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Water Research Jun 2024Micropollutants and bacteria are prevalent pollutants in wastewater, posing significant risks to ecosystems and human health. As peracetic acid (PAA) is being...
Regulating charge transfer for enhanced PAA activation over sulfur-doped magnetic CoFeO: A novel strategy for simultaneous micropollutants degradation and bacteria inactivation.
Micropollutants and bacteria are prevalent pollutants in wastewater, posing significant risks to ecosystems and human health. As peracetic acid (PAA) is being increasingly used as a disinfectant, activation of PAA by low-cost and high-performance activators is a promising strategy for wastewater treatment. In this study, the sulfur-doped magnetic CoFeO (SCFO) is successfully developed for efficient PAA activation to simultaneously decontaminate and disinfect wastewater. PAA/SCFO-0.3 exhibits exceptional performance, degrading 100 % of 8 μM sulfamethoxazole (SMX) with a first-pseudo reaction rate of 1.275 min, and achieving 5.3-log inactivation of Escherichia coli (E. coli) within 3 min at a PAA dosage of 0.2 mM and catalyst dosage of 0.025 g/L (initial pH 6.5). Scavenging experiments and electron paramagnetic resonance (EPR) analysis identify CHC(O)O and CHC(O)OO as the dominant reactive species for SMX degradation. The sulfur species in SCFO-0.3 facilitate Co regeneration and regulate charge transfer, promoting PAA activation for SMX degradation. Moreover, the PAA/SCFO-0.3 system demonstrates operational feasibility over a broad range of water matrices and has excellent stability and reusability (maintaining 93 % removal of SMX after 5 cycles), demonstrating its potential for industrial applications. This study provides insights into enhancing PAA activation through sulfur doping in transition metal catalysts and highlights the practical applicability of the PAA/SCFO-0.3 system as an advanced alternative to conventional disinfection for simultaneous decontamination and disinfection in wastewater.
Topics: Escherichia coli; Sulfur; Wastewater; Peracetic Acid; Cobalt; Ferric Compounds; Water Pollutants, Chemical
PubMed: 38640561
DOI: 10.1016/j.watres.2024.121595 -
Environmental Pollution (Barking, Essex... Jun 2024This study presents the synthesis of a novel composite catalyst, ZIF-67, doped on sodium bicarbonate-modified biochar derived from kumquat peels (ZIF-67@KSB3), for the...
This study presents the synthesis of a novel composite catalyst, ZIF-67, doped on sodium bicarbonate-modified biochar derived from kumquat peels (ZIF-67@KSB3), for the enhanced activation of peracetic acid (PAA) in the degradation of acetaminophen (APAP) in aqueous solutions. The composite demonstrated a high degradation efficiency, achieving 94.3% elimination of APAP at an optimal condition of 200 mg L catalyst dosage and 0.4 mM PAA concentration at pH 7. The degradation mechanism was elucidated, revealing that superoxide anion (O) played a dominant role, while singlet oxygen (O) and alkoxyl radicals (R-O) also contributed significantly. The degradation pathways of APAP were proposed based on LC-MS analyses and molecular electrostatic potential calculations, identifying three primary routes of transformation. Stability tests confirmed that the ZIF-67@KSB3 catalyst retained an 86% efficiency in APAP removal after five successive cycles, underscoring its durability and potential for application in pharmaceutical wastewater treatment.
Topics: Acetaminophen; Charcoal; Water Pollutants, Chemical; Zeolites; Peracetic Acid; Prunus armeniaca; Imidazoles; Wastewater; Catalysis; Waste Disposal, Fluid
PubMed: 38636839
DOI: 10.1016/j.envpol.2024.123970 -
Environmental Science & Technology May 2024Peracetic acid (PAA) oxidation catalyzed by metal-free carbons is promising for advanced water decontamination. Nevertheless, developing reaction-oriented and...
Peracetic acid (PAA) oxidation catalyzed by metal-free carbons is promising for advanced water decontamination. Nevertheless, developing reaction-oriented and high-performance carbocatalysts has been limited by the ambiguous understanding of the intrinsic relationship between carbon chemical/molecular structure and PAA transformation behavior. Herein, we comprehensively investigated the PAA activation using a family of well-defined sp/sp carbon hybrids from annealed nanodiamonds (ANDs). The activity of ANDs displays a volcano-type trend, with respect to the sp/sp ratio. Intriguingly, sp-C-enriched AND exhibits the best catalytic activity for PAA activation and phenolic oxidation, which is different from persulfate chemistry in which the sp network normally outperforms sp hybridization. At the electron-rich sp-C site, PAA undergoes a reduction reaction to generate a reactive complex (AND-PAA*) and induces an electron-transfer oxidation pathway. At the sp-C site adjacent to C═O, PAA is oxidized to surface-confined OH* and O* successively, which ultimately evolves into singlet oxygen (O) as the primary reactive species. Benefiting from the dual nonradical regimes on sp/sp hybrids, AND mediates a sustainable redox recycle with PAA to continuously generate reactive species to attack water contaminants, meanwhile maintaining structural/chemical integrity and exceptional reusability in cyclic runs.
Topics: Peracetic Acid; Catalysis; Nanodiamonds; Water Purification; Oxidation-Reduction; Water Pollutants, Chemical; Water
PubMed: 38634679
DOI: 10.1021/acs.est.3c10361 -
Cureus Mar 2024Introduction The disinfection of impressions is crucial to eliminate the viral and other microbial loads to prevent the cross contamination of diseases. The aim of this...
Introduction The disinfection of impressions is crucial to eliminate the viral and other microbial loads to prevent the cross contamination of diseases. The aim of this study was to compare the effect of different virucidal disinfecting methods on the dimensional accuracy and surface detail reproduction (SDR) of impression materials. Methods A total of 160 samples were fabricated with different impression materials using zinc oxide eugenol (Group 1), alginate (Group 2), polyether (Group 3), and addition silicone (Group 4) impression materials, each containing 40 samples (n=40). These groups were further divided into Subgroups A, B, C, and D (n=10) based on the disinfecting method used. Disinfection was carried out using 0.2% peracetic acid (A), a natural polymer of glucosamine (B), ultraviolet (UV) radiation (C), and ozonated water (D). The disinfected impressions were poured in type IV gypsum, and the obtained casts were checked for dimensional accuracy and surface detail reproduction (SDR). For dimensional accuracy, a one-way analysis of variance (ANOVA) test and, for surface detail reproduction, the chi-square test were used to compare the different subgroups of each impression material separately. Results Zinc oxide eugenol samples showed the lowest mean dimensional change when disinfected with 0.2% peracetic acid (1A=154.1 µm), and alginate showed the lowest mean dimensional change when disinfected using ozonated water (2D=134.9 µm). On the other hand, the lowest mean dimensional change observed in polyether and addition silicone samples was those which were disinfected using UV radiation (3C=100.9 µm and 4C=113.5 µm). Surface detail was reproduced adequately in most of the samples. Conclusion A 0.2% peracetic acid could be used to disinfect zinc oxide eugenol impressions, ozonated water for alginate impressions, and UV radiation for polyether and addition silicone impressions.
PubMed: 38623104
DOI: 10.7759/cureus.55931 -
Environmental Science & Technology Apr 2024The reaction of peracetic acid (PAA) and Fe(II) has recently gained attention due to its utility in wastewater treatment and its role in cloud chemistry. Aerosol-cloud...
The reaction of peracetic acid (PAA) and Fe(II) has recently gained attention due to its utility in wastewater treatment and its role in cloud chemistry. Aerosol-cloud interactions, partly mediated by aqueous hydroxyl radical (OH) chemistry, represent one of the largest uncertainties in the climate system. Ambiguities remain regarding the sources of OH in the cloud droplets. Our research group recently proposed that the dark and light-driven reaction of Fe(II) with peracids may be a key contributor to OH formation, producing a large burst of OH when aerosol particles take up water as they grow to become cloud droplets, in which reactants are consumed within 2 min. In this work, we quantify the OH production from the reaction of Fe(II) and PAA across a range of physical and chemical conditions. We show a strong dependence of OH formation on ultraviolet (UV) wavelength, with maximum OH formation at λ = 304 ± 5 nm, and demonstrate that the OH burst phenomenon is unique to Fe(II) and peracids. Using kinetics modeling and density functional theory calculations, we suggest the reaction proceeds through the formation of an [Fe(II)-(PAA)(HO)] complex, followed by the formation of a Fe(IV) complex, which can also be photoactivated to produce additional OH. Determining the characteristics of OH production from this reaction advances our knowledge of the sources of OH in cloudwater and provides a framework to optimize this reaction for OH output for wastewater treatment purposes.
Topics: Hydroxyl Radical; Aerosols; Peracetic Acid; Light; Kinetics; Iron
PubMed: 38619820
DOI: 10.1021/acs.est.3c10684 -
Journal of Hazardous Materials May 2024Photochemical active species generated from photosensitizers, e.g., dissolved organic matter (DOM), play vital roles in the transformation of micropollutants in water....
Photochemical active species generated from photosensitizers, e.g., dissolved organic matter (DOM), play vital roles in the transformation of micropollutants in water. Here, butanedione (BD), a redox-active moiety in DOM and widely found in nature, was employed to photo-transform naproxen (NPX) with peracetic acid (PAA) and HO as contrasts. The results obtained showed that the BD exhibited more applicable on NPX degradation. It works in the lake or river water under UV and solar irradiation, and its NPX degradation efficiency was 10-30 times faster than that of PAA and HO. The reason for the efficient transformation of pollutants is that the BD system was proved to be a non-free radical dominated mechanism. The quantum yield of BD (Ф) was calculated to be 0.064, which indicates that photophysical process is the dominant mode of BD conversion. By adding trapping agents, direct energy transfer from BD* to NPX (in anoxic environment) or dissolved oxygen (in aerobic environment) was proved to play a major role (> 91 %). Additionally, the BD process reduces the toxicity of NPX and promotes microbial growth after irradiation. Overall, this study significantly deepened the understanding of the transformation between BD and micropollutants, and provided a potential BD-based process for micropollutants removal under solar irradiation.
Topics: Naproxen; Water Pollutants, Chemical; Ultraviolet Rays; Photolysis; Energy Transfer; Hydrogen Peroxide; Peracetic Acid; Photochemical Processes
PubMed: 38608588
DOI: 10.1016/j.jhazmat.2024.134258 -
Environmental Pollution (Barking, Essex... May 2024With the acceleration of air cleaning activities in China, air pollution has entered a new stage characterized by seasonal interplay and predominance of fine particulate...
With the acceleration of air cleaning activities in China, air pollution has entered a new stage characterized by seasonal interplay and predominance of fine particulate matter (PM) and ozone (O) pollutants. However, the differing peak seasons of these two pollution preclude the use of a unified indicator for air pollution complex. Given that peroxyacetyl nitrate (PAN) originates from secondary formation and persists under low-temperature conditions for extended periods, it is vital to determine whether its concentration can be used as an indicator to represent air pollution, not only in summer but also in winter. Here, PAN observational data from 2018 to 2022 for Beijing were analyzed. The results showed that during photochemical pollution events in summer, secondary formation of PAN was intense and highly correlated with O (R = 0.8), while during PM pollution events in winter, when the lifetime of PAN is extended due to the low temperature, the PAN concentration was highly consistent with the PM concentration (R = 0.9). As a result, the PAN concentration essentially exhibited consistency with both the seasonal trends in the exceedance of air pollution (R = 0.6) and the air quality index (R = 0.8). When the daily average concentration exceeds 0.5 and 0.9 ppb, the PAN concentration can be used as a complementary indicator of the occurrence of primary and secondary standard pollution, respectively. This study demonstrated the unique role of PAN as an indicator of air pollution complex, highlighting the comprehensive ability for air quality characterization and reducing the burden of atmospheric environment management.
Topics: Air Pollutants; Air Pollution; Environmental Monitoring; Particulate Matter; Seasons; Ozone; Peracetic Acid; Beijing; China
PubMed: 38580062
DOI: 10.1016/j.envpol.2024.123905 -
Inorganic Chemistry Apr 2024The heme-containing chlorite dismutases catalyze the rapid and efficient decomposition of chlorite (ClO) to yield Cl and O, and the catalytic efficiency of chlorite...
The heme-containing chlorite dismutases catalyze the rapid and efficient decomposition of chlorite (ClO) to yield Cl and O, and the catalytic efficiency of chlorite dismutase from (Cld) in catalyzing the decomposition of bromite (BrO) was dependent on pH, which was supposed to be caused by the conversion of active Cpd I to the inactive Cpd II by proton-coupled electron transfer (PCET) from the pocket Tyr118 to the propionate side chain of heme at high pH. However, the direct evidence of PCET and how the pH affects the efficiency of Cld, as well as whether Cpd II is really inactive, are still poorly understood. Here, on the basis of the high-resolution crystal structures, the computational models in both acidic (pH 5.0) and alkaline (pH 9.0) environments were constructed, and a series of quantum mechanical/molecular mechanical calculations were performed. On the basis of our calculation results, the O-Br bond cleavage of BrO always follows the homolytic mode to generate Cpd II rather than Cpd I. It is different from the O-O cleavage of O/HO or peracetic acid catalyzed by the other heme-containing enzymes. Thus, in the subsequent O-O rebound reaction, it is the Fe(IV)═O in Cpd II that combines with the O-Br radical. Because the porphyrin ring in Cpd II does not bear an unpaired electron, the previously suggested PCET from Tyr118 to the propionate side chain of heme was not theoretically recognized in an alkaline environment. In addition, the O-O rebound step in an alkaline solution corresponds to an energy barrier that is larger than that in an acidic environment, which can well explain the pH dependence of the activity of Cld. In addition, the protonation state of the propionic acid side chains of heme and the surrounding hydrogen bond networks were calculated to have a significant impact on the barriers of the O-O rebound step, which is mainly achieved by affecting the reactivity of the Fe(IV)═O group in Cpd II. In an acidic environment, the relatively weaker coordination of the O2 atom to Fe leads to its higher reactivity toward the O-O rebound reaction. These observations may provide useful information for understanding the catalysis of chlorite dismutases.
Topics: Propionates; Hydrogen Peroxide; Catalysis; Protons; Hydrogen-Ion Concentration; Heme; Chlorides; Oxidoreductases; Betaproteobacteria
PubMed: 38572830
DOI: 10.1021/acs.inorgchem.4c00126 -
Bioresource Technology May 2024Excessive proliferation of algae in water depletes dissolved oxygen, resulting in the demise of aquatic life and environmental damage. This study delves into the...
Excessive proliferation of algae in water depletes dissolved oxygen, resulting in the demise of aquatic life and environmental damage. This study delves into the effectiveness of the dielectric barrier discharge (DBD) plasma activated peracetic acid (PAA) system in deactivating Chlorella. Within 15 min, the algae removal effectiveness reached 89 % under ideal trial conditions. DBD plasma activation of PAA augmented the concentration of reactive species such as ·OH, O, and organic radicals (RO·) in the solution, which are involved in the process of cell inactivation. Reactive oxygen species (ROS) within Chlorella cells continued to rise as a result of treatment-induced damage to the morphological structure and cell membrane of the organism. DNA and chlorophyll-a (Chl-a), were oxidized and destroyed by these invasive active compounds. This study presents an efficient advanced oxidation method to destroy algal cells and adds an alternative strategy for algal control in areas where eutrophication occurs.
Topics: Chlorella; Peracetic Acid; Plasma Gases; Reactive Oxygen Species; Chlorophyll; Chlorophyll A
PubMed: 38570100
DOI: 10.1016/j.biortech.2024.130651 -
Water Research May 2024This study used a simple mechanical ball milling strategy to significantly improve the ability of MnO to activate peracetic acid (PAA) for sustainable and efficient...
This study used a simple mechanical ball milling strategy to significantly improve the ability of MnO to activate peracetic acid (PAA) for sustainable and efficient degradation of organic micropollutant (like bisphenol A, BPA). BPA was successfully removed and detoxified via PAA activation by the bm-MnO within 30 min under neutral environment, with the BPA degradation kinetic rate improved by 3.4 times. Satisfactory BPA removal efficiency can still be achieved over a wide pH range, in actual water and after reuse of bm-MnO for four cycles. The change in hydrophilicity of MnO after ball milling evidently elevated the affinity of MnO for binding to PAA, while the reduction in particle size exposed more active sites contributing partially to catalytic oxidation. Further analysis revealed that BPA oxidation in the ball mill-treated MnO (bm-MnO)/PAA process mainly depends on the bm-MnO-PAA complex (i.e., Mn(III)-OO(O)CCH) mediated non-radical pathway rather than R-O• and Mn(IV). Especially, the existence of the Mn(III)-PAA complex was definitely verified by in situ Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Simultaneously, density functional theory calculations determined that PAA adsorbs readily on manganese sites thereby favoring the formation of Mn(III)-OO(O)CCH complexes. This study advances an in-depth understanding of the underlying mechanisms involved in the manganese oxide-catalyzed activation of PAA for superior non-radical oxidation of micropollutants.
PubMed: 38564895
DOI: 10.1016/j.watres.2024.121486