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Progress in Chemistry 2021, Vol. 33 Issue (3): 471-489 DOI: 10.7536/PC200562 Previous Articles   Next Articles

Special Issue: 金属有机框架材料

• Review •

Elimination of Emerging Organic Contaminants in Wastewater by Advanced Oxidation Process Over Iron-Based MOFs and Their Composites

Xiaohong Yi1,2, Chongchen Wang1,2,*()   

  1. 1 Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation, Beijing University of Civil Engineering and Architecture,Beijing 100044, China
    2 School of Environment and Energy Engineering, Beijing University of Civil Engineering and Architecture,Beijing 100044, China
  • Received: Revised: Online: Published:
  • Contact: Chongchen Wang
  • Supported by:
    the National Natural Science Foundation of China(51878023); the Beijing Natural Science Foundation(8202016); the Great Wall Scholars Training Program Project of Beijing Municipality Universities(CIT&TCD20180323); the Beijing Talent Project(2019A22); the BUCEA Post Graduate Innovation Project(PG2020038)
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The emergence of emerging organic contaminants(EOCs) has attracted increasing attention due to their wide distribution and persistence in aquatic ecosystems, as well as the potential threat to the health and safety of aquatic organisms. Traditional water treatment processes represented by activated sludge processes are generally insufficient to eliminate these persistent pollutants. For efficient removal of EOCs, advanced oxidation technology based on new materials is one of the most important advanced treatment technologies. Fe-MOFs and their composites have been widely used in many fields, especially in the catalytic oxidation of pollutants in wastewater. With the aid of the improvement of synthesis methods, post-synthetic modification and being composited with specific functional materials, Fe-MOFs can be used to effectively improve the adsorption performance, enhance the light absorption characteristics, and promote the effective separation of charge carriers. The review focuses on the progress of advanced oxidation processes(photocatalysis, Fenton-like reaction and sulfate radical($SO_{4}^{-·}$) mediated oxidation) of Fe-MOFs and their composites to remove emerging organic contaminants in wastewater. As well, the opportunities and challenges of Fe-MOFs in the field of EOCs removal are proposed.

Contents

1 Introduction

2 Preparation of Fe?MOFs and their composites for oxidative degradation of EOCs

2.1 MIL?100(Fe) and its composites

2.2 MIL?101(Fe) and its composites

2.3 MIL?53(Fe) and its composites

2.4 MIL?88(Fe) and its composites

3 The application of Fe?MOFs and their composites in advanced oxidation degradation of EOCs

3.1 Advanced oxidative degradation of drugs in wastewater by Fe?MOFs and their composites

3.2 Advanced oxidative degradation of environmental hormone in wastewater by Fe?MOFs and their composites

3.3 Advanced oxidative degradation of pesticide in wastewater by Fe?MOFs and their composites

3.4 Advanced oxidative degradation of multiple EOCs in wastewater by Fe?MOFs and their composites

4 The influencing factors of advanced oxidation degradation of EOCs by Fe?MOFs and their composites

4.1 The influence of physical properties of materials

4.2 The influence of operation conditions

4.3 The influence of active substances

5 Conclusions and prospects

Key words: emerging organic contaminants, metal-organic frameworks(MOFs), advanced oxidation process, catalysis, degradation
Fig.1 Diagrams of carboxylic acid ligands and Fe-MOFs structure:(a) 1,4-dicarboxybenzene;(b) MIL-53(Fe)[42];(c) MIL-88B(Fe)[42];(d) MIL-101(Fe)[42];(e) 1,3,5-benzenetricarboxylic acid;(f) MIL-100(Fe)[44];(g) fumaric acid;(h) MIL-88A(Fe)[43]
Table 1 The degradation performance of iron-based MOFs and their composites for EOCs
Catalysts/Dosage (g·L-1) Target Pollutants/Volume
(mL)/concentration
(mg·L-1)/pH 		Light Source Reaction Time (min) Degradation Efficiency (%) ref
Photocatalytic oxidation
WO3/MIL-53(Fe)/0.2 2,4-dichlorophenoxyacetic
acid/100/45/2.5		 sun light 240 ~100 45
CdS/MIL-53(Fe)/0.75 ketorolac tromethamine/100/10/6 85 W Oreva CFL bulb(λ≥ 420 nm) 330 80 46
MIL-88A/g-C3N4/1.0 tetracycline/100/10/NA 1000 W iodine tungsten lamp(λ≥ 420 m) 120 22 47
Ag/AgCl@MIL-88A(Fe)/0.4 ibuprofen/50/10/NA 500 W Xe lamp(λ≥ 420 nm) 210 100 48
BiOI/MIL-88B(Fe)/0.3 ciprofloxacin/100/10/NA 150 W Xe lamp(AM 1.5G) 270 80 49
MIL-100(Fe)/PANI/0.25 tetracycline/200/10/NA 300 W Xe lamp 120 84 36
Fenton-like reaction
1T-MoS2@MIL-53(Fe)+20 mmol/L·H2O2/0.4 ibuprofen/50/10/7.0 500 W Xe lamp(λ≥ 420 nm) 120 100 50
g-C3N4/PDI@NH2-MIL-53(Fe)+10 mmol/L·H2O2/0.4 tetracycline/50/50/6.0 5 W LED white lamp(380~800 nm) 40 90 51
g-C3N4/PDI@NH2-MIL-53(Fe)+10 mmol/L·H2O2/0.4 carbamazepine/50/50/6.0 5 W LED white lamp(380~800 nm) 150 78 51
g-C3N4/PDI@NH2-MIL-53(Fe)+10 mmol/L·H2O2/0.4 bisphenol A/50/50/6.0 5 W LED white lamp(380~800 nm) 10 100 51
g-C3N4/PDI@NH2-MIL-53(Fe)+10 mmol/L·H2O2/0.2 bisphenol A/50/2/6.0 5 W LED white lamp(380~800 nm) 10 100 51
MIL-88A(Fe)+100 μL H 2O2/0.2 bisphenol A/50/10/NA 350 mW LED visible light 60 ~100 52
PANI/MIL-88A(Fe)+20 μL H 2O2/0.2 bisphenol A/50/10/5.1 5 W LED visible light 30 100 53
CUS-MIL-100(Fe)+6 mmol/L H2O2/0.5 sulfamethazine/80/20/3.0 in dark 60 100 17
Pd@MIL-100(Fe)+40 μL H 2O2/0.125 theophylline/40/20/4.0 300 W Xe lamp(λ≥ 420 nm) 150 99.5 54
Pd@MIL-100(Fe)+40 μL H 2O2/0.125 ibuprofen /40/20/4.0 300 W Xe lamp(λ≥ 420 nm) 150 100 54
Pd@MIL-100(Fe)+40 μL H 2O2/0.125 bisphenol A/40/20/4.0 300 W Xe lamp(λ≥ 420 nm) 150 68 54
Pd-PTA-MIL-100(Fe)+40 μL H 2O2/0.125 theophylline/40/20/4.0 300 W Xe lamp(λ≥ 420 nm) 150 99.5 55
Pd-PTA-MIL-100(Fe)+40 μL H 2O2/0.125 ibuprofen/40/20/4.0 300 W Xe lamp(λ≥ 420 nm) 180 99.5 55
Table 1 (continued) The degradation performance of iron-based MOFs and their composites for EOCs
Catalysts/Dosage (g·L-1) Target Pollutants/Volume
(mL)/concentration
(mg·L-1)/pH 		Light Source Reaction Time (min) Degradation Efficiency (%) ref
WO3/MIL-100(Fe)+40 μL H 2O2/0.25 bisphenol A/80/10/3.0 25 W LED visible light 20 100 56
MIL-100(Fe)/g-C3N4+50 μL H 2O2/0.5 diclofenac sodium/200/0.1 mmol/L/NA 300 W Xe lamp 50 100 21
MIL-100(Fe)/Fe-SPC+40 mmol/L·H2O2/1.0 thiamethoxam/50/60/7.5 600 W ultrasonic probe 100 100 57
Cu2O/MIL-100(Fe/Cu)+49 mmol/L H2O2/0.5 thiacloprid/50/80/7.47 500 W Xe lamp 25 90 58
MIL-100(Fe)/TiO2+20 μL H 2O2/0.05 tetracycline /100/100/NA 450 W Xe arc lamp 60 85.8 59
MIL-100(Fe)@Fe3O4/CA+H2O2/0.2 tetracycline /50/10/5.0 150 W Xe lamp(λ≥ 400 nm) 210 85 60
M.MIL-100(Fe)@ZnO +10 mmol/L·H2O2/0.2 bisphenol A/50/5/2.0 LSH-500 W Xe arc lamp 60 ~100 61
M.MIL-100(Fe)@ZnO +10 mmol/L·H2O2/0.2 atrazine/50/5/2.0 LSH-500 W Xe arc lamp 120 >80 61
Oxidation of activated persulfate
AgIO3/MIL-53(Fe)+50 mg·L-1 PS/0.5 methyl malathion/100/20/5.0 sun light 120 93 37
AgIO3/MIL-53(Fe)+50 mg·L-1 PS/0.5 chlorpyrifos/100/20/5.0 sun light 120 97 37
AgIO3/MIL-53(Fe)+50 mg·L-1 PS/0.5 methyl malathion(binary mixture)/100/20/5.0 sun light 180 100 37
AgIO3/MIL-53(Fe)+50 mg·L-1 PS/0.5 chlorpyrifos(binary mixture)/100/20/5.0 sun light 180 50 37
MIL-88A@MIP+10.8 mmol/L PS/0.5 dibutyl phthalate/100/3.5/ not adjusted in dark 480 77.4 62
MIL-88A@MIP+10.8 mmol/L PS/0.5 dibutyl phthalate/100/4.0/ not adjusted in dark 480 >80.4 62
MIL-88A@MIP+10.8 mmol/L PS/0.5 dibutyl phthalate/100/5.0/ not adjusted in dark 480 80.4 62
MIL-88B(Fe)+2 mmol/L PS/0.6 bisphenol A/100/10/6.5~7.2 300 W Xe lamp(λ≥ 420 nm) 25 100 63
Bi12O17Cl2/MIL-100(Fe)+0.2 mmol/L PS/0.25 bisphenol A/200/10/5.2 300 W Xe lamp 40 100 64
g-C3N4/MIL-101(Fe)+1 mmol/L PS/0.5 bisphenol A/NA/10/NA 300 W Xe lamp(λ≥ 400 nm) 60 98 34
AQS-NH-MIL-101(Fe)+10 mmol/L PS/0.2 bisphenol A/25/60/5.76 in dark 120 97.7 35
Fig.2 The morphologies of (a) Pd/MIL-100(Fe)[54],(b) Pd-PTA-MIL-100(Fe)[55],(c) CUS-MIL-100(Fe)[17],(d) MIL-100(Fe)/Fe-SPC[57],(e) Cu2O/MIL(Fe/Cu)[58];(f) Cu2O/MIL(Fe)[58];(g) MIL-100(Fe)/Ti2[59];(h) M.MIL-100(Fe)@ZnO[61] and (i) MIL-100(Fe)@Fe3O4/CA[60]
Fig.3 The morphologies of (a) MIL-100(Fe)/g-C3N4[21],(b) MIL-100(Fe)/PANI[36],(c) WO3/MIL-100(Fe)[56] and (d) Bi12O17Cl2/MIL-100(Fe)[64]
Fig.4 The morphologies of (a) g-C3N4/MIL-101(Fe)[34] and (b) AQS-NH-MIL-101(Fe)[35]
Fig.5 The morphologies of(a) WO3/MIL-53(Fe)[45],(b) 1T-MoS2@MIL-53(Fe)[50],(c) CdS/MIL-53(Fe)[46],(d) AgIO3/MIL-53(Fe)[37] and (e) g-C3N4/PDI@NH2-MIL-53(Fe)[51]
Fig.6 The morphologies of(a) MIL-88A-1[52],(b) MIL-88A-2[52],(c) PANI/MIL-88A(Fe)[53],(d) MIL-88A/g-C3N4[47],(e) MIL-88A@MIP[62],(f) Ag/AgCl@MIL-88A(Fe)[48],(g) MIL-88B(Fe)[63],(h) MIL-88B(Fe)[49] and (i) BiOI/MIL-88B(Fe)[49]
Fig.7 The proposed pathways for the photo-Fenton degradation of BPA by (a) MIL-88A-2[52],(b) PANI/MIL-88A(Fe)[53] and (c) WO3/MIL-100(Fe)[56]
Fig.8 (a) Proposed transformation pathways for BPA degradation in M88/Vis/PS system;(b) risk assessment of BPA and its by-products via ECOSAR in M88/PS/Vis system;(c) the relative absorption intensity variation of M88/PS/Vis system to CCK-8;(d) the efficiency of BPA mineralization by the M88/PS/Vis system[63]
Fig.9 (a) BPA chemical structure;(b) HOMO and LUMO orbitals of BPA;(c) NPA charge distribution and Fukui index of BPA;(d) Proposed pathways of photocatalytic degradation toward BPA over BM200/light/PS system[64]
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