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

doi:10.1007/s11783-023-1728-7

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (10) : 128 https://doi.org/10.1007/s11783-023-1728-7

RESEARCH ARTICLE

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

Yali Chang^1,², Jianwei Cao²(

), Wenfeng Song², Zhi Wang²(

), Chenyang Xu¹(

), Mengzhuo Long^1,²

¹. School of Mechanical Electronic and Information Engineering, China University of Mining and Technology, Beijing 100083, China
². CAS Key Laboratory of Green Process and Engineering, National Engineering Research Center of Green Recycling for Strategic Metal Resources, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China

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Abstract

● 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.

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.

Keywords Dechlorinated fly ash SO₃ Heavy metal Chemical speciation Glass solidification

Corresponding Author(s): Jianwei Cao,Zhi Wang,Chenyang Xu

Issue Date: 29 May 2023

Cite this article:

Yali Chang,Jianwei Cao,Wenfeng Song, et al. Effects of sulfur on variations in the chemical speciation of heavy metals from fly ash glass[J]. Front. Environ. Sci. Eng., 2023, 17(10): 128.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1728-7
https://academic.hep.com.cn/fese/EN/Y2023/V17/I10/128

Tab.1 Compositions of the dechlorinated fly ash and coal fly ash used in this work (wt.%)

Tab.2 Oxide compositions of the group A base glass specimens (wt.%)

Tab.3 Oxide compositions of the group B base glass specimens (wt.%)

Tab.4 Details of Tessier’s five-step continuous chemical extraction method

Fig.1 Macroscopic morphologies and XRD patterns of glass samples.

Fig.2 The concentrations of various metals obtained from leaching trials with glass specimens.

Tab.5 Composition of the yellow phase found on sample A3 as determined by XRF (wt.%)

Fig.3 The proportions of (a) Mn, (b) Cr, (c) Ni, (d) Pb and (e) Zn in various states within glass specimens. (f) The proportions of heavy metals in various states in glass specimens having an M(CS/S) of 0.85 with and without the yellow surface phase.

Fig.4 FTIR spectra obtained from glass specimens having M(CS/S) of 0.28, 0.51 and 0.85.

Fig.5 The results of peak fitting of FTIR spectra obtained from specimens having M(CS/S) values of (a) 0.28, (b) 0.51 and (c) 0.85. (d) The NBO/T values of the glass specimens.

Fig.6 Proportions of (a) Mn, (b) Cr, (c) Ni, (d) Pb and (e) Zn in various glass specimens with M(CS/S) of 0.28, 0.51 and 0.85. (f) Variations in the proportions of Qⁿ structural units.

Fig.7 Variations in the quantities of Qⁿ structural units in the specimens having M(CS/S) values of (a) 0.28, (b) 0.51 and (c) 0.85. (d) NBO/T values of the raw glass powder and the glass after leaching of metals in the carbonate bound state.

Fig.8 The proportions of (a) Mn, (b) Cr, (c) Ni, (d) Pb and (e) Zn in various states in glass specimens having M(C/S) values of 0.25, 0.43 and 0.66.

Fig.9 The results of peak fitting of FTIR spectra obtained from specimens having M(C/S) values of (a) 0.25, (b) 0.43 and (c) 0.66. (d) The NBO/T values of the glass specimens.

Fig.10 Proportions of (a) Mn, (b) Cr, (c) Ni, (d) Pb and (e) Zn in various glass specimens with M(C/S) of 0.25, 0.43 and 0.66. (f) Variations in the proportions of Qⁿ structural units.

Fig.11 The results of the PCA of TS values for (a) Mn, (b) Cr, (c) Ni and (d) Pb.

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