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Progress in Chemistry 2021, Vol. 33 Issue (11): 2138-2149 DOI: 10.7536/PC201219 Previous Articles   Next Articles

• Review •

Micro-Interface Electron Transfer Oxidation Based on Persulfate Activation

Yong Feng1,2(), Yu Li1,2, Guangguo Ying1,2   

  1. 1 SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical, Chemistry of Environment, South China Normal University,Guangzhou 510006, China
    2 School of Environment, South China Normal University, Guangzhou 510006, China
  • Received: Revised: Online: Published:
  • Contact: Yong Feng
  • Supported by:
    National Natural Science Foundation of China(42077340); National Natural Science Foundation of China(52000080); Guangdong Basic and Applied Basic Research Foundation(2019A1515110988)
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Advanced oxidation processes based on persulfate activation have attracted increasing attention in the field of environmental remediation. However, the ubiquitous presence of radical scavengers in the environment limits the practical application of this technology. The latest publications show that the persulfate, under the activation of certain catalysts, can oxidize contaminants through the non-radical mechanism of electron transfer, and the catalyst mainly serves as an electron shuttle. This technology is not easily affected by common anions, such as chloride ions and bicarbonate ions, and natural organic matters and has high selectivity for the oxidation of target contaminants. Meanwhile, this technology may degrade pollutants without the need of direct contact between oxidants and pollutants, thereby avoiding the generation of toxic halogenated products due to the direct interaction between halogen ions and persulfate. This review mainly summarizes the types of common electron shuttles, the characterization methods of electron transfer processes, and the effects of common water components. Finally, the problems and application potential of this technology are proposed.

Contents:

1 Introduction

2 Mechanism and categories of interfacial electron transfer oxidation

2.1 Development and mechanism of interfacial electron transfer

2.2 Types of electron shuttles

2.3 Advantages and disadvantages of different electron shuttles

3 Identification of electron transfer mechanism

3.1 Radical measurements

3.2 Involvement of nonradical species

3.3 Electrochemical tests

3.4 Decomposition of persulfates

3.5 Theoretical calculation

4 Influencing factors of interfacial electron transfer

4.1 Factors influencing the catalytic reactivity

4.2 Factors influencing the adsorption reactivity

5 Effects of common water components

5.1 Chloride ions

5.2 Carbonate and bicarbonate ions

5.3 Natural organic matters

5.4 Treatment of wastewate by electron transfer

6 Applications of interfacial electron transfer

7 Conclusions and outlook

Key words: persulfate, electron transfer, microcontaminants, oxidative degradation, selective oxidation, matrix effects
Table 1 Physicochemical properties of persulfates
Properties PMS PDS
standard reduction potential(VNHE) 1.81 ± 0.03[15] 2.08[16]
O—O dissociation energy(kJ·mol-1) 150.6[17] 92[17]
dissociation constant 9.4 ± 0.1[18] -3.5[19]
rate constant with halide ion(M-1·s-1) pH-dependent[20]
kHS,Cl=(2.06 ± 0.03) × 10-3
kS,Cl=(3.8 ± 0.5) × 10-4
kHS,Br=(7.0 ± 0.1) × 10-1
kS,Br=(1.7 ± 0.3) × 10-1		 negligible[21]
rate constant with radical(M-1·s-1) pH-dependent[22]
k HS , S O 4 · -< 105
k S , S O 4 · -< 105
kHS,·OH= 1.7 × 107
kS,·OH= 2.1 × 109		 k PDS , S O 4 · -= 1.2 × 106[21]
kPDS,·OH< 106[21]
main activation method transition metal, base, UV light, carbonaceous materials transition metal, base, UV light, heat, microwave, ultrasound, carbonaceous materials
major reactive species SO4·-, ·OH, SO4·-,1O2 SO4·-, ·OH, SO4·-,1O2
Fig. 1 The development and mechanism of degradation of organic contaminants by catalyzed persulfates via interfacial electron transfer
Table 2 Oxidative removal of organic contaminants by activated persulfates via electron-transfer mechanism
Material types Activator Persulfate Contaminant Removal rate
CNT N-doped CNT PMS Phenol ~100%[30]
CNT PDS PDs ~100%[28]
CNT PMS 4-CP ~100%[12,31]
CNT PDS PCs 20%~100%[27,32]
Biochar Corncob biochar PDS SDZ 97.1%[33]
Reed biochar PDS Orange G ~100%[34]
Spirulina biochar PDS SMX ~100%[35]
Sawdust biochar PDS AO7 96%[36]
Shrimp shell biochar PDS 2,4-DCP ~100%[37]
Porous carbon N-doped porous carbon PMS BPA ~100%[38]
N-doped porous carbon PMS 4-CP ~100%[39]
mesoporous carbon PDS 2,4-DCP ~100%[40]
N-doped graphitic carbon PMS BPA 90%[41]
N-doped nanosphere PMS Phenol 97%[25]
Graphene-like nanosheets PDS SMX ~100%[42]
Transition metal(oxide) CuO PDS 2,4-DCP ~100%[29]
Iron-doped δ-MnO2 PMS BPA 95%[13,14]
Fig. 2 Identification of electron transfer mechanism during the activation of persulfate
Fig. 3 Effects of common water components on the advanced oxidation processes
Table 3 Effects of common water components on the degradation of organic contaminants via electron-transfer mechanism
Water matrixes Reaction conditions [Water matrices]/
[contaminant]		 Overall influence
Cl- [Cl-] = 5 mM, [PDS] = 20 μM, [2,4-DCP] = 5 μM, initial pH 5.8 1,000 NB[29]
[Cl-] = 17 mM, [PDS] = 6 mM, [SMX] = 79 μM 215 NB[35]
[Cl-] = 20 mM, [PDS] = 2 g/L, [2,4-DCP] = 1.2 mM 17 NB[66]
NOMs [humic acid] = 10 mg/L, [PDS] = 1 mM, [phenol] = 10 μM, initial pH 7 NA NB[47]
[humic acid] = 40 mg/L, [PDS] = 6 mM, [SMX] = 79 μM NA NB[35]
[Suwannee River NOM] = 50 mg/L, [HOPC] = 0.2 g/L, [PMS] = 2 mM, [BPA] = 50 μM NA NB[38]
HCO3- [HCO3-] = 7.2 mM, [PDS] = 6 mM, [SMX] = 79 μM 91 NB[35]
Table 4 Treatment of synthetic/practical wastewater by electron transfer-mediated technologies
Oxidative combination Synthetic/practical wastewater Water quality parameters Degradation performance
Fe0.15Mn0.85O2/PMSa Synthetic shale gas
produced water		 [Cl-] = 1840.6 mM, [Br-] = 9.3 mM,
[BPA] = 50 μM		 kDI water = 0.0029 min-1,
kwastewater = 0.0020 min-1 [13]
Graphitized nanodiamond/PDS Surface water [DOC] = 4.1 mg/L, [alkalinity] = 38 mg/L,
[conductivity] = 162.9 μS/cm, [phenol] = 10 μM		 No obvious difference[47]
Groundwater [DOC] = 0.3 mg/L, [alkalinity] = 40 mg/L, [conductivity] = 151.2 μS/cm, [phenol] = 10 μM
Sea water [DOC] = 1.3 mg/L, [conductivity] = 50 910 μS/cm, [phenol] = 10 μM
Hierarchically ordered
porous carbon/PMS		 Artificial drinking water [Suwannee River NOM] = 2 mg/L, [NaHCO3] = 252 mg/L, [CaCl2·2H2O] = 147 mg/L, pH 7.6 Near 100% after reaction for 1 min[38]
Artificial seawater [NaCl] = 245 mg/L, [NaBr] = 0.82 mg/L, [MgCl2·6H2O] = 110 mg/L, [CaCl2·2H2O] = 16 mg/L, [KCl] = 7.5 mg/L, pH 8.2
Wastewater treatment plant effluent [BOD] = 17.9 mg/L, pH 7.1
Fig. 4 Galvanic cell oxidation device based on(a) CNT membrane and(b) salt bridge
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