Monchegorsk ecology of beautiful tundra








Nature and origin of multicomponent aerial emissions of the copper-nickel smelter complex

Valery Barcan
Lapland Biosphere Reserve, Zeleny, 8; 184505, Monchegorsk, Murmansk Prov.,
Russia Received 5 February 2002;
accepted 12 August 2002


Abstract

The Severonickel Smelter Complex as well as other big nickel-copper smelter plants are the source of metallurgical dust emissions, enriched with toxic elements Ni, Cu, Pb, Zn and As. The phase composition of typical metallurgy dust is described as pentlandite (Ni,Fe)9S8, pyrrhotite Fe7S8(Nit), chalcopyrite CuFeS2, chalcosite Cu2S, covellite CuS, cuprite Cu20, tenorite CuO, and metal copper and nickel. The fine dust fractions are enriched by lead, zinc and arsenic oxides.
The obtained data can be turned to account when conducting the investigations of heavy metal behaviour in nature media, in particular soils.
2002 Elsevier Science Ltd. All rights reserved.

Keywords: Smelter technology; Nickel; Copper; Lead; Zinc and arsenic emissions

1. Preface

This work is accomplished on the practice of the Severonickel Smelter Complex (the town of Monchegorsk), processing sulfide raw materials. We have the basis to account that deductions may be disseminated to other similar enterprises. Dust and gaseous emissions of metallurgy plants processing sulfide materials into pure metals have similar composition, independently of location (Kola Peninsula and Taymir Peninsula in Russia, Canada, Australia, Finland, ex.), owing to similar raw materials (Polpherov, 1978) and the main metallurgy processes (Greyver, 1962; Lomako, 1968).

The production of nonferrous metals is very capital-capacious and, accordingly, inert process. The main processes used at Severonickel Complex until 1998 were described as far as 1962 (Greyver, 1962).
The smelter complex is a metallurgical enterprise with a complete production cycle, from the raw materials to the finished productspure electrolytic metals (Ni, Co and Cu), platinum metal concentrates and sulfuric acid. In the development of enterprises of this sort, the main emphasis was placed on maximizing the total output and on achieving technological perfection. The problems associated with the environmental effect of the smelter were largely ignored, and overall, they received only low priority when selecting the technology to be used or the investment policy. The first step to essential change of the process was made at 1998the electric melting of the ore was stopped, and the technological reconstruction of the smelter is now in progress, with the aim to reduce the volume of emissions to acceptable level. However, for the present, these changes are reversible simply the process is divided in the space (Monchegorsk-Norilsk).

2. Introduction

The irrevocable loss of metals from the plant as slags, dust and waste was at last the time 4.5-5% of the raw material. The emissions of Ni, Cu and S02 are shown in Tables 1 and 2. The total emissions is found in sum so big at the last 50 yearsnickel ~ 110000 tons, copper ~ 100000 tons and sulfur dioxide ~ 7 500 000 tonsthat even after its complete stop, the monitoring and study of their negative influence will remain actual for many decades.

Metallurgical slag contains toxic metals in immobile insoluble forms, and the slag heaps can cover several hectares of land. Metal-containing effluents pollute the neighbouring reservoirs, but represent local pollution sources only. Contrary to this, gaseous emissions from smelters such as Severonickel and Pechenganickel complexes in the Kola Peninsula and the Norilsk Smelter Complex in Siberia are global sources of atmospheric pollution (Kryuchkov and Makarova, 1989).

Airborne industrial emissions are distributed among three mediaair, water and soil. Gaseous pollutants, such as sulfur dioxide, nitrogen oxides and chlorine, are mainly present in the ambient air, although they are partly absorbed by soil and water. Particles of metallurgical dust, greater than 1 -2 um, are deposited on flat surfaces such as soil and water. Particles less than 1-2 jxm behave as gases, and remain in the air for indefinite periods and can be transported in the atmosphere for thousands kilometers (Kryuchkov and Makarova, 1989; Malachov and Zyrin, 1988).

The share of Severonickel Smelter Complex accounts for 94-96% of the total emissions of sulfur dioxide, and 100% of the emissions of nonferrous heavy metals at the central part of the Kola Peninsula (Poznyakov, 1993, 1999).



Table 1

Emissions S02 in atmosphere and utilization of sulfur at Severonickel Smelter Complex
Year Emissions SO2 (thousand tons per year) Utilization of sulfur of raw materials (%) Year Emissions SO2 (thousand tons per year) Utilization of sulfur of raw materials (%)
1969 94 33 1985 236 35
1970 101 32 1986 251 39
1971 111 31 1987 224 45
1972 118 30 1988 212 48
1973 215 21 1989 212 48
1974 259 18 1990 233 44
1975 274 19 1991 196 43
1976 268 20 1992 182 39
1977 246 22 1993 137 41
1978 244 30 1994 98 43
1979 189 39 1995 129 32
1980 206 38 1996 110 37
1981 187 39 1997 140 38
1982 239 34 1998 88 49
1983 278 23 1999 45 -
1984 257 32 2000 45 -
2001 44 76


The level of environmental contamination by emissions of Severonickel Smelter Complex is described as follows. The area about 4000 km2 around the plant is found to be contaminated by nickel and copper by the factor 6-1500 times more than European background, dependent on the distance and direction from the pollution source (Barcan and Silina, 1996). The soils sampled from the center of this airborne pollution, including the inhabited territory of the town of Monchegorsk, were found to be contaminated by nickel and copper to levels 450 and 250 times higher in comparison to the background, respectively9000 and 4000 mg/kg of soil (Barcan and Kovnatsky, 1998). By this reason, the plants (for example, berries, mushrooms, needles and leaves) growing over an area of at least 3000 km2 around the smelter complex are unsuitable for human consumption due to the elevated nickel concentration (Barcan et al., 1998).

Extremely low velocity of soil self-purification from the absorbed toxic metals (Iimura et al., 1977; Barcan, 2002) retains the urgency of their study on influence on the nature environment.

Unpublished bibliography connected with airborne emissions of Severonickel Smelter Complex includes about 1200 names, including summaries (Doncheva, 1978; Alexeyev, 1990; Norin and Yarmishko, 1990; Kozlov et al, 1993; Tikkanen and Niemelii, 1995; Reimann et al, 1996; Evdo-kimova, 1995; Lukina and Nikonov, 1996; Kozlov and Barcan, 2000; AMAP, 1998). However, all publications are characterized by the fact that the pollution source is considered as some sort of "black box". The technological characteristic of the pollution source and the form and chemical composition of the emitted compounds are not taken into account. Despite this, the properties and composition of the compounds are undoubtedly of great importance from the point of view of their interactions with nature media.

The aims of the study are to open for the ecologists the "black box" of the smelter by means of a brief description of the specific emissions linked to the main technological steps in ore processing and to emphasise the strong necessity to take into account both the physical properties and the chemical composition of the emitted dust particles in environmental research.



Table 2

Emissions in ambient air of nickel, copper and cobalt by Severonickel Smelter Complex (ton/year)
Years Nickel Copper Cobalt
1984 3110 2490 116
1985 3013 2420 82
1986 - - -
1987 - - -
1988 - - -
1989 - - -
1990 2712 1813 97
1991 2660 1740 97
1992 2118 1456 91
1993 1960 1049 89
1994 1619 934 82
1995 1366 726 56
1996 1309 700 41
1997 1350 760 37
1998 1304 874 35
1999 1128 856 32
2000 1126 873 34
2001 1212 827 44




3. The emission source

The main Ni- and Cu-containing minerals of Cu-Ni sulfide ores (Polpherov, 1978) are pentlandite (Ni,Fe)9S8 representing an isomorphous mixture of nickel and iron sulfides; pyrrhotite Fe7S8(Nit), containing solid solutions of nickel; and chalcopyrite CuFeS2. Other sulfide minerals, e.g. pyrite FeS2 cubanite CuFe2S3, occur rather rarely. Nickel is accompanied by cobalt, platinum metals, selenium, tellurium, gold and silver. The nickel content of the sulfide ores is 0.3-5.5%, copper 0.6-10% and cobalt 0.2%. The main mineral mass in the ore is magnetite (FeFe204), pyrrhotite and silicates of iron, aluminium, magnesium and calcium. The first operation is the melting of copper-nickel ores and circulating materials to form copper-nickel matte. As a result, the alloy simple sulfidesNi3S2, Cu2S and FeS, and the oxide alloyslagare obtained. From 13% to 25% of sulfur in the ore is emitted as sulfur dioxide in the ambient air. The dust clouds swirling up the smelter during many years consisted viz. of this gas.

The ores contain lead (0.002% average) as PbS, zinc (0.004-0.06% average) as ZnS and ZnO, and arsenic (0.005-0.03% average). The circulating products contain about 1% As as iron arsenate.
Ore smelting in the electric arc furnaces is accompanied by formation of the dust as a result of the evaporation of overheated smelt and sputtering. The gas flow carries much of the fine-grained material when feeding charge on the smelt surface in the furnace.
The gas from ore smelting is, after dust removal, subsequently emitted into the ambient air, partly through chimneys or sky-lights in the roof.
The copper-nickel matte is blown through with air and quartzite added to the iron slagging (the Bessemer process).

The bessemerizing gas contains up to 5-6% S02 and, after dust removal, passes to sulfuric acid production. A considerable proportion of the gas is emitted in the smelter building and subsequently passes out into the ambient air.

More gas and dust are emitted when the converter is turned off to pour out the alloy. The source of dust during besseme-rization is the formation of a multitude of small gas sprays in the turbulent alloy, and it is carried out by the gas flow.

The mixture of nickel, copper and cobalt sulfides formed as a result of the bessemerizing processBessemer matte is separated by flotation into nickel and copper concentrates, and these half-finished products are subsequently treated using a number of different techniques.
The treatment of the nickel concentrate (Ni3S2) is not accompanied by the essential emission of gas and dust in the ambient air because S02 is completely used for the sulfuric acid production, after the effective preliminated dust removal.
The anode nickel undergoes electrolytic refining to give the finished commercial productpure electrolytic nickel (99.97-99.99% Ni).
The half of sulfur, contained in copper concentrate, is emitted as S02 in the ambient air, as well as copper-bearing dust.
The obtained rough copper is refined by blistering and then electrolytic refining to give the finished commercial productpure electrolytic copper (99.95-99.99% Cu). The content of three metals in the liquid effluent formed during the hydrometallurgical production of nickel and copper is given in Table 3.
All the dust emission sources in the process chain are equipped with dust removal systems, but the large losses of metal in the form of dust are due to violations of technological principles, aged and defective equipment, etc. However, the losses could be relatively easily reduced. The total costs of the current gas purification systems, including depreciations, are only a few percent of production costs. Maximum tolerable emissions of S02 by Severonickel Smelter not more than 13 000-25 000 tons per year and emissions of nonferrous metals are totally not permissible (Kryuchkov and Makarova, 1989; Barcan, 1992).

The technological reconstruction of the Smelter is necessary for this aim, but this question is out of the framework of this paper.
The Severonickel Smelter is also a source of gaseous emissions of C02, CO, NOx, phenol, formaldehyde and polycyclic aromatic hydrocarbons, mainly benz(a)pyrene, sulfuric acid and sulfuric anhydride, hydrogen sulfide, chlorine, nickel tetracarbonyl, vanadium compounds, selenium dioxide and tellurium dioxide and manganese oxides (Table 4). Carbon and nitrogen oxides are formed as a result of the combustion of masut in the steam boiler and in the blister refining furnaces during the burning of self-coked electrodes in the electrical arc furnaces and the reduction of nickel monoxide by coke. The source of phenol and formaldehyde is the production of slag wadding in which phenol-formaldehyde resin is used as binder. 3,4-benz(a)pyrene is mainly formed during the burning of self-coked electrodes and masut combustion. The source of vanadium emissions is the combustion of masut, and of manganese during the melting of alloyed steel in the repair shop. Selenium, tellurium and cobalt are emitted together with nickel and copper. Nickel tetracarbonyl is emitted during the production of pure nickel powder, hydroaerosols of nickel and copper and chlorinewith ventilation gases of hydrometal shops. The source of sulfuric acid and sulfuric anhydride is sulfuric acid production. Table 4 is compiled by data of State Statistic reports, based on reports of the Environment Protection Department of the Severonickel Smelter Complex.



Table 3

Entrance of metals with sewage in natural reservoirs by Severonickel Smelter Complex (ton/year)
Years Nickel Copper Cobalt
1985 284 12 3.5
1986 213 5 5
1987 184 3 3
1988 138 2 2
1989 131 4 22.5
1990 123 5 2
1991 147 7 3
1992 84 5 2
1993 94 3 2.5
1994 54 2.5 1.5
1995 46 3 3
1996 54 4 2
1997 44 2.5 1.5
1998 32 3.5 0.5
1999 32 2.5 0.5
2000 20 2.5 0.6
2001 18 1.7 0.3




4. Investigation of metallurgical dusts of Severonickel Smelter Complex

4.1. Materials and methods: dust sampling and analysis

The dust samples were taken either from the gas flow near to the smoke ducts using special traps made from heat-resistant fabric, or from the last section of the electrostatic filters. The samples were always taken when the plant was working. The element content in the dust was determined by standard metallography methods (Volynsky, 1947; Vachro-meev, 1960; Isaenko et al, 1978). A total of 20 major elements were determined in the dust samples: Fe, Si, Al, Ca, Mg, S, Ni, Cu, Co, As, Cd, Cr, Mn, Pb, Zn, Se, Mo, Ti, V and W. The chemical analyses were conducted after extraction of the dust samples with a mixture of concentrated HC1 and HN03 (3:1, aqua regia). The total metal concentrations in the solution were determined as follows: Ni, Cu, Co, Fe, Zn and Pb by flame atomic absorption spectrometry on a Perkin Elmer 303 0B spectrometer; Al, Cr, Mn, Se, V, W, Ti, Sr, Mo, Ca and Mg on an AtomScan 25 emission ICP spectrometer (Thermo Jarrell Ash) and Cd and As on a Perkin Elmer 3030B spectrometer using a furnace cuvette. The total sulfur concentration in the dust was determined on a LECO CS-444 instrument by ignition in a current of oxygen and sulfur dioxide determination by infrared detection (LECO, 1991). The total silicon concentration in the dust was determined by a standard method involving alkaline melting (Ponomaryov, 1955).



Table 4

Pollutant emissions in ambient air by Severonickel Smelter Complex (ton/year)
1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 2001
Hydrocarbons 600 600 600 600 400 400 400 400 400 400 400 313
Benz(a)pyrene - - 0.06 0.06 0.06 0.053 0.014 0.014 0.015 0.013 0.013 0.010
H2SO4 318 302 262 245 251 197 206 267 184 212 195 115
H2S 28 28 28 28 18 18 18 18 18 18 18 16
Cl2 425 396 365 365 341 341 242 222 208 203 196 86
Phenol 8.6 8.6 8.6 8.6 1.7 1.7 0.9 0.8 0.7 0.7 0.7 0.5
Formaldehyde 553 553 553 553 108 64 33 28 24 4 4 3
Ni hydroaerosol 199 199 178 178 157 85 85 77 74 62 60 58
Cu hydroaerosol 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 2
Ni(CO)4 1.6 1.6 1.5 1.5 1.5 1.5 1.5 1.5 1.5 - - -
V205 48 48 48 57 60 40 39 37 46 47 45 62
Mn203 0.13 0.13 0.13 0.13 0.14 0.14 0.14 0.14 0.14 0.14 0.14 0.14
Se02 0.9 0.9 0.9 0.9 1.4 0.025 0.025 0.08 0.8 0.8 0.8 0.9
Te02 0.09 0.09 0.09 0.09 0.09 0.005 0.005 0.005 0.005 0.02 0.02 0.02




4.2. Results

The phase and chemical composition of the dusts, emitted by metallurgical processes and precipitated on the landscapes, are formed by the composition of initial and obtained products. At the same time, some elements like lead, zinc and arsenic are concentrated viz. in dusts, owing to high temperature volatility of their compounds.

The dust from the ore smelting mainly consists of the slag-forming compounds of iron, aluminium, magnesium, calcium and silicon, as well as sulfide minerals of nickel, copper and iron, which are both present in the ore (pen-tlandite, pyrrotite and chalcopyrite) and are formed during smeltingNi3S2, FeS2 and CuS (Table 5). The dust considerably is enriched with As to 0.1-0.6%, Pb to 0.2-0.3% and Zn to 0.4-1.4%, compared to the content in the ore. The sum of these elements in dust is equal or even more than that of nickel and copper (Table 6).



Table 5

Phase composition of metallurgical dusts of Severonickel Smelter Complex
Process Main phases

Melting of copper-nickel ores and concentrates
to obtain copper-nickel matte

pentlandite (Fe,Ni)9S8
pyrrotite Fe7S8
chalcopyrite CuFeS2
khyslevudite Ni3S2
pyrite FeS2
covellite CuS
silicates of Fe, As, Mg, Ca
As205
PbO
ZnO

Bessemerizing of copper-nickel matte

khyslevudite Ni3S2
Covellite CuS
Ni met
As205
PbO
ZnO
iron silicates

Processing of copper concentrate of matte flotation
(united dust of reverberatory melting, bessemerizing
of white matte and blister refining of rough copper)

chalcosite Cu2S
cuprite Cu20
tenorite CuO
Cu met

Kilning of nickel concentrate of matte flotation

khyslevudite Ni3S2
protoxide NiO
Ni met





The main structural components in the dust derived from the bessemerizing of copper-nickel matte include iron silicates, khyslevudite Ni3S2, covellite CuS and metal nickel (Table 5). The dust is enriched with As to 0.7-2%, Pb to 0.6-1.4% and Zn to 0.8-1.8%, which is equal or more than the content of nickel and copper (Table 6). The elevated molybdenum content is caused by loading nonferrous scrap metal into the converters. The dust produced during copper production mainly consists of chalcosite Cu2S, metal copper, cuprite Cu20 and tenorite CuO (Table 5). Copper is the main component (75%), and the following elements are iron, nickel and sulfur (Table 6).

The main structural components in the dust produced during the kilning of the Ni concentrate includes khyslevudite Ni3S2, protoxide NiO and metal nickel (Table 5). Nickel (33-45%), copper and iron are predominant (Table 6). The dust contains also considerable amounts of arsenic, lead, zinc and selenium. Sulfide copper-nickel ores, especially those from Norilsk, contain considerable amounts of platinum metals, gold and silver (Polpherov, 1978). The soils around Monchegorsk contain elevated concentrations of silver (Barcan and Kovnatsky, 1998).

The sum of elements in Table 6 is less than 100%. The rest includes oxygen, carbon, sorbed gases and other undetermined elements.
Thus, the main metal-containing compounds deposited on the landscape in the form of dust emissions from the smelter are pentlandite (Ni,Fe)9S8, pyrrotite Fe7Sg(Nit), chalcopyrite CuFeS2, chalcosite Cu2S, covellite CuS, cuprite Cu20, tenorite CuO, and metal copper and nickel. The fine fractions of the dust are enriched with lead, arsenic and zinc. The proportion of dust derived from different sources (metallurgical processes) varies according to the raw materials and the condition of the gas cleaning systems.

5. Conclusion

It is shown on the example of the copper-nickel Severonickel Smelter Complex that metallurgical dusts of non-ferrous plants are enriched with the toxic nonferrous metals: nickel, cobalt, copper, lead, zinc and arsenic.
The phase composition of typical metallurgy dust is described as pentlandite (Ni,Fe)9Sg, pyrrotite Fe7S8(NiT), chalcopyrite CuFeS2, chalcosite Cu2S, covellite CuS, cuprite Cu20, tenorite CuO, and metal copper and nickel.

The fine dust fractions are enriched by lead, zinc and arsenic oxides.
The obtained data can be turned to account when conducting the investigations of heavy metal behaviour in nature media, in particular soils.



Table 6

Concentrations of predominant elements in dusts of the main pyrometallurgical processes of Severonickel Smelter Complex
Element Detection limit (%) Process 1 Process 2 Process 3 Process 4
Al 0.0025 1.3-3.8 (1-4) 1.0 (1) < 0.0025 (1) -
As 0.0125 0.1-0.6 (1-6) 0.7-2.0 (1-3) 0.01 (1-5) 0.07-0.26 (1-5)
Ca 0.0025 1.0-2.3 (1-4) 0.35 (1) < 0.0025 (1) -
Cd 0.0025 0.02-0.03 (1-3) 0.04 (1) - -
Co 0.0125 0.05-0.20 (1-6) 0.2-0.6 (1-3) 0.03-0.50 (1-10) 0.9-1.5 (1-5)
Cr 0.0125 0.01-0.06 (1-2) 0.04 (1)
Cu 0.0125 1.3-4.3 (1-6) 3.1-5.3 (1-3) 24.1-76.3 (1-10) 2.0-6.4 (1-5)
Fe 0.0125 1.1-33.8 (1-6) 12.4-15.1 (1-3) 1.5-16.2 (1-10) 2.8-4.5 (1-5)
Mg 0.0025 2.3-5.1 (1-4) 0.3 (1) < 0.0025 (1) -
Mn 0.0125 0.06-0.07 (1-3) 0.05 (1) - -
Mo 0.0125 0.02-0.04 (1-2) 0.2 (1) - -
Ni 0.0025 1.3-8.4 (1-6) 3.1-6.4 (1-3) 0.9-11.0 (1-10) 32.9-45.4 (1-5)
Pb 0.0125 0.02-0.30 (1-5) 0.6-1.4 (1-3) 0.01-0.02 (1-4) 0.04-0.36 (1-5)
Stotal 0.0005 3.2-8.3 (1-5) 8.0-12.0 (1-2) 3.1-15.7 (1-10) 2.9-10.9 (1-5)
Se 0.0125 < 0.01 (1-4) 0.04 (1) - 0.07-1.0 (1-5)
Si 0.01 1.5-15.0 (1-4) 2.4 (1) 0.2 (1) -
Ti 0.0125 0.01-0.10 (1-3) 0.1 (1) - -
V 0.0125 < 0.01 (1-3) < 0.01 (1) - -
W 0.0125 0.03-0.09 (1-2) - - -
Zn 0.0020 0.4-1.4 (1-5) 0.8-1.8 (1) 0.01-0.02 (1-4) 0.002-0.17 (1-5)


"-" No data.
Processes 1 - Melting of copper-nickel ores and concentrates to obtain copper-nickel matte.
Processes 2 - Bessemerizing of copper-nickel matte.
Processes 3 - Treatment of copper concentrate (united dust of reverberatory melting, bessemerizing of white matte and blister refining of rough copper).
Processes 4 - Kilning of nickel concentrate of matte flotation.
In brackets - number of samples.


Acknowledgements

The author thanks Dr. Mikhail Kozlov, Senior Resercher from the University of Turku, for discussions, and Dr. John Derome, Senior Scientist from the Finnish Forest Research Institute, for help with the English language.

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