Stabilization/solidification mechanisms of tin tailings and fuming slag-based geopolymers for different heavy metals

Highlights

● Immobilization efficiency of cations (Cu, Zn, Mn) was higher than that of anions (As, Cr).

● Cr₂O₇^2– is converted to CrO₄^2– and combines with OH^– to form Cr(OH)₃ precipitates.

● Cations are embedded in aluminosilicate lattice while anions are form precipitates.

Abstract

Tin mine tailings (TMT) and fuming slag (FS) contain many heavy metals (As, Cr, Cu, Zn and Mn) that cause severe pollution to the environment. Herein, geopolymers were prepared using TMT, FS and flue gas desulfurization gypsum (FGDG) to immobilize heavy metals, and their compressive strength and heavy metal leaching toxicity were investigated. It was first determined that T4F5 (TMT:FS = 4:5) sample exhibited the highest compressive strength (7.83 MPa). T4F5 achieved 95% immobilization efficiency for As and Cr, and nearly 100% for Cu, Zn and Mn, showing good immobilization performance. A series of characterization analyses showed that heavy metal cations can balance the charge in the geopolymer and replace Al in the geopolymer structure to form covalent bonds. In addition, about 2%–20% of heavy metal Fe was immobilized in hydration products, heavy metal hydroxides and non-bridging Si–O and Al–O coordination with silica-aluminate matrices. AsO₃^3– was oxidized into AsO₄^3–, which may form Ca–As or Fe–As precipitates. Cr₂O₇^2– was converted to CrO₄^2– under alkaline environment and then combined with OH^– to form Cr(OH)₃ precipitates. Mn²⁺ may react directly with dissolved silicate to form Mn₂SiO₄ and also form Mn(OH)₂ precipitates. The unstable Mn(OH)₂ can be further oxidized to MnO₂. The heavy metal cations were immobilized in the silicoaluminate lattice, while the anions tended to form insoluble precipitates. These results may benefit the industry and government for better handling of TMT, FS and solid wastes containing the abovementioned five heavy metals.

Graphical abstract

Keywords

Heavy metals / Cementitious materials / Tin tailings / Stabilization/solidification / Redox

References

[1] AbadelA AAlbidah A SAltheebA HAlrshoudiF AAbbasH SalloumY A A (2021). Effect of molar ratios on strength, microstructure & embodied energy of metakaolin geopolymer. Advances in Concrete Construction 11: 127–140

[2] Ahmari S, Zhang L. (2013). Durability and leaching behavior of mine tailings-based geopolymer bricks. Construction & Building Materials, 44: 743–750

[3] Biswal B K, Zhu W, Yang E H. (2020). Investigation on Pseudomonas aeruginosa PAO1-driven bioleaching behavior of heavy metals in a novel geopolymer synthesized from municipal solid waste incineration bottom ash. Construction & Building Materials, 241: 118005

[4] Boca Santa R A A, Soares C, Riella H G. (2016). Geopolymers with a high percentage of bottom ash for solidification/immobilization of different toxic metals. Journal of Hazardous Materials, 318: 145–153

[5] ChangYCao JSongWWangZXuC LongM (2023). Effects of sulfur on variations in the chemical speciation of heavy metals from fly ash glass. Frontiers of Environmental Science & Engineering 17(10): 128 10.1007/s11783–023-1783–023

[6] Chen Q Y, Ke Y J, Zhang L N, Tyrer M, Hills C D, Xue G. (2009). Application of accelerated carbonation with a combination of Na₂CO₃ and CO₂ in cement-based solidification/stabilization of heavy metal-bearing sediment. Journal of Hazardous Materials, 166(1): 421–427

[7] Chen Y, Chen F, Zhou F, Lu M, Hou H, Li J, Liu D, Wang T. (2022). Early solidification/stabilization mechanism of heavy metals (Pb, Cr and Zn) in Shell coal gasification fly ash based geopolymer. Science of the Total Environment, 802: 149905

[8] Ei-Eswed B I, Aldagag O M, Khalili F I. (2017). Efficiency and mechanism of stabilization/solidification of Pb(II), Cd(II), Cu(II), Th(IV) and U(VI) in metakaolin based geopolymers. Applied Clay Science, 140: 148–156

[9] Faheem M, Huang X, Li S, Xia M, Zhang M L, Liu Q, Hassan M A S, Jiao B Q, Yu L, Li D W. (2018). Strength evaluation by using polycarboxylate superplasticizer and solidification efficiency of Cr⁶⁺, Pb²⁺ and Cd²⁺ in composite based geopolymer. Journal of Cleaner Production, 188: 807–815

[10] Fu B, Liu G, Mian M M, Sun M, Wu D. (2019). Characteristics and speciation of heavy metals in fly ash and FGD gypsum from Chinese coal-fired power plants. Fuel, 251: 593–602

[11] Gao W, Ni W, Zhang Y, Li Y, Shi T, Li Z. (2020). Investigation into the semi-dynamic leaching characteristics of arsenic and antimony from solidified/stabilized tailings using metallurgical slag-based binders. Journal of Hazardous Materials, 381: 120992

[12] Guo B, Pan D A, Liu B, Volinsky A A, Fincan M, Du J F, Zhang S G. (2017). Immobilization mechanism of Pb in fly ash-based geopolymer. Construction & Building Materials, 134: 123–130

[13] Gworek B, Dmuchowski W, Koda E, Marecka M, Baczewska A, Brągoszewska P, Sieczka A, Osiński P. (2016). Impact of the municipal solid waste Łubna landfill on environmental pollution by heavy metals. Water, 8(10): 470

[14] Hu S, Zhong L, Yang X, Bai H, Ren B, Zhao Y, Zhang W, Ju X, Wen H, Mao S. . (2020). Synthesis of rare earth tailing-based geopolymer for efficiently immobilizing heavy metals. Construction & Building Materials, 254: 119273

[15] Huang T, Zhou L, Cao Z, Zhang S, Liu L. (2021). A microwave irradiation-persulfate-formate system for achieving the detoxification and alkali-activated composite geopolymerization of the chromate-contaminated soil. Ecotoxicology and Environmental Safety, 217: 112233

[16] Huang X, Huang T, Li S, Muhammad F, Xu G, Zhao Z, Yu L, Yan Y, Li D, Jiao B. (2016). Immobilization of chromite ore processing residue with alkali-activated blast furnace slag-based geopolymer. Ceramics International, 42(8): 9538–9549

[17] Huang X, Zhuang R, Muhammad F, Yu L, Shiau Y C, Li D. (2017). Solidification/stabilization of chromite ore processing residue using alkali-activated composite cementitious materials. Chemosphere, 168: 300–308

[18] Ji Z, Pei Y. (2019). Bibliographic and visualized analysis of geopolymer research and its application in heavy metal immobilization: a review. Journal of Environmental Management, 231: 256–267

[19] Ji Z, Pei Y. (2020). Immobilization efficiency and mechanism of metal cations (Cd²⁺, Pb²⁺ and Zn²⁺) and anions (AsO₄^3– and Cr₂O₇^2–) in wastes-based geopolymer. Journal of Hazardous Materials, 384: 121290

[20] KimJ HLee J Y (2019). An optimum condition of MICP indigenous bacteria with contaminated wastes of heavy metal. Journal of Material Cycles and Waste Management, 21(7): 239–247

[21] Kulikowska D, Gusiatin Z M, Bułkowska K, Kierklo K. (2015). Humic substances from sewage sludge compost as washing agent effectively remove Cu and Cd from soil. Chemosphere, 136: 42–49

[22] Lan J, Dong Y, Sun Y, Fen L, Zhou M, Hou H, Du D. (2021). A novel method for solidification/stabilization of Cd(II), Hg(II), Cu(II), and Zn(II) by activated electrolytic manganese slag. Journal of Hazardous Materials, 409: 124933

[23] Li Q, Zhong Z, Du H, Zheng X, Zhang B, Jin B. (2022). Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: analysis of stabilizing heavy metals. Frontiers of Environmental Science & Engineering, 16(7): 85

[24] Li Y, Liu X, Li Z, Ren Y, Wang Y, Zhang W. (2021). Preparation, characterization and application of red mud, fly ash and desulfurized gypsum based eco-friendly road base materials. Journal of Cleaner Production, 284: 124777

[25] Liew Y M, Heah C Y, Mohd Mustafa A B, Kamarudin H. (2016). Structure and properties of clay-based geopolymer cements: a review. Progress in Materials Science, 83: 595–629

[26] Liu J, Hu L, Tang L, Ren J. (2021). Utilisation of municipal solid waste incinerator (MSWI) fly ash with metakaolin for preparation of alkali-activated cementitious material. Journal of Hazardous Materials, 402: 123451

[27] Mabroum S, Moukannaa S, El Machi A, Taha Y, Benzaazoua M, Hakkou R. (2020). Mine wastes based geopolymers: a critical review. Cleaner Engineering and Technology, 1: 100014

[28] Pan D A, Li L L, Wu Y F, Liu T T, Yu H L (2018). Characteristics and properties of glass-ceramics using lead fuming slag. Journal of Cleaner Production, 175(5): 251–256

[29] Ren B, Zhao Y, Bai H, Kang S, Zhang T, Song S. (2021). Eco-friendly geopolymer prepared from solid wastes: a critical review. Chemosphere, 267: 128900

[30] Sithole N T, Ntuli F, Okonta F. (2020). Fixed bed column studies for decontamination of acidic mineral effluent using porous fly ash-basic oxygen furnace slag based geopolymers. Minerals Engineering, 154: 106397

[31] TanL, YuC, WangM, Zhang S, SunJ, DongS, SunJ (2019). Synergistic effect of adsorption and photocatalysis of 3D g-C₃N₄-agar hybrid aerogels. Applied Surface Science, 467–468: 286–292 10.1016/j.apsusc.2018.10.067

[32] Tang L, Yang G D, Zeng G M, Cai Y, Li S S, Zhou Y Y, Pang Y, Liu Y Y, Zhang Y, Luna B. (2014). Synergistic effect of iron doped ordered mesoporous carbon on adsorption-coupled reduction of hexavalent chromium and the relative mechanism study. Chemical Engineering Journal, 239: 114–122

[33] Usman Kankia M, Baloo L, Mohammed B S, Hassan S B, Haruna S, Danlami N, Affiana Ishak E, Nurliyana Samahani W. (2021). Effects of petroleum sludge ash in fly ash-based geopolymer mortar. Construction & Building Materials, 272: 121939

[34] Wang A, Liu H, Hao X, Wang Y, Liu X, Li Z. (2019). Geopolymer synthesis using garnet tailings from molybdenum mines. Minerals, 9(1): 48

[35] Wang Y, Han F, Mu J. (2018). Solidification/stabilization mechanism of Pb(II), Cd(II), Mn(II) and Cr(III) in fly ash based geopolymers. Construction & Building Materials, 160: 818–827

[36] Xia M, Muhammad F, Zeng L, Li S, Huang X, Jiao B, Shiau Y C, Li D. (2019). Solidification/stabilization of lead-zinc smelting slag in composite based geopolymer. Journal of Cleaner Production, 209: 1206–1215

[37] XiaYQiuD LyvZZhangJ SinghNShih KTangY (2022). Controlled sintering for cadmium stabilization by beneficially using the dredged river sediment. Frontiers of Environmental Science & Engineering 17(5): 61

[38] Ye N, Chen Y, Yang J K, Liang S, Hu Y, Xiao B, Huang Q, Shi Y, Hu J, Wu X. (2016). Co-disposal of MSWI fly ash and Bayer red mud using an one-part geopolymeric system. Journal of Hazardous Materials, 318: 70–78

[39] Yunsheng Z, Wei S, Qianli C, Lin C. (2007). Synthesis and heavy metal immobilization behaviors of slag based geopolymer. Journal of Hazardous Materials, 143(1–2): 206–213

[40] Zhan X, Kirkelund G M. (2021). Electrodialytic remediation of municipal solid waste incineration fly ash as pre-treatment before geopolymerisation with coal fly ash. Journal of Hazardous Materials, 412: 125220

[41] Zhang P, Wang K X, Li Q F, Wang J, Ling Y. (2020a). Fabrication and engineering properties of concretes based on geopolymers/alkali-activated binders: a review. Journal of Cleaner Production, 258: 120896

[42] Zhang Q, Cao X, Sun S, Yang W, Fang L, Ma R, Lin C, Li H. (2022). Lead zinc slag-based geopolymer: demonstration of heavy metal solidification mechanism from the new perspectives of electronegativity and ion potential. Environmental Pollution, 293: 118509

[43] Zhang Y, Gao W, Ni W, Zhang S, Li Y, Wang K, Huang X, Fu P, Hu W. (2020b). Influence of calcium hydroxide addition on arsenic leaching and solidification/stabilisation behaviour of metallurgical-slag-based green mining fill. Journal of Hazardous Materials, 390: 122161

[44] Zhang Y, Liu X, Xu Y, Tang B, Wang Y. (2020c). Preparation of road base material by utilizing electrolytic manganese residue based on Si–Al structure: mechanical properties and Mn²⁺ stabilization/solidification characterization. Journal of Hazardous Materials, 390: 122188

[45] Zheng L, Wang W, Gao X B. (2016). Solidification and immobilization of MSWI fly ash through aluminate geopolymerization: based on partial charge model analysis. Waste Management, 58: 270–279

[46] Zhou H, Liu G, Zhang L, Zhou C, Mian M M, Cheema A I. (2021). Strategies for arsenic pollution control from copper pyrometallurgy based on the study of arsenic sources, emission pathways and speciation characterization in copper flash smelting systems. Environmental Pollution, 270: 116203

Acknowledgements

This work was financially supported by the National Key R&D Program of China (No. 2019YFC1904202), the State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming (No. CNMRCUKF20) and the Center for Analysis and Testing of Kunming University of Science and Technology (No. 2020P20171130007).

Conflict of Interests

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-024-1816-3 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2024 Higher Education Press 2024