Insights into the dissolution kinetics of copper–nickel tailings for CO₂ mineral sequestration

Abstract

Copper–nickel tailings (CNTs), consisting of more than 80wt% magnesium-bearing silicate minerals, show great potential for CO₂ mineral sequestration. The dissolution kinetics of CNTs in HCl solution was investigated through a leaching experiment and kinetic modeling, and the effects of reaction time, HCl concentration, solid-to-liquid ratio, and reaction temperature on the leaching rate of magnesium were comprehensively studied. Results show that the suitable leaching conditions for magnesium in CNTs are 2 M HCl, a solid-to-liquid ratio of 50 g·L⁻¹, and 90°C, at which the maximum leaching rate of magnesium is as high as 83.88%. A modified shrinking core model can well describe the leaching kinetics of magnesium. The dissolution of magnesium was dominated by a combination of chemical reaction and product layer diffusion, with a calculated apparent activation energy of 77.51 kJ·mol⁻¹. This study demonstrates the feasibility of using CNTs as a media for CO₂ mineral sequestration.

Keywords

copper–nickel tailings / dissolution kinetics / magnesium leaching / shrinking core model / CO₂ mineral sequestration

References

[1] Qian CG, Li CQ, Huang P, et al.. Research progress of CO₂ capture and mineralization based on natural minerals. Int. J. Miner. Metall. Mater., 2024, 31(61208

[2] International Energy Agency. Global Energy Review: CO₂ Emissions in 2021, 2022, Paris, IEA

[3] J.R. Fernández, An overview of advances in CO₂ capture technologies, Energies, 16(2023), No. 3, art. No. 1413.

[4] Metz B, Davidson O, Coninck HD, Loos M, Meyer L. IPCC Special Report on Carbon Dioxide Capture and Storage, 2005, Cambridge, Cambridge University Press442

[5] Sanna A, Dri M, Maroto-Valer M. Carbon dioxide capture and storage by pH swing aqueous mineralisation using a mixture of ammonium salts and antigorite source. Fuel, 2013, 114: 153

[6] Y. González, A. Navarra, R.I. Jeldres, and N. Toro, Hydrometallurgical processing of magnesium minerals–A review, Hydrometallurgy, 201(2021), art. No. 105573.

[7] Sanna A, Hall MR, Maroto-Valer M. Post-processing pathways in carbon capture and storage by mineral carbonation (CCSM) towards the introduction of carbon neutral materials. Energy Environ. Sci., 2012, 5(77781

[8] MacDowell N, Florin N, Buchard A, et al.. An overview of CO₂ capture technologies. Energy Environ. Sci., 2010, 3(111645

[9] Wang WM, Lu AH, Tao WD, Zhang WQ. Experimental study on acid solubility of tailings sand in Jinchuan copper–nickel mine. Acta Petrol. Mineral., 2005, 24(6633

[10] Wang HX. Chelating Agents-Induced Bioaccumulation of Pb/Zn by Plants of Tailings Waste Lands, 2011, Nanjing, Nanjing Agricultural University2

[11] Wang WM, Lu AH, Wang CQ, Zhang WQ. Thermodynamic analysis on diluted acid leaching process of tailings from copper nickel mine. Nonferrouss Met., 2007, 59(4102

[12] Liu WG, Peng XY, Liu WB, Zhang NX, Wang XY. A cost-effective approach to recycle serpentine tailings: Destruction of stable layered structure and solvent displacement crystallization. Int. J. Min. Sci. Technol., 2022, 32(3595

[13] Dlugogorski BZ, Balucan RD. Dehydroxylation of serpentine minerals: Implications for mineral carbonation. Renewable Sustainable Energy Rev., 2014, 31: 353

[14] Li JJ, Hitch M. Mechanical activation of ultramafic mine waste rock in dry condition for enhanced mineral carbonation. Miner. Eng., 2016, 95: 1

[15] Turianicová E, Baláž P, Tuček L, et al.. A comparison of the reactivity of activated and non-activated olivine with CO₂. Int. J. Miner. Process., 2013, 123: 73

[16] Li JJ, Hitch M. Ultra-fine grinding and mechanical activation of mine waste rock using a high-speed stirred mill for mineral carbonation. Int. J. Miner. Metall. Mater., 2015, 22(101005

[17] M. Chen, C. Wang, Q. Shi, H.M. Hu, Q.W. Zhang, and Z. Li, Enhanced simultaneous CO₂ mineralization and cadmium immobilization in a wide pH range by using ball-milled serpentine, Chem. Eng. J., 474(2023), art. No. 145558.

[18] Zulumyan N, Isahakyan A, Beglaryan H, Melikyan S. A study of thermal decomposition of antigorite from dunite and lizardite from peridotite. J. Therm. Anal. Calorim., 2018, 131(21201

[19] Werner M, Hariharan S, Zingaretti D, Baciocchi R, Mazzotti M. Dissolution of dehydroxylated lizardite at flue gas conditions: I. Experimental study. Chem. Eng. J., 2014, 241: 301

[20] Hariharan S, Repmann-Werner M, Mazzotti M. Dissolution of dehydroxylated lizardite at flue gas conditions: III. Near-equilibrium kinetics. Chem. Eng. J., 2016, 298: 44

[21] Frimmel FH. Book review: Chemistry of the solid-water interface. Processes at the mineral-water and particle-water interface in natural systems. By W. Stumm. Angew. Chem. Int. Ed. Engl., 1993, 32(71105

[22] Hariharan SB, Werner M, Zingaretti D, Baciocchi R, Mazzotti M. Dissolution of activated serpentine for direct flue-gas mineralization. Energy Procedia, 2013, 37: 5938

[23] C.D. Breuil, L. César-Pasquier, G. Dipple, J.F. Blais, M.C. Iliuta, and G. Mercier, Mineralogical transformations of heated serpentine and their impact on dissolution during aqueous-phase mineral carbonation reaction in flue gas conditions, Minerals, 9(2019), No. 11, art. No. 680.

[24] C.D. Breuil, L.C. Pasquier, G. Dipple, J.F. Blais, M.C. Iliuta, and G. Mercier, Impact of particle size in serpentine thermal treatment: Implications for serpentine dissolution in aqueous-phase using CO₂ in flue gas conditions, Appl. Clay Sci., 182(2019), art. No. 105286.

[25] H. Beglaryan, A. Isahakyan, N. Zulumyan, S. Melikyan, and A. Terzyan, A study of magnesium dissolution from serpentinites composed of different serpentine group minerals, Miner. Eng., 201(2023), art. No. 108171.

[26] McCutcheon J, Dipple GM, Wilson S, Southam G. Production of magnesium-rich solutions by acid leaching of chrysotile: A precursor to field-scale deployment of microbially enabled carbonate mineral precipitation. Chem. Geol., 2015, 413: 119

[27] P.Y. Shi, Y.Z. Liu, Q.Y. Chao, and M.F. Jiang, A convenient and user-friendly hydrometallurgical process for preparing porous siliceous adsorbents using ascharite tailings: Mechanism of structural change and evaluation of adsorption properties, Colloids Surf. A, 681(2024), art. No. 132787.

[28] Sun JZ, Wen JK, Chen BW, Wu B. Mechanism of Mg²⁺ dissolution from olivine and serpentine: Implication for bioleaching of high-magnesium nickel sulfide ore at elevated pH. Int. J. Miner. Metall. Mater., 2019, 26(91069

[29] Arce GLAF, Soares Neto TG, Ávila I, Luna CMR, Carvalho JA. Leaching optimization of mining wastes with lizardite and brucite contents for use in indirect mineral carbonation through the pH swing method. J. Cleaner Prod., 2017, 141: 1324

[30] Sirota V, Selemenev V, Kovaleva M, et al.. Preparation of crystalline Mg(OH)₂ nanopowder from serpentinite mineral. Int. J. Min. Sci. Technol., 2018, 28(3499

[31] Sierra C, Chouinard S, Pasquier LC, Mercier G, Blais JF. Feasibility study on the utilization of serpentine residues for Mg(OH)₂ production. Waste Biomass Valorization, 2018, 9(101921

[32] Singh V, Rautela R, Durbha KS, Murthy YR. Study of the kinetics of the magnesium leaching from serpentine bearing chromite overburden rocks for mineral carbonation. Miner. Process. Extr. Metall., 2020, 129(3–4282

[33] O.S. Baigenzhenov, T.A. Chepushtanova, A.Z. Altmyshbayeva, et al., Investigation of thermodynamic and kinetic regularities of asbestos waste leaching processes, Results Eng., 21(2024), art. No. 102000.

[34] Fan TT, Wang XS, Gao Y, Zhang XY. Investigating the interaction mechanism and effect of different calcium sulfate whiskers on performance of asphalt binder. Constr. Build. Mater., 2019, 224: 515

[35] Ma JY, Zhang YF, Qin YH, Wu ZK, Wang TL, Wang CW. The leaching kinetics of K-feldspar in sulfuric acid with the aid of ultrasound. Ultrason. Sonochem., 2017, 35: 304

[36] Teir S, Revitzer H, Eloneva S, Fogelholm CJ, Zevenhoven R. Dissolution of natural serpentinite in mineral and organic acids. Int. J. Miner. Process., 2007, 83(1–236

[37] Liu Y, Olsen AA, Rimstidt JD. Mechanism for the dissolution of olivine series minerals in acidic solutions. Am. Mineral., 2006, 91(2–3455

[38] Wang XL, Maroto-Valer MM. Dissolution of serpentine using recyclable ammonium salts for CO₂ mineral carbonation. Fuel, 2011, 90(31229

[39] Ferrufino GLAA, Okamoto S, Dos Santos JC, et al.. CO₂ sequestration by pH-swing mineral carbonation based on HCl/NH₄OH system using iron-rich lizardite 1T. J. CO2 Util., 2018, 24: 164

[40] Alexander G, Maroto-Valer MM, Gafarova-Aksoy P. Evaluation of reaction variables in the dissolution of serpentine for mineral carbonation. Fuel, 2007, 86(1–2273

[41] Jang NH, Park SK, Shim HM, Kim HT. Comparison of pretreatment method for the enhancement of CO₂ mineralogied sequestration using by serpentine. Appl. Chem. Eng., 2010, 21(124

[42] Farhang F, Rayson M, Brent G, Hodgins T, Stockenhuber M, Kennedy E. Insights into the dissolution kinetics of thermally activated serpentine for CO₂ sequestration. Chem. Eng. J., 2017, 330: 1174

[43] Gao WC, Wen JK, Li ZB. Dissolution kinetics of magnesium from calcined serpentine in NH₄Cl solution. Ind. Eng. Chem Res., 2014, 53(197947

[44] Viti C. Serpentine minerals discrimination by thermal analysis. Am. Mineral., 2010, 95(4631

[45] Bloise A. Thermal behaviour of actinolite asbestos. J. Mater. Sci., 2019, 54(1811784

[46] Benhelal E, Rashid MI, Rayson MS, et al.. Direct aqueous carbonation of heat activated serpentine: Discovery of undesirable side reactions reducing process efficiency. Appl. Energy, 2019, 242: 1369

[47] Rashid MI, Benhelal E, Anderberg L, et al.. Aqueous carbonation of peridotites for carbon utilisation: A critical review. Environ. Sci. Pollut. Res., 2022, 29(5075161

[48] A.A. Fara, M.R. Rayson, G.F. Brent, T.K. Oliver, M. Stockenhuber, and E.M. Kennedy, Formation of magnesite and hydromagnesite from direct aqueous carbonation of thermally activated lizardite, Environ. Prog. Sustainable Energy, 38(2019), No. 3, art. No. e13244.

[49] Irfan MF, Usman MR, Rashid A. A detailed statistical study of heterogeneous, homogeneous and nucleation models for dissolution of waste concrete sample for mineral carbonation. Energy, 2018, 158: 580

[50] X.Y. Peng, W.G. Liu, W.B. Liu, et al., Fluorite enhanced magnesium recovery from serpentine tailings: Kinetics and reaction mechanisms, Hydrometallurgy, 201(2021), art. No. 105571.

[51] Li N, Zhang YF, Kong DJ, Zhou QL, Chen X, Hui SE. Fluid particle group reaction model and experimental verification. Adv. Powder Technol., 2013, 24(1200

[52] Renedo MJ, Fernández J. Kinetic modelling of the hydrothermal reaction of fly ash, Ca(OH)₂ and CaSO₄ in the preparation of desulfurant sorbents. Fuel, 2004, 83(4–5525

[53] Gullett BK, Jozewicz W, Stefanski LA. Reaction kinetics of calcium-based sorbents with hydrogen chloride. Ind. Eng. Chem. Res., 1992, 31(112437

RIGHTS & PERMISSIONS

University of Science and Technology Beijing