热液条件下Au络合物迁移行为的热力学模拟计算

马璐瑶; 马勋娇

doi:10.3969/j.issn.2097-0013.2025.01.006

热液条件下Au络合物迁移行为的热力学模拟计算

东华理工大学地球科学学院，江西南昌 330013

基金项目: 东华理工大学研究生创新基金（DHYC-202407）

详细信息

作者简介: 马璐瑶（1999—），女，硕士研究生，主要从事热液地球化学研究，E-mail：mly000602@163.com

中图分类号: P595；P618.51

收稿日期: 2024-12-03

修回日期: 2025-01-18

刊出日期: 2025-03-20

Thermodynamic Simulation of Migration Behavior of Au Complex Under Hydrothermal Conditions

School of Earth Sciences, East China University of Technology, Nanchang 330013, Jiangxi, China

Received Date: 03 December 2024

Revised Date: 18 January 2025

Publish Date: 20 March 2025

摘要

摘要:
金矿床的形成主要依赖于成矿热液将地下深部金元素运移至地壳浅部并促使其沉淀、富集，该过程在很大程度上取决于金络合物在热液环境中的稳定性。深入探究富金流体形成与迁移的具体条件，关键在于明晰影响热液中金络合物稳定性的物理化学因素。本文以热力学理论为基础，对地球化学模拟软件GEM-Selektor的数据库进行补充后，按照自然热液环境设计了不同的流体体系，并对其进行金的溶解度计算。研究结果表明，热液流体若呈现高温状态，同时具有较高的氧逸度，并富含HS⁻和S₃⁻等还原性硫配体时，将更有助于金的溶解。Au-HS⁻络合物相较于Au-Cl⁻络合物展现出更高的稳定性，尤其是Au(HS)S₃⁻的存在，显著提升了成矿流体在演化阶段萃取金的能力及运输效率。
- 地球化学 /
- 热力学模拟 /
- 金络合物 /
- 热液流体
Abstract:
The formation of gold deposits mainly depends on the transport of gold elements from deep underground to shallow crust by ore-forming hydrothermal fluids and their precipitation and enrichment, a process that largely depends on the stability of gold complexes in hydrothermal environments. The key to exploring the specific conditions for the formation and migration of gold-rich fluids is to clarify the physicochemical factors that affect the stability of gold complexes in the hydrothermal fluids. Based on the thermodynamic theory and after the supplementary database of the geochemical simulation software GEM-Selektor, different fluid systems are designed according to the natural hydrothermal environment, and the gold solubility calculations are carried out in this study. The results show that hydrothermal fluids with high temperature, high oxygen fugacity, and rich in reducing sulfur ligands, such as HS⁻ and S₃⁻ are more conducive to gold dissolution, and that Au-HS⁻ complexes exhibit higher stability than Au-Cl⁻ complexes, especially the presence of Au(HS)S₃⁻, which significantly enhances the extraction capacity and transport efficiency of gold in the evolutionary stage of the ore-forming fluids.
- geochemistry /
- thermodynamic simulation /
- gold complex /
- hydrothermal fluid

HTML全文

图 1 金络合物浓度(a)和硫物种浓度(b)随温度的变化情况

Figure 1.

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图 2 金络合物的浓度随pH (a)和氧逸度(b)的变化情况

Figure 2.

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图 3 金络合物的浓度随盐度(a)和总硫含量(b)的变化情况

Figure 3.

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图 4 与三种主要类型金矿床有关的热液体系达到平衡时金络合物的浓度

Figure 4.

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表 1 软件及数据库来源

Table 1. Software and database sources

软件及数据库	来源
GEM-Selektor	http://gems.web.psi.ch/
SUPCRT92	http://pdukonline.co.uk/download
SLOP98 database	http://geopig.asu.edu/supcrt_data.html

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表 2 金的络合物在不同温度下平衡时的浓度（mol/L）

Table 2. Concentration (mol/L) of gold complexes in equilibrium at different temperatures

温度（℃）	200	300	400	500	600
Au(HS)H₂S	7.10×10⁻¹³	3.98×10⁻¹⁷	5.64×10⁻¹⁵	1.15×10⁻¹⁰	8.83×10⁻⁴
Au(HS)S₃⁻	8.75×10⁻²⁶	3.23×10⁻¹⁶	2.37×10⁻⁸	7.08×10⁻⁴	1.44×10⁻¹
Au(HS)⁻	1.09×10⁻¹⁰	2.39×10⁻⁸	1.33×10⁻⁶	4.91×10⁻⁷	3.53×10⁻⁹
Au(HS)₂⁻	1.67×10⁻¹¹	9.46×10⁻⁷	1.13×10⁻²	3.01×10⁻¹	1.56×10⁻¹
Au(OH)	7.35×10⁻¹²	1.80×10⁻¹⁰	3.14×10⁻⁹	6.65×10⁻¹⁰	3.92×10⁻¹²
Au(OH)₂⁻	6.53×10⁻²⁰	8.94×10⁻¹⁸	5.66×10⁻¹⁶	1.59×10⁻¹⁶	1.36×10⁻¹⁸
AuCl₂⁻	5.67×10⁻¹⁵	8.62×10⁻¹²	7.71×10⁻⁹	5.22×10⁻⁸	1.05×10⁻⁸
AuCl	3.61×10⁻¹⁶	2.86×10⁻¹³	7.86×10⁻¹¹	2.01×10⁻¹⁰	1.03×10⁻¹¹

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表 3 含硫配体在不同温度下平衡时的浓度(mol/L)

Table 3. Concentration (mol/L) of sulfur-containing ligands in equilibrium at different temperatures

温度（℃）	200	300	400	500	600
H₂S₂O₃	2.66×10⁻²⁷	1.27×10⁻²¹	1.92×10⁻¹⁷	2.21×10⁻¹⁴	6.06×10⁻¹²
HS₂O₃⁻	4.42×10⁻²⁴	6.31×10⁻¹⁹	4.15×10⁻¹⁵	1.00×10⁻¹²	5.89×10⁻¹¹
S₂O₃²⁻	2.81×10⁻²¹	4.51×10⁻¹⁸	4.91×10⁻¹⁴	4.48×10⁻¹²	2.30×10⁻¹⁰
SO₂	5.57×10⁻²²	8.03×10⁻¹⁸	1.07×10⁻¹⁴	1.63×10⁻¹²	5.78×10⁻¹¹
HSO₄⁻	1.24×10⁻¹⁶	1.06×10⁻¹²	9.15×10⁻¹⁰	4.88×10⁻⁸	8.77×10⁻⁷
SO₄²⁻	1.82×10⁻¹⁴	7.38×10⁻¹³	5.55×10⁻¹⁰	7.20×10⁻⁹	8.92×10⁻⁸
S₃⁻	4.64×10⁻²¹	3.82×10⁻¹⁵	2.10×10⁻¹⁰	5.15×10⁻⁷	3.75×10⁻⁴
S₂²⁻	3.56×10⁻¹⁶	2.03×10⁻¹⁴	2.52×10⁻¹¹	5.98×10⁻¹⁰	1.45×10⁻⁸
S₃²⁻	1.17×10⁻²¹	1.59×10⁻¹⁸	1.89×10⁻¹⁴	2.25×10⁻¹²	1.71×10⁻¹⁰
S₄²⁻	2.43×10⁻²⁷	9.35×10⁻²³	1.11×10⁻¹⁷	6.91×10⁻¹⁵	1.74×10⁻¹²
S₅²⁻	4.15×10⁻³³	4.20×10⁻²⁷	5.20×10⁻²¹	1.75×10⁻¹⁷	1.54×10⁻¹⁴
H₂S	3.46×10⁻¹⁰	3.35×10⁻⁹	2.49×10⁻⁸	9.31×10⁻⁸	2.00×10⁻⁷
HS⁻	8.86×10⁻⁷	1.12×10⁻⁵	1.00×10⁻⁴	2.19×10⁻⁴	4.08×10⁻⁴
S²⁻	2.90×10⁻¹⁹	3.37×10⁻¹⁹	5.71×10⁻¹⁷	8.25×10⁻¹⁶	4.05×10⁻¹⁴

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表 4 金的络合物在不同pH值下平衡时的浓度（mol/L）

Table 4. Concentration (mol/L) of gold complexes in equilibrium at different pH values

pH值	2	3	4	5	6	7	8	9	10	11
Au(HS)S₃⁻	1.37×10⁻¹	8.97×10⁻²	1.98×10⁻³	4.83×10⁻⁴	2.68×10⁻⁴	1.00×10⁻⁴	1.92×10⁻⁶	2.43×10⁻⁸	5.24×10⁻¹⁰	3.12×10⁻¹²
Au(HS)⁻	2.21×10⁻⁴	1.21×10⁻⁴	2.65×10⁻⁵	1.20×10⁻⁵	1.00×10⁻⁵	4.13×10⁻⁶	1.10×10⁻⁶	2.57×10⁻⁷	7.07×10⁻⁸	1.26×10⁻⁸
Au(HS)₂⁻	6.77×10⁻⁴	1.04×10⁻³	1.26×10⁻³	4.35×10⁻³	5.34×10⁻²	2.51×10⁻¹	2.51×10⁻¹	2.50×10⁻¹	2.46×10⁻¹	2.23×10⁻¹
Au(OH)	2.10×10⁻⁷	1.85×10⁻⁷	1.78×10⁻⁷	1.26×10⁻⁷	7.20×10⁻⁸	3.84×10⁻⁸	2.48×10⁻⁸	1.52×10⁻⁸	9.74×10⁻⁹	5.58×10⁻⁹
AuCl₂⁻	2.04×10⁻⁴	2.15×10⁻⁵	2.40×10⁻⁶	2.10×10⁻⁷	1.29×10⁻⁸	4.42×10⁻¹⁰	3.20×10⁻¹¹	1.68×10⁻¹²	1.27×10⁻¹³	5.12×10⁻¹⁵
AuCl	9.45×10⁻⁶	8.82×10⁻⁷	8.99×10⁻⁸	6.49×10⁻⁹	3.82×10⁻¹⁰	1.35×10⁻¹¹	9.68×10⁻¹³	5.18×10⁻¹⁴	3.95×10⁻¹⁵	1.49×10⁻¹⁶

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表 5 金的络合物在不同氧逸度下平衡时的浓度（mol/L）

Table 5. Concentration (mol/L) of gold complexes at equilibrium with different oxygen fugacity

log₁₀(f_O2)	−39	−37	−35	−33	−31	−29	−27	−25	−23	−21
Au(HS)S₃⁻	1.10×10⁻⁸	1.40×10⁻⁸	1.60×10⁻⁸	2.10×10⁻⁷	1.32×10⁻⁵	4.35×10⁻³	6.37×10⁻²	2.60×10⁻¹³	2.95×10⁻²¹	1.44×10⁻³³
Au(HS)⁻	1.40×10⁻⁷	1.60×10⁻⁷	1.80×10⁻⁷	8.30×10⁻⁷	2.26×10⁻⁶	7.24×10⁻⁶	1.04×10⁻⁵	1.19×10⁻⁸	8.64×10⁻¹¹	4.19×10⁻¹⁴
Au(HS)₂⁻	5.29×10⁻³	5.31×10⁻³	5.49×10⁻³	6.89×10⁻³	1.97×10⁻²	1.83×10⁻²	1.43×10⁻²	3.15×10⁻⁹	8.13×10⁻¹⁴	6.36×10⁻²¹
Au(OH)	5.93×10⁻¹¹	6.58×10⁻¹¹	8.18×10⁻¹¹	6.35×10⁻¹⁰	3.30×10⁻⁹	1.49×10⁻⁸	1.09×10⁻⁷	7.44×10⁻⁷	1.51×10⁻⁶	4.49×10⁻⁶
AuCl₂⁻	5.14×10⁻¹⁰	5.79×10⁻¹⁰	7.22×10⁻¹⁰	8.92×10⁻⁹	1.85×10⁻⁸	8.55×10⁻⁸	2.75×10⁻⁷	1.94×10⁻⁶	3.99×10⁻⁶	1.20×10⁻⁵
AuCl	1.13×10⁻¹¹	1.79×10⁻¹¹	2.78×10⁻¹¹	1.38×10⁻¹⁰	6.65×10⁻¹⁰	3.79×10⁻⁹	1.39×10⁻⁸	8.94×10⁻⁸	1.84×10⁻⁷	5.52×10⁻⁷

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表 6 金的络合物在不同盐度下平衡时的浓度（mol/L）

Table 6. The concentration (mol/L) of gold complexes in equilibrium at different salinities

盐度w（wt.% NaCl_eq）	3.5	5.8	11.7	17.6	23.4	29.3
Au(HS)S₃⁻	4.49×10⁻⁵	4.08×10⁻⁵	3.65×10⁻⁵	2.06×10⁻⁵	2.52×10⁻⁵	3.45×10⁻⁵
Au(HS)⁻	5.93×10⁻⁶	5.58×10⁻⁶	5.50×10⁻⁶	3.21×10⁻⁶	3.16×10⁻⁶	3.65×10⁻⁶
Au(HS)₂⁻	1.07×10⁻³	1.10×10⁻³	9.21×10⁻⁴	1.48×10⁻³	1.81×10⁻³	1.84×10⁻³
Au(OH)	5.20×10⁻⁸	4.78×10⁻⁸	4.77×10⁻⁸	2.29×10⁻⁸	2.26×10⁻⁸	2.74×10⁻⁸
AuCl₂⁻	1.74×10⁻⁸	2.52×10⁻⁸	5.85×10⁻⁸	8.80×10⁻⁸	1.17×10⁻⁷	1.60×10⁻⁷
AuCl	1.83×10⁻⁹	2.07×10⁻⁹	3.41×10⁻⁹	4.18×10⁻⁹	4.79×10⁻⁹	5.84×10⁻⁹

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表 7 金的络合物在不同S浓度的热液中平衡时的浓度(mol/L)

Table 7. The concentration (mol/L) of gold complexes at equilibrium in the hydrothermal solution with different S concentrations

S浓度（wt.%）	0	0.5	1	1.5	2	2.5	3	3.5	4
Au(HS)S₃⁻	9.05×10⁻²³	1.40×10⁻²	3.93×10⁻²	6.81×10⁻²	9.87×10⁻²	1.30×10⁻¹	1.62×10⁻¹	1.95×10⁻¹	2.28×10⁻¹
Au(HS)⁻	3.00×10⁻¹⁰	3.30×10⁻⁵	4.19×10⁻⁵	4.75×10⁻⁵	5.16×10⁻⁵	5.49×10⁻⁵	5.79×10⁻⁵	6.02×10⁻⁵	6.24×10⁻⁵
Au(HS)₂⁻	3.50×10⁻¹²	3.80×10⁻²	5.66×10⁻²	6.90×10⁻²	7.84×10⁻²	8.60×10⁻²	9.28×10⁻²	9.84×10⁻²	1.04×10⁻¹
Au(OH)	9.61×10⁻⁸	1.01×10⁻⁷	1.06×10⁻⁷	1.09×10⁻⁷	1.11×10⁻⁷	1.13×10⁻⁷	1.15×10⁻⁷	1.17×10⁻⁷	1.18×10⁻⁷
AuCl₂⁻	2.80×10⁻⁷	2.85×10⁻⁷	2.94×10⁻⁷	2.99×10⁻⁷	3.03×10⁻⁷	3.07×10⁻⁷	3.08×10⁻⁷	3.12×10⁻⁷	3.13×10⁻⁷
AuCl	6.60×10⁻⁹	7.02×10⁻⁹	7.41×10⁻⁹	7.68×10⁻⁹	7.88×10⁻⁹	8.05×10⁻⁹	8.19×10⁻⁹	8.32×10⁻⁹	8.43×10⁻⁹

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表 8 三种主要类型金矿床热液体系平衡时金络合物浓度(mol/L)表

Table 8. Gold complexes concentration (mol/L) table at equilibrium of hydrothermal system in three main types of gold deposits

矿床类型	斑岩型	浅成低温热液型	造山型
Au(HS)H₂S	1.67×10⁻⁵	3.07×10⁻²⁰	8.77×10⁻¹²
Au(HS)S₃⁻	5.18×10⁻⁶	3.10×10⁻¹⁸	4.02×10⁻¹⁰
Au(HS)⁻	9.16×10⁻⁸	2.58×10⁻⁸	2.99×10⁻⁷
Au(HS)₂⁻	1.79×10⁻²	1.10×10⁻⁶	7.61×10⁻²
Au(OH)	5.05×10⁻⁷	3.21×10⁻¹⁰	4.35×10⁻⁹
AuCl₂⁻	1.20×10⁻⁶	5.65×10⁻¹⁴	2.00×10⁻¹²
AuCl	8.01×10⁻⁹	5.26×10⁻¹⁵	1.06×10⁻¹³

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热液条件下Au络合物迁移行为的热力学模拟计算

东华理工大学地球科学学院，江西 南昌 330013

作者简介: 马璐瑶（1999—），女，硕士研究生，主要从事热液地球化学研究，E-mail：mly000602@163.com

Thermodynamic Simulation of Migration Behavior of Au Complex Under Hydrothermal Conditions

School of Earth Sciences, East China University of Technology, Nanchang 330013, Jiangxi, China

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东华理工大学地球科学学院，江西南昌 330013