Sulfide-modified zerovalent iron for enhanced antimonite sequestration: Characterization, performance, and reaction mechanisms

Shasha Huang, Chunhua Xu, Qianqian Shao, Yahao Wang, Bingliang Zhang, Baoyu Gao, Weizhi Zhou, Paul Tratnyek

Research output: Contribution to journalArticle

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Abstract

Zerovalent iron (ZVI) is commonly used for water treatment under aerobic conditions such as sequestration of metals. Sulfide-modified ZVI (S-ZVI) is attracting increasing attention for its easy preparation and high reactivity with environmental pollutants. The processes responsible for contaminant removal can be a complex mixture of redox, sorption, and coprecipitation processes. In this paper, ZVI and S-ZVI were used to sequester antimonite (Sb(III)). The rates of Sb(III) sequestration were determined in open, well-mixed, batch reactors. The effects of various experimental variables were investigated, including pH, iron dose, initial concentrations of Sb(III), aging time of the ZVI and S-ZVI, addition of Fe2+, mixing rate, etc. The results showed that S-ZVI can significantly enhance the Sb(III) sequestration, and under basic conditions in this study, the kobs (0.018 min−1) obtained in the S-ZVI system was approximately 15 times higher than the 0.0012 min−1 obtained in the ZVI system. Solid phase characterizations were conducted to assess the influence of sulfidation on the morphology and surface geochemistry of ZVI. Scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectroscopy (EDS) confirmed the presence of sulfur. X-ray photoelectron spectroscopy (XPS) indicated the oxidation of Sb(III) to Sb(V) and adsorption and coprecipitation onto the iron oxides is the mainly sequestration process. The FeS layer on ZVI is more conductive than oxides and therefore accelerates electron transfer. In addition sulfidation promotes the corrosion of iron and the formation of ferrous iron, which further enhances the ferric iron oxide formation, thereby favoring adsorption and oxidation of Sb(III).

Original languageEnglish (US)
Pages (from-to)539-547
Number of pages9
JournalChemical Engineering Journal
Volume338
DOIs
StatePublished - Apr 15 2018

Fingerprint

stibnite
Sulfides
Iron
sulfide
iron
Coprecipitation
Iron oxides
iron oxide
X-ray spectroscopy
antimonite
adsorption
Adsorption
oxidation
Environmental Pollutants
Oxidation
Geochemistry
pollutant
Batch reactors
oxic conditions
Complex Mixtures

Keywords

  • Antimony
  • Oxidation
  • Sequestration
  • Sulfidation
  • Zerovalent iron

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

Cite this

Sulfide-modified zerovalent iron for enhanced antimonite sequestration : Characterization, performance, and reaction mechanisms. / Huang, Shasha; Xu, Chunhua; Shao, Qianqian; Wang, Yahao; Zhang, Bingliang; Gao, Baoyu; Zhou, Weizhi; Tratnyek, Paul.

In: Chemical Engineering Journal, Vol. 338, 15.04.2018, p. 539-547.

Research output: Contribution to journalArticle

Huang, Shasha ; Xu, Chunhua ; Shao, Qianqian ; Wang, Yahao ; Zhang, Bingliang ; Gao, Baoyu ; Zhou, Weizhi ; Tratnyek, Paul. / Sulfide-modified zerovalent iron for enhanced antimonite sequestration : Characterization, performance, and reaction mechanisms. In: Chemical Engineering Journal. 2018 ; Vol. 338. pp. 539-547.
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abstract = "Zerovalent iron (ZVI) is commonly used for water treatment under aerobic conditions such as sequestration of metals. Sulfide-modified ZVI (S-ZVI) is attracting increasing attention for its easy preparation and high reactivity with environmental pollutants. The processes responsible for contaminant removal can be a complex mixture of redox, sorption, and coprecipitation processes. In this paper, ZVI and S-ZVI were used to sequester antimonite (Sb(III)). The rates of Sb(III) sequestration were determined in open, well-mixed, batch reactors. The effects of various experimental variables were investigated, including pH, iron dose, initial concentrations of Sb(III), aging time of the ZVI and S-ZVI, addition of Fe2+, mixing rate, etc. The results showed that S-ZVI can significantly enhance the Sb(III) sequestration, and under basic conditions in this study, the kobs (0.018 min−1) obtained in the S-ZVI system was approximately 15 times higher than the 0.0012 min−1 obtained in the ZVI system. Solid phase characterizations were conducted to assess the influence of sulfidation on the morphology and surface geochemistry of ZVI. Scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectroscopy (EDS) confirmed the presence of sulfur. X-ray photoelectron spectroscopy (XPS) indicated the oxidation of Sb(III) to Sb(V) and adsorption and coprecipitation onto the iron oxides is the mainly sequestration process. The FeS layer on ZVI is more conductive than oxides and therefore accelerates electron transfer. In addition sulfidation promotes the corrosion of iron and the formation of ferrous iron, which further enhances the ferric iron oxide formation, thereby favoring adsorption and oxidation of Sb(III).",
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T1 - Sulfide-modified zerovalent iron for enhanced antimonite sequestration

T2 - Characterization, performance, and reaction mechanisms

AU - Huang, Shasha

AU - Xu, Chunhua

AU - Shao, Qianqian

AU - Wang, Yahao

AU - Zhang, Bingliang

AU - Gao, Baoyu

AU - Zhou, Weizhi

AU - Tratnyek, Paul

PY - 2018/4/15

Y1 - 2018/4/15

N2 - Zerovalent iron (ZVI) is commonly used for water treatment under aerobic conditions such as sequestration of metals. Sulfide-modified ZVI (S-ZVI) is attracting increasing attention for its easy preparation and high reactivity with environmental pollutants. The processes responsible for contaminant removal can be a complex mixture of redox, sorption, and coprecipitation processes. In this paper, ZVI and S-ZVI were used to sequester antimonite (Sb(III)). The rates of Sb(III) sequestration were determined in open, well-mixed, batch reactors. The effects of various experimental variables were investigated, including pH, iron dose, initial concentrations of Sb(III), aging time of the ZVI and S-ZVI, addition of Fe2+, mixing rate, etc. The results showed that S-ZVI can significantly enhance the Sb(III) sequestration, and under basic conditions in this study, the kobs (0.018 min−1) obtained in the S-ZVI system was approximately 15 times higher than the 0.0012 min−1 obtained in the ZVI system. Solid phase characterizations were conducted to assess the influence of sulfidation on the morphology and surface geochemistry of ZVI. Scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectroscopy (EDS) confirmed the presence of sulfur. X-ray photoelectron spectroscopy (XPS) indicated the oxidation of Sb(III) to Sb(V) and adsorption and coprecipitation onto the iron oxides is the mainly sequestration process. The FeS layer on ZVI is more conductive than oxides and therefore accelerates electron transfer. In addition sulfidation promotes the corrosion of iron and the formation of ferrous iron, which further enhances the ferric iron oxide formation, thereby favoring adsorption and oxidation of Sb(III).

AB - Zerovalent iron (ZVI) is commonly used for water treatment under aerobic conditions such as sequestration of metals. Sulfide-modified ZVI (S-ZVI) is attracting increasing attention for its easy preparation and high reactivity with environmental pollutants. The processes responsible for contaminant removal can be a complex mixture of redox, sorption, and coprecipitation processes. In this paper, ZVI and S-ZVI were used to sequester antimonite (Sb(III)). The rates of Sb(III) sequestration were determined in open, well-mixed, batch reactors. The effects of various experimental variables were investigated, including pH, iron dose, initial concentrations of Sb(III), aging time of the ZVI and S-ZVI, addition of Fe2+, mixing rate, etc. The results showed that S-ZVI can significantly enhance the Sb(III) sequestration, and under basic conditions in this study, the kobs (0.018 min−1) obtained in the S-ZVI system was approximately 15 times higher than the 0.0012 min−1 obtained in the ZVI system. Solid phase characterizations were conducted to assess the influence of sulfidation on the morphology and surface geochemistry of ZVI. Scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectroscopy (EDS) confirmed the presence of sulfur. X-ray photoelectron spectroscopy (XPS) indicated the oxidation of Sb(III) to Sb(V) and adsorption and coprecipitation onto the iron oxides is the mainly sequestration process. The FeS layer on ZVI is more conductive than oxides and therefore accelerates electron transfer. In addition sulfidation promotes the corrosion of iron and the formation of ferrous iron, which further enhances the ferric iron oxide formation, thereby favoring adsorption and oxidation of Sb(III).

KW - Antimony

KW - Oxidation

KW - Sequestration

KW - Sulfidation

KW - Zerovalent iron

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