matte phases are calculated with varying matte grades and tion. So, it is very important to understand the behaviors of
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1 A Thermodynamic Model of Nickel Smelting and Direct High-Grade Nickel Matte Smelting Processes: Part II. Distribution Behaviors of Ni, Cu, Co, Fe, As, Sb, and Bi PENGFU TAN and DIETER NEUSCHÜTZ A thermodynamic model has been developed to predict the distribution behavior of Ni, Cu, Co, Fe, S, As, Sb, and Bi in nickel smelting and direct high-grade nickel matte smelting processes. The model has been validated by numerous experimental data and industrial data with a wide range of operating conditions. The effect of operating conditions on the distributions of Ni, Cu, Co, As, Sb, and Bi among the gas, matte, and slag phases has been investigated. It was found that the distribution behavior of Ni, Co, Cu, As, Sb, and Bi in the nickel smelting furnace depends on process parameters such as the smelting temperature, matte grade, oxygen enrichment, Fe/SiO 2 ratio in the slag, Cu/Ni ratio in charge, and oil/air ratio. The parameters also have an influence on the behavior of Fe 3 O 4 in the slag. I. INTRODUCTION A. Matte Grade THE extractive smelting process consists of a series of The matte grade is the most important operating parameter steps to eliminate impurities from the objective metal. The in the nickel smelting process. The fractional distributions controlled behavior of Ni, Cu, Co, As, Sb, and Bi in the of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and nickel smelting process is critical to the success of the operaa matte phases are calculated with varying matte grades and tion. So, it is very important to understand the behaviors of 96.8 pct oxygen enrichment in the blowing air at 1573 K. the elements, in order to recover valuable metals such as The results are shown in Figure 1. The terms (X) g, X Sl, Ni, Cu, and Co or to eliminate detrimental impurities such and {X} Mt represent the fractional distributions of X in the as As, Sb, and Bi. The thermodynamic model developed gas, slag, and matte phases, respectively. The content of previously [1] can be used to predict the behavior of these Fe 3 O 4 in the slag vs the matte grade is shown in Figure 2. elements in the nickel smelting process. The values of (As) g and (Sb) g decrease as the matte grade increases. The value of (Bi) g increases with increasing matte grade up to a level of 25 pct (Cu Ni) in the matte, then II. RESULTS AND DISCUSSION decreases slightly with increasing matte grade up to 45 pct (Cu Ni) in the matte, and then increases in the higher Four types of operating conditions were investigated at region. The values of As Sl and Sb Sl increase as the matte the plant-scale level by INCO Metals Company (Sudburg, grade increases to 35 and 45 pct, respectively, and then Canada), and excellent materials balances were obtained for the furnace. [2] The average accountability for as much as 11 decrease in the higher-matte-grade range. The value of Bi Sl increases with increasing matte grade. The values of {As} elements (Ni, Cu, Co, Fe, S, As, Bi, Si, Al, Ca, and Mg) Mt and {Sb} Mt decrease in the lower-matte-grade range, then was 99.3 pct. The industrial distributions of As, Bi, Ni, Cu, increase in the higher-matte-grade range with increasing Co, Fe, Si, Ca, Al, and Mg in the four modes were compared matte grade. with the predicted data from the thermodynamic model in The values of Ni Sl, Cu Sl, and Co Sl increase with this work, and good agreement was obtained. [1] The content of increasing matte grade, but {Ni} Mt, {Cu} Mt, and {Co} Mt Fe3 O 4 in the slag in the four modes was also in agreement with the predicted values. [1] decrease with increasing matte grade. This means that the The operation conditions and the compositions of the charges for these test modes were recovery rate of valuable metals such as nickel, copper, and presented in detail. [2] These are necessary for this modeling cobalt is lower in the higher-matte-grade range, especially work. So, the industrial operation conditions and the compophase is over 95 pct at 20 pct (Ni Cu) in the matte, but for cobalt. The fractional distribution of cobalt in the matte sitions of the charges in mode 1 of INCO Metals Company [2] are chosen as the conditions of simulation in this work. The it is only 30 pct when the matte grade decreases to 70 pct, content of As, Sb, and Bi in the concentrate was assumed as shown in Figure 1. to be 0.1 pct, respectively. The distribution coefficients of As, Sb, and Bi between The effect of operating conditions on the Ni, Cu, Co, As, the slag and matte vs the matte grade are shown in Figure Sb, and Bi distributions among the gas, matte, and slag are 3. It can be seen that the distribution coefficients of As and simulated, and the results are shown in the following text. Sb are significantly affected by the matte grade. The values of L s/m As and L s/m Sb decrease as the matte grade increases, while L s/m Bi is almost constant vs the matte grade in the range between 22 pct and 70 pct (Cu Ni) in the matte. The PENGFU TAN, Ph.D., Research Fellow, and DIETER NEUSCHÜTZ, value of L s/m Sb is higher than L s/m As in this matte-grade range. Professor, Dr. -Ing, are with the Institute of Theoretical Process Metallurgy, Aachen University of Technology (RWTH Aachen), Kopernikusstr. 16, Font et al. [4] pointed out that the oxidic species for arsenic, D Aachen, Germany. antimony, and bismuth are prevailing in the slag phase, and Manuscript submitted March 17, they exist mainly in the slag as AsO 1.5, SbO 1.5, and BiO 1.5. So, METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 32B, APRIL
2 Fig. 1 Fractional distribution of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against matte grade. Fig. 2 The content of Fe 3 O 4 in slag against matte grade. the following reactions among the matte, slag, and gaseous phases can be established: Fig. 3 Distribution coefficients of As, Sb, and Bi between slag and matte against matte grade. {X} 3/4 O 2 (g) (XO 1.5 ) [1] matte and slag, respectively; and { X } and ( XO1.5 ) are the activity coefficients of X in the matte and of XO 1.5 in the slag, respectively. Here, {n t } and (n t ) are the mole amounts of 100 g in the where ( ) and { } denote the slag and matte phases, respec- For a given temperature, the equilibrium constant of the tively. The term X represents As, Sb, or Bi. reaction (K 1 ) is constant, the activity coefficients of AsO 1.5, The distribution coefficients of X (L s/m X ) are calculated SbO 1.5, and BiO 1.5 in the slag and the ratio of (n t )/{n t } are using the following equation: [4] almost constant, [4] and the oxygen partial pressure increases with increasing matte grade. [1] So, the main reason that the L s/m X K 1 po 3/4 3 (n t) {n t } { X } [2] ( XO1.5 ) distribution coefficients of As and Sb decrease with increasing matte grade is the significant change of their activity coefficients in the matte, according to Eq. [2]. The activity 354 VOLUME 32B, APRIL 2001 METALLURGICAL AND MATERIALS TRANSACTIONS B
3 operations. The higher content of magnetite in the slag leads to the higher viscosity of the slag. If the magnetite is saturated in the slag, it will deposit in the bottom of the smelting furnace. This leads to a reduction of the smelting volume in the furnace. The content of Fe 3 O 4 in the slag increases significantly as the matte grade increases, as can be seen in Figure 2. The content of Fe 3 O 4 in the slag is only 3 pct at 25 pct (CU Ni) in the matte, and it increases to 35 pct when the matte grade increases to 70 pct. The reason for this is that the oxygen partial pressure increases with increas- ing matte grade. The calculations also show that the oxygen partial pressure increases from to bar as the matte grade increases from 20 to 70 pct. coefficients of As and Sb in the matte decrease remarkably as the matte grade increases, as shown in Figure 4. It is noted that the activity coefficient of bismuth in the matte decreases slightly with increasing matte grade. On the contrary, the oxygen partial pressure increases slightly as the matte grade increases. So, the distribution coefficient of bismuth does not change that much, according to Eq. [2]. Figure 4 also shows that As Sb Bi. This means that the chemical affinity between As and the matte is higher than that between Sb or Bi and the matte. The magnetite in the slag has an influence on the industrial Fig. 4 Raoultian activity coefficients of As, Sb, and Bi in matte against matte grade. B. Temperature The fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases are calculated with varying smelting temperatures and 96.8 pct oxygen enrichment in the blowing air at a fixed air/charge ratio (0.164 N m 3 /kg); these are shown in Figure 5. The calculations show that the matte grade increases from 26.9 to 33.6 pct as the temperature increases from 1473 to 1773 K at the fixed air/ charge ratio. The distributions of As, Sb, and Bi in the gas increase significantly with increasing temperature, because the higher temperature leads to the higher partial pressure of their gaseous species. The distributions of As, Sb, and Bi in the slag decrease slightly, but the distributions of Ni, Cu, and Co in the slag increase slightly as the temperature increases. The distributions of As, Sb, Bi, Cu, and Co in the Fig. 5 Fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against smelting temperature. METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 32B, APRIL
4 matte decrease with increasing temperature. So, the higher The above results suggest that the higher smelting temperature may be used in the industrial nickel smelting process temperature benefits the elimination of arsenic, antimony, and bismuth by means of volatilization, but does not benefit in order to eliminate arsenic, antimony, and bismuth and the recovery of copper and cobalt. lower the content of magnetite in the slag. In particular, the The calculations show that L s/m As, L s/m Sb, and L s/m Bi decrease higher temperature is necessary when a matte with a higher as the temperature increases, while L s/m Cx and L s/m Co increase as grade is produced directly. This is because the elimination the temperature increases, and L s/m Ni is almost constant in the rate of arsenic and antimony at the higher matte grade is temperature range from 1473 to 1773 K. At the same time, lower, and the content of Fe 3 O 4 in the slag is higher. L s/m Sb L s/m As L s/m Bi, and L s/m Co L s/m Cu L s/m Ni in this temperature range. The content of magnetite in the slag decreases as the C. Oxygen Enrichment temperature increases, as shown in Figure 6. So, the higher The fractional distributions of As, Sb, Bi, Ni, Cu, and Co temperature leads to a lower content of Fe 3 O 4 in the slag. among the gas, slag, and matte phases are calculated with varying oxygen enrichments in the blowing air at a fixed matte grade (30 pct) at 1573 K, and are shown in Figure 7. The distributions of As, Sb, and Bi in the gas decrease remarkably with increasing oxygen enrichment in the blowing air. The reason is that the volume of gas produced by the oxidation of iron and sulfur in the matte decreases with an increased content of oxygen in the blowing air at the fixed matte grade. So, the amounts of arsenic, antimony, and bismuth carried by the gas also decrease. The distributions of As, Sb, and Bi in the slag increase significantly with increasing oxygen enrichment. The values of {As} Mt and {Sb} Mt increase in the lower-oxygen-enrichment range, then decrease in the higher-oxygen-enrichment range with increasing matte grade. The distributions of Cu, Ni, and Co in the slag and matte seem to be independent of the oxygen Fig. 6 The content of Fe 3 O 4 in slag against smelting temperature. enrichment at a given matte grade. Fig. 7 Fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against oxygen enrichment (matte grade 30). 356 VOLUME 32B, APRIL 2001 METALLURGICAL AND MATERIALS TRANSACTIONS B
5 Fig. 8 Fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against the content of Fe in matte. The calculations show that L s/m As, L s/m Sb, and L s/m Bi increase as the oxygen enrichment increases, but L s/m Cu, L s/m Co, and L s/m Ni are almost constant in the oxygen-enrichment range between 21 and 100 pct. These results suggest that the use of oxygen or oxygenenriched air as the blowing gas in the nickel smelting process benefits the elimination of As, Sb, and Bi by means of slagging and has little influence on the recovery of valuable metals such as copper, nickel, and cobalt. The oxygen enrichment has no influence on the content of magnetite in the slag. D. The Content of Fe in the Matte The fractional distribution of As, Sb, Ni, Cu, and Co among the gas, slag, and matte phases are calculated with Fig. 9 The content of Fe 3 O 4 in slag against the content of Fe in matte. varying contents of iron in the matte and with a 96.8 pct oxygen enrichment in the blowing air at 1573 K. The results are shown in Figure 8. decrease, while the fractional distributions of nickel, copper, The values of (As) g and (Sb) g increase as the content of and cobalt in the matte increase with an increasing content Fe in the matte increases. The value of (Bi) g decreases as of iron in the matte. the content of Fe in the matte increase to 20 pct, increases The content of Fe 3 O 4 in the slag decreases significantly slightly as the content of Fe in the matte increases to 40 from 35 to 3 pct as the content of Fe in the matte increases pct, and then decreases in the higher-fe-content range. The from 5 to 40 pct, as shown in Figure 9. values of As Sl and Sb Sl increase as the content of Fe increases to 35 and 25 pct, respectively, and then decrease in the higher-fe-content range. The value of Bi Sl decreases E. The Fe/SiO 2 Mass Ratio in Slag as the content of Fe increases. The values of {As} Mt and {Sb} Mt decrease in the lower-fe-content range, then increase The fractional distributions of As, Sb, Bi, Ni, Cu, and Co in the higher-fe-content range as the content of Fe in the among the gas, slag, and matte phases are calculated with matte increases. The values of Ni Sl, Cu Sl, and Co Sl varying Fe/SiO 2 mass ratios in the slag and a 96.8 pct oxygen METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 32B, APRIL
6 Fig. 10 Fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against the Fe/SiO 2 ratio in slag (matte grade 30). F. The Concentration of SO 2 in Gas The fractional distributions of As, Sb, and Bi among the gas, slag, and matte phases are calculated with varying concentrations of SO 2 in the gas at a fixed matte grade (30 pct) at 1573 K and are shown in Figure 12. The distributions of As, Sb, and Bi in the gas decrease remarkably with an increasing concentration of SO 2 in the gas. The distributions of As, Sb, and Bi in the slag increase as the concentration of SO 2 in the gas increases. The values of {As} Mt and {Sb} Mt increase in the lower range of SO 2 concentrations then decrease slightly in the higher range of SO 2 concentrations with increasing matte grade. Fig. 11 The content of Fe 3 O 4 in slag against the Fe/SiO 2 ratio in slag (matte grade 30). enrichment in the blowing air, at a fixed matte grade (30 pct) at 1573 K. The results are shown in Figure 10. The values of (As) g, (Sb) g, (Bi) g, {As} Mt, {Sb} Mt, and {Co} Mt decrease slightly with an increasing Fe/SiO 2 mass ratio in the slag. The values of As Sl, Sb Sl, Bi Sl, and Co Sl increase slightly as the Fe/SiO 2 ratio increases. As can be shown in Figure 11, the content of Fe 3 O 4 in the slag increases remarkably from 0.55 to 12.8 pct as the Fe/SiO 2 mass ratio increases from 0.7 to 1.5. When the Fe/ SiO 2 ratio in the slag increases, the activity coefficient of Fe 3 O 4 in the slag decreases. [3] So, the content of magnetite increases with an increasing Fe/SiO 2 ratio in the slag. G. The Content of As, Sb, and Bi in the Charge The fractional distributions of As, Sb, and Bi are calculated with varying contents of As, Sb, and Bi in the charge and 96.8 pct oxygen in the blowing air, at a fixed matte grade (28 pct) at 1573 K. The results are shown in Figure 13. It is noted that the fractional distributions of As, Sb, and Bi are almost independent of the mass percentage of As, Sb, and Bi in the charge, at least in the range of actual impurity contents in the nickel-copper concentrates (less than 1 pct). It should be noted that the content of As, Sb, and Bi in the concentrate was assumed to be 0.1 pct in the calculations, respectively. Apparently, the predicted distributions of As, Sb, and Bi based on the assumption are reasonable and close to those found in practice. 358 VOLUME 32B, APRIL 2001 METALLURGICAL AND MATERIALS TRANSACTIONS B
7 Fig. 12 Fractional distributions of As, Sb, and Bi among the gas, slag, and matte phases against the concentration of SO 2 in gas (matte grade 30). Fig. 13 Fractional distributions of As, Sb, and Bi among the gas, slag, and matte phases against the content of As, Sb, and Bi in charge (matte grade 28). H. The Oil/Air Ratio as the Cu/Ni mass ratio increases, and Bi Sl is almost constant. The calculations show that the activity coefficients of The fractional distributions of As, Sb, and Bi are calcu- As, Sb, and Bi in the matte at the same matte grade (30 pct) lated with varying oil/air ratios and 96.8 pct oxygen in the increase with an increasing Cu/Ni ratio in the matte. The blowing air, at a fixed matte grade (30 pct) at 1573 K, and reason is that the chemical affinity between these impurity are shown in Figure 14. It is seen that the distributions of elements and the nickel in the matte is higher than that As, Sb, and Bi in the slag decrease with an increasing oil/ between these elements and the copper in the matte. [4] So, air ratio when the matte grade is constant, and the distribu- {As} Mt, {Sb} Mt, and {Bi} Mt decrease as the Cu/Ni ratio in tions of As, Sb, and Bi in the matte increase as the oil/air the matte increases. ratio increases. The oil/air ratio has no influence on the distribution coefficients of Ni, Cu, and Co between the slag and matte with a fixed matte grade. The gas is diluted by some combustion products of oil III. CONCLUSIONS such as CO 2 and H 2 O as the oil/air ratio increases at the The effect of operating conditions on the distributions of fixed matte grade and temperature. As, Sb and Bi volatilize Ni, Cu, Co, As, Sb, and Bi among the gas, matte, and slag into the gaseous phase, but Ni, Cu, and Co do not volatilize phases in nickel smelting processes and the behavior of in the smelting process. The is the reason why the oil/air magnetite in the slag have been investigated with a wide ratio has an influence on the distribution of As, Sb, and Bi, range of operating conditions. The operating conditions used but no influence on the distribution of Ni, Cu, and Co. in the calculations cover the practical ones in the Outokumpu flash-smelting process, the Outokumpu direct high-grade I. The Cu/Ni Mass Ratio in the Charge matte smelting process, and the INCO flash-smelting process. The fractional distributions of As, Sb, and Bi are calculated The partial elimination of arsenic and antimony by means with varying Cu/Ni ratios in the charge and 96.8 pct of slagging can be achieved effectively in the lower-matte- oxygen in the blowing air, at a fixed matte grade (30 pct) grade range, while that of bismuth can be done in the higher- at 1573 K, and are shown in Figure 15. The distributions matte-grade range. On the other hand, the elimination of of As, Sb, and Bi in the matte decrease with an increasing impurities by means of volatilization is not effective with Cu/Ni mass in the charge, while As Sl and Sb Sl increase increasing matte grades. The lower matte grade improves METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 32B, APRIL
8 Fig. 14 Fractional distributions of As, Sb, Bi, Ni, Cu, and Co among the gas, slag, and matte phases against the oil/air ratio (matte grade 30). Fig. 15 Fractional distribution of As, Sb, and Bi among the gas, slag and matte phases against the Cu/Ni ratio in charge (matte grade 30). the recovery of nickel, copper, and cobalt and leads to the lower content of magnetite in the slag. It should be said that the lower matte grade does not decrease the energy consumption. The higher smelting temperature improves the elimination of As, Sb, and Bi by means of volatilization and leads to the lower content of magnetite in the slag. It is suggested that the higher temperature be used in the direct highgrade nickel matte smelting process. A higher oxygen enrichment in the blowing gas does not improve the elimination of arsenic, antimony, and bismuth by means of volatilization because the volume of gas decreases, but it improves the elimination of these impurity elements by means of slagging. The oxygen enrichment has no influence on the recovery of copper and cobalt and has only little influence on the content of magnetite in the slag. The Fe/SiO 2 mass ratio in the slag and the oil/air ratio affect slightly the distributions of As, Sb, Bi, Ni, and Cu in the smelting process, but the Fe/SiO 2 ratio has a significant influence on the content of magnetite in the slag. The elimination of As, Sb, and Bi from the nickel-copper matte by volatilization and slagging increases with an 360 VOLUME 32B, APRIL 2001 METALLURGICAL AND MATERIALS TRANSACTIONS B
9 increasing Cu/Ni mass ratio in the charge. The fractional REFERENCES distributions of impurity elements such as arsenic, antimony, and bismuth among the gas, slag, and matte are 1. P. Tan and D. Neuschütz: Metall. Mater. Trans. B, 2001, vol. 32B, almost independent of their content in the charge. pp M.Y. Solar, R.J. Neal, T.N. Antonioni, and M.C. Bell: J. Met., 1979, ACKNOWLEDGMENT vol. 31 (1), pp N. Kemori, T. Kimura, Y. Mori, and S. Goto: Pyrometallurgy 87, The authors thank Professor Chuanfu Zhang (Central- IMM, London, 1987, pp South University of Technology, Changsha, People s Repub- 4. J. Font, M. Hino, and K. Itagaki: Mater. Trans., JIM, 1998, vol. 39 lic of China) for his constructive suggestions. (8), pp METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 32B, APRIL
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