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Front. Environ. Sci. Eng.    2024, Vol. 18 Issue (5) : 56    https://doi.org/10.1007/s11783-024-1816-3
Stabilization/solidification mechanisms of tin tailings and fuming slag-based geopolymers for different heavy metals
Xian Zhou1,2, Zhengfu Zhang1(), Hui Yang1
1. School of Materials Science and Engineering, Kunming University of Science and Technology, Kunming 650093, China
2. Kunming Metallurgical Research Institute Co., Ltd., Kunming 650031, China
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Abstract

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

● Cr2O72– is converted to CrO42– and combines with OH– to form Cr(OH)3 precipitates.

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

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. AsO33– was oxidized into AsO43–, which may form Ca–As or Fe–As precipitates. Cr2O72– was converted to CrO42– 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.
Keywords Heavy metals      Cementitious materials      Tin tailings      Stabilization/solidification      Redox     
Corresponding Author(s): Zhengfu Zhang   
Issue Date: 18 January 2024
 Cite this article:   
Xian Zhou,Zhengfu Zhang,Hui Yang. Stabilization/solidification mechanisms of tin tailings and fuming slag-based geopolymers for different heavy metals[J]. Front. Environ. Sci. Eng., 2024, 18(5): 56.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1816-3
https://academic.hep.com.cn/fese/EN/Y2024/V18/I5/56
Sample CaO SiO2 Al2O3 Fe2O3 SO3 TiO2 As Cr Cu Zn Mn LOI
TMTFSFGDG 18936 21301 2660.5 16370.2 2349 0.830.04 0.70.09– 0.020.04– 0.070.1– 0.040.4– 0.50.5– 11.216.514.2
Tab.1  Chemical compositions of TMT, FS and FGDG (wt.%)
Sample TMT FS FGDG AsO33– Cr2O72– Cu2+ Mn2+ Zn2+ Reagent w/b
T8F1 80 10 10 0 0 0 0 0 — 0.3
T6F3 60 30 10 0 0 0 0 0 — 0.3
T4F5 40 50 10 0 0 0 0 0 — 0.3
T2F7 20 70 10 0 0 0 0 0 — 0.3
T4F5-As 40 50 10 4 0 0 0 0 Na3AsO3 0.3
T4F5-Cr 40 50 10 0 4 0 0 0 K2Cr2O7 0.3
T4F5-Cu 40 50 10 0 0 4 0 0 CuSO4 0.3
T4F5-Zn 40 50 10 0 0 0 4 0 ZnSO4 0.3
T4F5-Mn 40 50 10 0 0 0 0 4 MnSO4 0.3
Tab.2  Design scheme for synthesis of geopolymer (wt.%)
Fig.1  Chemical fractions of heavy metals ((a) TMT; (b) FS).
Fig.2  Compressive strength of geopolymers.
Fig.3  XRD patterns of geopolymer without heavy metals: ((a) 3 d; (b) 28 d).
Species Movement Wavenumbers Corresponding phase
H–O–H Stretching vibration 3413.9−3549.3 Free water
H–O–H Bending vibration 1617.5−1639.3 Crystallized water
C–O Stretching vibration 1431−1431.9 CaCO3
Si–O–Si/Al Stretching vibration 996.1−1031.1 N–A–S–H
S–O Bending vibration 614.7−622.9 Gypsum
Si–O–Si Bending vibration 445.5−452.2 Silicates
Tab.3  Species, wavenumbers and corresponding phases
Fig.4  FTIR spectra of geopolymer without heavy metals: ((a) 3 d; (b) 28 d).
Sample Compressive strength at 3 d Compressive strength at 73 d Compressive strength at 28 d
MPa Change (%) MPa Change (%) MPa Change (%)
T4F5 5.29 ± 0.52 – 7.14 ± 0.36 34.97 7.83 ± 0.39 9.66
T4F5-As 2.84 ± 0.26 – 3.54 ± 0.34 24.65 3.68 ± 0.46 3.95
T4F5-Cr 4.21 ± 0.51 – 5.29 ± 0.43 25.65 5.66 ± 0.34 6.99
T4F5-Cu 4.52 ± 0.35 – 5.84 ± 0.26 29.20 6.07 ± 0.42 3.94
T4F5-Zn 3.98 ± 0.28 – 4.96 ± 0.31 27.51 5.26 ± 0.45 6.05
T4F5-Mn 3.18 ± 0.21 – 4.57 ± 0.32 43.71 5.39 ± 0.19 17.94
Tab.4  Compressive strength of geopolymers containing heavy metals
Fig.5  Leaching results and immobilization efficiency of heavy metals.
Fig.6  SEM-EDS mapping images of geopolymer samples containing heavy metals ((a) T4F5-As; (b) T4F5-Cr; (c) T4F5-Cu; (d) T4F5-Zn; (e) T4F5-Mn; (f) T4F5).
Samples T4F5 T4F5-As T4F5-Cr T4F5-Cu T4F5-Zn T4F5-Mn
Na+ (mg/L) 15.7 18.6 17.2 82.5 74.9 97.2
Tab.5  Leaching concentrations of Na+ in samples containing heavy metals
Fig.7  XRD patterns and FTIR spectra of geopolymers with different heavy metals ((a) 3 d XRD pattern; (b) 28 d XRD pattern; (c) 28 d FTIR spectra; (d) BCR extraction results).
Fig.8  XPS full spectra of T4F5 samples containing heavy metals.
Fig.9  Schematic of heavy metal immobilization mechanism.
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