Physicochemical Models for Ore Formation Processes at Mercury Deposits a.a. Obolensky, l.v. Gushchina, And a.s. Borisenko

7/29/2019 Physicochemical Models for Ore Formation Processes at Mercury Deposits a.a. Obolensky, l.v. Gushchina, And a.s.

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Russian Geology Geologiya

and Geophysics i Geofizika

Vol. 47, No. 12, pp. 1344-1359, 2006 UDC 550.41,546.59+;553.499

PHYSICOCHEMICAL MODELS

FOR ORE FORMATION PROCESSES AT MERCURY DEPOSITS

A.A. Obolensky, L.V. Gushchina, and A.S. Borisenko

Institute of Geology and Mineralogy, Siberian Branch of the RAS,

3 prosp. Akad. Koptyuga, Novosibirsk, 630090, Russia

We report results of computer modeling of physicochemical ore formation processes at

mercury deposits accumulated during the development of secondary-hydrothermal and

mixed-fluid ore-forming systems. Exogenous chloride brines, oil waters of artesian basins,

and petroleum pools are shown to serve as secondary mercury reservoirs and geochemical

barriers.

Modeling of possible mechanisms of mercury transfer and deposition in the form of cinnabar

(-HgS) was performed for ore-forming solutions of different compositions. Four mainthermodynamic models have been constructed using the Chiller program: (1) simple cooling

(cooling only), for recent thermal springs, (2) mixing of high-chloride hydrothermal solutions

with cold hydrosulfuric waters (mixing model), for telethermal deposits, (3) isoenthalpic

boiling (P = f(T)), and (4) solutionrock interaction (rock titration model).

Mercury deposits, ore-forming systems, composition of hydrothermal solutions, forms of

mercury transfer, metal-bearing capacity of solutions, thermodynamic modeling

INTRODUCTION

Study of geology, genesis, and regularities of mercury-deposit localization was one of the main avenues of

research of Academician V.A. Kuznetsov. Beginning with studying the Chagan-Uzun deposit [Kuznetsov, 1934]

and having discovered the Aktash deposit in Gorny Altai [Kuznetsov and Mukhin, 1936] and others in Kuznetsk

Alatau and Gornaya Shoria [Kuznetsov, 1939, 1940], he substantiated the concept of the West Siberian [Kuznetsov,

1943] and, later (after the discovery and study of Hg deposits in Tuva, West and East Sayans), Altai-Sayan

[Kuznetsov, 1958] mercury provinces. Having established the relationship of Central Asian Hg deposits with

Mesozoic tectonomagmatic activity, Kuznetsov recognized the Central Asian mercury belt as a global geologic

structure controlling the localization of Hg deposits [Kuznetsov, 1974].

Along with metallogeny problems, classification of mercury deposits was developed on the basis of recognized

ore associations [Kuznetsov et al., 1996], and the key genesis problems were studied, such as sources of ore matter

[Kuznetsov and Obolensky, 1970], mineral composition of ores, types of metasomatic wallrocks [Kuznetsov et al.,

1978], relationship of Hg deposits with magmatism, nature and sources of ore-forming hydrothermal solutions

[Obolensky et al., 1979], and physicochemical conditions of mercury transfer and deposition established in

thermobarogeochemical studies of fluid inclusions and thermodynamic modeling [Belevantsev et al., 1982]. Inrecent years, types of low-temperature hydrothermal ore-forming systems and their evolution in various geodynamic

settings [Borisenko, 1999; Obolensky et al., 1999; Obolenskiy and Naumov, 2003] and conditions of localization

of large mercury deposits [Distanov et al., 1998; Borisenko et al., 2005, 2006a] have been described.

In this paper we present results of computer modeling of ore formation processes at the main types of Hg

deposits. As we established earlier, such deposits are localized in structures of various geodynamic settings

[Obolenskiy and Naumov, 2003]:

1. On active continental margins:

In suprasubduction fault zones and in obducted oceanic crust in frontal parts of subduction zones

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(Californian type). This type includes the New Almaden and New Idria listwaenite-cinnabar Hg deposits on the

California Coast Range, Tamvatnei deposit on the Chukchi Peninsula, etc.

In areas of subaerial suprasubduction volcanism (Toscana type). Typical ore provinces are Toscana in

Italy, Transcarpathia, Kamchatka, New Zealand, etc.

In back-arc rifting zones (Nevada type). An example is the ore belt in the Basin and Range Province in

the western USA with the Opalite, Cordero, and other deposits.

2. In orogenic belts. These Hg deposits are confined to regional thrusts related to strike-slip faults (Tien

Shan type). Typical examples are the Khaidarkan, Chauvai, Chonkoi (Ulug-Too), and other deposits in Kirghizia

and the Aktash and Chagan-Uzun deposits in Gorny Altai.

3. In zones of continental rifts and paleorifts (aulacogens), which are still of high tectonic and magmatic

activity (Donetsk type). An example is the Donetsk Basin ore province with the Nikitovka and other Hg deposits.

4. In areas of within-plate rifting related to mantle plumes (Almaden type). Such deposits occur in the

Iberian (Almaden, El Entridicho, Las Cuevas, etc.) and South Chinese (Wan Shan) provinces.

Though Hg deposits formed in different geodynamic settings, this process was related to the development of

similar-type secondary-hydrothermal and mixed-fluid systems [Borisenko, 1999]. Each ore-forming system is

characterized by specific composition of hydrothermal solutions (determined by the paleohydrogeologic setting of

its evolution) and different gradients of change in physicochemical parameters: temperature, pressure, and

composition and concentration of solutions, which determine their acidityalkalinity (pH) and redox potential (Eh).

These parameters govern the form of transfer and conditions of deposition of ore-forming components at

geochemical barriers. The composition and concentration of hydrothermal solutions determine their possiblemetal-bearing capacity and ore potential. The existing concepts of the composition and concentration of

mineral-forming solutions at Hg deposits rest upon the studies of modern thermal springs depositing Hg minerals,

mainly detailed examinations of fluid inclusions in minerals of ores from Hg deposits (Fig. 1) [Obolensky et al.,

1979; Obolensky and Borisenko, 1979]. Mineral-forming solutions are of diverse compositions and can be

subdivided into three major groups according to the predominance of dissolved components: (1) sulfide-chloride

(with and without CO2), (2) sulfide-bicarbonate-chloride, and (3) sulfide-carbonate solutions. For model

computations, we chose solutions of each group (Table 1).

The most specific feature of Hg-bearing hydrothermal solutions is their polygenous nature and mantle sources

of Hg, which is confirmed by the presence of mantle 3He in them (Table 2) and the change in 3He/4He during

the ore formation [Naumov et al., 2004].

Along with the composition and concentration of hydrothermal solutions that formed Hg deposits, modeling

of ore formation processes requires knowledge of their metal-bearing capacity and ore potential [Belevantsev et

al., 1982]. Based on the generalized and supplemented available literature data on the mercury solubility in aqueouselectrolyte solutions in the system HgH2OH2SCl

CO2 at 25250 C, pH = 112, and different concentrations

of complexing ligands (HS, S2, Cl), we performed computer modeling in order to estimate the possible

metal-bearing capacities and ore potentials of different types of hydrothermal ore-forming solutions at Hg deposits

(Table 3). The metal-bearing capacity was evaluated with regard to the presence of two Hg species, Hg(II) and

Hg(0) (we used the refined constants of water solubility of Hg [Gushchina et al., 1989] and the transition

Hg(II) Hgaq0 at high temperatures [Gushchina et al., 1990]), and mercury chloride complexes [Gushchina et al.,

1994]. The presented data show strong temperature, CCl, and CS2 dependences of the Hg-bearing capacity of

hydrotherms. We have also established an important role of Hgaq0 in mercury transfer in low-chloride and low-sulfide

solutions.

Computing modeling has shown that some types of hydrothermal solutions can transfer and deposit large

amounts of Hg. For example, the Hg-bearing capacity of sulfide-chloride-CO2 and sulfide-carbonate solutions can

reach 0.41.3 g/kg H2O (Table 3). Note that at high temperatures, mercury is transported with fluids mainly asHg(0). Our studies confirmed the assumption on the prevailing participation of concentrated high-Hg ore-forming

solutions in the formation of large and, especially, unique Hg deposits (Fig. 2, Table 4).

The mechanism of Hg transfer, factors determining concentration of Hg-ores in some types of ore-forming

systems, and amounts of these ores were studied using the Chiller program (Solveq) [Reed, 1982] and enclosed

Soltherm-98 thermodynamic database supplemented with earlier obtained thermodynamic parameters of mixed

Hg(II) complexes [Belevantsev et al., 1982] and Sb(III) chlorine complexes and monosulfide [Belevantsev et al.,

1998a,b; Obolenskiy and Gushchina, 1999; Gushchina et al., 2000] and based on the SUPCRT92 thermodynamic

database [Johnson et al., 1992]. The program permits computation of equilibria in high-concentration solutions.

The concentrations of components in the initial aqueous solutions were calculated in mole/kg H2O. The redox

potentials of the model solutions were specified based on the sulfidesulfate equilibrium (Table 5).

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We have constructed four main thermodynamic models of the possible mechanisms of mercury transfer and

deposition in the form of cinnabar (-HgS) for ore-forming solutions of different compositions: (1) simple cooling

(cooling only), for recent thermal springs, (2) mixing of high-chloride hydrothermal solutions with cold

hydrosulfuric waters (mixing model), for telethermal deposits, (3) isoenthalpic boiling (P = f(T)), and (4)

solutionrock interaction (rock titration model).

ORE FORMATION IN MODERN THERMAL SOURCES

Systems of modern thermal springs are localized in subaerial-volcanism areas on active continental margins

and island arcs. Examples are the Wilbur Springs, Sulfur Bank, Sulfur Springs in California, Apapel and Uzonon the Kamchatka Peninsula, Ngawha, Blue Pool, and Acid Springs in New Zealand [Shikina et al., 1982; Davey

and van Moert, 1986; Karpov, 1988; Sorokin et al., 1988; Chudaev et al., 2000; Giggenboch et al., 2003]. As

these are real hydrothermal ore-forming systems which can serve as a prototype of paleohydrothermal systems, it

is important to recognize equilibrium Hg, Sb, and As species in them and elucidate some regularities of sulfide

mineral formation in the system H2OClH2SSbHgAs. For modeling ore formation processes in thermal-spring

systems, we used the cooling model [Gushchina et al., 2004].

The considered thermodynamic models are based on the physicochemical parameters and chemical

composition of thermal waters (Table 6). But for the systems to be electrically neutral, the concentrations of

prevailing Cl, SO42, and Na+ in the solutions were changed to obtain equivalent concentrations of cations and

anions.

Fig. 1. Composition of solutions of gas-liquid inclusions in minerals of Hg, Sb, and As ores.

Solutions: I NaClCaCl2; II NaClCO2; III NaHCO3NaCl; IV Na2CO3NaCl.

Deposits: 1 Hg (with Hg-containing sulfosalts); 2 Sb and Sb-Hg deposits; 3 As and

As-Hg: 1 Chazadyr, 2 Slavyanka, 3 Terligkhai, 4 Arzak, 5 Torasair, 6

Kurumdu-Aira, 7 Dzhylkydal, 8 Tyute, 9 Gorkhon, 10 Kadyrel, 11 Uzunsair,

12 Izerlig, 13 Tebek, 14 Aktash (Hg), 15 Chagan-Uzun, 16 Kurai, 17 Aktyul,

18 Cheremshanka, 19 Galkhaya, 20 Karasu, 21 Wan Shan, 22 Palyan, 23

Nikitovka, 24 Dzhizhikrut, 25 Barun-Shiveya, 26 Ust-Ege, 27 Khaidarkan, 28

Kadamzhai, 29 Tyrgetui, 30 Sarasa, 31 Aktash (As-Hg), 32 Lukhum, 33

Minkyule, 34 Elbrus, 35 Kodis-Dzeri, 36 Uzon, 37 Aktash (As), 38 Almaden,

39 Las Cuevas [Borisenko et al., 1974; Obolensky et al., 1979; Higueras et al., 2000].

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Table 1

Chemical Composition of Solutions for Thermodynamic Modeling

Group

no.

Composition

of solution

Concentration of

main components

[Cl] (ionic

strength)pH at 25 C Note

(mole/kg H2O)

1 NaCl

CaCl2

2.1 1.4 4.9 6.3 3.6 CH2S= 10

1

2 NaCl

CO2

0.9 0.5 0.9 0.9 3.2 CH2S= 10

1

3 NaCl

NaHCO3

0.9 0.6 0.9 1.5 8.5 8.3 CH2S= 10

1

CH2S= 10

4

4 NaCl

Na2CO3

1.7 0.5 1.7 3.1 12.2 11.5 CH2S= 10

1

CH2S= 10

4

Table 2

3He/4He Values in Ore-Forming Fluids from Hg Deposits

Deposit 3He/4He106

Nikitovka (Ukraine) 0.12

Khaidarkan (Kirghizia) 0.06

Wan Shan (China) 0.38

Aktash (Altai) 0.28

Dzhikidal (Altai) 1.6]

Sulfur Bank1 (USA) 19.419.9

Uzon

2

(Kamchatka) 611.3New Zealand3 3.17.4

Steamboat Springs1 (USA) 1.488.36

Note. 1 after [Torgersen and Jenkins, 1981]; 2 after [Rozhkov, 1979]; 3 after [Torgersen et al., 1982].

Table 3

Possible Metal-Bearing Capacity of Hydrotherms (from CHg at 250 C)

Group no.

Composition

of solution

[Cl]

(ionic

strength)pH250 C

0Possible content of Hg (g/kg H2O)

(mole/kg H2O) CH2S= 101

(a) CH2S= 104

(b)

1 NaCl

CaCl2

4.9 6.3 3 5103 0.4

2 NaCl

CO2

0.9 0.9 3 7104 0.05

3 NaCl

NaHCO3

0.9 1.5 8 3103 0.05

4 NaCl

Na2CO3

1.7 3.1 11 0.3 1.3

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The gas phase of the Wilbur Springs, Sulfur Bank (California), Ngawha, Blue Pool, Acid Springs (New

Zealand), and hot Apapel spring waters is composed of CO2 and CH4, and the mineral phase, of quartz and

cinnabar. The mineral phase of the Uzon caldera hydrotherm (Kamchatka) also contains orpiment and antimonite.

The results obtained are listed in Fig. 3.

Note that the waters of all considered thermal springs contain mercury as Hgaq0 . Its concentration reaches

5104 mole/kg H2O in the Blue Pool and Acid Springs acid waters at 250 C. This species is also predominantin H2S-free waters of these and the Apapel springs at low temperatures. Solutions rich in sulfides at temperatures

of up to 150 C are dominated by HgSHS, which produces cinnabar by the reaction

HgSHSaq =-HgSsol + HSaq

. (1)

In the Uzon caldera hydrotherms, arsenic is present as HAsO2 and H2AsO3 hydrocomplexes, which produce

arsenic sulfide:

2HAsO2aq + 3H2Saq = As2S3sol + 4H2O. (2)

Antimony is present in the hydrotherms as Sb(OH)3aq and forms antimonite following the reaction

Fig. 2. Hg content in ore-forming solutions of deposits (1)

and thermal springs (2) with different Hg reserves.

Table 4

Contents of Hg in Ore-Forming Solutions at Some Deposits [Borisenko, 1999]

Deposit Thom, C Csol, wt.% Main componentHg concentration*,

g/kg H2O

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Sb(OH)3aq + 1.5H2Saq = 0.5Sb2S3sol + 3H2O. (3)

At high temperatures, Sb can be transported as SbS2 and HSb2S4

, which form when the concentration of

dissolved H2S in the hot fluids increases. Near-neutral hydrotherms usually lack mercury chloride complexes though

contain Cl (Table 5), but acid brines (Blue Pool and Acid Springs) are characterized by the formation of Hg(II)

chloride complexes at high temperatures (>200 C) (Fig. 3).

Thus, mercury is transported with modern thermal springs as Hgaq0 , whose content increases with temperature,

and HgSHS, which exists in hydrosulfuric waters at < 200 C. The main factors responsible for cinnabar deposition

from waters are their cooling and decrease in sulfide sulfur concentration. Since Sb and As are transported with

hydrotherms mainly as HAsO2aq and Sb(OH)3aq, the deposition of their sulfides, in contrast to mercury sulfide,

requires not only a temperature decrease but also the presence of dissolved H2S.Thermodynamic modeling showed that simple cooling of solutions compositionally similar to the Apapel,

Blue Pool, and Acid Springs waters can result in the deposition of quartz, calcite, and magnesite but not cinnabar.

Since the concentration of Hgaq0 does not reach its saturation limit (pK50 C = 5.76), Hgliq is not deposited. But

Sorokin et al. [1988] notes that mercury sulfide can sometimes be produced through local concentration of sulfide

sulfur. The model solutions compositionally similar to the Sulfur Bank, Wilbur Springs, and Ngawha waters

containing sulfide sulfur deposit the same minerals and cinnabar (-HgS) when cooling from 250 to 100 C. The

solution compositionally close to the Sb,As,Hg-containing Uzon hydrotherms deposits quartz, Ca and Mg

carbonates, and antimonite (Sb2S3) when cooling from 250 to 150 C; on subsequent cooling to 100 C and below,

orpiment (As2S3) and cinnabar are produced.

Thus, the joint transfer of Sb and As in the form of hydroxyl complexes (Sb(OH) 3, HAsO2, H2AsO3) and

Table 5

Equilibrium Concentrations (mole/kg H2O) of Components in Initial Model Solutions

Component

Concentration in solution at 250 CConcentration in solution

at 150 C

I II III IV V VI a VI b VII

pH = 5.4 7.3 7.3 5.5 4.6 4.7 8.4

HS 1.00104 1.00101 1.00102 1.00101 1.00102 1.00103 1.00104 1.00102

SO42 1.00104 1.00105 1.00105 1.00105 1.00104 1.00104 1.00105 1.00105

Na+ 3.60 9.00101 1.70 9.00101 1.70 2.00 2.00101

Cl 4.40 9.00101 1.70 1.00 1.70 4.15 7.52101

Hg2+ 1.15103 4.09104 8.73104 2.65104 1.12104 1.00104 4.00104

HCO3 2.03102 2.78102 3.60102 5.37103 1.28102 9.54103 1.55101

K+ 8.00101 1.00101 1.00102

Fe2+

1.131010 1.00102 1.00103 1.00102 1.00103

SiO2aq 5.96103 5.92103 1.00103 1.00101

Sb(OH)3 4.10102 4.11103

Al3+ 1.00102 1.00105 1.00102

Mg2+ 1.00102 2.00101

TiO2 1.00104 1.00104

Ba2+ 1.00102

Mn2+ 1.00104 1.00104

Ca2+ 1.00 7.00102

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Table6

CharacteristicsandChemic

alCompositionofModernTherm

alSpringWaters

Spring

T,C

pH at

20C

Concen

tration,mole/kgH2O103

mole/kgH2O107

References

Na+

NH4+

K+

Ca2+SiO2

Al3+

Mg2+

Cl

SO42

HC

O3

H2S

Hg

As

Sb

SulfurBank

(California)

69

6.8

51.8

25.7

0.59

0.50

.7

2.3

18.2

6.2

53.9

0.35

1.00

Shikinaetal.,1982;

Karpov,1988

WilburSprings

(California)

57

7.2

398

16.8

11.8

0.044

.9

2.4

310

0.24

121

5.20

11.0

Ngawha

(NewZealand)

484898

6.46.47.6

36.0

36.1

35.6

8.28.2

1.61.621.8

1.90.200.58

3

.0

1.00.10

3535.238.3

3.63.610.17

5.57

5.57

4.84

0.18

0.176

0.18

4.980.50.17

2.7

Shikinaetal.,1982;

Karpov,1988;

Daveyandvan

Mo

ort,1986

AcidSprings,Blue

Pool(WhiteIsland,

NewZealand)

7993

1.41.3

0.26

14.7

6.76.1

16.3

0.82

0.086.65

0.60

0.55

0.006

0.89

0.158.17

1.125.2

0.170.02

0.01

0.01

0.002

0.002

0.030.03

Giggenbachetal.,

2003

UpperApapel

(Kamchatka)

9795

8.28.0

1721.7

0.38

0.26

1.530

0.01

4.925.1

1.305.71

3.30

3.11

200 C), as Hgaq0 . In H2S-free waters, Hgaq

0 remains the main Hg species

even at low temperatures. We have established that fluids can transport mercury in the form of Hg gas, whichaccumulates in the gas phase as a result of the transition of Hg(II) sulfides and Hg aq

0 into the latter. Cinnabar is

deposited from hydrotherms as the temperature drops and sulfide sulfur is concentrated. Since Sb and As are

transported with hydrotherms mainly as complexes Sb(OH)3 and HAsO2, the deposition of their sulfides, in contrast

to Hg sulfides, requires not only a temperature decrease but also the presence of dissolved H 2S.

In acid chloride solutions with low concentrations of S2, prevailing forms of mercury transfer at high

temperatures are chloride complexes HgCln2n . On cooling, the solutions deposit cinnabar, which is caused by the

increase in their concentration of sulfide sulfur on their mixing with H2S-containing solutions or by the metasomatic

replacement of the sulfide-enriched host rocks.

In near-neutral or alkaline NaHCO3NaCl and Na2CO3NaCl solutions, mercury is transported in the form

of sulfide complexes HgS22 and HgSHS and, partly, as Hgaq

0 , and antimony is transferred as SbS2 or Sb(OH)3.

The main factors responsible for the cinnabar deposition from these solutions are their cooling and decrease in

their sulfide sulfur concentration; antimony sulfide deposition requires, in addition, a decrease in pH of the solutionand the presence of dissolved H2S in it. Isoenthalpic boiling (P = f(T)) of the solutions and condensation of the

cooling gas phase (Hggas and H2Sgas) also lead to cinnabar deposition.

Thus, these types of solutions seem to play a leading role in the formation of most known hydrothermal

mercury deposits because they are most widespread in natural hydrothermal systems and deposit concentrated ores.

At the above-considered Hg deposits differing in the composition of ore-forming hydrothermal solutions,

wallrock metasomatism develops in different ways. The deposits produced by sulfide-chloride solutions show weak

pre-ore and intense syn-ore rock metasomatism. Ore deposition there completes syn-ore rock metasomatism. The

deposits formed by sulfide-chloride-carbon dioxide solutions abound in both pre-ore and syn-ore metasomatites.

First cinnabar generations are produced at the beginning of syn-ore metasomatism, whereas most of ores are

deposited together with kaolinite (dickite) at its final stage. At the deposits produced by sulfide-bicarbonate-car-

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bonate solutions, pre-ore metasomatites drastically dominate over syn-ore ones. Ore deposition there completes

syn-ore metasomatism.

The considered models of the formation of Hg deposits shed light on many moot points of their genesis,

such as their spatial separation from other types of mineralization and magmatism manifestations, the high

metal-bearing capacity and widely varying chemical composition of their ore-forming solutions (usually

corresponding to the composition of particular exogenous waters), the mantle source of their Hg (Sb, As), and the

supply of their S, Ba, Sr, Ni, Co, and Pb from the host rocks, as follows from the isotope-geochemical data.

We have established that exogenous waters play an important role in the formation of Hg deposits as they

are not only a medium for Hg accumulation but also a source of many elements (Ba, Sr, S, etc.) and serve as an

effective geochemical barrier for ore deposition (H2S, SO22, O, etc.). In the geological context, their participation

in the ore formation is expressed as a paleohydrogeologic control of Hg mineralization at regional and local levels

[Borisenko, 1990].

We thank Prof. M.Reed, Oregon University, USA, for kind provision of the Chiller program and Prof.

V.I. Belevantsev for help in study of mercury solubility.

This work was supported by grants 04-05-64485 and 04-05-64485 from the Russian Foundation for Basic

Research, Scientific School grant 4933.2006.5, and grant DSP.2.1.1.702 from the Ministry for Russian Science

and Education.

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Received 23 June 2006

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Physicochemical Models for Ore Formation Processes at Mercury Deposits a.a. Obolensky, l.v. Gushchina, And a.s. Borisenko