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化学进展 2022, Vol. 34 Issue (4): 870-883 DOI: 10.7536/PC210435 前一篇   后一篇

• 综述 •

微生物铁氧化还原作用对水中砷锑去除影响的研究进展

张双玉, 胡韵璇, 李成, 徐新华*()   

  1. 浙江大学环境与资源学院 环境工程系 杭州 310058
  • 收稿日期:2021-04-22 修回日期:2021-06-28 出版日期:2022-04-24 发布日期:2021-07-29
  • 通讯作者: 徐新华
  • 基金资助:
    国家自然科学基金项目(21976153)
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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:2021-04-22 Revised:2021-06-28 Online:2022-04-24 Published:2021-07-29
  • Contact: Xinhua Xu
  • Supported by:
    National Natural Science Foundation of China(21976153)

砷锑污染在全球领域广泛存在,与常规的铁氧化物相比,微生物铁氧化生成的含Fe(Ⅲ)矿物对水中砷/锑(As/Sb)具有更强的吸附能力,并因其高效、实用和环境友好而具有广阔的应用前景,但微生物铁还原也可能导致被吸附的As/Sb再次释放。本文综述了微生物铁氧化还原作用对As/Sb去除影响的研究进展,归纳了铁矿物“合成-溶解-转化”的微生物循环过程以及该循环伴随的水中As/Sb固定、溶解与转化机理,整合了微生物合成Fe(Ⅲ)矿物的矿物学性质、对As/Sb固定的热动力学规律和络合机制,总结了微生物合成Fe(Ⅲ)矿物对As/Sb去除的影响因素,基于该研究的现存问题展望了利用微生物铁氧化还原作用去除As/Sb的发展方向。

关键词： 微生物, 铁矿物, 氧化还原, 除As/Sb

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
()
图1 Acidovorax菌株BoFeN1氧化Fe(Ⅱ)合成不同种类的Fe(Ⅲ)矿物(橙色、蓝色、棕色矿物是不同结晶度的Fe(Ⅲ)(氢)氧化物)[24]
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
表1 微生物参与Fe氧化还原去除砷锑
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
图2 微生物铁循环
Fig. 2 Microbial iron cycle
图3 微生物参与Fe(Ⅲ)还原过程As(Ⅴ)的转化
Fig. 3 Microorganisms participation in the transformation of As(Ⅴ) in Fe(Ⅲ) reduction process
图4 聚苯胺空心微球/Fe3O4纳米材料吸附水溶液As机理[81]
Fig. 4 Aqueous As adsorption mechanism by hollow polyaniline microsphere/Fe3O4 nanocomposite[81]
图5 铁(氢)氧化物-Sb(Ⅴ)共边(上)和共角(下)配位结构模型(O原子为红色)[55]
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
表2 砷锑与铁矿物配位机制
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
表3 共存阴离子对铁矿物砷锑去除影响a)
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
表4 pH对铁矿物砷锑去除的影响
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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