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Progress in Chemistry 2022, Vol. 34 Issue (4): 870-883 DOI: 10.7536/PC210435 Previous Articles   Next Articles

• Review •

Effect of Microbial Iron Redox on Aqueous Arsenic and Antimony Removal

Shuangyu Zhang, Yunxuan Hu, Cheng Li, Xinhua Xu()   

  1. Department of Environment Engineering,College of Environmental and Resource Sciences, Zhejiang University,Hangzhou 310058,China
  • Received: Revised: Online: Published:
  • Contact: Xinhua Xu
  • Supported by:
    National Natural Science Foundation of China(21976153)
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Arsenic and antimony pollution is widespread around the world. Compared with the conventional iron oxide, Fe(Ⅲ) minerals formed by microbial oxidation have a stronger adsorption capacity for aqueous As/Sb. There are wide application prospects of these minerals because of the advantages of high removal efficiency, practicability and environmental friendliness. However, the microbial reduction of the Fe(Ⅲ) minerals may lead to the release of adsorbed As/Sb. This paper reviewed the process of effect of microbial participated iron redox process on As/Sb removal. The microbial cycle of “synthesis, dissolution and transformation” of iron minerals and the mechanism of immobilization, dissolution and transformation of aqueous As/Sb associated with this cycle are concluded. The mineralogy of Fe(Ⅲ) minerals synthesized by microorganisms is illustrated. The thermal dynamics and coordination mechanism of the binding of Fe(Ⅲ) minerals with As/Sb are explained. The factors affecting As/Sb removal by microbial synthesized Fe(Ⅲ) minerals are summarized. Based on the existing problems in this field, the outlook of As/Sb removal by microbial iron redox has prospected.

Contents

1 Introduction

2 Immobilization of As/Sb with synthesis of Fe(Ⅲ) minerals by microorganisms

2.1 Synthesis of Fe(Ⅲ) minerals

2.2 As/Sb immobilization and valence state transformation

3 Release and secondary immobilization of As/Sb with transformation of Fe(Ⅲ) minerals by microorganisms

3.1 Reduction of Fe(Ⅲ) minerals

3.2 As/Sb release and secondary immobilization

3.3 As/Sb valence state transformation

4 Mechanism of As/Sb immobilization by microbial synthesized Fe(Ⅲ) minerals

4.1 Mineralogy of microbial synthesis of Fe(Ⅲ) minerals

4.2 Adsorption thermodynamics of As/Sb by Fe(Ⅲ) minerals

4.3 Complexation mechanism of As/Sb with Fe(Ⅲ) minerals

5 Influencing factors of As/Sb immobilization by microbial synthesized Fe(Ⅲ) minerals

5.1 Species of As/Sb and iron minerals

5.2 Coexisting anions

5.3 Organic matter

5.4 pH

6 Conclusion and outlook

Key words: microorganism, iron minerals, redox, As/Sb removal
Fig. 1 Formation of different biogenic Fe(Ⅲ) minerals during Fe(Ⅱ) oxidation by the nitrate-reducing Acidovorax strain BoFeN1 (The orange, blue and brown minerals are ferric (oxyhydr)oxides of different crystallinity)[24]. Copyright 2011, Mineralogical Society of America
Table 1 Microorganisms participation in Fe redox to remove arsenic and antimony
Microbes Fe concentration Iron products Target Removal performance ref
Fe(Ⅱ)-oxidizing
denitrifying bacteria BoFeN1		 3.5 mM Fe(Ⅱ) Superparamagnetic goethite, ferrihydirte and Lepidocrocite 20 μM As(Ⅲ)、As(Ⅴ) 98.9% As(Ⅴ) removal efficiency
and 97.1% As(Ⅲ) removal
efficiency		 29
KS - 98.9% removal efficiency As(Ⅴ)
and 99.6% As(Ⅲ) removal
efficiency
SW2 ND* 98.4% removal efficiency As(Ⅴ)
and 99.6% As(Ⅲ)
removal efficiency
As(Ⅲ)-oxidizing
denitrifying bacteria		 20 mg/L Fe(Ⅱ) Hematite and amorphous Fe(Ⅲ) (hydr)oxides 0.5 mg/L
As(Ⅲ)		 97.2(±3.3)% As removal efficiency 38
Fe(Ⅱ)-oxidizing
denitrifying bacteria		 9.0 mM Fe(Ⅱ) Fe(Ⅲ) (hydr)oxides 100 and 500 μM As(Ⅲ) > 96% As removal efficiency 36
Fe(Ⅲ)-reducing
bacteria MR-1		 6~8 mM As-bearing
Fe(Ⅲ) minerals		 Secondary Fe(Ⅱ) and
Fe(Ⅱ)/Fe(Ⅲ)
minerals		 As(Ⅲ) and
As(Ⅴ) in
Fe(Ⅲ) minerals		 Aqueous As(Ⅲ) and As(Ⅴ)
concentrations increased and decresed
respectively		 40
Fe(Ⅲ)-reducing
bacteria MR-1		 5~7 mM As(Ⅴ)-
bearing Fe(Ⅲ)
(Oxyhydr)oxides		 Vivianite and siderite As(Ⅴ) in
Fe(Ⅲ)
(oxyhydr)oxides		 As(Ⅴ) oxided to As(Ⅲ) and
absorbed to Fe(Ⅱ)/Fe(Ⅲ) minerals		 50
Bacteria from military shooting range soils 29 500 mg/kg Fe 71% Sb(Ⅲ)-goethite
and 10% Sb(Ⅴ)-
goethite		 20 mg/kg Sb in soils Sb(Ⅲ) concentrations correlated with Fe(Ⅱ) concentrations 46
Fe(Ⅲ)-reducing
bacteria CN32		 20 g/L Sb(Ⅴ)-
bearing ferrihydrite		 FeOOH polymorphs,
feroxyhyte and goethite		 456 ± 52 μmol/g Sb(Ⅴ) Aqueous Sb(Ⅴ)
concentrations
decreased		 53
Fig. 2 Microbial iron cycle
Fig. 3 Microorganisms participation in the transformation of As(Ⅴ) in Fe(Ⅲ) reduction process
Fig. 4 Aqueous As adsorption mechanism by hollow polyaniline microsphere/Fe3O4 nanocomposite[81]
Fig. 5 Structure model of Fe (hydro) oxide-Sb(Ⅴ) edge sharing (above) and corner sharing (below) coordinations (O atoms are shown in red)[55]. Copyright 2020, American Chemical Society
Table 2 Coordination mechanism between arsenic/antimony and iron minerals
Iron minerals Target As/Sb-Fe interatomic distance (Å) Coordination complex ref
Siderate-goethite bimineral As(Ⅴ) 3.34~3.35 2C 76
3.45~3.50 1V
As(Ⅲ) 3.33~3.35 2C
3.45~3.52 1V
Goethite As(Ⅲ) 3.378 ± 0.014 2C 79
Two-Line Ferrihydrite and
hematite		 As(Ⅲ) 2.90 ± 0.05 2E 80
3.35 ± 0.05 2C
Goethite and lepidocrocite As(Ⅲ) 3.3~3.4 2C 80
3.5~3.6 1V
Goethite As(Ⅴ) 3.60 1V 82
3.24~3.26 2C
2.83~2.85 2E
Magnetite As(Ⅴ) 3.35~3.39 ±0.04 2C 85
- Outer-sphere
As(Ⅲ) 3.50~3.53 ± 0.04 3C
3.28~3.30 ± 0.04 Species with low surface coverage
Ferrihydrite Sb(Ⅴ) 3.10~3.11 2E 54
3.51~3.55 2C
3.07~3.09 2E
3.53~3.57 2C
Goethite Sb(Ⅴ) 3.08~3.11 2E 54
3.11~3.13 2E (In the chains)
3.33~3.36 2E (In the row)
3.55~3.58 2C
Goethite Sb(Ⅴ) 3.07~3.08 2E 88
Sb(Ⅲ) 3.46 2C
Goethite Sb(Ⅴ) - 2E 90
- Outer-sphere
Sb(Ⅲ) 3.46 2C
Table 3 Effect of coexisting anions on arsenic and antimony removal by iron mineralsa)
Anion Target Effect Mechanism ref
N As(Ⅴ) A* Acceleration of nitrate-dependent Fe(Ⅱ) oxidation and Fe(Ⅲ) minerals formation 59
As(Ⅲ) O* Reduction of N contributes to As(Ⅲ) oxidation in microbes 97
Sb(Ⅲ) A Oxidation of Sb(Ⅲ) and inhibition of iron reduction 98
Sb(Ⅲ) N* - 106
Sb(Ⅴ) N - 113
P As(Ⅲ) and As(Ⅴ) I* Phosphate competes with arsenic adsorption surface sites on iron minerals 103
As(Ⅲ) and As(Ⅴ) I Phosphate ions have strong interaction with As(OH)3 and As 104
Sb(Ⅴ) I Affect of pH with the addition of phosphate 105
Sb(Ⅲ) I Sb(OH)3 and P compete for the same sites on goethite 106
Si As(Ⅲ) and As(Ⅴ) I Si can bind to Fh through ligand exchange 107
As(Ⅲ) and As(Ⅴ) I Polymeric Si can diminish As rentention on hematite 108
As(Ⅲ) I Si competes the eletrostatic attration sites with As 114
HC/C As(Ⅲ) I HC/C competition behavior varies with pH 109
As(Ⅲ) and As(Ⅴ) I C can form bidentate binuclear inner-shpere surface complexes on hematite 110
Table 4 Effect of pH on arsenic and antimony removal by iron minerals
Iron minerals Target Effect ref
Maghemite As(Ⅴ) Removal percentage dropped from 68.16% to 6.67% with pH increasing from10 to 11 74
HFO and goethite As(Ⅲ) and As(Ⅴ) As(Ⅴ) has a higher affinity for solids below pH = 5~6 and it is opposite above pH = 7~8 103
Goethite Sb(Ⅲ) Strong absorption affinity on pH 3~12 90
Sb(Ⅴ) Maximum adsorption below pH 7 90
Fe-Mn bimetal composite Sb(Ⅴ) Adsorption capacity of Sb(Ⅴ) decreased at pH of 9 113
Fe3O4@TA@UiO-66 As(Ⅲ) and Sb(Ⅲ) Adsorption behaviors of As(Ⅲ) and Sb(Ⅲ) were pH independent 14
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