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Environmental Applications of Catalytic Ozonation
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Environmental Applications of Catalytic Ozonation

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Green Chemistry".

Deadline for manuscript submissions: closed (30 June 2019) | Viewed by 27071

Special Issue Editors

Prof. Dr. Fernando J. Beltrán Novillo

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Guest Editor
Departamento de Ingenieria Química y Química Física, Instituto Universitario de Investigación del Agua, Cambio Climático y Sostenibilidad Universidad de Extremadura, 06187 Badajoz, Spain
Interests: water ozonation; advanced oxidation processes; catalysis engineering; environmental remediation; photocatalysis
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Pedro Modesto Alvarez Pena

E-Mail Website
Guest Editor
Departamento de Ingeniería Química y Química Física, Universidad de Extremadura, Badajoz, Spain
Interests: advanced oxidation processes; catalyst preparation and characterization; water and wastewater treatment technologies
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Ozone, an allotropic form of oxygen, is known to react with organics in water through two reaction mechanisms: selective direct reaction with some organics having specific moieties, and unselective reaction through free radical oxygen species (ROS), mainly hydroxyl radicals, coming from ozone decomposition. In spite of the high reactivity of ozone, its application in water treatment did not take off until the end of the 1970s, when ozone was confirmed as an alternative oxidant to chlorine to reduce the formation of organohalogen compounds during drinking water disinfection. A decade later, research on the combination of ozone and UV radiation or hydrogen peroxide showed ways to increase hydroxyl radical concentrations, giving rise to the appearance of advanced oxidation processes (AOPs). Later, different AOPs have been extensively investigated (Fenton, photocatalytic oxidation, etc.) Among them, catalytic ozonation has attracted interest for water treatment in spite of the costs associated with the generation and dissolution of ozone in water. In fact, in the period 1990–2018, more than 650 works have been published on this subject. At the turn of the century, another ozone-based AOP called the interest of the scientific community: photocatalytic ozonation, or the combination of catalysts, radiation, and ozone. In the period 2005–2018, the literature has reported more than 100 publications on this emerging AOP. In addition to water treatment applications, catalytic ozonation is receiving attention as a method to control volatile organic compounds (VOCs) emissions.

This Special Issue is dedicated to catalytic ozonation processes with the aim to collect findings on aspects related to the synthesis and characterization of catalysts, the removal of organics, the mechanism and kinetics of the processes, the combination of catalytic ozonation with other elements and operations, such as membranes, carbon adsorption, and biological oxidation, the application in the treatment of wastewater, and the control of gaseous emissions.

Prof. Fernando J. Beltrán Novillo
Dr. Pedro M. Álvarez
Guest Editors

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Keywords

  • Ozonation
  • Catalytic ozonation
  • Photocatalytic ozonation
  • Advanced oxidation processes
  • Water and wastewater treatment
  • Air purification
  • Heterogeneous catalysis
  • Reaction kinetics
  • Reaction mechanism

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Published Papers (6 papers)

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Research

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11 pages, 3452 KiB  
Article
Catalytic Ozonation of Organics in Reverse Osmosis Concentrate with Catalysts Based on Activated Carbon
by Xieyang Xu, Zhilin Xia, Laisheng Li, Qi Huang, Can He and Jianbing Wang
Molecules 2019, 24(23), 4365; https://doi.org/10.3390/molecules24234365 - 29 Nov 2019
Cited by 4 | Viewed by 3052
Abstract
Acid-washed activated carbon (AC-A), nitric acid modified activated carbon (AC-NO2), aminated activated carbon (AC-NH2) and cerium-loaded activated carbon (Ce/AC) were prepared and characterized by BET procedure, Boehm titration and SEM. Their performances were investigated for the ozonation of p-chlorobenzoic [...] Read more.
Acid-washed activated carbon (AC-A), nitric acid modified activated carbon (AC-NO2), aminated activated carbon (AC-NH2) and cerium-loaded activated carbon (Ce/AC) were prepared and characterized by BET procedure, Boehm titration and SEM. Their performances were investigated for the ozonation of p-chlorobenzoic acid (p-CBA) in its solution and organic compounds in reverse osmosis concentrate (ROC). Nitration and amination had little effect on the surface area of catalyst, but increased the concentration of surface acid and basic functional group respectively. After loading Ce, the surface area of the catalyst decreased, and amount of Ce particles were agglomerated on the surface of activated carbon. All the four catalysts can improve the removal rate of the organics in water. Among the four catalysts, Ce/AC shows the highest catalytic activity. The removal rates of p-CBA, TOC and three target pollutants (e.g., tetracycline, metoprolol, atrazine) are 99.6%, 70.38%, 97.76%, 96.21% and 96.03%, respectively. Hydroxyl radical (·OH) was proved to be the core of catalytic reaction mechanism for Ce/AC, with the contribution rate to p-CBA removal of 91.4%. The surface groups and the Ce loaded on AC were the initiator for the rapid generation of ·OH. Electron transfer between electron-rich structures and cerium oxide might be a synergistic effect that can increase catalytic activity of Ce loaded on AC. Catalytic ozonation with Ce/AC is a promising ROC treatment technology due to its efficiency and possibilities for improvement. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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21 pages, 6843 KiB  
Article
Removal of Reactive Dyes in Textile Effluents by Catalytic Ozonation Pursuing on-Site Effluent Recycling
by Enling Hu, Songmin Shang and Ka-Lok Chiu
Molecules 2019, 24(15), 2755; https://doi.org/10.3390/molecules24152755 - 29 Jul 2019
Cited by 46 | Viewed by 6408
Abstract
The textile wash-off process consumes substantial amounts of water, which generates large volumes of wastewater that pose potential pollution issues for the environment. In the present study, catalytic ozonation was applied to degrade residual dyes present in rinsing effluents from wash-off processes towards [...] Read more.
The textile wash-off process consumes substantial amounts of water, which generates large volumes of wastewater that pose potential pollution issues for the environment. In the present study, catalytic ozonation was applied to degrade residual dyes present in rinsing effluents from wash-off processes towards the aim of recycling the waste effluents. A magnetic catalyst was prepared for promoting dye degradation by catalytic ozonation. Via a hydrothermal reaction, highly magnetic manganese ferrite (MnFe2O4) particles were successfully loaded on carbon aerogel (CA) materials (MnFe2O4@CA). The results showed that the developed catalyst strikingly promoted the degradation of dye contaminants by catalytic ozonation, in terms of color removal and reduction of chemical oxidation demand (COD) in rinsing effluents. COD removal efficiency in catalytic ozonation was enhanced by 25% when compared with that achieved by ozonation alone under the same treatment conditions. Moreover, we confirmed that after catalytic ozonation, the rinsing effluents could be recycled to replace fresh water without any evident compromise in the color quality of fabrics. The color difference (ΔEcmc(2:1)) between fabrics treated with recycled effluents and water was not more than 1.0, suggesting that the fabrics treated with recycled effluents displayed acceptable color reproducibility. Although colorfastness and color evenness of fabrics treated with recycled effluents were slightly poorer than those of fabrics treated with water, they were still within the acceptable tolerance. Therefore, the present study validated that catalytic ozonation was a promising technology for saving water and wastewater elimination in textile dyeing. It provides a feasibility assessment of catalytic ozonation for recycling waste effluents to reduce water dependence in textile production. Furthermore, we show a new perspective in on-site recycling waste effluents by catalytic ozonation and enrich the knowledge on feasible approaches for water management in textile production. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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14 pages, 3516 KiB  
Article
Optimization of the Electro-Peroxone Process for Micropollutant Abatement Using Chemical Kinetic Approaches
by Huijiao Wang, Lu Su, Shuai Zhu, Wei Zhu, Xia Han, Yi Cheng, Gang Yu and Yujue Wang
Molecules 2019, 24(14), 2638; https://doi.org/10.3390/molecules24142638 - 20 Jul 2019
Cited by 11 | Viewed by 4098
Abstract
The electro-peroxone (E-peroxone) process is an emerging electrocatalytic ozonation process that is enabled by in situ producing hydrogen peroxide (H2O2) from cathodic oxygen reduction during ozonation. The in situ-generated H2O2 can then promote ozone (O3 [...] Read more.
The electro-peroxone (E-peroxone) process is an emerging electrocatalytic ozonation process that is enabled by in situ producing hydrogen peroxide (H2O2) from cathodic oxygen reduction during ozonation. The in situ-generated H2O2 can then promote ozone (O3) transformation to hydroxyl radicals (•OH), and thus enhance the abatement of ozone-refractory pollutants compared to conventional ozonation. In this study, a chemical kinetic model was employed to simulate micropollutant abatement during the E-peroxone treatment of various water matrices (surface water, secondary wastewater effluent, and groundwater). Results show that by following the O3 and •OH exposures during the E-peroxone process, the abatement kinetics of a variety of model micropollutants could be well predicted using the model. In addition, the effect of specific ozone doses on micropollutant abatement efficiencies could be quantitatively evaluated using the model. Therefore, the chemical kinetic model can be used to reveal important information for the design and optimization of the treatment time and ozone doses of the E-peroxone process for cost-effective micropollutant abatement in water and wastewater treatment. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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18 pages, 1929 KiB  
Article
Ozone-Based Advanced Oxidation Processes for Primidone Removal in Water using Simulated Solar Radiation and TiO2 or WO3 as Photocatalyst
by Manuel A. Figueredo, Eva M. Rodríguez, Manuel Checa and Fernando J. Beltran
Molecules 2019, 24(9), 1728; https://doi.org/10.3390/molecules24091728 - 3 May 2019
Cited by 21 | Viewed by 4675
Abstract
In this work, primidone, a high persistent pharmacological drug typically found in urban wastewaters, was degraded by different ozone combined AOPs using TiO2 P25 and commercial WO3 as photocatalyst. The comparison of processes, kinetics, nature of transformation products, and ecotoxicity of [...] Read more.
In this work, primidone, a high persistent pharmacological drug typically found in urban wastewaters, was degraded by different ozone combined AOPs using TiO2 P25 and commercial WO3 as photocatalyst. The comparison of processes, kinetics, nature of transformation products, and ecotoxicity of treated water samples, as well as the influence of the water matrix (ultrapure water or a secondary effluent), is presented and discussed. In presence of ozone, primidone is rapidly eliminated, with hydroxyl radicals being the main species involved. TiO2 was the most active catalyst regardless of the water matrix and the type of solar (global or visible) radiation applied. The synergy between ozone and photocatalysis (photocatalytic ozonation) for TOC removal was more evident at low O3 doses. In spite of having a lower band gap than TiO2 P25, WO3 did not bring any beneficial effects compared to TiO2 P25 regarding PRM and TOC removal. Based on the transformation products identified during ozonation and photocatalytic ozonation of primidone (hydroxyprimidone, phenyl-ethyl-malonamide, and 5-ethyldihydropirimidine-4,6(1H,5H)-dione), a degradation pathway is proposed. The application of the different processes resulted in an environmentally safe effluent for Daphnia magna. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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18 pages, 1989 KiB  
Review
Advances in Treatment of Brominated Hydrocarbons by Heterogeneous Catalytic Ozonation and Bromate Minimization
by Asogan N. Gounden and Sreekantha B. Jonnalagadda
Molecules 2019, 24(19), 3450; https://doi.org/10.3390/molecules24193450 - 23 Sep 2019
Cited by 9 | Viewed by 3860
Abstract
The formation of carcinogenic bromate ions is a constraint when ozone is used for the remediation of water containing brominated organic materials. With its strong oxidizing ability, ozone rapidly transforms bromide in aqueous media to bromate, through a series of reactions involving hydroxyl [...] Read more.
The formation of carcinogenic bromate ions is a constraint when ozone is used for the remediation of water containing brominated organic materials. With its strong oxidizing ability, ozone rapidly transforms bromide in aqueous media to bromate, through a series of reactions involving hydroxyl radicals. Several strategies, such as limiting the ozone concentration, maintaining pH < 6, or the use of ammonia or hydrogen peroxide were explored to minimize bromate generation. However, most of the above strategies had a negative effect on the ozonation efficiency. The advanced oxidation processes, using catalysts together with ozone, have proven to be a promising technology for the degradation of pollutants in wastewater, but very few studies have been conducted to find ways to minimize bromate formation during this approach. The proposed article, therefore, presents a comprehensive review on recent advances in bromate reduction in water by catalytic ozonation and proposes reaction mechanisms associated with the catalytic process. The main aim is to highlight any gaps in the reported studies, thus creating a platform for future research and a quest to find environment friendly and efficacious catalysts for minimizing bromate formation in aqueous media during ozonation of brominated organic compounds. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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30 pages, 572 KiB  
Review
Graphene-Based Catalysts for Ozone Processes to Decontaminate Water
by Fernando J. Beltrán, Pedro M. Álvarez and Olga Gimeno
Molecules 2019, 24(19), 3438; https://doi.org/10.3390/molecules24193438 - 22 Sep 2019
Cited by 25 | Viewed by 4169
Abstract
The use of graphene-based materials as catalysts in both ozone and ozone/radiation processes is creating interest among researchers devoted to the study of advanced oxidation processes (AOPs) for the degradation of organic pollutants in water. In this review, detailed explanations of catalytic and [...] Read more.
The use of graphene-based materials as catalysts in both ozone and ozone/radiation processes is creating interest among researchers devoted to the study of advanced oxidation processes (AOPs) for the degradation of organic pollutants in water. In this review, detailed explanations of catalytic and photocatalytic ozonation processes mediated by graphene-based materials are presented, focusing on aspects related to the preparation and characterization of catalysts, the nature of the water pollutants treated, the type of reactors and radiation sources applied, the influence of the main operating variables, catalyst activity and stability, and kinetics and mechanisms. Full article
(This article belongs to the Special Issue Environmental Applications of Catalytic Ozonation)
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