The coupling of sand with ZVI/oxidants achieved proportional and highly efficient removal of arsenic

Highlights

• Simply doping sands with ZVI achieved an even activation of ZVI by oxidants.

• Sand doping facilitated proportional As trapping along the ZVI/oxidants column.

• ZVI/sand/oxidants are highly efficient for arsenic removal.

• ZVI/sand/oxidants reduced significantly the Fe²⁺ leaching and effluent turbidity.

• More than 54% of arsenic was reduced to As(III) in ZVI/sand/oxidants system.

Abstract

The coupling of zero-valent iron (ZVI) with common oxidants has recently achieved very rapid and highly efficient removal of Heavy metals from wastewater. However, the uniform activation of ZVI throughout the column and the proportional removal of target contaminants are urgently required for the prevention of premature filter clogging and the extension of the effective column operational time. In this study, we successfully achieved this objective by simply doping granular sand with ZVI at appropriate weight ratios. When pure ZVI packed column was spiked with oxidants, the majority of As trapping occurred between the column inlet and the first sampling point. In a packed column with a 1:20 mixture of ZVI and sand, the average As removal efficiency was 36 (1st), 13.1 (2nd), 18.5 (3rd), 19.2 (4th) and 5.9% (5th outlet). The overall arsenic removal performance of the composite filling system of ZVI/sand was equally as efficient as that of the previous pure ZVI-packed system. Moreover, the leaching of Fe was significantly reduced with an increased sand ratio, resulting in clearer water with less turbidity. The results of X-ray photoelectron spectroscopy (XPS) demonstrated that more than 54% of the arsenic was reduced to As(III). X-ray diffraction (XRD) and scanning electron microscopy (SEM) confirmed the extensive corrosion of the ZVI surface, which resulted in various species of iron oxyhydroxides responsible for the highly efficient sequester of arsenic through reduction, adsorption, and coprecipitation.

Graphical abstract

Keywords

Arsenic / ZVI / Sand / Oxidants / Fixed-bed Column / Removal

References

[1] Chen G (2004). Electrochemical technologies in wastewater treatment. Separation and Purification Technology, 38(1): 11–41

[2] Da̧browski A, Hubicki Z, Podkościelny P, Robens E(2004). Selective removal of the heavy metal ions from waters and industrialwastewaters by ion-exchange method.  Chemosphere,  56(2): 91–106

[3] De Klerk R J, Jia Y, Daenzer R, Gomez M A, Demopoulos G P (2012). Continuous circuit coprecipitation of arsenic(V) with ferric iron by lime neutralization: Process parameter effects on arsenic removal and precipitate quality. Hydrometallurgy, 111– 112: 65–72

[4] Ding C, Cheng W, Sun Y, Wang X (2015). Effects of Bacillus subtilis on the reduction of U(VI) by nano-Fe⁰. Geochimica et Cosmochimica Acta, 165: 86–107

[5] Guan X, Sun Y, Qin H, Li J, Lo I M, He D, Dong H (2015). The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures: The development in zero-valent iron technology in the last two decades (1994–2014). Water Research, 75: 224–248

[6] Guo X, Yang Z (2014). A method to rapidly remove the heavy metals from water. CN104276646A, PA

[7] Guo X, Yang Z, Dong H, Guan X, Ren Q, Lv X, Jin X (2016). Simple combination of oxidants with zero-valent-iron (ZVI) achieved very rapid and highly efficient removal of heavy metals from water. Water Research, 88: 671–680

[8] Guo X, Yang Z, Jin X (2014). A method to remove nitrate from water by ZVI/oxidants/zeolite. CN104341055A

[9] Guo X, Yang Z, Liu H, Lv X, Tu Q, Ren Q, Xia X, Jing C (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

[10] Kaliwon B F I (2015). A study on artificial hexavalent chromium removal by using zero valent iron reactor and sand filter in electrochemical reduction process. In: InCIEC 2014 (pp. 1003–1009). Singapore: Springer,

[11] Kanel S R, Manning B, Charlet L, Choi H (2005). Removal of arsenic (III) from groundwater by nanoscale zero-valent iron. Environmental Science & Technology, 39(5): 1291–1298

[12] Kim Y H, Ko S O, Yoo H C (2002). Simultaneous removal of tetrachlorocarbon and chromium (VI) using zero valent iron. Journal-Korean Society of Environmental Engineers, 24(11): 1949–1956

[13] Lackovic J A, Nikolaidis N P, Dobbs G M (2000). Inorganic arsenic removal by zero-valent iron. Environmental Engineering Science, 17(1): 29–39

[14] Li Y, Guo X, Dong H, Luo X, Guan X, Zhang X, Xia X (2018). Selenite removal from groundwater by zero-valent iron (ZVI) in combination with oxidants. Chemical Engineering Journal, 345: 432–440

[15] Liang L, Guan X, Shi Z, Li J, Wu Y, Tratnyek P G (2014). Coupled effects of aging and weak magnetic fields on sequestration of selenite by zero-valent iron. Environmental Science & Technology, 48(11): 6326–6334

[16] Luo H, Jin S, Fallgren P H, Colberg P J, Johnson P A (2010). Prevention of iron passivation and enhancement of nitrate reduction by electron supplementation. Chemical Engineering Journal, 160(1): 185–189

[17] Matlock M M, Howerton B S, Atwood D A (2002). Chemical precipitation of heavy metals from acid mine drainage. Water Research, 36(19): 4757–4764

[18] Mondal P, Bhowmick S, Jullok N, Ye W, Van Renterghem W, Van den Berghe S, Van der Bruggen B (2014). Behavior of As(V) with ZVI–H₂O system and the reduction to As(0). Journal of Physical Chemistry C, 118(37): 21614–21621

[19] Nikolaidis N P, Dobbs G M, Lackovic J A (2003). Arsenic removal by zero-valent iron: Field, laboratory and modeling studies. Water Research, 37(6): 1417–1425

[20] Noubactep C (2010). Metallic iron for safe drinking water worldwide. Chemical Engineering Journal, 165(2): 740–749

[21] Noubactep C (2015). Metallic iron for environmental remediation: A review of reviews. Water Research, 85: 114–123

[22] Noubactep C, Caré S (2011). Designing laboratory metallic iron columns for better result comparability. Journal of Hazardous Materials, 189(3): 809–813

[23] O’Carroll D, Sleep B, Krol M, Boparai H, Kocur C (2013). Nanoscale zero-valent iron and bimetallic particles for contaminated site remediation. Advances in Water Resources, 51: 104–122

[24] Peng X, Xi B, Zhao Y, Shi Q, Meng X, Mao X, Jiang Y, Ma Z, Tan W, Liu H, Gong B (2017). Effect of arsenic on the formation and adsorption property of ferric hydroxide precipitates in ZVI treatment. Environmental Science & Technology, 51(17): 10100–10108

[25] Sellers R M (1980). Spectrophotometric determination of hydrogen peroxide using potassium titanium(IV) oxalate. Analyst (London), 105(1255): 950–954

[26] Sleiman N, Deluchat V, Wazne M, Mallet M, Courtin-Nomade A, Kazpard V, Baudu M (2016). Phosphate removal from aqueous solution using ZVI/sand bed reactor: Behavior and mechanism. Water Research, 99: 56–65

[27] Sun F, Osseo-Asare K A, Chen Y, Dempsey B A (2011). Reduction of As(V) to As(III) by commercial ZVI or As(0) with acid-treated ZVI. Journal of Hazardous Materials, 196: 311–317

[28] Sun Y, Li J, Huang T, Guan X (2016). The influences of iron characteristics, operating conditions and solution chemistry on contaminants removal by zero-valent iron: A review. Water Research, 100: 277–295

[29] Westerhoff P, James J (2003). Nitrate removal in zero-valent iron packed columns. Water Research, 37(8): 1818–1830

[30] Xie M, Shon H K, Gray S R, Elimelech M (2016). Membrane-based processes for wastewater nutrient recovery: Technology, challenges, and future direction. Water Research, 89: 210–221

[31] Yang Z, Shan C, Zhang W, Jiang Z, Guan X, Pan B (2016). Temporospatial evolution and removal mechanisms of As(V) and Se(VI) in ZVI column with H₂O₂ as corrosion accelerator. Water Research, 106: 461–469

[32] Zhu B W, Lim T T (2007). Catalytic reduction of chlorobenzenes with Pd/Fe nanoparticles: Reactive sites, catalyst stability, particle aging, and regeneration. Environmental Science & Technology, 41(21): 7523–7529

[33] Zhu F, Ma S, Liu T, Deng X (2018). Green synthesis of nano zero-valent iron/Cu by green tea to remove hexavalent chromium from groundwater. Journal of Cleaner Production, 174: 184–190

[34] Zhu H, Jia Y, Wu X, Wang H (2009). Removal of arsenic from water by supported nano zero-valent iron on activated carbon. Journal of Hazardous Materials, 172(2–3): 1591–1596

Acknowledgements

Authors greatly acknowledge the support from the National Natural Science Foundation of China (Grant No. 21876011), National Key Research and Development Program of China (Grant No. 2017YFA0605001), and Fund for Innovative Research Group of the National Natural Science Foundation of China (Grant No. 51721093).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-020-1273-6 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2020 Higher Education Press