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Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Environmental Nanoscience and Nanotechnology".

Deadline for manuscript submissions: closed (15 September 2022) | Viewed by 32268

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Prof. Dr. Joaquim Esteves Da Silva

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Chemistry Research Unit (CIQUP), Institute of Molecular Sciences (IMS), Department of Geosciences, Environment and Spatial Plannings, Faculty of Sciences, University of Porto (FCUP), Rua do Campo Alegre s/n, 4169-007 Porto, Portugal
Interests: environmental sciences; soil physical chemistry; climate change
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Special Issue Information

Dear Colleagues,

Water quality is a leading currently environmental concern enrolled on priority environmental agendas. Water used for humans, animals and agriculture will only have enough quality if superficial and groundwater is not contaminated from untreated sewages discharges. One common pollutant family in the water are the dyes resulting from several industrial activities, mainly from textiles. Indeed, textile industries are responsible for this global environmental problem due to the high amount of dyes present in sewages and to the difficulty in their degradation. Advanced oxidation processes (AOP) are being used for the treatment of dye contaminated sewages. Moreover, AOP are being coupled to nanomaterials in order to increase the degradation yields.

Accordingly to the nanomaterials properties, they have a role on the dye degradation by adsorption, photocatalysis, chemical and biological treatment. Besides carbonaceous and titanium dioxide and lanthanum and bismuth titanates, many other nanomaterials and their modifications are being proposed for water remediation.

This Special Issue of Nanomaterials aims to cover the most recent advances in nanomaterials designed to be used in dye degradation in water or in the coupling of nanomaterials with AOP of water contaminated with dyes.

Prof. Dr. Joaquim Esteves da Silva
Guest Editor

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Keywords

Textile dyes
Textiles sewage
Water remediation
Titanium dioxide
Metal oxides nanomaterials
Carbonaceous nanomaterials
Photocalyst nanomaterials
Adsorbent nanomaterials
Catalyst nanomaterials
Upconversion nanomaterials

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Published Papers (9 papers)

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Research

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15 pages, 2401 KiB

Open AccessArticle

Oxygen Vacancy-Mediated Activates Oxygen to Produce Reactive Oxygen Species (ROS) on Ce-Modified Activated Clay for Degradation of Organic Compounds without Hydrogen Peroxide in Strong Acid

by Tianming Wu, Jing Cui, Changjiang Wang, Gong Zhang, Limin Li, Yue Qu and Yusheng Niu

Nanomaterials 2022, 12(24), 4410; https://doi.org/10.3390/nano12244410 - 10 Dec 2022

Cited by 10 | Viewed by 2594

Abstract

The treatment of acid wastewater to remove organic matter in acid wastewater and recycle valuable resources has great significance. However, the classical advanced oxidation process (AOPs), such as the Fenton reaction, encountered a bottleneck under the conditions of strong acid. Herein, making use of the oxidation properties of CeAY (CeO₂@acid clay), we built an AOPs reaction system without H₂O₂ under a strong acid condition that can realize the transformation of organic matter in industrial wastewater. The X-ray photoelectron spectroscopy (XPS) proved that the CeAY based on Ce³⁺ as an active center has abundant oxygen vacancies, which can catalyze O₂ to produce reactive oxygen species (ROS). Based on the electron spin-resonance spectroscopy spectrum and radical trapping experiments, the production of •O₂^– and •OH can be determined, which are the essential factors of the degradation of organic compounds. In the system of pH = 1.0, when 1 mg CeAY is added to 10 mL of wastewater, the degradation efficiency of an aniline solution with a 5 mg/L effluent concentration is 100%, and that of a benzoic acid solution with a 100 mg/L effluent concentration is 50% after 10 min of reaction. This work may provide novel insights into the removal of organic pollutants in a strong acid water matrix. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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15 pages, 4390 KiB

Open AccessArticle

UV-Based Advanced Oxidation Processes of Remazol Brilliant Blue R Dye Catalyzed by Carbon Dots

by Inês M. F. Cardoso, Rita M. F. Cardoso, Luís Pinto da Silva and Joaquim C. G. Esteves da Silva

Nanomaterials 2022, 12(12), 2116; https://doi.org/10.3390/nano12122116 - 20 Jun 2022

Cited by 10 | Viewed by 2785

Abstract

UV-based advanced oxidation processes (AOPs) (UV/H₂O₂ and UV/S₂O₈²⁻) with a titanium(IV)-doped carbon dot, TiP-CD, as a catalyst were developed for the decomposition of Remazol Brilliant Blue R (Reactive Blue 19), an anthraquinone textile dye (at T = 25 °C and pH = 7). The Ti-CD, with marked catalytic UV properties, was successfully synthesized by the one-pot hydrothermal procedure, using L-cysteine as carbon precursor, ethylenediamine as nitrogen source, PEG (polyethylene glycol) as a capping agent, and titanium(IV) isopropoxide (precursor of TiO₂ doping). Contrary to azo dyes (methyl orange, orange II sodium salt, and reactive black 5), which achieved complete degradation in a time interval less than 30 min in the developed AOP systems (UV/H₂O₂, UV/S₂O₈²⁻, and UV/TiO₂), the RBB-R showed relatively low degradation rates and low discoloration rate constants. In the presence of the catalyzer, the reaction rate significantly increased, and the pseudo-first-order rate constants for the RBB-R discoloration were UV/3.0 mM H₂O₂/TIP-CD-0.0330 min⁻¹ and UV/1.02 mM S₂O₈²⁻/TIP-CD-0.0345 min⁻¹. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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16 pages, 4528 KiB

Open AccessArticle

Mesoporous Nano-Sized BiFeVOx.y Phases for Removal of Organic Dyes from Wastewaters by Visible Light Photocatalytic Degradation

by Niyazi A. S. Al-Areqi, Muhamad Umair, Ahmed M. Senan, Ahlam Al-Alas, Afraah M. A. Alfaatesh, Saba Beg, Kashif-ur-Rehman Khan, Sameh A. Korma, Mohamed T. El-Saadony, Mohammed A. Alshehri, Ahmed Ezzat Ahmed, Ahmed M. Abbas, Riyad A. Alokab and Ilaria Cacciotti

Nanomaterials 2022, 12(8), 1383; https://doi.org/10.3390/nano12081383 - 18 Apr 2022

Cited by 4 | Viewed by 2453

Abstract

With an increasing demand for industrial dyes in our daily lives, water conditions have become worse. Recently, the removal of such environmentally hazardous pollutants from wastewaters through photocatalytic degradation has been drawing increased attention. Three mesoporous nanophases of BiFeVOx.y as (Bi₂Fe^IIIV_1−yO_5.5−y) visible light photocatalysts were synthesized in this study using ethylene glycol-citrate sol-gel synthesis combined with microwave- assisted calcination. X-ray diffraction (XRD), differential thermal analysis (DTA), FTIR spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy coupled with energy dispersive X-ray spectrometry (SEM-EDS), nitrogen adsorption-desorption isotherms, and UV-Vis diffuse reflectance spectrophotometry (UV-Vis/DRS) were used to characterize the BiFeVOx.y photocatalysts. The visible light-induced photocatalytic activities of the BiFeVOx.y phases were evaluated by the degradation of methylene blue (MB) dye in aqueous solution at pH ~10.0. The results of this study show that the combination of doping strategy with the utilization of advanced synthesis methods plays an important role in improving the structure and surface properties of BiFeVOx.y phases, and thereby enhancing their adsorption and photocatalytic efficiencies. The synthesized mesoporous tetragonal γ-BiFeVOx.y nanophase has been proven to be a potential visible-light photocatalyst for the degradation of organic dyes. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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17 pages, 3796 KiB

Open AccessArticle

Copper(II)-Doped Carbon Dots as Catalyst for Ozone Degradation of Textile Dyes

by Rita M. F. Cardoso, Inês M. F. Cardoso, Luís Pinto da Silva and Joaquim C. G. Esteves da Silva

Nanomaterials 2022, 12(7), 1211; https://doi.org/10.3390/nano12071211 - 4 Apr 2022

Cited by 23 | Viewed by 3451

Abstract

A catalytic ozonation advanced oxidation process (AOP) with a copper(II)-doped carbon dot as catalyst, Cu-CD (using L-cysteine and polyethylene glycol (PEG) as precursors and passivation agents), was developed for textile wastewater treatment (T = 25 °C and pH = 7). Four dyes were analyzed—Methyl Orange (MO), Orange II sodium salt (O-II), Reactive Black 5 (RB-5) and Remazol Brilliant Blue R (RBB-R), as well as a real effluent from the dying and printing industry. The Cu-CD, with marked catalytic ozonation properties, was successfully synthesized by one-pot hydrothermal procedure with a size of 4.0 nm, a charge of −3.7 mV and a fluorescent quantum yield of 31%. The discoloration of the aqueous dye solutions followed an apparent first-order kinetics with the following rate constants (k_ap in min⁻¹): MO, 0.210; O-II, 0.133; RB-5, 0.177; RBB-R, 0.086. In the presence of Cu-CD, the following apparent first-order rate constants were obtained (k_ap^c in min⁻¹) with the corresponding increase in the rate constant without catalyst (%Inc): MO, 1.184 (464%); O-II, 1.002 (653%); RB-5, 0.709 (301%); RBB-R, 0.230 (167%). The presence of sodium chloride (at a concentration of 50 g/L) resulted in a marked increase of the discoloration rate of the dye solution due to generation of other radicals, such as chlorine and chlorine oxide, resulting from the reaction of ozone and chloride. Taking into consideration that the real textile effluent under research has a high carbonate concentration (>356 mg/L), which inhibits ozone decomposition, the discoloration first-order rate constants without and with Cu-CD (k_ap = 0.0097 min⁻¹ and k_ap^c = 0.012 min⁻¹ (%Inc = 24%), respectively) were relatively small. Apparently, the Cu-CD, the surface of which is covered by a soft and highly hydrated caramelized PEG coating, accelerates the ozone decomposition and dye adsorption, increasing its degradation. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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16 pages, 3978 KiB

Open AccessArticle

Physicochemical and Photocatalytic Properties under Visible Light of ZnO-Bentonite/Chitosan Hybrid-Biocompositefor Water Remediation

by Imane Aadnan, Omar Zegaoui, Abderrahim El Mragui and Joaquim Carlos Gomes Esteves da Silva

Nanomaterials 2022, 12(1), 102; https://doi.org/10.3390/nano12010102 - 29 Dec 2021

Cited by 15 | Viewed by 2294

Abstract

In this investigation, a hybrid-biocomposite “ZnO-Bentonite/Chitosan” was synthesized using inexpensive and environmentally friendly materials (Bentonitechitosan) and (ZnO). It was used as a photocatalyst for water remediation. The structural, optical, thermal, and morphological properties of the synthesized hybrid-biocomposite were investigated using XRD, FTIR spectroscopy, UV-vis diffuse reflectance spectroscopy, TGA, XPS, and SEM-EDS. The thermal measurements showed that the decomposition of CS was postponed progressively by adding PB and ZnO, and the thermal stability of the synthesized hybrid-biocomposite was improved. The characterization results highlighted strong interactions between the C–O, C=O, -NH₂, and OH groups of chitosan and the alumina-silica sheets of bentonite on the one side, and between the functional groups of chitosan (-NH₂, OH) and ZnO on the other side. The photocatalytic efficiency of the prepared hybrid-biocomposite was assessed in the presence of Methyl Orange (MO). The experiments carried out in the dark showed that the MO removal increased in the presence of Zn-PB/CS hybrid-biocomposite (86.1%) by comparison with PB (75.8%) and CS (65.4%) materials. The photocatalytic experiments carried out under visible light showed that the MO removal increased 268 times in the presence of Zn-PB/CS by comparison withZnO.The holes trapping experiments indicated that they are the main oxidative active species involved in the MO degradation under both UV-A and visible light irradiations. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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14 pages, 4283 KiB

Open AccessArticle

Facile Synthesis of Carbon- and Nitrogen-Doped Iron Borate as a Highly Efficient Single-Component Heterogeneous Photo-Fenton Catalyst under Simulated Solar Irradiation

by Shan-Yuan Hsiao, En-Xuan Lin and Pei-Yuin Keng

Nanomaterials 2021, 11(11), 2853; https://doi.org/10.3390/nano11112853 - 26 Oct 2021

Cited by 6 | Viewed by 2697

Abstract

The development of a heterogeneous catalyst for use in environmental remediation remains a challenging and attractive research endeavor. Specifically, for Fenton reactions, most research approaches have focused on the preparation of iron-containing heterostructures as photo-Fenton catalysts that utilize visible light for enhancing the degradation efficiency. Herein, the synthesis and novel application of C,N-doped iron borates are demonstrated as single-component heterogeneous photo-Fenton catalysts with high Fenton activity under visible light. Under the optimal conditions, 10 mg of the catalyst is shown to achieve effective degradation of 10 ppm methylene blue (MB) dye, Rhodamine B (RhB) dye, and tetracycline (TC) under simulated solar irradiation with a first-order rate constant of k = 0.218 min⁻¹, 0.177 min⁻¹, and 0.116 min⁻¹, respectively. Using MB as a model system, the C,N-doped iron borate exhibits 10- and 26-fold increases in catalytic activity relative to that of the 50 nm hematite nanoparticles and that of the non-doped iron borate, respectively, in the presence of H₂O₂ under the simulated solar irradiation. Furthermore, the optimum reaction conditions used only 320 equivalents of H₂O₂ with respect to the concentration of dye, rather than the several thousand equivalents of H₂O₂ used in conventional heterogeneous Fenton catalysts. In addition, the as-prepared C,N-doped iron borate achieves 75% MB degradation after 20 min in the dark, thus enabling the continuous degradation of pollutants at night and in areas with poor light exposure. The stability and recyclability of C,N-doped iron borate for the oxidation of MB was demonstrated over three cycles with insignificant loss in photo-Fenton activity. The high Fenton activity of the C,N-doped iron borate is considered to be due to the synergistic action between the negatively-charged borate ligands and the metal center in promoting the Fenton reaction. Moreover, carbon and nitrogen doping are shown to be critical in modifying the electronic structure and increasing the conductivity of the catalyst. In view of its synthetic simplicity, high efficiency, low cost of reagents, and minimal cost of operation (driven by natural sunlight), the as-prepared heterogeneous single-component metal borate catalyst has potential application in the industrial treatment of wastewater. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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20 pages, 5401 KiB

Open AccessArticle

Synthesis of Fe₃O₄@mZrO₂-Re (Re = Y/La/Ce) by Using Uniform Design, Surface Response Methodology, and Orthogonal Design & Its Application for As³⁺ and As⁵⁺ Removal

by Easar Alam, Qiyan Feng, Hong Yang, Jiaxi Fan, Sameena Mumtaz and Farida Begum

Nanomaterials 2021, 11(9), 2177; https://doi.org/10.3390/nano11092177 - 25 Aug 2021

Cited by 6 | Viewed by 2856

Abstract

In this study, iron oxide (Fe₃O₄) was coated with ZrO₂, and doped with three rare earth elements((Y/La/Ce), and a multi-staged rare earth doped zirconia adsorbent was prepared by using uniform design U₁₄, Response Surface methodology, and orthogonal design, to remove As³⁺ and As⁵⁺ from the aqueous solution. Based on the results of TEM, EDS, XRD, FTIR, and N₂-adsorption desorption test, the best molar ratio of Fe₃O₄:TMAOH:Zirconium butoxide:Y:La:Ce was selected as 1:12:11:1:0.02:0.08. The specific surface area and porosity was 263 m²/g, and 0.156 cm³/g, respectively. The isothermal curves and fitting equation parameters show that Langmuir model, and Redlich Peterson model fitted well. As per calculations of the Langmuir model, the highest adsorption capacities for As³⁺ and As⁵⁺ ions were recorded as 68.33 mg/g, 84.23 mg/g, respectively. The fitting curves and equations of the kinetic models favors the quasi second order kinetic model. Material regeneration was very effective, and even in the last cycle the regeneration capacities of both As³⁺ and As⁵⁺ were 75.15%, and 77.59%, respectively. Adsorption and regeneration results suggest that adsorbent has easy synthesis method, and reusable, so it can be used as a potential adsorbent for the removal of arsenic from aqueous solution. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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Review

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28 pages, 3393 KiB

Open AccessReview

Challenges and Recent Advances in Enzyme-Mediated Wastewater Remediation—A Review

by Khadega A. Al-Maqdi, Nada Elmerhi, Khawlah Athamneh, Muhammad Bilal, Ahmed Alzamly, Syed Salman Ashraf and Iltaf Shah

Nanomaterials 2021, 11(11), 3124; https://doi.org/10.3390/nano11113124 - 19 Nov 2021

Cited by 53 | Viewed by 5809

Abstract

Different classes of artificial pollutants, collectively called emerging pollutants, are detected in various water bodies, including lakes, rivers, and seas. Multiple studies have shown the devastating effects these emerging pollutants can have on human and aquatic life. The main reason for these emerging pollutants in the aquatic environment is their incomplete removal in the existing wastewater treatment plants (WWTPs). Several additional treatments that could potentially supplement existing WWTPs to eliminate these pollutants include a range of physicochemical and biological methods. The use of enzymes, specifically, oxidoreductases, are increasingly being studied for their ability to degrade different classes of organic compounds. These enzymes have been immobilized on different supports to promote their adoption as a cost-effective and recyclable remediation approach. Unfortunately, some of these techniques have shown a negative effect on the enzyme, including denaturation and loss of catalytic activity. This review focuses on the major challenges facing researchers working on the immobilization of peroxidases and the recent progress that has been made in this area. It focuses on four major areas: (1) stability of enzymes upon immobilization, enzyme engineering, and evolution; (2) recyclability and reusability, including immobilization on membranes and solid supports; (3) cost associated with enzyme-based remediation; and (4) scaling-up and bioreactors. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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13 pages, 320 KiB

Open AccessEditor’s ChoiceReview

Advanced Oxidation Processes Coupled with Nanomaterials for Water Treatment

by Inês M. F. Cardoso, Rita M. F. Cardoso and Joaquim C. G. Esteves da Silva

Nanomaterials 2021, 11(8), 2045; https://doi.org/10.3390/nano11082045 - 11 Aug 2021

Cited by 75 | Viewed by 5828

Abstract

Water quality management will be a priority issue in the near future. Indeed, due to scarcity and/or contamination of the water, regulatory frameworks will be increasingly strict to reduce environmental impacts of wastewater and to allow water to be reused. Moreover, drinking water quality standards must be improved in order to account for the emerging pollutants that are being detected in tap water. These tasks can only be achieved if new improved and sustainable water treatment technologies are developed. Nanomaterials are improving the ongoing research on advanced oxidation processes (AOPs). This work reviews the most important AOPs, namely: persulfate, chlorine and NH₂Cl based processes, UV/H₂O₂, Fenton processes, ozone, and heterogeneous photocatalytic processes. A critical review of the current coupling of nanomaterials to some of these AOPs is presented. Besides the active role of the nanomaterials in the degradation of water contaminants/pollutants in the AOPs, the relevance of their adsorbent/absorbent function in these processes is also discussed. Full article

(This article belongs to the Special Issue Development of Nanomaterials for Advanced Oxidation Processes of Dye Degradation and Water Remediation)

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