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化学进展 2021, Vol. 33 Issue (11): 2138-2149 DOI: 10.7536/PC201219 前一篇   后一篇

• 综述 •

基于过硫酸盐活化的微界面电子转移氧化技术

冯勇1,2,*(), 李谕1,2, 应光国1,2   

  1. 1 华南师范大学环境研究院 广东省化学品污染与环境安全重点实验室 环境理论化学教育部重点实验室 广州 510006
    2 华南师范大学环境学院 广州 510006
  • 收稿日期:2020-12-11 修回日期:2021-01-05 出版日期:2021-11-20 发布日期:2021-03-04
  • 通讯作者: 冯勇
  • 基金资助:
    国家自然科学基金项目(42077340); 国家自然科学基金项目(52000080); 广东省基础与应用基础研究基金(2019A1515110988)
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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:2020-12-11 Revised:2021-01-05 Online:2021-11-20 Published:2021-03-04
  • 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)

基于过硫酸盐活化的高级氧化技术是当前环境领域的研究热点。然而,环境中广泛存在的基质严重地制约了这一技术的实际应用。最新研究表明,在某些催化剂的作用下,过硫酸盐能够以电子转移的非自由基机制氧化降解污染物,而催化剂主要起电子转移媒介的作用。这一技术不易受水环境中氯离子、碳酸氢根离子等常见阴离子和天然有机物的影响,对目标污染物的氧化去除具有较高的选择性。同时,实验现象初步显示这一技术有望实现污染物的降解而无须使其与氧化剂直接接触,从而能够避免氧化剂和卤素阴离子的作用。本文着重综述了常见电子媒介的类型、电子转移机制的表征方法和常见基质对电子转移过程的影响,提出了这一技术存在的问题并对其应用前景进行了展望。

关键词： 过硫酸盐, 电子转移, 微污染物, 氧化降解, 选择性氧化, 基质效应

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
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表1 过硫酸盐的物理化学特性
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
图1 催化过硫酸盐界面电子转移氧化降解有机污染物的发展历程和机制
Fig. 1 The development and mechanism of degradation of organic contaminants by catalyzed persulfates via interfacial electron transfer
表2 活化过硫酸盐电子转移氧化去除有机污染物
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]
图2 催化过硫酸盐电子转移机制的鉴定流程
Fig. 2 Identification of electron transfer mechanism during the activation of persulfate
图3 水中常见基质影响高级氧化反应的机理示意图
Fig. 3 Effects of common water components on the advanced oxidation processes
表3 水中常见基质对电子转移氧化有机物污染物的影响
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]
表4 电子转移技术净化(模拟)实际废水
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
图4 基于(a)CNT膜和(b)盐桥的原电池氧化降解装置示意图[12,13]
Fig. 4 Galvanic cell oxidation device based on(a) CNT membrane and(b) salt bridge
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