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Trends in Catalytic Wet Peroxide Oxidation Processes

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A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Environmental Catalysis".

Deadline for manuscript submissions: closed (30 April 2019) | Viewed by 52322

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Prof. Dr. Asuncion Quintanilla

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Guest Editor

Chemical Engineering Department, Universidad Autónoma de Madrid, Campus de Cantoblanco, 28049 Madrid, Spain
Interests: environmental engineering; wastewater treatment; advanced oxidation processes; heterogeneous catalysis; metal-free catalysts; nanomaterials and nanotechnology; 3D-printing; structured catalysts and reactors; kinetics and reactor modeling

Prof. Dr. Macarena Munoz

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Co-Guest Editor

Chemical Engineering Department, Universidad Autónoma de Madrid, Campus de Cantoblanco, 28049 Madrid, Spain
Interests: advanced oxidation processes; catalytic hydrodechlorination; catalytic wet peroxide oxidation; cyanotoxins; design, preparation and characterization of catalysts; environmental engineering; heterogeneous catalysis; magnetic catalysts; microplastics; pollutants of emerging concern; wastewater treatment

Special Issue Information

Dear Colleagues,

This Special Issue aims to report recent advances and future challenges in the field of catalytic wet peroxide oxidation. This technology has shown great potential as an environmentally-friendly and sustainable alternative for water treatment. At present, the main barriers that limit their implementation in practice are associated with the reusability/durability of the catalysts and the cost-efficiency of the process and scale-up. In this context, the subjects that will be preferably covered by this Special Issue are focused on the improvement of CWPO performance seeking for its industrial implementation: (i) the exploration of novel catalysts (nanocatalysts, free-metal and magnetic catalysts), paying special attention to their durability and reusability; (ii) the development of industrial-scale heterogeneous catalysts (robust structured catalysts); (iii) the intensification of CWPO by energetically-assisted approaches with light, microwave, or ultrasound; (iv) the determination of reaction kinetics and mechanisms; (v) the modelling and simulation of reactors; (vi) the application of CWPO to the treatment of real industrial wastewaters, pollutants of emerging concern, and pathogens inactivation (disinfection); (vii) the environmental impact of the process, considering both the aqueous and gas phases; and (viii) the economic evaluation and scale up challenges of CWPO. This Special Issue will preferably include research papers, but sound critical overviews of the state-of-the-art in this field are also welcome. Authors with expertise in CWPO are cordially invited to submit their manuscripts to Catalysts.

Prof. Asuncion Quintanilla
Dr. Macarena Munoz
Guest Editors

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Keywords

catalytic wet peroxide oxidation
design, preparation, and characterization of catalysts
metal-free catalysts
magnetic catalysts
nanocatalysts
structured catalysts
kinetics and reactor engineering
industrial wastewater
pollutants of emerging concern
disinfection
technology scale-up

Published Papers (12 papers)

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Editorial

Jump to: Research, Review

2 pages, 167 KiB

Open AccessEditorial

Editorial Catalysts: Special Issue on Trends in Catalytic Wet Peroxide Oxidation Processes

by Asunción Quintanilla and Macarena Munoz

Catalysts 2019, 9(11), 918; https://doi.org/10.3390/catal9110918 - 04 Nov 2019

Cited by 3 | Viewed by 1530

Abstract

The catalytic wet peroxide oxidation (CWPO) process is an advanced oxidation technology that has shown great potential for the decontamination of wastewater [...] Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

Research

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22 pages, 4562 KiB

Open AccessArticle

Wet Peroxide Oxidation of Chlorobenzenes Catalyzed by Goethite and Promoted by Hydroxylamine

by David Lorenzo, Carmen M. Dominguez, Arturo Romero and Aurora Santos

Catalysts 2019, 9(6), 553; https://doi.org/10.3390/catal9060553 - 20 Jun 2019

Cited by 18 | Viewed by 3705

Abstract

In this work, the abatement of several chlorobenzenes commonly found as pollutants in the aqueous phase has been carried out by catalytic wet peroxide oxidation using goethite as the catalyst and hydroxylamine as the promotor. Spiked water with monochlorobenzene and different positional isomers of dichlorobenzene, trichlorobenzene, and tetrachlorobenzene, at concentrations ranging from 0.4 to 16.9 mg L⁻¹ was treated. Runs were carried out batch-way, at room conditions, without headspace. The heterogeneous catalyst was commercial goethite, with a specific surface area (S_BET) of 10.24 m² g⁻¹ and a total iron content of 57.3 wt%. Iron acts as a catalyst of hydrogen peroxide decomposition to hydroxyl radicals. Hydroxylamine (in a range from 0 to 4.9 mM) was added to enhance the iron redox cycle from Fe (III) to Fe (II), remarkably increasing the radical production rate and therefore, the conversion of chlorobenzenes. Iron was stable (not leached to the aqueous phase) even at the lowest pH tested (pH = 1). The effect of pH (from 2 to 7), hydrogen peroxide (from 1 to 10 times the stoichiometric dosage), hydroxylamine, and catalyst concentration (from 0.25 to 1 g/L) was studied. Pollutant removal increased with hydroxylamine and hydrogen peroxide concentration. An operating conditions study demonstrated that the higher the hydroxylamine and hydrogen peroxide concentrations, the higher the removal of pollutants. The optimal pH value and catalyst concentration was 3 and 0.5 g L⁻¹, respectively. Operating with 2.4 mM of hydroxylamine and 10 times the stoichiometric H₂O₂ amount, a chlorobenzenes conversion of 90% was achieved in 2.5 h. Additionally, no toxic byproducts were obtained. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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14 pages, 4805 KiB

Open AccessArticle

Degradation of Crystal Violet by Catalytic Wet Peroxide Oxidation (CWPO) with Mixed Mn/Cu Oxides

by Ana María Campos, Paula Fernanda Riaño, Diana Lorena Lugo, Jenny Alejandra Barriga, Crispín Astolfo Celis, Sonia Moreno and Alejandro Pérez

Catalysts 2019, 9(6), 530; https://doi.org/10.3390/catal9060530 - 13 Jun 2019

Cited by 16 | Viewed by 3518

Abstract

The environment protection has been the starting point for the development of new technologies, which allow the control of highly toxic substances present in the effluents of various industries, whose removal is not feasible by conventional methods. In this research, mixed oxide catalysts Mn and Cu in different molar ratios were prepared from the autocombustion method and characterized by XRD, XRF, TPR-H₂, and N₂ adsorption–desorption isotherms. The solids were evaluated in the catalytic wet peroxide oxidation of crystal violet (CV) with mild conditions of reaction: 25 °C, normal pressure, airflow of 2 mL/min, and H₂O₂ 0.1 M (2 mL/h). The experimental results indicated degradations of 100% of CV, conversion of the total organic carbon (TOC) of 74%, and elimination of chemical oxygen demand (COD) of 71% in 90 min of reaction. Additionally, the selectivity was monitored by CG-MS, finding that there was almost complete mineralization in a short reaction time, generating intermediate products such as carboxylic acids, alcohols, and amines that do not cause a serious risk to the environment. The Mn–Cu catalyst with molar ratios of 1:2 was the most promising catalyst, displaying a cooperative effect between the two metals, and demonstrating the importance of the redox properties for the elimination of CV dye in wastewater. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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16 pages, 3381 KiB

Open AccessArticle

Condensation By-Products in Wet Peroxide Oxidation: Fouling or Catalytic Promotion? Part II: Activity, Nature and Stability

by Asunción Quintanilla, Jose L. Diaz de Tuesta, Cristina Figueruelo, Macarena Munoz and Jose A. Casas

Catalysts 2019, 9(6), 518; https://doi.org/10.3390/catal9060518 - 11 Jun 2019

Cited by 3 | Viewed by 2437

Abstract

The deposition of condensation by-products onto the catalyst surface upon wet peroxide and wet air oxidation processes has usually been associated with catalyst deactivation. However, in Part I of this paper, it was demonstrated that these carbonaceous deposits actually act as catalytic promoters in the oxygen-assisted wet peroxide oxidation (WPO-O₂) of phenol. Herein, the intrinsic activity, nature and stability of these species have been investigated. To achieve this goal, an up-flow fixed bed reactor packed with porous Al₂O₃ spheres was used to facilitate the deposition of the condensation by-products formed in the liquid phase. It was demonstrated that the condensation by-products catalyzed the decomposition of H₂O₂ and a higher amount of these species leads to a higher degree of oxidation degree The reaction rates, conversion values and intermediates’ distribution were analyzed. The characterization of the carbonaceous deposits on the Al₂O₃ spheres showed a significant amount of condensation by-products (~6 wt.%) after 650 h of time on stream. They are of aromatic nature and present oxygen functional groups consisting of quinones, phenols, aldehydes, carboxylics and ketones. The initial phenol concentration and H₂O₂ dose were found to be crucial variables for the generation and consumption of such species, respectively. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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15 pages, 2801 KiB

Open AccessArticle

Condensation By-Products in Wet Peroxide Oxidation: Fouling or Catalytic Promotion? Part I. Evidences of an Autocatalytic Process

by Asunción Quintanilla, Jose L. Diaz de Tuesta, Cristina Figueruelo, Macarena Munoz and Jose A. Casas

Catalysts 2019, 9(6), 516; https://doi.org/10.3390/catal9060516 - 11 Jun 2019

Cited by 11 | Viewed by 2613

Abstract

The present work is aimed at the understanding of the condensation by-products role in wet peroxide oxidation processes. This study has been carried out in absence of catalyst to isolate the (positive or negative) effect of the condensation by-products on the kinetics of the process, and in presence of oxygen, to enhance the oxidation performance. This process was denoted as oxygen-assisted wet peroxide oxidation (WPO-O₂) and was applied to the treatment of phenol. First, the influence of the reaction operating conditions (i.e., temperature, pH₀, initial phenol concentration, H₂O₂ dose and O₂ pressure) was evaluated. The initial phenol concentration and, overall, the H₂O₂ dose, were identified as the most critical variables for the formation of condensation by-products and thus, for the oxidation performance. Afterwards, a flow reactor packed with inert quartz beads was used to facilitate the deposition of such species and thus, to evaluate their impact on the kinetics of the process. It was found that as the quartz beads were covered by condensation by-products along reaction, the disappearance rates of phenol, total organic carbon (TOC) and H₂O₂ were increased. Consequently, an autocatalytic kinetic model, accounting for the catalytic role of the condensation by products, provides a well description of wet peroxide oxidation performance. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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11 pages, 3006 KiB

Open AccessArticle

Catalytic Degradation of Textile Wastewater Effluent by Peroxide Oxidation Assisted by UV Light Irradiation

by Sarto Sarto, Paesal Paesal, Irine Bellina Tanyong, William Teja Laksmana, Agus Prasetya and Teguh Ariyanto

Catalysts 2019, 9(6), 509; https://doi.org/10.3390/catal9060509 - 04 Jun 2019

Cited by 6 | Viewed by 3847

Abstract

Textile industries produce a complex wastewater which is difficult to be treated. In this work, a catalytic degradation of wastewater effluent composed of sulphur black coloring agent discharged by industry was studied. UV lamp power, peroxide concentration, pH, and iron oxide catalyst were varied to determine the best conditions for oxidative treatment. Kinetic parameters were evaluated based on the reaction model proposed. In the absence of iron oxide catalyst, chemical oxygen demand (COD) and biological oxygen demand (BOD) degradation of up to 80% and 75%, respectively, were observed as resulting from using an H₂O₂ concentration of 0.61 moles/L, UV lamp power of 30 watts, and pH of 6. When using an iron oxide catalyst combined with UV light irradiation, the degradation rate could be increased significantly, while similar final COD and BOD degradation percentages resulted. It is found that the reaction rate order was shifted from first order to second order when using an H₂O₂/UV/Fe₂O₃ system. The results could be an alternative for treating textile industry wastewater, and the parameters obtained can be used for equipment scale-up. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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14 pages, 1851 KiB

Open AccessArticle

Enhanced Degradation of Phenol by a Fenton-Like System (Fe/EDTA/H₂O₂) at Circumneutral pH

by Selamawit Ashagre Messele, Christophe Bengoa, Frank Erich Stüber, Jaume Giralt, Agustí Fortuny, Azael Fabregat and Josep Font

Catalysts 2019, 9(5), 474; https://doi.org/10.3390/catal9050474 - 22 May 2019

Cited by 35 | Viewed by 6973

Abstract

This work deals with the degradation of phenol based on the classical Fenton process, which is enhanced by the presence of chelating agents. Several iron-chelating agents such as ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), diethylenetriamine pentaacetic acid (DTPA), and ethylenediamine-N,N’-diacetic acid (EDDA) were explored, although particular attention was given to EDTA. The effect of the molar ligand to iron ratio, EDTA:Fe, initial pH, and temperature on the oxidation process was studied. The results demonstrate that the proposed alternative approach allows the capacity for degrading phenol to be extended from the usual acidic pH (around 3.0) to circumneutral pH range (6.5–7.5). The overall feasibility of the process depends on the concentration of the chelating agent and the initial pH of the solution. The maximum phenol conversion, over 95%, is achieved using a 0.3 to 1 molar ratio of EDTA:Fe, stoichiometric ratio of H₂O₂ at an initial pH of 7.0, and a temperature of 30 °C after 2 hours of reaction, whereas only 10% of phenol conversion is obtained without EDTA. However, in excess of ligand (EDTA:Fe > 1), the generation of radicals seems to be strongly suppressed. Improvement of the phenol removal efficiency at neutral pH also occurs for the other chelating agents tested. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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14 pages, 3490 KiB

Open AccessEditor’s ChoiceArticle

Activation of Persulfate by Biochars from Valorized Olive Stones for the Degradation of Sulfamethoxazole

by Elena Magioglou, Zacharias Frontistis, John Vakros, Ioannis D. Manariotis and Dionissios Mantzavinos

Catalysts 2019, 9(5), 419; https://doi.org/10.3390/catal9050419 - 03 May 2019

Cited by 53 | Viewed by 5526

Abstract

Biochars from spent olive stones were tested for the degradation of sulfamethoxazole (SMX) in water matrices. Batch degradation experiments were performed using sodium persulfate (SPS) as the source of radicals in the range 250–1500 mg/L, with biochar as the SPS activator in the range 100–300 mg/L and SMX as the model micro-pollutant in the range 250–2000 μg/L. Ultrapure water (UPW), bottled water (BW), and secondary treated wastewater (WW) were employed as the water matrix. Removal of SMX by adsorption only was moderate and favored at acidic conditions, while SPS alone did not practically oxidize SMX. At these conditions, biochar was capable of activating SPS and, consequently, of degrading SMX, with the pseudo-first order rate increasing with increasing biochar and oxidant concentration and decreasing SMX concentration. Experiments in BW or UPW spiked with various anions showed little or no effect on degradation. Similar experiments in WW resulted in a rate reduction of about 30%, and this was attributed to the competitive consumption of reactive radicals by non-target water constituents. Experiments with methanol and t-butanol at excessive concentrations resulted in partial but generally not complete inhibition of degradation; this indicates that, besides the liquid bulk, reactions may also occur close to or on the biochar surface. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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11 pages, 1970 KiB

Open AccessArticle

Solar-Driven Removal of 1,4-Dioxane Using WO₃/nγ-Al₂O₃ Nano-catalyst in Water

by Xiyan Xu, Shuming Liu, Yong Cui, Xiaoting Wang, Kate Smith and Yujue Wang

Catalysts 2019, 9(4), 389; https://doi.org/10.3390/catal9040389 - 25 Apr 2019

Cited by 15 | Viewed by 4031

Abstract

Increasing demand for fresh water in extreme drought regions necessitates potable water reuse. However, current membrane-based water reclamation approaches cannot effectively remove carcinogenic 1,4-dioxane. The current study reports on the solar-driven removal of 1,4-dioxane (50 mg L⁻¹) using a homemade WO₃/nγ-Al₂O₃ nano-catalyst. Characterization methods including scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray fluorescence (XRF) analyses are used to investigate the surface features of the catalyst. The 1,4-dioxane mineralization performance of this catalyst under various reaction conditions is studied. The effect of the catalyst dosage is tested. The mean oxidation state carbon (MOSC) values of the 1,4-dioxane solution are followed during the reaction. The short chain organic acids after treatment are measured. The results showed that over 75% total organic carbon (TOC) removal was achieved in the presence of 300 mg L⁻¹ of the catalyst with a simulated solar irradiation intensity of 40 mW cm⁻². Increasing the dose of the catalyst from 100 to 700 mg L⁻¹ can improve the treatment efficiency to some extent. The TOC reduction curve fits well with an apparent zero-order kinetic model and the corresponding constant rates are within 0.0927 and 0.1059 mg L⁻¹ s⁻¹, respectively. The MOSC values of the 1,4-dioxane solution increase from 1.3 to 3 along the reaction, which is associated with the formation of some short chain acids. The catalyst can be effectively reused 7 times. This work provides an oxidant-free and energy saving approach to achieve efficient removal of 1,4-dioxane and thus shows promising potential for potable reuse applications. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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16 pages, 3649 KiB

Open AccessArticle

Kinetic and Mechanistic Study on Catalytic Decomposition of Hydrogen Peroxide on Carbon-Nanodots/Graphitic Carbon Nitride Composite

by Zhongda Liu, Qiumiao Shen, Chunsun Zhou, Lijuan Fang, Miao Yang and Tao Xia

Catalysts 2018, 8(10), 445; https://doi.org/10.3390/catal8100445 - 11 Oct 2018

Cited by 20 | Viewed by 5065

Abstract

The metal-free CDots/g-C₃N₄ composite, normally used as the photocatalyst in H₂ generation and organic degradation, can also be applied as an environmental catalyst by in-situ production of strong oxidant hydroxyl radical (HO·) via catalytic decomposition of hydrogen peroxide (H₂O₂) without light irradiation. In this work, CDots/g-C₃N₄ composite was synthesized via an electrochemical method preparing CDots followed by the thermal polymerization of urea. Transmission electron microscopy (TEM), X-Ray diffraction (XRD), Fourier Transform Infrared (FTIR), N₂ adsorption/desorption isotherm and pore width distribution were carried out for characterization. The intrinsic catalytic performance, including kinetics and thermodynamic, was studied in terms of catalytic decomposition of H₂O₂ without light irradiation. The second-order rate constant of the reaction was calculated to be (1.42 ± 0.07) × 10⁻⁹ m·s⁻¹ and the activation energy was calculated to be (29.05 ± 0.80) kJ·mol⁻¹. Tris(hydroxymethyl) aminomethane (Tris) was selected to probe the produced HO· during the decomposing of H₂O₂ as well as to buffer the pH of the solution. The composite was shown to be base-catalyzed and the optimal performance was achieved at pH 8.0. A detailed mechanism involving the adsorb-catalyze double reaction site was proposed. Overall, CDots/g-C₃N₄ composite can be further applied in advanced oxidation technology in the presence of H₂O₂ and the instinct dynamics and the mechanism can be referred to further applications in related fields. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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Review

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33 pages, 5611 KiB

Open AccessReview

Wastewater Treatment by Catalytic Wet Peroxidation Using Nano Gold-Based Catalysts: A Review

by Carmen S.D. Rodrigues, Ricardo M. Silva, Sónia A.C. Carabineiro, F.J. Maldonado-Hódar and Luís M. Madeira

Catalysts 2019, 9(5), 478; https://doi.org/10.3390/catal9050478 - 23 May 2019

Cited by 16 | Viewed by 4631

Abstract

Nowadays, there is an increasing interest in the development of promising, efficient, and environmentally friendly wastewater treatment technologies. Among them are the advanced oxidation processes (AOPs), in particular, catalytic wet peroxidation (CWPO), assisted or not by radiation. One of the challenges for the industrial application of this process is the development of stable and efficient catalysts, without leaching of the metal to the aqueous phase during the treatment. Gold catalysts, in particular, have attracted much attention from researchers because they show these characteristics. Recently, numerous studies have been reported in the literature regarding the preparation of gold catalysts supported on various supports and testing their catalytic performance in the treatment of real wastewaters or model pollutants by CWPO. This review summarizes this research; the properties of such catalysts and their expected effects on the overall efficiency of the CWPO process, together with a description of the effect of operational variables (such as pH, temperature, oxidant concentration, catalyst, and gold content). In addition, an overview is given of the main technical issues of this process aiming at its industrial application, namely the possibility of using the catalyst in continuous flow reactors. Such considerations will provide useful information for a faster and more effective analysis and optimization of the CWPO process. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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18 pages, 2651 KiB

Open AccessReview

Application of Catalytic Wet Peroxide Oxidation for Industrial and Urban Wastewater Treatment: A Review

by Juan José Rueda Márquez, Irina Levchuk and Mika Sillanpää

Catalysts 2018, 8(12), 673; https://doi.org/10.3390/catal8120673 - 19 Dec 2018

Cited by 66 | Viewed by 7171

Abstract

Catalytic wet peroxide oxidation (CWPO) is emerging as an advanced oxidation process (AOP) of significant promise, which is mainly due to its efficiency for the decomposition of recalcitrant organic compounds in industrial and urban wastewaters and relatively low operating costs. In current study, we have systemised and critically discussed the feasibility of CWPO for industrial and urban wastewater treatment. More specifically, types of catalysts the effect of pH, temperature, and hydrogen peroxide concentrations on the efficiency of CWPO were taken into consideration. The operating and maintenance costs of CWPO applied to wastewater treatment and toxicity assessment were also discussed. Knowledge gaps were identified and summarised. The main conclusions of this work are: (i) catalyst leaching and deactivation is one of the main problematic issues; (ii) majority of studies were performed in semi-batch and batch reactors, while continuous fixed bed reactors were not extensively studied for treatment of real wastewaters; (iii) toxicity of wastewaters treated by CWPO is of key importance for possible application, however it was not studied thoroughly; and, (iv) CWPO can be regarded as economically viable for wastewater treatment, especially when conducted at ambient temperature and natural pH of wastewater. Full article

(This article belongs to the Special Issue Trends in Catalytic Wet Peroxide Oxidation Processes)

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