云南腾冲热海高温地热水中汞的地球化学异常及其指示意义

doi:10.13745/j.esf.sf.2019.9.7

摘要/Abstract

摘要：

汞是环境中典型有害组分,深部地热系统可能是环境中汞的重要来源之一,但当前地热成因汞的研究程度很低。本文以腾冲火山带热海水热区为研究区,开展了热泉中汞的水文地球化学研究。热海水热区内排泄的中性热泉含有异常高浓度的汞,但酸性热泉则绝大多数未检出汞。热海热泉中的汞与典型的岩浆来源组分氯相同,均主要来源于岩浆流体的混合。在中性热泉中,Hg(II)是汞的占优势地位的价态,Hg²⁺与不同形态硫化物的配合则是决定Hg(II)的形态分布的直接因素,但pH可通过控制水中硫化物的形态分布来影响Hg(II)的形态分布。Hg(II)不易挥发,故中性热泉中汞含量普遍较高;但酸性热泉中的汞受泉口氧化还原电位较高的影响,以Hg(0)为主要价态,且因Hg(0)易挥发而导致总汞含量极低。就中性热泉而言,其汞含量对水热区断裂分布有重要指示作用,原因为沿不同断裂上升的中性地热水经历的冷却方式不同,最终导致热泉汞含量也表现出显著差异。热泉汞含量对水热系统结构研究有借鉴意义。

关键词: 热泉, 汞, 存在形态, 地球化学异常, 断裂

Abstract:

Mercury (Hg) is a typical undesirable constituent in the environment. One of potential sources of environmental mercury is deep geothermal systems. However, systematic studies on geothermal mercury are sparse. Here, we conducted a hydrogeochemical study on Hg in hot springs in the Rehai hydrothermal area in the Tengchong volcanic region. The results showed that Hg is rich in the neutral hot springs in the Rehai area but was not detected in most acidic Rehai hot springs. Moreover, the geothermal mercury in Rehai, like chlorine, a typical magma-derived component, primarily comes from magmatic fluid. In the neutral hot springs, Hg(II) is the predominant form of mercury. Complexation of Hg²⁺ with different sulfide species directly determines Hg(II) speciation, but hot spring pH values can also have an effect to some degrees by controlling sulfide speciation. Because Hg(II) is not prone to volatilization, the neutral hot springs generally have high mercury concentrations. However, volatile Hg(0) is the major form of mercury in acidic Rehai hot springs due to their much higher redox potentials, resulting in very low total mercury concentrations in acidic springs. Mercury in neutral hot springs can be an effective indicator for fault distribution in Rehai, because mercury concentration in ascending neutral spring waters varies distinctively depending on the water cooling process along fault. Geothermal mercury is of great significance for studying the structures of hydrothermal systems.

Key words: hot spring, mercury, speciation, geochemical anomaly, fault

中图分类号:

郭清海, 吴启帆. 云南腾冲热海高温地热水中汞的地球化学异常及其指示意义[J]. 地学前缘, 2020, 27(1): 103-111.

GUO Qinghai, WU Qifan. Hydrogeochemical anomaly of mercury in the high-temperature geothermal waters in the Rehai hydrothermal area in Tengchong, Yunnan and its indications[J]. Earth Science Frontiers, 2020, 27(1): 103-111.

图/表 12

图1 热海水热区地质简图(左)和热泉采样位置(右)

Fig.1 Simplified geological map of the Rehai hydrothermal area (Left) and sampling locations (Right)

表1 水样采集信息、现场测试指标和汞含量

Table 1 Summary of water sampling information, in-situ parameters and mercury concentrations

样品编号	采样位置	所属子区	pH	t/℃	EC/(μS·cm^-1)	DO质量浓度/(mg·L^-1)	Hg质量浓度/(μg·L^-1)
LGG-HT	老滚锅	硫磺塘	4.87	72.3	902.3	n.d.	n.d.
LGG-LT	老滚锅	硫磺塘	4.60	56.2	916.7	1.46	n.d.
DRTY-01	地热体验区	硫磺塘	1.60	46.7	4 639	5.84	n.d.
DRTY-02	地热体验区	硫磺塘	1.80	68.3	2 184	0.34	n.d.
DRTY-03	地热体验区	硫磺塘	1.93	71.8	1 494	0.21	n.d.
DRTY-04	地热体验区	硫磺塘	2.14	62.6	1 317	0.24	n.d.
DRTY-10	地热体验区	硫磺塘	1.59	49.9	5 857	1.40	n.d.
DRTY-11	地热体验区	硫磺塘	2.19	82.9	604.5	0.49	n.d.
WGQ	文光泉	硫磺塘	5.36	38.4	382.8	0.09	n.d.
ZZQ	珍珠泉	硫磺塘	3.46	93.0	558.9	0.58	0.024
TQL	听泉楼	硫磺塘	8.12	82.9	3 552	0.20	0.796
YJQ-L	眼镜泉-左	硫磺塘	8.31	91.8	3 753	0.53	1.046
GMQ	鼓鸣泉	硫磺塘	8.30	92.5	3 601	0.31	0.939
HTJ-L	怀胎井-左	硫磺塘	7.56	92.2	3 473	0.52	0.939
HTJ-R	怀胎井-右	硫磺塘	6.77	82.4	2 752	0.38	0.765
DGG	大滚锅	硫磺塘	6.87	85.7	4 419	0.30	1.472
XKT-L	霞客亭-左	澡塘河	7.32	79.9	2 236	0.94	0.486
XKT-R	霞客亭-右	澡塘河	7.64	94.8	2 362	0.37	0.455
ZTH	澡塘河热泉	澡塘河	7.51	80.7	2 326	0.56	0.405
HMZ	蛤蟆嘴	澡塘河	7.70	74.5	2 814	0.27	0.422
HMZP-R	蛤蟆嘴坡-右	澡塘河	7.13	93.1	2 436	0.23	0.524

表2 热泉水化学和氢氧同位素组成

Table 2 Hydrochemical and water isotopic compositions of the hot springs

样品编号	组分质量浓度/(mg·L^-1)															As质量浓度/ (μg·L^-1)	δD/‰	δ¹⁸O/‰
样品编号	HCO₃	CO₃	SO₄	Cl	F	Br	Na	K	Ca	Mg	Fe	Si	Li	B	硫化物	As质量浓度/ (μg·L^-1)	δD/‰	δ¹⁸O/‰
LGG-HT	0.0	0.00	436.2	42.8	2.69	0.29	208.4	38.2	6.64	1.05	0.47	139.1	2.86	1.33	0.17	35.7	n.a.	n.a.
LGG-LT	0.0	0.00	490.2	45.5	2.50	0.32	210.2	38.8	6.96	1.09	0.45	141.3	2.90	1.34	0.00	28.8	-53	-7.6
DRTY-01	0.0	0.00	3 548	30.1	2.33	n.d.	46.2	136.9	26.6	3.93	46.0	120.2	3.36	0.30	2.20	46.5	-58	-7.3
DRTY-02	0.0	0.00	1 894	29.5	2.33	n.d.	7.72	19.1	16.0	1.78	27.7	69.3	0.49	0.20	0.17	100	-55	-8.1
DRTY-03	0.0	0.00	667.0	12.6	1.04	n.d.	11.4	19.7	1.95	1.03	12.5	76.9	1.72	0.08	0.20	127	-60	-7.7
DRTY-04	0.0	0.00	694.6	10.1	0.91	n.d.	26.0	44.7	1.82	1.11	20.4	178.5	4.12	0.14	0.12	261	-67	-9.3
DRTY-10	0.0	0.00	15 590	50.9	15.2	n.d.	29.8	209.8	35.6	8.74	60.2	132.6	3.21	0.39	0.05	n.d.	-59	-9.6
DRTY-11	0.0	0.00	320.4	4.95	n.d.	n.d.	0.42	1.83	0.17	0.05	0.81	11.7	0.06	0.01	0.04	4.4	-56	-7.2
WGQ	60.8	0.01	175.1	5.53	1.21	n.d.	82.5	27.8	8.82	1.22	2.01	107.2	1.29	0.06	0.75	51.9	n.a.	n.a.
ZZQ	38.4	0.00	163.3	52.7	1.34	0.33	84.3	35.1	4.47	0.98	1.31	83.2	0.75	1.29	0.04	88.6	-64	-7.2
TQL	886	59.8	45.4	596.3	16.4	1.87	677.5	102.2	1.97	0.28	n.d.	108.9	8.04	9.88	2.60	751	n.a.	n.a.
YJQ-L	851	98.3	55.0	635.6	17.1	1.96	701.5	119.5	1.80	0.27	n.d.	121.0	8.35	10.07	5.90	897	n.a.	n.a.
GMQ	854	81.4	46.7	588.1	16.3	1.72	671.0	115.3	1.93	0.29	n.d.	134.8	8.04	9.73	5.20	837	-67	-7.5
HTJ-L	913	34.0	49.9	583.1	16.2	1.85	639.0	106.7	1.62	0.29	n.d.	114.4	7.58	9.19	4.20	802	-66	-7.7
HTJ-R	739	6.38	68.8	433.8	12.6	1.61	507.5	84.9	2.13	0.32	n.d.	116.2	6.11	7.41	2.10	593	n.a.	n.a.
DGG	1 256	5.73	40.8	738.1	19.9	2.35	858.0	150.0	1.77	0.26	n.d.	152.0	9.90	12.01	0.24	1 059	-65	-7.3
XKT-L	641	6.62	69.4	323.1	9.91	1.27	408.0	71.4	6.18	0.60	n.d.	72.3	4.66	5.56	0.17	305	n.a.	n.a.
XKT-R	720	14.2	46.3	309.3	9.67	n.d.	437.6	76.5	4.01	0.36	0.01	77.2	5.18	5.80	0.71	257	n.a.	n.a.
ZTH	691	11.1	59.6	338.7	10.5	n.d.	436.1	76.2	3.87	0.51	n.d.	79.4	4.99	5.88	0.60	255	-65	-8.4
HMZ	585	9.88	39.7	270.7	9.29	1.22	355.6	64.2	13.7	1.84	n.d.	65.1	4.15	5.03	0.31	151	n.a.	n.a.
HMZP-R	722	8.65	45.3	326.9	10.2	n.d.	429.6	73.7	6.72	0.63	0.15	75.5	4.89	5.88	0.43	264	n.a.	n.a.

表2 热泉水化学和氢氧同位素组成

Table 2 Hydrochemical and water isotopic compositions of the hot springs

样品编号	组分质量浓度/(mg·L^-1)															As质量浓度/ (μg·L^-1)	δD/‰	δ¹⁸O/‰
样品编号	HCO₃	CO₃	SO₄	Cl	F	Br	Na	K	Ca	Mg	Fe	Si	Li	B	硫化物	As质量浓度/ (μg·L^-1)	δD/‰	δ¹⁸O/‰
LGG-HT	0.0	0.00	436.2	42.8	2.69	0.29	208.4	38.2	6.64	1.05	0.47	139.1	2.86	1.33	0.17	35.7	n.a.	n.a.
LGG-LT	0.0	0.00	490.2	45.5	2.50	0.32	210.2	38.8	6.96	1.09	0.45	141.3	2.90	1.34	0.00	28.8	-53	-7.6
DRTY-01	0.0	0.00	3 548	30.1	2.33	n.d.	46.2	136.9	26.6	3.93	46.0	120.2	3.36	0.30	2.20	46.5	-58	-7.3
DRTY-02	0.0	0.00	1 894	29.5	2.33	n.d.	7.72	19.1	16.0	1.78	27.7	69.3	0.49	0.20	0.17	100	-55	-8.1
DRTY-03	0.0	0.00	667.0	12.6	1.04	n.d.	11.4	19.7	1.95	1.03	12.5	76.9	1.72	0.08	0.20	127	-60	-7.7
DRTY-04	0.0	0.00	694.6	10.1	0.91	n.d.	26.0	44.7	1.82	1.11	20.4	178.5	4.12	0.14	0.12	261	-67	-9.3
DRTY-10	0.0	0.00	15 590	50.9	15.2	n.d.	29.8	209.8	35.6	8.74	60.2	132.6	3.21	0.39	0.05	n.d.	-59	-9.6
DRTY-11	0.0	0.00	320.4	4.95	n.d.	n.d.	0.42	1.83	0.17	0.05	0.81	11.7	0.06	0.01	0.04	4.4	-56	-7.2
WGQ	60.8	0.01	175.1	5.53	1.21	n.d.	82.5	27.8	8.82	1.22	2.01	107.2	1.29	0.06	0.75	51.9	n.a.	n.a.
ZZQ	38.4	0.00	163.3	52.7	1.34	0.33	84.3	35.1	4.47	0.98	1.31	83.2	0.75	1.29	0.04	88.6	-64	-7.2
TQL	886	59.8	45.4	596.3	16.4	1.87	677.5	102.2	1.97	0.28	n.d.	108.9	8.04	9.88	2.60	751	n.a.	n.a.
YJQ-L	851	98.3	55.0	635.6	17.1	1.96	701.5	119.5	1.80	0.27	n.d.	121.0	8.35	10.07	5.90	897	n.a.	n.a.
GMQ	854	81.4	46.7	588.1	16.3	1.72	671.0	115.3	1.93	0.29	n.d.	134.8	8.04	9.73	5.20	837	-67	-7.5
HTJ-L	913	34.0	49.9	583.1	16.2	1.85	639.0	106.7	1.62	0.29	n.d.	114.4	7.58	9.19	4.20	802	-66	-7.7
HTJ-R	739	6.38	68.8	433.8	12.6	1.61	507.5	84.9	2.13	0.32	n.d.	116.2	6.11	7.41	2.10	593	n.a.	n.a.
DGG	1 256	5.73	40.8	738.1	19.9	2.35	858.0	150.0	1.77	0.26	n.d.	152.0	9.90	12.01	0.24	1 059	-65	-7.3
XKT-L	641	6.62	69.4	323.1	9.91	1.27	408.0	71.4	6.18	0.60	n.d.	72.3	4.66	5.56	0.17	305	n.a.	n.a.
XKT-R	720	14.2	46.3	309.3	9.67	n.d.	437.6	76.5	4.01	0.36	0.01	77.2	5.18	5.80	0.71	257	n.a.	n.a.
ZTH	691	11.1	59.6	338.7	10.5	n.d.	436.1	76.2	3.87	0.51	n.d.	79.4	4.99	5.88	0.60	255	-65	-8.4
HMZ	585	9.88	39.7	270.7	9.29	1.22	355.6	64.2	13.7	1.84	n.d.	65.1	4.15	5.03	0.31	151	n.a.	n.a.
HMZP-R	722	8.65	45.3	326.9	10.2	n.d.	429.6	73.7	6.72	0.63	0.15	75.5	4.89	5.88	0.43	264	n.a.	n.a.

图2 热海水热区所有热泉样品的Giggenbach Na-K-Mg三角图 ○:中性热泉;□:蒸汽加热型酸性热泉;△:受到中性地热水混合的蒸汽加热型酸性热泉。

Fig.2 Giggenbach's Na-K-Mg triangular diagram of all hot spring samples collected from the Rehai hydrothermal area. Symbols: ○Neutral hot springs; □Steam-heated acidic hot springs; △Steam-heated acidic hot springs mixing with some neutral geothermal waters.

图3 热泉氢氧同位素组成及对其地热化学成因的指示

Fig.3 Plot of δD vs. δ18O for the hot spring samples and indications for geothermal geochemical origin

图4 热海不同类型地热水地球化学成因概念模型图

Fig.4 A conceptual model of the geochemical origin of various geothermal waters in Rehai

表3 热泉中汞的不同形态的含量的模拟计算结果

Table 3 Simulated concentrations of various Hg species in the Rehai hot springs

样品编号	汞质量浓度/(mol·L^-1)
	Hg(0)	Hg(I)	Hg(II)
	Hg	H $g 2 2 +$	HgH $S 2 -$	Hg $S 2 2 -$	Hg(HS)₂	Hg(OH)₂
ZZQ	1.08E-10	1.13E-32	1.49E-14	1.18E-19	1.14E-11	8.96E-32
TQL	3.98E-12	0.00E+00	2.55E-09	1.38E-09	3.75E-11	4.21E-30
YJQ-L	2.90E-10	5.01E-40	2.62E-09	2.30E-09	2.44E-11	4.21E-30
GMQ	9.13E-11	0.00E+00	2.49E-09	2.09E-09	2.40E-11	4.83E-30
HTJ-L	9.41E-11	2.85E-40	3.82E-09	5.73E-10	2.03E-10	2.45E-31
HTJ-R	1.24E-10	3.14E-39	2.72E-09	5.98E-11	9.21E-10	6.98E-32
DGG	5.46E-10	2.15E-36	5.30E-09	1.76E-10	1.34E-09	1.29E-29
XKT-L	3.38E-13	2.16E-40	2.07E-09	1.52E-10	2.02E-10	2.51E-29
XKT-R	6.73E-10	1.89E-38	1.33E-09	2.09E-10	6.16E-11	3.83E-30
ZTH	6.05E-12	0.00E+00	1.71E-09	1.97E-10	1.08E-10	3.00E-30
HMZ	3.61E-14	0.00E+00	1.74E-09	2.93E-10	7.19E-11	1.86E-29
HMZP-R	5.19E-10	8.93E-38	1.75E-09	8.51E-11	2.62E-10	2.28E-30

表3 热泉中汞的不同形态的含量的模拟计算结果

Table 3 Simulated concentrations of various Hg species in the Rehai hot springs

样品编号	汞质量浓度/(mol·L^-1)
	Hg(0)	Hg(I)	Hg(II)
	Hg	H $g 2 2 +$	HgH $S 2 -$	Hg $S 2 2 -$	Hg(HS)₂	Hg(OH)₂
ZZQ	1.08E-10	1.13E-32	1.49E-14	1.18E-19	1.14E-11	8.96E-32
TQL	3.98E-12	0.00E+00	2.55E-09	1.38E-09	3.75E-11	4.21E-30
YJQ-L	2.90E-10	5.01E-40	2.62E-09	2.30E-09	2.44E-11	4.21E-30
GMQ	9.13E-11	0.00E+00	2.49E-09	2.09E-09	2.40E-11	4.83E-30
HTJ-L	9.41E-11	2.85E-40	3.82E-09	5.73E-10	2.03E-10	2.45E-31
HTJ-R	1.24E-10	3.14E-39	2.72E-09	5.98E-11	9.21E-10	6.98E-32
DGG	5.46E-10	2.15E-36	5.30E-09	1.76E-10	1.34E-09	1.29E-29
XKT-L	3.38E-13	2.16E-40	2.07E-09	1.52E-10	2.02E-10	2.51E-29
XKT-R	6.73E-10	1.89E-38	1.33E-09	2.09E-10	6.16E-11	3.83E-30
ZTH	6.05E-12	0.00E+00	1.71E-09	1.97E-10	1.08E-10	3.00E-30
HMZ	3.61E-14	0.00E+00	1.74E-09	2.93E-10	7.19E-11	1.86E-29
HMZP-R	5.19E-10	8.93E-38	1.75E-09	8.51E-11	2.62E-10	2.28E-30

图5 中性热泉中Hg(II)的四种存在形式( HgHS 2 -, HgS 2 2 -,Hg(HS)2,Hg(OH)2)的含量与硫化物含量(a)和pH(b)的关系

Fig.5 Relations between concentrations of four Hg(II) species ( HgHS 2 -, HgS 2 2 -, Hg(HS)2, Hg(OH)2) and sulfide concentration (a) or pH (b) in neutral hot springs

图6 热泉中汞含量与氯(a)、砷(b)含量的关系

Fig.6 Relations between Hg and Cl (a) or As (b) concentrations in the hot springs

表4 热泉样品对辰砂和黑辰砂的饱和指数

Table 4 Saturation indices of hot spring samples with respects to cinnabar and meta-cinnabar

样品编号	饱和指数		样品编号	饱和指数
样品编号	辰砂	黑辰砂	样品编号	辰砂	黑辰砂
ZZQ	-5.81	-6.41	DGG	-2.96	-3.56
TQL	-3.69	-4.29	XKT-L	-2.62	-3.22
YJQ-L	-4.69	-5.29	XKT-R	-4.81	-5.41
GMQ	-4.74	-5.34	ZTH	-3.31	-3.90
HTJ-L	-4.89	-5.49	HMZ	-2.33	-2.93
HTJ-R	-3.84	-4.43	HMZP-R	-4.44	-5.04

表5 硫磺塘热泉和澡塘河热泉中主要化学组分的含量对比

Table 5 Comparison of major chemical compositions of the Liuhuangtang and Zaotanghe hot springs

子区	数值类型	质量浓度/(μg·L^-1)		质量浓度/(mg·L^-1)
子区	数值类型	Hg	As	Cl	F	Br	Na	K	Ca	Mg	Li	Si	B
硫磺塘	最大值	1.472	1 059	738.1	19.9	2.35	858.0	150.0	2.13	0.32	9.90	152.0	12.01
硫磺塘	最小值	0.765	593	433.8	12.6	1.61	507.5	84.9	1.62	0.26	6.11	108.9	7.41
澡塘河	最大值	0.524	305	338.7	10.5	1.27	437.6	76.5	13.67	1.84	5.18	79.4	5.88
澡塘河	最小值	0.405	151	270.7	9.3	1.22	355.6	64.2	3.87	0.36	4.15	65.1	5.03

图7 中性热泉中汞含量空间分布及其与断裂的关系

Fig.7 Spatial distribution of mercury contents in neutral hot springs and its relations to faults

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