Remediation of arsenic contaminated soil by sulfidated zero-valent iron

doi:10.1007/s11783-020-1377-z

Front. Environ. Sci. Eng.

2021, Vol. 15

Issue (5) : 83 https://doi.org/10.1007/s11783-020-1377-z

RESEARCH ARTICLE

Remediation of arsenic contaminated soil by sulfidated zero-valent iron

Junlian Qiao^1,², Yang Liu^1,², Hongyi Yang^1,², Xiaohong Guan^1,², Yuankui Sun^1,²(

)

¹. State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
². Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

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Abstract

• Sulfidation significantly enhanced As(V) immobilization in soil by zerovalent iron.

• S-ZVI promoted the conversion of exchangeable As to less mobile Fe-Mn bound As.

• Column test further confirmed the feasibility of sulfidated ZVI on As retention.

• S-ZVI amendment and magnetic separation markedly reduced TCLP leachability of As.

In this study, the influences of sulfidation on zero-valent iron (ZVI) performance toward As(V) immobilization in soil were systemically investigated. It was found that, compared to unamended ZVI, sulfidated ZVI (S-ZVI) is more favorable to immobilize As(V) in soil and promote the conversion of water soluble As to less mobile Fe-Mn bound As. Specifically, under the optimal S/Fe molar ratio of 0.05, almost all of the leached As could be sequestrated by>0.5 wt.% S-ZVI within 3 h. Although the presence of HA could decrease the desorption of As from soil, HA inhibited the reactivity of S-ZVI to a greater extent. Column experiments further proved the feasibility of applying S-ZVI on soil As(V) immobilization. More importantly, to achieve a good As retention performance, S-ZVI should be fully mixed with soil or located on the downstream side of As migration. The test simulating the flooding conditions in rice culture revealed there was also a good long-term stability of soil As(V) after S-ZVI remediation, where only 0.7% of As was desorbed after 30 days of incubation. Magnetic separation was employed to separate the immobilized As(V) from soil after S-ZVI amendment, where the separation efficiency was found to be dependent of the iron dosage, liquid to soil ratio, and reaction time. Toxicity characteristic leaching procedure (TCLP) tests revealed that the leachability of As from soil was significantly reduced after the S-ZVI amendment and magnetic separation treatment. All these findings provided some insights into the remediation of As(V)-polluted soil by ZVI.

Keywords Soil As(V) Sulfidation Zero-valent iron Magnetic separation

Corresponding Author(s): Yuankui Sun

Issue Date: 17 December 2020

Cite this article:

Junlian Qiao,Yang Liu,Hongyi Yang, et al. Remediation of arsenic contaminated soil by sulfidated zero-valent iron[J]. Front. Environ. Sci. Eng., 2021, 15(5): 83.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1377-z
https://academic.hep.com.cn/fese/EN/Y2021/V15/I5/83

Fig.1 Effect of sulfidation on the performance of ZVI in remediating As-laden paddy soils in terms of the desorption (a, c) and speciation (b, d) of As. Reaction conditions: initial As in soil= 105.5 mg/kg, soil/solution= 2 g/10 mL, iron loading=1.0 wt.% for Figs. (a) and (b). S/Fe molar ratio=0.05 for Figs. (c) and (d), T = 25°C, incubation time= 15 d for Figs. (b) and (d).

Fig.2 Effect of S-ZVI addition on the desorption of As from As-laden paddy soils under different operating conditions (soil/solution= 2 g/10 mL, S/Fe molar ratio= 0.05, S-ZVI= 0 or 5 g/kg (0.5 wt.%), T = 25°C).

Fig.3 Cumulative As desorption in the effluents of different columns: (A) without S-ZVI, (B) filled S-ZVI homogeneously throughout the column, (C) filled S-ZVI in the bottom half of the column, (D) filled S-ZVI in the top half of the column. Reaction conditions: the flow rate of pure water= 0.75–0.90 mL/h; S-ZVI= 3 g; soil dosage= 60 g; T = 25°C.

Fig.4 The spatial distribution and speciation of As at the end of the column experiments.

Fig.5 Effect of the changeover of anoxic and oxic condition on the release of As from the S-ZVI treated soils in pure water. Reaction conditions: Soils were collected from Column B, As_tot = 578.9 mg/kg, Fe_tot = 180.0 g/kg, soil/solution= 1 g/10 mL.

Fig.6 Effect of operating conditions on the recovery of As from S-ZVI treated soils by magnetic separation (As_tot = 105.5 mg/kg).

Fig.7 TCLP leachability of As from soils treated by S-ZVI and magnetic separation (As_tot = 105.5 mg/kg).

1	S R Al-Abed, G Jegadeesan, J Purandare, D Allen (2007). Arsenic release from iron rich mineral processing waste: Influence of pH and redox potential. Chemosphere, 66(4): 775–782 https://doi.org/10.1016/j.chemosphere.2006.07.045
2	M W Anders, R J Bull, K P Cantor, D Chakraborti, C J Chen, A B Deangelo (2004). IARC monographs on the evaluation of carcinogenic risks to humans. Lyon: IARC Press
3	S Bae, W Lee (2014). Influence of riboflavin on nanoscale zero-valent iron reactivity during the degradation of carbon tetrachloride. Environmental Science & Technology, 48(4): 2368–2376 https://doi.org/10.1021/es4056565
4	S Bang, M D Johnson, G P Korfiatis, X G Meng (2005). Chemical reactions between arsenic and zero-valent iron in water. Water Research, 39(5): 763–770 https://doi.org/10.1016/j.watres.2004.12.022
5	S Bhattacharjee, S Ghoshal (2018). Optimal design of sulfidated nanoscale zerovalent iron for enhanced trichloroethene degradation. Environmental Science & Technology, 52(19): 11078–11086 https://doi.org/10.1021/acs.est.8b02399
6	M Biterna, A Arditsoglou, E Tsikouras, D Voutsa (2007). Arsenate removal by zero valent iron: Batch and column tests. Journal of Hazardous Materials, 149(3): 548–552 https://doi.org/10.1016/j.jhazmat.2007.06.084
7	J Buschmann, A Kappeler, U Lindauer, D Kistler, M Berg, L Sigg (2006). Arsenite and arsenate binding to dissolved humic acids: Influence of pH, type of humic acid, and aluminum. Environmental Science & Technology, 40(19): 6015–6020 https://doi.org/10.1021/es061057+
8	S Comba, A Di Molfetta, R Sethi (2011). A comparison between field applications of nano-, micro-, and millimetric zero-valent iron for the remediation of contaminated aquifers. Water, Air, and Soil Pollution, 215(1–4): 595–607 https://doi.org/10.1007/s11270-010-0502-1
9	H K Das, A K Mitra, P K Sengupta, A Hossain, F Islam, G H Rabbani (2004). Arsenic concentrations in rice, vegetables, a fish in Bangladesh: A preliminary study. Environment International, 30(3): 383–387 https://doi.org/10.1016/j.envint.2003.09.005
10	J Dong, Y S Zhao, R Zhao, R Zhou (2010). Effects of pH and particle size on kinetics of nitrobenzene reduction by zero-valent iron. Journal of Environmental Sciences (China), 22(11): 1741–1747 https://doi.org/10.1016/S1001-0742(09)60314-4
11	X M Dou, R Li, B Zhao, W Y Liang (2010). Arsenate removal from water by zero-valent iron/activated carbon galvanic couples. Journal of Hazardous Materials, 182(1–3): 108–114 https://doi.org/10.1016/j.jhazmat.2010.06.004
12	D Fan, R P Anitori, B M Tebo, P G Tratnyek, J S Lezama Pacheco, R K Kukkadapu, M H Engelhard, M E Bowden, L Kovarik, B W Arey (2013). Reductive sequestration of pertechnetate (99TcO4‒) by nano zerovalent iron (nZVI) transformed by abiotic sulfide. Environmental Science & Technology, 47(10): 5302–5310 https://doi.org/10.1021/es304829z
13	D Fan, Y Lan, P G Tratnyek, R L Johnson, J Filip, D M O’Carroll, Nunez A Garcia, A Agrawal (2017). Sulfidation of iron-based materials: A review of processes and implications for water treatment and remediation. Environmental Science & Technology, 51(22): 13070–13085 https://doi.org/10.1021/acs.est.7b04177
14	X H Guan, H Y Yang, Y K Sun, J L Qiao (2019). Enhanced immobilization of chromium(VI) in soil using sulfidated zero-valent iron. Chemosphere, 228: 370–376 https://doi.org/10.1016/j.chemosphere.2019.04.132
15	X J Guo, Z Yang, H Liu, X F Lv, Q S Tu, Q D Ren, X H Xia, C Y Jing (2015). Common oxidants activate the reactivity of zero-valent iron (ZVI) and hence remarkably enhance nitrate reduction from water. Separation and Purification Technology, 146: 227–234 https://doi.org/10.1016/j.seppur.2015.03.059
16	Y L Han, W L Yan (2016). Reductive dechlorination of trichloroethene by zero-valent iron nanoparticles: Reactivity enhancement through sulfidation treatment. Environmental Science & Technology, 50(23): 12992–13001 https://doi.org/10.1021/acs.est.6b03997
17	C S He, D He, R N Collins, S Garg, Y Mu, T D Waite (2018). Effects of good’s buffers and pH on the structural transformation of zero valent iron and the oxidative degradation of contaminants. Environmental Science & Technology, 52(3): 1393–1403 https://doi.org/10.1021/acs.est.7b04030
18	F He, D Zhao, C Paul (2010). Field assessment of carboxymethyl cellulose stabilized iron nanoparticles for in situ destruction of chlorinated solvents in source zones. Water Research, 44(7): 2360–2370 https://doi.org/10.1016/j.watres.2009.12.041
19	S S Huang, C H Xu, Q Q Shao, Y H Wang, B L Zhang, B Y Gao, W Z Zhou, P G Tratnyek (2018). Sulfide-modified zerovalent iron for enhanced antimonite sequestration: Characterization, performance, and reaction mechanisms. Chemical Engineering Journal, 338: 539–547 https://doi.org/10.1016/j.cej.2018.01.033
20	C A Jones, W P Inskeep, D R Neuman (1997). Arsenic transport in contaminated mine tailings following liming. Journal of Environmental Quality, 26(2): 433–439 https://doi.org/10.2134/jeq1997.00472425002600020014x
21	H B Jung, M A Charette, Y Zheng (2009). Field, laboratory, and modeling study of reactive transport of groundwater arsenic in a coastal aquifer. Environmental Science & Technology, 43(14): 5333–5338 https://doi.org/10.1021/es900080q
22	I Kögel-Knabner, W Amelung, Z H Cao, S Fiedler, P Frenzel, R Jahn, K Kalbitz, A Kolbl, M Schloter (2010). Biogeochemistry of paddy soils. Geoderma, 157(1–2): 1–14 https://doi.org/10.1016/j.geoderma.2010.03.009
23	M M Krol, A J Oleniuk, C M Kocur, B E Sleep, P Bennett, Z Xiong, D M O’Carroll (2013). A field-validated model for in situ transport of polymer-stabilized nZVI and implications for subsurface injection. Environmental Science & Technology, 47(13): 7332–7340 https://doi.org/10.1021/es3041412
24	R E Macur, J T Wheeler, T R Mcdermott, W P Inskeep (2001). Microbial populations associated with the reduction and enhanced mobilization of arsenic in mine tailings. Environmental Science & Technology, 35(18): 3676–3682 https://doi.org/10.1021/es0105461
25	M S H Mak, P H Rao, I M C Lo (2009). Effects of hardness and alkalinity on the removal of arsenic(V) from humic acid-deficient and humic acid-rich groundwater by zero-valent iron. Water Research, 43(17): 4296–4304 https://doi.org/10.1016/j.watres.2009.06.022
26	D O’Carroll, B Sleep, M Krol, H Boparai, C Kocur (2013). Nanoscale zero valent iron and bimetallic particles for contaminated site remediation. Advances in Water Resources, 51: 104–122 https://doi.org/10.1016/j.advwatres.2012.02.005
27	X Peng, B D Xi, Y Zhao, Q T Shi, X G Meng, X H Mao, Y H Jiang, Z F Ma, W B Tan, H L Liu, B Gong (2017). Effect of arsenic on the formation and adsorption property of ferric hydroxide precipitates in ZVI treatment. Environmental Science & Technology, 51(17): 10100–10108 https://doi.org/10.1021/acs.est.7b02635
28	T Phenrat, P Hongkumnerd, J Suk-In, V Khum-In (2019). Nanoscale zerovalent iron particles for magnet-assisted soil washing of cadmium-contaminated paddy soil: Proof of concept. Environmental Chemistry, 16(6): 446–458 https://doi.org/10.1071/EN19028
29	P Rao, M S Mak, T Liu, K C Lai, I M Lo (2009). Effects of humic acid on arsenic(V) removal by zero-valent iron from groundwater with special references to corrosion products analyses. Chemosphere, 75(2): 156–162 https://doi.org/10.1016/j.chemosphere.2008.12.019
30	A D Redman, D L Macalady, D Ahmann (2002). Natural organic matter affects arsenic speciation and sorption onto hematite. Environmental Science & Technology, 36(13): 2889–2896 https://doi.org/10.1021/es0112801
31	Y M Su, A S Adeleye, Y X Huang, X F Zhou, A A Keller, Y L Zhang (2016). Direct synthesis of novel and reactive sulfide-modified nano iron through nanoparticle seeding for improved cadmium-contaminated water treatment. Scientific Reports, 6, 24358 https://doi.org/10.1038/srep24358
32	Y K Sun, X H Guan, J M Wang, X G Meng, C H Xu, G M Zhou (2014). Effect of weak magnetic field on arsenate and arsenite removal from water by zerovalent iron: An XAFS investigation. Environmental Science & Technology, 48(12): 6850–6858 https://doi.org/10.1021/es5003956
33	C L Tang, Y H Huang, H Zeng, Z Q Zhang (2014). Reductive removal of selenate by zero-valent iron: The roles of aqueous Fe2+ and corrosion products, and selenate removal mechanisms. Water Research, 67: 166–174 https://doi.org/10.1016/j.watres.2014.09.016
34	A Tessier, P G C Campbell, M Bisson (1979). Sequential extraction procedure for the speciation of particulate trace-metals. Analytical Chemistry, 51(7): 844–851 https://doi.org/10.1021/ac50043a017
35	J Wang, P M Wang, Y Gu, P M Kopittke, F J Zhao, P Wang (2019). Iron-manganese (oxyhydro)oxides, rather than oxidation of sulfides, determine mobilization of Cd during soil drainage in paddy soil systems. Environmental Science & Technology, 53(5): 2500–2508 https://doi.org/10.1021/acs.est.8b06863
36	Y J Zavala, J M Duxbury (2008). Arsenic in rice: I. Estimating normal levels of total arsenic in rice grain. Environmental Science & Technology, 42(10): 3856–3860 https://doi.org/10.1021/es702747y
37	Z Zhou, Q Alhadidi, K Quiñones Deliz, H Yamaguchi Greenslet, J C Bonzongo (2020). Removal of oxyanion forming elements from contaminated soils through combined sorption onto zero-valent iron (ZVI) and magnetic separation: Arsenic and chromium as case studies. Soil & Sediment Contamination, 29(2): 180–191 https://doi.org/10.1080/15320383.2019.1696279

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