Effects of sulfur on variations in the chemical speciation of heavy metals from fly ash glass

Highlights

● A higher sulfur content reduced the curing rate of Cr in glass.

● Depolymerization increased the amounts of heavy metals in the carbonate bound state.

● Reducing the CaO/SiO₂ ratio increased the proportion of stable heavy metals.

Abstract

This work designed a new CaO-Al₂O₃-SiO₂-SO₃ glass for the immobilization of multiple heavy metals found in dechlorinated fly ash having high amounts of calcium and sulfur. Increasing the (CaO + SO₃)/SiO₂ mass ratio (M(CS/S)) from 0.28 to 0.85 was found to lower the proportions of Mn, Ni and Zn in an unstable state, while an M(CS/S) ratio of 0.51 gave the lowest proportions of unstable Cr and Pb. Decreasing the degree of polymerization of the glassy network increased the proportions of Mn, Cr, Ni, Pb and Zn in the carbonate bound state. The leaching out of metals in this state was the primary cause of degradation of Q³ structural units in the glassy network. The amount of Mn in the iron-manganese oxide bound state was increased by increasing the number of Q² units in the silicate network. Decreasing the CaO/SiO₂ mass ratio (M(C/S)) raised the proportions of Mn, Ni and Zn in the unstable state. An M(C/S) value of 0.43 lowered the proportions of unstable Cr and Pb. A principal components analysis determined that the leaching of toxic heavy metals from the glass was primarily related to the proportions of these metals in the unstable state while there were no evident correlations between leaching and the proportions in stable states.

Graphical abstract

Keywords

Dechlorinated fly ash / SO₃ / Heavy metal / Chemical speciation / Glass solidification

References

[1] Chen C G , Sun C J , Gau S H , Wu C W , Chen Y L . (2013). The effects of the mechanical–chemical stabilization process for municipal solid waste incinerator fly ash on the chemical reactions in cement paste. Waste Management (New York, N.Y.), 33(4): 858–865

[2] Crum J, Maio V, Mccloy J, Scott C, Riley B, Benefiel B, Vienna J, Archibald K, Rodriguez C, Rutledge V, Zhu Z, Ryan J, Olszta M (2014). Cold crucible induction melter studies for making glass ceramic waste forms: a feasibility assessment. Journal of Nuclear Materials, 444(1–3): 481–492

[3] Crum J V , Turo L , Riley B , Tang M , Kossoy A . (2012). Multi-phase glass-ceramics as a waste form for combined fission products: alkalis, alkaline earths, lanthanides, and transition metals. Journal of the American Ceramic Society, 95(4): 1297–1303

[4] Cyr M , Idir R , Escadeillas G . (2012). Use of metakaolin to stabilize sewage sludge ash and municipal solid waste incineration fly ash in cement-based materials. Journal of Hazardous Materials, 243: 193–203

[5] Ferraro A , Farina I , Race M , Colangelo F , Cioffi R , Fabbricino M . (2019). Pre-treatments of MSWI fly-ashes: a comprehensive review to determine optimal conditions for their reuse and/or environmentally sustainable disposal. Reviews in Environmental Science and Biotechnology, 18(3): 453–471

[6] Fuentes A , Lloréns M , Sáez J , Aguilar M I , Ortuño J F , Meseguer V F . (2008). Comparative study of six different sludges by sequential speciation of heavy metals. Bioresource Technology, 99(3): 517–525

[7] Griffiths P R . (1983). Fourier transform infrared spectrometry. Science, 222(4621): 297–302

[8] Hou H B , He X H , Zhu S J , Zhang D J . (2006). The cement solidification of municipal solid waste incineration fly ash. Journal of Wuhan University of Technology (Materials Science), 21(4): 137–140

[9] Huang T , Zhang S , Liu L . (2019). Immobilization of trace heavy metals in the electrokinetics-processed municipal solid waste incineration fly ashes and its characterizations and mechanisms. Journal of Environmental Management, 232: 207–218

[10] Krausova K , Gautron L , Karnis A , Catillon G , Borensztajn S . (2016). Glass ceramics and mineral materials for the immobilization of lead and cadmium. Ceramics International, 42(7): 8779–8788

[11] Li M , Xiang J , Hu S , Sun L S , Su S , Li P S , Sun X X . (2004). Characterization of solid residues from municipal solid waste incinerator. Fuel, 83(10): 1397–1405

[12] Ma W , Fang Y , Chen D , Chen G , Xu Y , Sheng H , Zhou Z . (2017). Volatilization and leaching behavior of heavy metals in MSW incineration fly ash in a DC arc plasma furnace. Fuel, 210: 145–153

[13] Ma W , Shi W , Shi Y , Chen D , Liu B , Chu C , Li D , Li Y , Chen G . (2021). Plasma vitrification and heavy metals solidification of MSW and sewage sludge incineration fly ash. Journal of Hazardous Materials, 408: 124809

[14] Pan Y , Wu Z , Zhou J , Zhao J , Ruan X , Liu J , Qian G . (2013). Chemical characteristics and risk assessment of typical municipal solid waste incineration (MSWI) fly ash in China. Journal of Hazardous Materials, 261: 269–276

[15] Sun T , Chen J , Lei X , Zhou C . (2014). Detoxification and immobilization of chromite ore processing residue with metakaolin-based geopolymer. Journal of Environmental Chemical Engineering, 2(1): 304–309

[16] Tessier A , Campbell P G , Bisson M . (1979). Sequential extraction procedure for the speciation of particulate trace metals. Analytical Chemistry, 51(7): 844–851

[17] Tian X , Rao F , Li C , Ge W , Lara N O , Song S , Xia L . (2021). Solidification of municipal solid waste incineration fly ash and immobilization of heavy metals using waste glass in alkaline activation system. Chemosphere, 283: 131240

[18] 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

[19] Wey M Y , Ou W Y , Liu Z S , Tseng H H , Yang W Y , Chiang B C . (2001). Pollutants in incineration flue gas. Journal of Hazardous Materials, 82(3): 247–262

[20] Yue Y , Zhang J , Sun F , Wu S , Pan Y , Zhou J , Qian G . (2019). Heavy metal leaching and distribution in glass products from the co-melting treatment of electroplating sludge and MSWI fly ash. Journal of Environmental Management, 232: 226–235

[21] Zhang J, Liu J, Li C, Jin Y, Nie Y, Li J (2009). Comparison of the fixation effects of heavy metals by cement rotary kiln co-processing and cement based solidification/stabilization. Journal of Hazardous Materials, 165(1–3): 1179–1185

[22] Zhang J , Zhang S , Liu B . (2020a). Degradation technologies and mechanisms of dioxins in municipal solid waste incineration fly ash: A review. Journal of Cleaner Production, 250: 119507

[23] Zhang Y , Liu S , Ouyang S , Zhang X , Zhao Z , Jia X , Du Y , Deng L , Li B . (2020b). Transformation of unstable heavy metals in solid waste into stable state by the preparation of glass-ceramics. Materials Chemistry and Physics, 252: 123061

[24] Zhao M , Cao J , Geng X , Song W , Wang Z . (2020a). Structural origin of CaO-MgO-Al₂O₃-SiO₂-Fe₂O₃ glass crystallization: iron-containing clusters. Journal of Non-Crystalline Solids, 547: 120295

[25] Zhao M , Cao J , Wang Z , Li G . (2019). Insight into the dual effect of Fe₂O₃ addition on the crystallization of CaO-MgO-Al₂O₃-SiO₂ glass-ceramics. Journal of Non-Crystalline Solids, 513: 144–151

[26] Zhao S , Liu B , Ding Y , Zhang J , Wen Q , Ekberg C , Zhang S . (2020b). Study on glass-ceramics made from MSWI fly ash, pickling sludge and waste glass by one-step process. Journal of Cleaner Production, 271: 122674

[27] Zhao S , Wen Q , Zhang X , Liu B , Zhang S . (2021). Migration, transformation and solidification/stabilization mechanisms of heavy metals in glass-ceramics made from MSWI fly ash and pickling sludge. Ceramics International, 47(15): 21599–21609

[28] Zhou J , Wu S , Pan Y , Zhang L , Cao Z , Zhang X , Yonemochi S , Hosono S , Wang Y , Oh K , Qian G . (2015). Enrichment of heavy metals in fine particles of municipal solid waste incinerator (MSWI) fly ash and associated health risk. Waste Management (New York, N.Y.), 43: 239–246

[29] Zou C , Cao J , Zhao M , Wang Z , Lu J . (2019). Combined sodium and fluorine promote diopside continuous growth to achieve one-step crystallization in CaO-Al₂O₃-SiO₂-Fe₂O₃ glass-ceramics. Journal of the European Ceramic Society, 39(15): 4979–4987

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 52070181 and 51934006).

RIGHTS & PERMISSIONS

2023 Higher Education Press