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Progress in Chemistry 2021, Vol. 33 Issue (8): 1426-1439 DOI: 10.7536/PC200771 Previous Articles   Next Articles

• Review •

Activation Methods of Advanced Oxidation Processes Based on Sulfate Radical and Their Applications in The Degradation of Organic Pollutants

Wenliang Han(), Linyang Dong   

  1. Department of Environmental Science and Engineering, College of Chemical Engineering, Huaqiao University,Xiamen 361021, China
  • Received: Revised: Online: Published:
  • Contact: Wenliang Han
  • Supported by:
    National Natural Science Foundation of China(41203077); Natural Science Foundation of Fujian, China(2018J01065)
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Advanced oxidation processes(AOPs) based on sulfate radical(SO4.-) have attracted more and more attention due to their high degradation ability and adaptability to new types of organic pollutants. Compared with hydroxyl radical(·OH), SO4.- has better selectivity, higher reduction potential, longer half-life, wider pH range and lower cost, so it can degrade pollutants more effectively. SO4.- can be produced by persulfate(PS) such as peroxymonosulfate(PMS), peroxydisulfate(PDS), etc. which are activated by thermal, mechanochemical, transition metal, carbonaceous materials, alkali, ultraviolet(UV), electrochemical methods, etc. Advantages and disadvantages of different activation methods and the research progress of their applications in the degradation of organic pollutants are analyzed. Three degradation mechanisms(addition, hydrogen abstraction and direct electron transfer) of pollutants with different functional groups by SO4.- are summarized. The degradation pathways, degradation products, and research progress of persistent organic pollutants(POPs), “pseudo-persistent organic pollutants”, i.e. pharmaceuticals and personal care products(PPCPs), and organic dyes by SO4.- are reviewed. Moreover, future research directions of this technique are prospected.

Contents

1 Introduction

2 Activation methods of persulfate(PS)

2.1 Thermal activation

2.2 Mechanochemical activation

2.3 Transition metal activation

2.4 Carbonaceous materials activation

2.5 Alkali activation

2.6 Ultraviolet(UV) activation

2.7 Electrochemical activation

3 Degradation of organic pollutants by sulfate radical

3.1 Persistent organic pollutants(POPs)

3.2 Pharmaceuticals and personal care products(PPCPs)

3.3 Organic dyes

4 Conclusion and outlook

Key words: sulfate radical, advanced oxidation processes, peroxymonosulfate(PMS), peroxydisulfate(PDS), activation method, persistent organic pollutants(POPs), organic dyes
Fig. 1 Mechanism of SO4.- produced by the activation of peroxymonosulfate(PMS) or peroxydisulfate(PDS) by transition metals
Table 1 Degradation of organic pollutants by transition metal activated PS
Class Pollutant Conc.
(μM)		 PS Conc.
(mM)		 Activator Conc. pH T(℃) t(h) kobs
()		 Degradation
rate		 ref
POPs BDE-47 3.1 PDS 71.4 23,032∶1 nZVI 1000 mg/L 6~11 25 48 — 64% 39
BDE-209 10.4 PDS 200 19,183∶1 Fe2+ 100 mM 3~7 — 6 0.48 66% 41
CB-28 3.9 PDS 2 500∶1 V4+ 1 mM 5.5 25 25 0.03 80% 34
phenanthrenea 5.6 PDS 2 357∶1 V2O3 100 mg/L 3~5 25 3.6 7.15 88% 42
PPCPs carbamazepine 21.2 PMS 1.66 78∶1 Co3MnFeO6 200 mg/L 3~10 35 0.5 10.98 100% 36
tetracycline 225 PDS 5 22∶1 Ag/AgCl/(0.05)FeX 1000 mg/L 3.5 25 2 — 100% 43
norfloxacin 15 PMS 1 67∶1 Co0.4Fe2.6O4 200 mg/L 6~8.5 40 0.05 122.40 ~100% 44
norfloxacin 31.3 PMS 2 64∶1 Co(Ⅱ)/TiO2 500 mg/L 3~9 25 1 29.88 ~100% 37
ofloxacin 27.7 PMS 2 72∶1 Co(Ⅱ)/TiO2 500 mg/L 3~9 25 0.5 73.20 100% 37
Organic dyes rhodamine B 104.4 PMS 2 19∶1 Co(Ⅱ)/TiO2 500 mg/L 3~9 25 0.6 — ~100% 37
acid orange 7 56.9 PMS 0.55 10∶1 Mn-Fe/LDH 200 mg/L 5~9 25 0.5 8.28 97.6% 45
p-chloronitrobenzene 2697 PDS 200 74∶1 ZVI 1 mmol/g 3~6.8 25 8 — 90% 46
Other pollutants bisphenol A 100 PMS 2 20∶1 Mn/Fe3O4 200 mg/L 7~11 15 0.5 43.20 100% 47
p-nitrophenol 359.4 PDS 9 25∶1 CuFe2O4 30 000 mg/L 6 25 1 — 89% 48
benzotriazole 167.9 PDS 5 30∶1 Cu(Ⅱ)/V2O5 200 mg/L 9 — 2 — 97% 35
Table 2 Degradation of organic pollutants by UV activated PS
Class Pollutant Conc. (μM) PS Conc. (μM) M PS / Pollutant Wavelength(nm) pH t(h) Degradation rate ref
Anodyne antipyrine 26.5 PDS 520 19.6∶1 253.7 7.2 1.00 80% 69
Antihypertensive drugs atenolol 20 PMS 80 4∶1 254 7 0.50 ~80% 70
Antibiotics(sulfonamides) sulfadiazine 20 PDS — — — 6.5 0.30 97% 71
Antibiotics
(fluoroquinolones)		 ciprofloxacin
norfloxacin
levofloxacin		 40 PDS 500 12.5∶1 254 6.5 0.16 42%
25%
1%		 67
Antibiotics(β-lactams) cephalexin
oxacillin		 40 PDS 500 12.5∶1 254 6.5 0.16 84%
88%		 67
POPs endosulfan 2.45 PDS 49 20∶1 254 7 1.30 90% 25
Table 3 Advantages and disadvantages of different PS activation methods
Activation method Advantages Disadvantages
Thermal easy operation; no chemicals addition high cost; poor stability
Mechanochemical rapid reaction; no chemicals addition suitable for solid pollutants
Transition metal high degradation efficiency; easy operation;
no special device and low energy consumption		 metal ions leaching; poor stability and efficiency;
high cost for large-scale remediation
Alkali suitable for pollutants that can react with ·OH restricted by pH; equipment corrosion;
precipitation of metal ions
UV safe ; no secondary pollution poor reusability; high energy consumption;
high requirements for PS concentration
Carbonaceous materials high degradation efficiency; cheap and easy to get restricted by pH; poor stability
Electrochemical economic and environmental friendly;
controllable process; high degradation efficiency		 pretreatment needed; electrode passivation
Fig. 2 Direct electron transfer pathway for the degradation of organic pollutants by SO4.-[78]
Table 4 Degradation of POPs by SO4.-
Class POPs Conc. (μM) PS Conc. (μM) Activator Conc. pH T(℃) t(h) kobs() Degradation rate ref
OCPs endosulfan 2.45 PDS 49 20∶1 UV — 7 25 1.3 — 90% 25
lindane 3.43 PMS 250 73∶1 UV/Fe2+ 0.05 mM 3 25 0.6 5.05 98% 87
DDT 2.82 PMS 2000 710∶1 Co2+ 40 mM 3~5 40 2 21.60 100% 102
PCBs CB-28 3.9 PDS 2000 513∶1 V2O3 1.33 mM 5.9 25 4 0.89 100% 98
CB-28 1.94 PMS 200 103∶1 CuFe2O4 0.42 mM 7 25 8 0.49 89% 96
CB-1 20 PMS 400 20∶1 Fe2+ 0.2 mM 3 25 4 1.31 90% 103
PBDEs BDE-47 3.1 PDS 71 400 23 032∶1 nZVI 1000 mg/L 6~11 25 48 — 64% 39
BDE-209 5.2 PDS 100 000 19 183∶1 BC-nZVI 200 mM 3 40 4 0.30 82% 50
BDE-209 10.4 PDS 200 000 19 183∶1 Fe2+ 100 mM 3 25 4 0.18 51% 93
PFASs PFOA 120 PDS 12 000 100∶1 AC-Fe 1000 mg/L 2.5 25 10 0.21 64% 95
PFOA 0.5 PDS 20 000 40 000∶1 heat — 2 85 8 0.83 98% 99
PFOS 0.92 PDS 84 000 91 304∶1 heat — — 90 70 — 0% 100
PAHs phenanthrene 5.6 PDS 2000 357∶1 V2O3 100 mg/L 3~5 25 3.6 7.15 88% 42
Intermediate p-chloroaniline 500 PDS 2500 5∶1 AC 5000 mg/L 3~9 20 0.5 — 98% 104
Fig. 3 Degradation pathway of CB-28 by SO4.-[96,98]
Fig. 4 Degradation pathway of BDE-209 by SO4.-[41,50,65]
Table 5 Degradation of antibiotics by SO4.-
Class Antibiotic Conc.
(mM)		 PS Conc. (mM) MPS∶ Pollutant Activator Conc. pH T(℃) t(h) kobs(h-1) Degradation rate ref
Fluoroquinolones ciprofloxacin 0.04 PDS 0.5 12.5∶1 UV254 — 6.5 — 0.16 — 70% 67
norfloxacin 0.03 PDS 4.4 147∶1 BC 800 mg/L 6.5 25 5 0.57 ~100% 56
Sulfonamides sulfathiazole 0.10 PDS 5 50∶1 Cu2+ 0.5 mM 7 25 72 0.04 95% 114
sulfamethazine 0.18 PMS 1 5.6∶1 CuCo2O4 100 mg/L 5 25 0.5 8.46 95% 111
Tetracyclines tetracycline 0.34 PDS 11.1 32.9∶1 Fe 3500 mg/L 3.6 — 3 — 81.6% 115
β-Lactams cephalosporin 0.10 PDS 1.1 11∶1 Cu2+ 0.05 mM 7 — 2 — ~100% 26
Table 6 Degradation of organic dyes by SO4.-
Organic dye Conc. (mM) PS Conc. (mM) MPS/Pollutant Activator Conc. pH T(℃) t(min) kobs(h-1) Degradation rate ref
Acid orange 7 0.2 PDS 4 20∶1 CoMn2O4/rGO 50 mg/L 7 25 20 — 100% 52
Acid orange 7 0.06 PMS 0.55 9.7∶1 Mn-Fe/LDH 200 mg/L 5~9 25 30 8.28 98% 45
Acid orange G 0.11 PMS 0.28 2.5∶1 Co-Mn/LDH 25 mg/L 3~10 25 4 50.40 100% 118
Methylene blue 0.16 1.8∶1 — 100%
Rhodamine B 0.10 2.7∶1 — 100%
Methyl orange 0.15 1.8∶1 — 100%
p-Chloronitrobenzene 2.7 PDS 200 74.1∶1 ZVI 1.0 mmol/g 3~7 25 480 — 90% 46
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