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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2023 , Vol. 35 >Issue 8: 1258 - 1265

DOI: https://doi.org/10.7536/PC221214

Review

Peracetic Acid-Based Advanced Oxidation Processes and Its Applications in Water Disinfection

  • Yining Li ,
  • Minghao Sui , *
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  • College of Environment Science and Engineering, Tongji University,Shanghai 200092, China
*Corresponding author e-mail:

Received date: 2022-12-28

  Revised date: 2023-03-27

  Online published: 2023-05-10

Supported by

National Natural Science Foundation of China(2019YFC0408801)

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Abstract

Recent research has revealed that PAA-based advanced oxidation processes (AOP) can simultaneously destroy developing micropollutants in water while having a greater disinfection efficacy than PAA alone. This paper summarizes the activation mechanism of PAA-based AOP and its use in water disinfection. According to recent study, UV/PAA has a good treatment effect in the cutting-edge problems of water disinfection, such as the removal of algae and algal toxins, the inactivation of fungus and antibiotic-resistant bacteria, etc. It is awaiting more investigation. There are few AOPs in the realm of water disinfection that activate PAA in other ways, but they have significant research promise. Identification of potential disinfection by-products found in AOP of PAA may also become a focus of future research.

Contents

1 Introduction

2 Peracetic acid-based advanced oxidation processes and activation mechanism

2.1 Radiation activation

2.2 Metal catalysts activation

2.3 Activated carbon catalysts activation

3 Recent advances of peracetic acid-based advanced oxidation processes in water disinfection

3.1 Recent advances of bacterial inactivation

3.2 Recent advances of fungus and algae inactivation

3.3 Recent advances of virus inactivation

3.4 Recent advances of DBPs

4 Conclusion and outlook

Key words： peracetic acid; advanced oxidation processes; activation mechanism; water disinfection

Cite this article

Yining Li , Minghao Sui . Peracetic Acid-Based Advanced Oxidation Processes and Its Applications in Water Disinfection[J]. Progress in Chemistry, 2023 , 35(8) : 1258 -1265 . DOI: 10.7536/PC221214

1 Introduction

In recent decades, advanced oxidation processes (AOP) have developed rapidly in the field of water treatment, which can be roughly divided into photocatalytic method, Fenton method, sulfate radical advanced oxidation technology, hydroxyl radical advanced oxidation technology, etc. The emergence of many new materials or the further development of existing materials have brought new opportunities for AOP.Bimetallic oxides and their complexes, activated carbon modified by transition metals, QDs/g-C3N4, metal/carbon composites derived from metal-organic frameworks (MOFs), and peroxides are the materials that have been studied and have good effects in the field of water treatment disinfection, among which the advanced oxidation technology based on peracetic acid (peracetic acid,PAA,CH3C(O)OOH) in peroxides has attracted much attention[1⇓⇓~4][5].
PAA disinfectant is a mixture composed of H2O2, PAA, water and acetic acid (CH3COOH). It is explosive when the concentration is greater than 45%, and it is easy to decompose when the concentration is low, and the lower the concentration, the easier it is to decompose. Some studies have shown that the half-life of PAA in 15 mg·L-1 is about 3 to 5 days for PAA in 10 h,6 g·L-1. In practical use, low temperature storage or addition of stabilizers can delay decomposition[6][7][8]. PAA itself is a strong oxidant, E0=1.96 eV, higher than H2O2(E0=1.8 eV) and chlorine dioxide (E0=1.5 eV), which has a good inactivation effect on a variety of microorganisms[9]. As a disinfectant, compared with other disinfection methods, PAA has simpler equipment requirements, less dependence on the physical and chemical properties and composition of the water to be treated, and better cost-effectiveness. It was first used in sewage treatment in Europe, and then accepted by North America. In 2012, the United States Environmental Protection Agency (USEPA) approved the use of PAA in wastewater disinfection.Compared with chlorine disinfection, PAA produces little or almost no DBPs. Nowadays, the research on PAA in water treatment is still a hot spot. It has been shown that PAA can be used to disinfect municipal sewage, industrial wastewater, sludge, drinking water and ballast water[10][11].
Activation of PAA can produce a variety of reactive oxygen radicals, including ·OH(E0=2.72 eV), methyl radical (·CH3), peracyl radical (CH3C(O)O·,E0=2.24 eV;CH3C(O)OO·,E0=1.60 eV), etc., which may play a better role than other AOPs in complex water matrices, such as water containing hydroxyl radical scavengers such as natural organic matter (NOM), carbonate/bicarbonate ions[12][13]. In recent years, PAA-based AOP has attracted more and more attention from researchers, but there are few reviews. Shi et al., Correa-Sanchez et al. And Kiejza et al. Focused on the research progress of PAA-based AOP in the degradation of organic pollutants.Ao et al. Introduced its application in water purification and water disinfection, but at present, the research on AOP based on PAA has been greatly expanded in activation process and water disinfection, and it is necessary to make a more comprehensive summary[14⇓~16][9]. In this paper, the PAA-based AOP process and its activation mechanism are summarized, and the research progress of PAA-based AOP in water disinfection is systematically described, and suggestions for the development of related technologies are provided.

2 Advanced Oxidation Technology and Activation Mechanism Based on Peracetic Acid

There are two ways of decomposition of PAA: non-free radical decomposition and free radical decomposition. The non-radical decomposition includes the self-decomposition reaction of PAA and the reaction between PAA and water (Formula 1, 2), and the H2O2 present in the system will react with the anion of PAA (Formula 3)[17]. Free radical decomposition, that is, the activation technology needed for advanced oxidation process, includes energy activation, metal activation and catalyst activation.
Peracetic acid-based AOPs can generate HO ·, CH3COO·, CH3C(O)OO·, ·CH3,HO2·, ·OOCH2C(O)O-, CH3OO·, O2-·, ·CH2C(O)O- and other free radicals.The free radicals that play a major role in degrading pollutants or inactivating pathogens are HO ·, CH3COO·, and CH3C(O)OO·,Among them, HO · can oxidize toxic pollutants in water into non-toxic or easily decomposed compounds by microorganisms, which can be mainly divided into three reactions: dehydrogenation, electrophilic addition, and electron transfer, and can inactivate pathogens by destroying cell membranes/walls, enzymes, and genetic materials[18][19,20]; However, RO · (mainly CH3COO· and CH3C(O)OO·) is more selective in the degradation of pollutants, for example, it reacts significantly with some naphthyl compounds, and its inactivation of pathogens often occurs together with HO ·, which has not been studied separately[21].
2 C H 3 C ( O ) O O H → 2 C H 3 C ( O ) O H + O 2
C H 3 C ( O ) O O H + H 2 O ↔ C H 3 C ( O ) O H + H 2 O 2
C H 3 C ( O ) O O - + H 2 O 2 → C H 3 C ( O ) O - + H 2 O + O 2

2.1 Energy activation

2.1.1 Ultraviolet activation

UV activation of PAA is the most studied at present, usually using 254 nm ultraviolet light. The first step of this activation technology is that the peroxide bond of PAA is broken under ultraviolet irradiation to form HO · and CH3C(O)O· (Formula 4), and HO · and CH3C(O)O· react with PAA to form CH3C(O)OO· (Formula 5, 6), respectively.
$\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OOH}\xrightarrow{\text{hv}}\text{HO}\cdot +\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{O}\cdot $
$\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OOH+HO}\cdot \to \text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OO}\cdot +{{\text{H}}_{\text{2}}}\text{O}$
$\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OOH}+\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{O}\cdot \to \text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OO}\cdot +\text{C}{{\text{H}}_{3}}\text{COOH}$
In addition, CH3C(O)O· undergoes unimolecular decay to produce ·CH3 (Equation 7), which reacts rapidly with oxygen to produce CH3OO· (Equation 8).
C H 3 C ( O ) O · → C H 3 · + C O 2
C H 3 · + O 2 → C H 3 O O ·
CH3OO· will undergo bimolecular decay to produce CH3O· and other substances (formula 9~11),CH3O· will undergo rearrangement and oxidation in the system to produce HOCH2OO· (formula 12, 13).This substance reacts with hydroxyl and undergoes self-decay to produce superoxide anion radical (O2-·) and HO2·, respectively (formulas 14, 15).
C H 3 O O · + C H 3 O O · → H C H O + C H 3 O H + O 2
C H 3 O O · + C H 3 O O · → 2 H C H O + H 2 O 2
C H 3 O O · + C H 3 O O · → 2 C H 3 O · + O 2
C H 3 O · → · C H 2 O H
· C H 2 O H + O 2 → H O C H 2 O O ·
H O C H 2 O O · + O H - → H C H O + O 2 - · + H 2 O
H O C H 2 O O · → H C H O + H O 2 ·
In addition to the above chemical reactions, CH3C(O)OO· undergoes double decay to form CH3C(O)O· (formula 16),CH3C(O)O· undergoes radical coupling reaction (formula 17); HO · reacts with acetate ion to form ·CH2C(O)O- (formula 18), which reacts with oxygen to form ·OOCH2C(O)O- (formula 19)[22].
2 C H 3 C ( O ) O O · → 2 C H 3 C ( O ) O · + O 2
C H 3 C ( O ) O · + C H 3 C ( O ) O · → ( C H 3 C ( O ) O ) 2
H O · + C H 3 C ( O ) O - → · C H 2 C ( O ) O - + H 2 O
· C H 2 C ( O ) O - + O 2 → · O O C H 2 C ( O ) O -
Previous studies have shown that in the UV-activated PAA system, when the molar ratio of [PAA]0/[H2O2]0 is 0.5 – 3.0,The abundance of active oxygen groups from high to low is HO2·, ·OOCH2C(O)O-, CH3OO·,CH3C(O)OO· 、O2-· 、HO·、CH3COO· 、·CH3 、·CH2C(O)O- ,In this study, the kinetic reaction rates of each chemical reaction in the UV activated PAA system were calculated in detail, and the quantum yield of PAA at UV 254 mm was obtained[23]. Fig. 1 is a summary of the mechanism of UV activation of PAA.
图1 UV活化PAA机理[23]

Fig.1 Mechanism of Ultraviolet Activation of PAA[23].Copyright 2020, American Chemical Society

2.1.2 Thermal activation

There are few studies on thermally activated PAA, and the research report on the degradation of micro-pollutants in water by thermally activated PAA technology appeared only in 2020. According to the research, there are two ways of PAA decomposition in the thermally activated PAA system: free radical decomposition and non-free radical decomposition, and non-free radical decomposition is the main decomposition mode (Fig. 2)[17]. In the degradation of SMX pollutants, the degradation effect of thermally activated PAA was better than that of thermally activated H2O2 and thermally activated persulfate (PS) under the same conditions (86% vs 0%, 27%), and the contribution of active oxygen radicals in the system was greater, so increasing the proportion of PAA radical decomposition was worth discussing in the subsequent study of thermally activated PAA[24].
图2 热活化PAA机理[17]

Fig.2 Mechanism of Thermal Activation of PAA[17].Copyright 2020, American Chemical Society

Wang et al. Investigated the decomposition process of PAA at 20 ~ 60 ℃ under neutral pH conditions, and the experiment showed that the decomposition rate of PAA would increase with the increase of temperature, and under the action of heat energy, the peroxide bond would be broken to form HO · and CH3C(O)O· (Formula 20).HO · and CH3C(O)O· react with PAA to form CH3C(O)OO· (formula 5, 6),In this activation system, the peroxy group of CH3C(O)OO- will attack the central C atom of CH3C(O)OOH to produce singlet oxygen (1O2), CH3C(O)O· and acetic acid (Formula 21). In addition, the reactions in the system are Formula 7, 8, 16, 17, etc.
$\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OOH}\xrightarrow{\Delta }\text{HO}\cdot +\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{O}$
$\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{O}{{\text{O}}^{-}}+\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OOH}\to {}^{1}{{\text{O}}_{2}}+\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{O}\cdot +\text{C}{{\text{H}}_{3}}\text{C}\left( \text{O} \right)\text{OH}$

2.1.3 Ultrasonic activation

Ultrasound (US) is also a common means of activation in previous AOP, but there are few studies on the activation of PAA by US. In 2013, there was a study on the homolytic degradation of phenol by PAA catalyzed by ultrasound-assisted MnO2, and it was found that US assistance did improve the degradation efficiency[25]. In 2020, a study mentioned the use of US to activate PAA to oxidize algae cells, and found that in the case of [PAA]=10 mg·L-1, PAA could hardly rupture algae cells without US activation, while both US and UV activated PAA damaged the integrity of algae cells, but the damage effect of US/PAA was not as good as that of UV/PAA, which may be due to the fact that the reactive oxygen radicals produced by UV activation were more reactive than those activated by US[26].

2.2 Metal activation

Transition metals are commonly used catalysts in advanced oxidation processes. It has been reported that metal ions catalyze peracids in two competitive pathways (Equations 22 and 23), resulting in the formation of RC (O) O · (Equation 22) and RC (O) OO · (Equation 24)[27]. Based on the current research on activated PAA, the main transition metals used are iron, copper, cobalt, manganese, silver and so on.
M ( n - 1 ) + + R C ( O ) O O H → R C ( O ) O · + M n + + H O -
M ( n - 1 ) + + R C ( O ) O O H → R C ( O ) O - + M n + + H O ·
M n + + R C ( O ) O O H → R C ( O ) O O · + M ( n - 1 ) + + H +

2.2.1 Iron-based metal activation

In the Fenton-type advanced oxidation process, Fe2+ is the most commonly used catalyst due to its low cost and environmentally friendly characteristics, PAA has also been proved to be an oxidant in the Fenton-type process, and the Fe2+/PAA system has been proved to be the most effective at pH = 3.0, in which the reactions are shown in Formula 5 ~ 19 and Formula 25 ~ 28[28].
F e 2 + + C H 3 C ( O ) O O H → F e 3 + + C H 3 C ( O ) O · + O H -
F e 2 + + C H 3 C ( O ) O O H → F e 3 + + C H 3 C ( O ) O - + · O H
F e 2 + + C H 3 C ( O ) O O H → F e O 2 + + C H 3 C ( O ) O H + H +
F e 3 + + C H 3 C ( O ) O O H → F e 2 + + C H 3 C ( O ) O O · + H +
Although both Fe3+ and Fe2+ can react with H2O2, the reaction rate is not in the same order of magnitude as Equation 25, 26, 28, which has little effect on the system. In the Fe2+/PAA system, compared with the Fe3+,PAA, it is more inclined to react with the Fe2+, and the reaction rate of the (Fe2+-PAA,k=1.10×105~1.56×104M-1·s-1,pH=3.0~8.1;Fe3+-PAA,k=2.72 M-1·s-1,pH=3.0),pH=3.0 is about 4 orders of magnitude.Therefore, the regeneration of Fe2+ is poor. Recently, molybdenum disulfide has been used to accelerate the circulation of Fe3+/Fe2+, which significantly enhances the degradation effect of PAA on pollutants[28][29][30].
Zero-valent iron (ZVI) and sulfurized zero-valent iron (S-ZVI) are also used to activate PAA, which can ensure the continuous release of Fe2+. Studies have confirmed that ZVI/PAA can achieve rapid removal of tetracycline (TC) under weak acidic or nearly neutral conditions, in which the complex of Fe2+-TC plays a major role in activation, which is better than that of Fe2+ alone[31]. However, the mechanism of PAA activation by S-ZVI is completely different. Sulfidation enhances the ability of electron donation and electron transfer of ZVI, which makes PAA better activated[32].

2.2.2 Cu-based metal activation

Compared with other heterogeneous catalysts, copper-based oxides have shorter induced activation time and longer activation duration[33]. It has been confirmed that copper-based oxides can effectively activate PAA to produce active oxygen radicals, which have a good degradation or inactivation effect on carbamazepine and fungal spores. ZVC activated PAA has the best removal effect on diclofenac at pH = 3.0.The increase of pH will inhibit the precipitation of copper ions, and it is found that Cu+ is an effective activator in the system. The main active substances are HO ·, RO · and 1O2, and the main reactions are shown in Formula 21 and Formulas 29 to 32[34][35][36].
C u 2 + + C H 3 C ( O ) O O H → C u + + C H 3 C ( O ) O O · + H +
C u + + C H 3 C ( O ) O O H → C u 2 + + C H 3 C ( O ) O · + O H -
C u + + C H 3 C ( O ) O O H → C u 2 + + C H 3 C ( O ) O - + · O H
C u + + H 2 O 2 → C u 2 + + · O H + O H -
The research on Cu2+/PAA system is very limited. Wang et al showed that the degradation effect of Cu2+/PAA system on diclofenac was similar to that of PAA system alone, but carbonate/bicarbonate could enhance the catalytic ability of Cu2+, which may be due to the formation of CuCO3 and CuCO3(OH)- in the system[37].

2.2.3 Cobalt base metal activation

The research results of PAA activation by Co2+ show that HO · is almost not produced in the system, and the degradation effect of various aromatic organic compounds (sulfamethoxazole, bisphenol A, naproxen, carbamazepine, etc.) is significantly better than that of acidic or alkaline under neutral conditions. When the initial pH is 3.0 ~ 8.2, the K of PAA degradation by Co2+ is 1.70×101~6.67×102M-1·s-1,Co3+ and the K of PAA degradation is 3.91×100~4.57×102M-1·s-1,RO·, which is the main active substance. The activation mechanism is as follows (Formula 33, 34):[38,39][39]
C o 2 + + C H 3 C ( O ) O O H → C o 3 + + C H 3 C ( O ) O · + O H -
C o 3 + + C H 3 C ( O ) O O H → C o 2 + + C H 3 C ( O ) O O · + H +
In addition, it has been shown that Co3O4 (containing both Co2+ and Co3+) can effectively activate PAA, and RO · is the main active substance[40]. Cobalt ferrite (CoFe2O4) has also been studied as an activator of PAA. The CoFe2O4-PAA system has achieved efficient removal of a variety of micro-pollutants. The advantage of this catalyst is that the strong Fe-Co interaction significantly inhibits the leaching of cobalt ions[41].

2.2.4 Manganese-based metal activation

The activation of PAA by Mn2+ has not been widely studied. In the current study, Mn2+/PAA was used to degrade acid orange, and the effect was better under alkaline conditions (pH = 9.5). Sabine et al proposed that the activation system would undergo complex redox reactions, and MnVI=O was the actual catalytic active intermediate. Mn2+ began to activate PAA effectively at about pH 8.5, and the highly active intermediate MnVI=O reached an ideal stable state at pH 9.5. Inactive intermediates such as Mn(OH)2, MnCO3, and insoluble MnO2 begin to form after pH values greater than 9.5. It was also pointed out that an appropriate amount of H2O2 could maintain the catalytic activity of the system[42].
The activation of PAA by manganese-based oxides has recently attracted much attention. Mn3O4, PAA was successfully activated to produce active oxygen radical RO ·, which removed almost 100% of sulfamethoxazole in 12 min at pH = 6.5. This system is a radical reaction pathway, and the main chemical reactions are shown in Equations 5, 6, 35, and 36[43].
M n 2 + / M n 3 + + C H 3 C ( O ) O O H → M n 3 + / M n 4 + +   C H 3 C ( O ) O · + O H -
M n 3 + / M n 4 + + C H 3 C ( O ) O O H → M n 2 + / M n 3 + +   C H 3 C ( O ) O O · + H +

2.2.5 Activation of other metal catalyst

Some studies have used molybdenum disulfide (MoS2) to activate PAA, and the removal effect of sulfonamide pollutants was greater than 60% at pH = 3.0[27]; Ruthenium ion (Ru3+) can also activate PAA to form free radicals, and the system can remove almost 100% of micropollutants such as sulfamethoxazole, trimethoprim, carbamazepine and diclofenac in about 2 min at pH = 7.0[44]; Synergistic effect of Ag+/PAA system in disinfection field has been proved by research[45].

2.3 Carbon catalyst activation

Carbon-based materials, such as activated carbon, graphene oxide and carbon nanotubes, are good catalytic materials in AOP. However, there is only one report on the activation of PAA by activated carbon fiber (ACF)[46]. The results showed that the active dye Red X-3B could be effectively degraded in a wide pH range (3. 0 ~ 11.0) by the system of free electron transfer from ACF to PAA, which resulted in the active radical HO · and CH3COO·,ACF/PAA, and the degradation rate of Red X-3B was still 94% after 10 times of ACF recovery[46]. Therefore, there is still a huge research space for the activation of PAA by environmentally friendly carbon-based catalysts.
Table 1 is a summary of studies on PAA-based AOP degradation of organic pollutants.
表1 基于PAA的AOP降解有机污染物的研究概述

Table 1 Overview of studies employing PAA-based AOPs for removing organic compounds

Precesses Target Contamiants pH kobs Priaary Radicals ref
UV/PAA BZF 7.1 (2.40± 0.06)×10-2 min-1 HO· 46
UV/PAA DCF 7.1 1.38± 0.03 min-1HO· 46
UV/PAA CA 7.1 (2.30±0.03)×10-1 min-1 HO· 46
UV/PAA IBP 7.1 (8.83±0.15)×10-2 min-1 HO· 46
UV/PAA NAP 7.1 (3.07±0.07)×10-1 min-1 HO· 46
UV/PAA CBZ 7.1 (8.25±0.31)×10-2 min-1 HO· 46
Fe2+/PAA MB 3.0~8.2 0.17~1.75 s-1 HO· 27
Fe2+/PAA NPX 3.0~8.2 0.45~2.33 s-1 HO· 27
Fe2+/PAA BPA 3.0~8.2 0.21~0.75 s-1 HO· 27
nCuO/PAA CBZ 7 0.07 min-1 CH3C(O)OO· 33
ZVC/PAA DCF 2.0~11.0 0.1034~0.0017 min-1 HO· 35
Cu2+-HCO3-
(CO32-)/PAA		 DCF 9.3 0.0835 min-1 RO· 36
nCo3O4/PAA CBZ 7 0.03 min-1 RO· 42
Co2+/PAA SMX 7 0.1322 min-1 CHSC(O)OO· 37
Co2+/PAA BPA 7 (2.98±0.01)×10-4
(3.34±0.24)×10-2s-1		 CH3C(O)
OO·		 38
Co2+/PAA NAP 7 (4.05±0.01)×10-4
(8.12±0.38)×10-2s-1		 CH3C(O)
OO·		 38
Co2+/PAA SMX 7 (1.60±0.00)×10-4
(1.95±0.08)×10-2s-1		 CH3C(O)
OO·		 38
Co2+/PAA CBZ 7 (2.32±0.03)×10-4
(3.23±0.07)×10-3s-1		 CH3C(O)
OO·		 38
Mn2+/PAA Orange Ⅱ 7 6.05×10-2s-1 MnⅣ=O 41
MoS2/PAA SMX 7 0.128 min-1 HO· 26
US/MnO2/PAA Phenol 7 0.89 min-1 - 24

3 Research progress of peracetic acid-based advanced oxidation technology in water treatment disinfection

At present, the inactivation of bacteria, fungi, algae, viruses and other pathogenic microorganisms in water by PAA-AOP has been reported, and most of the studies focused on the UV/PAA system.

3.1 Study on inactivation of bacteria in water by PAA-AOP

In the study of inactivating bacteria in water, some studies have shown that UV/PAA process can inactivate 6-log Escherichia coli (E. coli), Enterococcus durans (E. durans) and Staphylococcus epidermidis (S. Epider midis, a drug-resistant bacterium) within 2.5 min, 3.5 min and 2.0 min, respectively, but the inactivation mechanisms are not the same. For the inactivation of E. coli, the contributions of free radicals, PAA, synergistic effect and UV are similar, and for E. durans, the contribution of RO · is similar[47]. In addition, Ag+ and Cu2+ have a synergistic effect on PAA, which can enhance the disinfection effect[45]. PAA was also applied to the UV/TiO2 process, and it was found that UV/TiO2 in the presence of PAA could completely inactivate the PAA;100~500 mg·L-1 of E.coli(0.5~2 mg·L-1 in 10 ~ 20 min (TiO2), and ultrasonic assistance could further improve the inactivation efficiency[48].
Due to the widespread use of antibiotics in daily life, in addition to antibiotic resistant bacteria (ARB), antibiotic resistance genes (ARGs) may also appear in water bodies. Sewage treatment plants are important reservoirs of ARGs and ARBs. These ARGs can be roughly divided into sulfonamides, quinolones, macrolides, tetracyclines, β-lactams, etc[49].
There are studies on the removal of ARGs in the UV/PAA process. Some scholars controlled the UV dose at 108 mJ·cm-2,[PAA]0=4 mg·L-1 and found that most of the resistance genes in the secondary sewage were effectively removed, which was mainly due to the production of active oxygen free radicals (RO ·, HO ·). Unlike the traditional NaClO disinfection, which removed ARGs by destroying the DNA of bacteria, the UV/PAA system directly inhibited the expression of key genes involved in the reproduction of ARGs[50].

3.2 Research progress on inactivation of algae and fungi in water by PAA-AOP

In recent years, with the acceleration of industrialization and the increase of diversity of human activities, seasonal eutrophication and algal blooms occur frequently in natural waters, and traditional coagulation treatment may lead to secondary pollution of high levels of coagulant residues.Some algal cells contain potent neurotoxins and hepatotoxins, which are released when the cell membrane is damaged, and the oxidation processes currently used to remove algae and algal toxins produce DBPs.Therefore, it is necessary to find new inactivation strategies, and fungi are also recognized as emerging environmental pollutants, which have been detected in surface water sources, drinking water treatment plants, and distribution water systems, posing potential health risks to humans (allergies, asthma, pneumonia, etc.), and posing challenges to traditional water treatment processes[51][52][53].
Recently, AOP technology using PAA to solve the above problems has attracted attention. The inactivation rate of Microcystis aeruginosa by UV/PAA system under neutral conditions was 3.17-ln (95.79%), while the inactivation rate by UV/H2O2 system was only 0.33-ln under the same conditions.The results also showed that RO · played a leading role in the inactivation of algae, and the diffusion of PAA also promoted the inactivation of algae. The main mechanism was that UV/PAA system destroyed the protein, lipid and nucleic acid functional groups of algae cells[54]. UV/PAA system could effectively remove -LR and -MR at pH = 7.7, which was better than that of UV/H2O2 system under the same conditions, and RO · was helpful to the degradation of the two microcystins at this pH[52]. In addition, UV/PAA process can also inactivate Aspergillus niger and Aspergillus flavus (pH = 5.0 ~ 7.0). In this experiment, four main factors contribute to the inactivation efficiency: UV > free radicals (mainly HO ·) > PAA > synergistic effect. There are two explanations for the synergistic effect: 1) PAA may inactivate catalase and improve the efficiency of free radicals as disinfectants[55][56]; 2) PAA may diffuse into the cell[47].
Other PAA-based advanced oxidation technologies have not been widely studied in the inactivation of algae and fungi in water. Some studies have focused on copper oxide (CuO), which can activate peroxymonosulfate (PMS) and has a rapid and good inactivation effect on fungi in water.However, CuO/PAA had better inactivation effect on Aspergillus niger and Aspergillus flavus than CuO/PMS under the same conditions (5-log vs < 0.2-log), and there was no significant difference between the performance in surface water and PBS[57][35].

3.3 Research progress of PAA-AOP inactivation of viruses in water

Studies on virus inactivation by PAA-AOP in water are very limited. Pilot-scale studies have found that UV/PAA treatment has a better inactivation effect on SC phage in secondary and tertiary effluent than PAA alone[58]. Koivunen et al. Found that 2.58-log MS2 phage could be inactivated at a [PAA]0=15 mg·L-1,UV dose of 38 mJ·cm-2[56].

3.4 Research Progress on DBPs

Several studies have confirmed that PAA alone produces no or very few disinfection by-products, including aldehydes, epoxides, chlorinated and brominated DBPs, and N-nitrosamines, in a typical drinking water or wastewater disinfection process, but the carboxylic acid content in water after PAA disinfection usually increases[18]. There are different conclusions about whether PAA can produce genotoxic DBPs in surface drinking water disinfection. Maffei et al. Used comet assay and human leukocyte micronucleus test to evaluate that PAA can cause DNA damage.However, more studies have shown that the use of PAA to disinfect drinking water does not detect DNA damage, or may reduce the genotoxic load of raw water, which has a great correlation with the quality of raw water[59][60][61][59⇓~61]. Therefore, the co-carcinogenic effect of PAA cannot be completely ruled out.
There is no systematic study on the possible disinfection by-products of PAA-AOP.

4 Conclusion and prospect

PAA-based AOPs mostly act through free radical pathways. Compared with HO ·, RO · can adapt to more complex water quality backgrounds and may be more selective in inactivating certain pathogenic microorganisms. Current studies have confirmed that PAA-based AOPs can inactivate microorganisms in water, including bacteria, viruses, protozoa and fungi. Compared with the advanced oxidation processes based on H2O2 or persulfate, PAA-based AOP is still a relatively new disinfection method to solve the emerging problems of water environment, and there are still many gaps to be explored.At present, most of the studies are focused on the UV activated PAA system, but the inactivation species are relatively limited, and there is room for further mechanism discussion. In the transition metal activated system, there are only studies on Cu and Ag, and the number is very small.The research on activated PAA such as Fe2+/Fe3+, Co2+, heterogeneous forms of transition metals, nanomaterials and carbon materials for water treatment disinfection is still blank, and it is necessary to develop more heterogeneous catalysts. In addition, the synergistic effect between activator and PAA is not clear.The identification of possible disinfection by-products has been largely neglected, and the organic matter content in the water treated by PAA-AOP may also be high, which are the problems that need to be paid attention to in the future research of PAA-AOP.

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