88E-20 0 MS01-4 1.27E-07 4.38E-08 34.80 8.20E-08 65.20 8.75E-16 0 MS02 4.18E-07 2.08E-07 50.07 2.07E-07 49.93 1.35E-22 0 MS03 8.10E-07 3.74E-07 46.36 4.32E-07 53.64 1.24E-17 0 MLJ01 9.62E-06 7.78E-06 80.91 1.83E-06 19.09 1.68E-30 0 MLJ02 1.78E-05 7.48E-06 42.05 1.03E-05 57.95 4.28E-31 0 MLJ03 4.83E-06 5.05E-07 10.47 4.31E-06 89.53 1.82E-31 0 MLJ04 1.76E-05 2.35E-06 13.40 1.52E-05 86.60 2.27E-33 0 MLJ05 1.65E-05 9.92E-07 6.03 1.54E-05 93.97 1.27E-29 0 MLJ06 7.32E-06 9.47E-07 12.98 6.35E-06 87.02 2.61E-28 0 MLJ07 4.91E-07 2.19E-07 44.75 2.70E-07 55.25 7.08E-29 0 MLJ08 2.59E-07 4.75E-08 18.35 2.11E-07 81.65 6.73E-33 0 QZM01 1.39E-06 1.22E-06 88.24 1.63E-07 11.76 1.72E-14 0 QZM02 7.07E-08 6.83E-08 96.50 2.47E-09 3.50 9.10E-22 0 QZM03
QZM041.35E-06
9.46E-081.08E-06
8.55E-0880.16
90.332.68E-07
9.14E-0919.84
9.671.62E-22
3.65E-240
0QZM05 1.71E-06 1.37E-06 80.35 3.35E-07 19.65 2.04E-20 0 QZM06 1.58E-07 1.37E-07 86.90 2.07E-08 13.10 1.58E-24 0 QZM07 1.89E-06 1.42E-06 74.87 4.76E-07 25.13 2.75E-21 0 QZM08 1.25E-07 6.86E-08 54.84 5.65E-08 45.16 2.91E-23 0 QZM09 8.97E-08 8.37E-08 93.38 5.94E-09 6.62 1.03E-27 0 QZM10 8.08E-08 1.04E-08 12.88 7.04E-08 87.12 1.08E-24 0 LL00 6.83E-08 6.83E-08 99.98 6.34E-13 0 7.34E-12 0.01 LL01 7.58E-08 2.83E-08 37.38 8.39E-16 0 2.37E-08 31.15 LL02 7.01E-08 7.01E-08 99.94 5.45E-13 0 1.99E-11 0.03 LL03 7.80E-08 7.78E-08 99.75 1.99E-10 0.25 9.51E-16 0 LL04 5.74E-08 5.60E-08 97.48 8.22E-15 0 7.23E-10 1.25 LL05 7.17E-08 7.17E-08 100 7.02E-13 0 2.39E-13 0 LL06 6.11E-08 1.80E-08 29.40 5.99E-15 0 2.16E-08 35.12 LL07 7.50E-08 7.38E-08 98.30 1.28E-09 1.70 9.06E-17 0 LL08 5.94E-08 5.88E-08 98.94 6.32E-10 1.06 8.91E-19 0 注：E-07即10-7，依此类推.
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