Sustainable Green Nanotechnologies for Innovative Purifications of Water

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

Deadline for manuscript submissions: closed (31 March 2023) | Viewed by 9901

Special Issue Editors

Department of Chemistry, Biochemistry and Environmental Protection, University of Novi Sad Faculty of Sciences, 21000 Novi Sad, Serbia
Interests: environmental chemistry; advanced oxidation processes; photocatalytic decomposition; emerging organic pollutants; wastewater purification; kinetic methods of analysis; nanoparticles; semiconductors
Department of Food Technology, University North, 48000 Koprivnica, Croatia
Interests: general statistics; research methodology; experimental design; mathematical modeling; multivariate analysis; novel food processing and extraction technologies
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Protecting aquatic ecosystems from pollution and hydromorphological changes and preserving the sustainability of water is crucial for current and future generations, as well as for maintaining political stability at any level. In general, a comprehensive water policy aims at ensuring that a sufficient quantity of good-quality water is available for both human needs and the environment, through regulating the main sources of pollution (e.g., from agriculture, industry, urban wastewaters), water usages (surface, groundwater, and drinking water), and integrated water management. The current priority is to find innovative solutions for the development of cost-effective, economically feasible, and sustainable environmentally friendly technologies for purifications of water.

This Special Issue focuses on advances in semiconductor materials (powders, ceramics, glass ceramics, thin films) processing, characterization, and their multidisciplinary applications. Especially welcomed are papers with a focus on sustainable green nanotechnology, synthesis of semiconductor materials from plant extracts, various precursors, and doping agents (based on non-metals, transition metals) for the removal of (emerging) organic pollutants (e.g., pesticides, pharmaceuticals, dyes from ultrapure, drinking, surface, ground, and wastewaters). This includes the application of “reagent-free, waste-free” advanced oxidation processes (AOPs). Topics regarding individual, as well as additive and synergistic effects obtained by operating hybrid AOPs (including photocatalysis, subcritical water treatments, ultrasound, plasma-based AOP, (photo)-Fenton, catalytic ozonation) are also welcomed.

Articles presented in this Special Issue will cover various topics, ranging from the synthesis and characterization of semiconductors (metal oxides, metal chalcogenides, metal–organic frameworks) to their specific applications of which foremost is the progress in photocatalysis, subcritical water treatments, and advanced oxidation processes in general. Additionally, of particular interest are applications of optical sensor systems as broad indicators of water quality during different treatments.

Prof. Dr. Daniela Šojić Merkulov
Dr. Predrag Putnik
Guest Editors

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Keywords

  • Green nanotechnologies
  • Metal oxides, metal chalcogenides, metal–organic frameworks
  • Synthesis and characterization of semiconductor materials
  • Powders, ceramics, glass ceramics, thin films
  • Environmental remediation
  • Advanced oxidation processes
  • Photocatalysis
  • Subcritical water treatment
  • Ultrasound
  • Plasma-based AOP
  • (Photo)-Fenton
  • Catalytic ozonation
  • Hybrid AOPs
  • Adsorption
  • Sensing
  • Optical sensor
  • Localized surface plasmon resonance

Published Papers (6 papers)

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Research

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15 pages, 2537 KiB  
Article
Exceptional Sorption of Heavy Metals from Natural Water by Halloysite Particles: A New Prospect of Highly Efficient Water Remediation
by Michał Stor, Kamil Czelej, Andrzej Krasiński and Leon Gradoń
Nanomaterials 2023, 13(7), 1162; https://0-doi-org.brum.beds.ac.uk/10.3390/nano13071162 - 24 Mar 2023
Cited by 4 | Viewed by 1279
Abstract
Halloysite particles, with their unique multilayer nanostructure, are demonstrated here as highly efficient and readily available sorbent of heavy metals that can be easily scaled up and used in large-scale water remediation facilities. The various methods of raw material purification were applied, and [...] Read more.
Halloysite particles, with their unique multilayer nanostructure, are demonstrated here as highly efficient and readily available sorbent of heavy metals that can be easily scaled up and used in large-scale water remediation facilities. The various methods of raw material purification were applied, and their effects were verified using techniques such as BET isotherm (determination of specific surface area and size of pores), XRF analysis (composition), and SEM imaging (determination of morphology). A series of adsorption experiments for aqueous solutions of metal ions (i.e., lead, cadmium) were carried out to quantify the sorption capacity of halloysite particles for selected heavy metals. The ability of adequately activated halloysite to efficiently remove heavy metal ions from water solutions was confirmed. The value of the zeta potential of raw and purified halloysite particles in water was determined. This enables us to understand its importance for the sorption of positively charged ions (metal, organics) at various pH values. The adsorption process conducted in the pH range of 6.0–6.5 showed significant improvement compared to the acidic conditions (pH value 3.0–3.5) and resulted in a high sorption capacity of lead ions—above 24.3 mg/g for the sulphuric acid-treated sample. The atomic scale ab initio calculations revealed a significant difference in adsorption energy between the external siloxane surface and cross-sectional interlayer surface, resulting in pronounced adsorption anisotropy. A low energy barrier was calculated for the interlayer migration of heavy metals into the halloysite interior, facilitating access to the active sites in these regions, thus significantly increasing the sorption capacity and kinetics. DFT (density functional theory) calculations supporting this study allowed for predicting the sorption potential of pure halloysite structure towards heavy metals. To confront it with experimental results, it was crucial to determine proper purification conditions to obtain such a developed structure from the mineral ore. The results show a massive increase in the BET area and confirm a high sorption potential of modified halloysite towards heavy metals. Full article
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17 pages, 3342 KiB  
Article
Reusable Fe2O3/TiO2/PVC Photocatalysts for the Removal of Methylene Blue in the Presence of Simulated Solar Radiation
by Ivana Jagodić, Imre Guth, Svetlana Lukić-Petrović, Dragana Tamindžija, Daniela Šojić Merkulov, Nina Finčur, Szabolcs Bognár, Predrag Putnik and Nemanja Banić
Nanomaterials 2023, 13(3), 460; https://0-doi-org.brum.beds.ac.uk/10.3390/nano13030460 - 23 Jan 2023
Cited by 2 | Viewed by 1521
Abstract
Currently, environmental pollution by various organic pollutants (e.g., organic dyes) is a serious, emerging global issue. The aqueous environment is highly exposed to the harmful effects of these organic compounds. Furthermore, the commonly applied conventional purification techniques are not sufficient enough. Heterogeneous photocatalysis [...] Read more.
Currently, environmental pollution by various organic pollutants (e.g., organic dyes) is a serious, emerging global issue. The aqueous environment is highly exposed to the harmful effects of these organic compounds. Furthermore, the commonly applied conventional purification techniques are not sufficient enough. Heterogeneous photocatalysis and the photo-Fenton process are effective, low-cost and green alternatives for the removal of organic pollutants. In this study, different iron(III) oxide/titanium(IV) oxide/polyvinyl chloride (Fe2O3/TiO2/PVC) nanocomposites in tablet form were investigated in the photodegradation of methylene blue (MB) under simulated sunlight, and their possible antibacterial effects were examined. The newly synthesized nanocomposites were characterized by scanning electron microscope, X-ray diffraction, UV–Vis diffuse reflectance spectroscopy, and Raman spectroscopy. The results showed a hematite crystal form in the case of Fe2O3(2) and Fe2O3 samples, while the Fe2O3(1) sample showed a combination of hematite and synthetic mineral akaganeite. The highest photocatalytic efficiency was achieved in the presence of Fe2O3/TiO2/PVC, when 70.6% of MB was removed. In addition, the possible photo-cleaning and reuse of the mentioned photocatalyst was also examined. Based on the results, it can be seen that the activity did not decrease after five successive runs. Nanocomposites also exhibited mild antibacterial effects against the two tested Gram-positive bacteria (S. aureus and B. cereus). Full article
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22 pages, 2451 KiB  
Article
Sustainable Removal of Tolperisone from Waters by Application of Photocatalysis, Nanotechnology, and Chemometrics: Quantification, Environmental Toxicity, and Degradation Optimization
by Szabolcs Bognár, Predrag Putnik, Ivana Maksimović, Branko Velebit, Marina Putnik-Delić and Daniela Šojić Merkulov
Nanomaterials 2022, 12(23), 4199; https://0-doi-org.brum.beds.ac.uk/10.3390/nano12234199 - 25 Nov 2022
Cited by 3 | Viewed by 1117
Abstract
Environmental pollution is an emerging global issue. Heterogenous photocatalytic degradation, which belongs to the advanced oxidation processes, is a promising sustainable technique for the removal of harmful pollutants (e.g., pharmaceuticals) from natural resources (surface and underground waters), as well as wastewaters. In our [...] Read more.
Environmental pollution is an emerging global issue. Heterogenous photocatalytic degradation, which belongs to the advanced oxidation processes, is a promising sustainable technique for the removal of harmful pollutants (e.g., pharmaceuticals) from natural resources (surface and underground waters), as well as wastewaters. In our study, we examined the efficiency of photocatalytic degradation (with TiO2 and ZnO as photocatalysts) of tolperisone hydrochloride (TLP) and the effect of TLP and its degradation intermediates on germination, photosynthetic capacity, and biomass production of wheat. According to the UFLC-DAD and LC–ESI–MS results, we found that the complete degradation of TLP can be reached after 60.83 min of UV irradiation using TiO2 as a photocatalyst. Furthermore, we determined that germination, biomass production, and chlorophyll b (Chl b) were not related to the percentage of TLP after irradiation. Chlorophyll a (Chl a) (r = −0.61, p ≤ 0.05), Chl a+b (r = −0.56, p ≤ 0.05), and carotenoid (car) (r = −0.57, p ≤ 0.05) were strongly inversely (negatively) correlated with TLP, while Chl a+b/car (r = 0.36, p ≤ 0.05) was moderately (positively) related. Full article
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15 pages, 2968 KiB  
Article
A Rational Analysis on Key Parameters Ruling Zerovalent Iron-Based Treatment Trains: Towards the Separation of Reductive from Oxidative Phases
by Iván Sciscenko, Antonio Arques, Carlos Escudero-Oñate, Melina Roccamante, Ana Ruiz-Delgado, Sara Miralles-Cuevas, Sixto Malato and Isabel Oller
Nanomaterials 2021, 11(11), 2948; https://0-doi-org.brum.beds.ac.uk/10.3390/nano11112948 - 03 Nov 2021
Cited by 6 | Viewed by 1408
Abstract
The development of treatment trains for pollutant degradation employing zerovalent iron has been attracting a lot of interest in the last few years. This approach consists of pre-treatment only with zerovalent iron, followed by a Fenton oxidation taking advantage of the iron ions [...] Read more.
The development of treatment trains for pollutant degradation employing zerovalent iron has been attracting a lot of interest in the last few years. This approach consists of pre-treatment only with zerovalent iron, followed by a Fenton oxidation taking advantage of the iron ions released in the first step. In this work, the advantages/disadvantages of this strategy were studied employing commercial zerovalent iron microparticles (mZVI). The effect of the initial amount of mZVI, H2O2, pH, conductivity, anions and dissolved oxygen were analysed using p-nitrobenzoic acid (PNBA) as model pollutant. 83% reduction of PNBA 6 µM into p-aminobenzoic acid (PABA) was achieved in natural water at an initial pH 3.0 and 1.4 g/L of mZVI, under aerobic conditions, in 2 h. An evaluation of the convenience of removing mZVI after the reductive phase before the Fenton oxidation was investigated together with mZVI reusability. The Fenton step against the more reactive PABA required 50 mg/L of H2O2 to achieve more than 96% removal in 15 min at pH 7.5 (final pH from the reductive step). At least one complete reuse cycle (reduction/oxidation) was achieved with the separated mZVI. This approach might be interesting to treat wastewater containing pollutants initially resistant to hydroxyl radicals. Full article
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14 pages, 2054 KiB  
Article
Environmental Photocatalytic Degradation of Antidepressants with Solar Radiation: Kinetics, Mineralization, and Toxicity
by Nina Finčur, Daniela Šojić Merkulov, Predrag Putnik, Vesna Despotović, Nemanja Banić, Marina Lazarević, Dragana Četojević-Simin, Jasmina Agbaba and Biljana Abramović
Nanomaterials 2021, 11(3), 632; https://0-doi-org.brum.beds.ac.uk/10.3390/nano11030632 - 03 Mar 2021
Cited by 9 | Viewed by 2274
Abstract
This work is focused on the kinetics, mineralization, and toxicological assessments of the antidepressant drug amitriptyline hydrochloride (AMI) in UV or solar illuminated aqueous suspensions of ZnO, TiO2 Degussa P25, and TiO2 Hombikat. ZnO was proven to be the most effective [...] Read more.
This work is focused on the kinetics, mineralization, and toxicological assessments of the antidepressant drug amitriptyline hydrochloride (AMI) in UV or solar illuminated aqueous suspensions of ZnO, TiO2 Degussa P25, and TiO2 Hombikat. ZnO was proven to be the most effective photocatalyst, and it was used for all further experiments under solar irradiation. The highest reaction rate was observed at 1.0 mg/mL of catalyst loading. In the investigated initial concentration range (0.0075–0.3000 mmol/L), the degradation rate of AMI increased with the increase of initial concentration in the investigated range. The effects of H2O2, (NH4)2S2O8, and KBrO3, acting as electron acceptors, along with molecular oxygen were also studied. By studying the effects of ethanol and NaI as a hydroxyl radical and hole scavenger, respectively, it was shown that the heterogeneous catalysis takes place mainly via free hydroxyl radicals. In the mineralization study, AMI photocatalytic degradation resulted in ~30% of total organic carbon (TOC) decrease after 240 min of irradiation; acetate and formate were produced as the organic intermediates; NH4+, NO3, NO2 ions were detected as nitrogen byproducts. Toxicity assessment using different mammalian cell lines, showed that H-4-II-E was the most sensitive one. Full article
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Review

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32 pages, 4042 KiB  
Review
Sustainable Green Nanotechnologies for Innovative Purifications of Water: Synthesis of the Nanoparticles from Renewable Sources
by Szabolcs Bognár, Predrag Putnik and Daniela Šojić Merkulov
Nanomaterials 2022, 12(2), 263; https://0-doi-org.brum.beds.ac.uk/10.3390/nano12020263 - 14 Jan 2022
Cited by 15 | Viewed by 3377
Abstract
Polluting the natural water resources is a serious global issue, which is confirmed by the fact that today at least 2 billion people consume water from contaminated sources. The conventional wastewater treatment methods cannot effectively remove the persistent pollutants (e.g., drugs, organic dyes, [...] Read more.
Polluting the natural water resources is a serious global issue, which is confirmed by the fact that today at least 2 billion people consume water from contaminated sources. The conventional wastewater treatment methods cannot effectively remove the persistent pollutants (e.g., drugs, organic dyes, pesticides) from the aqueous environment. Heterogeneous photocatalysis is a promising and sustainable alternative for water remediation. It is based on the interaction between light irradiation and the semiconductors (e.g., TiO2, ZnO) as photocatalysts, but these compounds, unfortunately, have some disadvantages. Hence, great attention has been paid to the nanotechnology as a possible way of improvement. Nanomaterials have extraordinary properties; however, their conventional synthesis is often difficult and requires a significant amount of dangerous chemicals. This concise topical review gives recent updates and trends in development of sustainable and green pathways in the synthesis of nanomaterials, as well as in their application for water remediation. In our review we put emphasis on the eco-friendly, mostly plant extract-based materials. The importance of this topic, including this study as well, is proved by the growing number of publications since 2018. Due to the current serious environmental issues (e.g., global warming, shortage of pure and quality water), it is necessary for the traditional TiO2 and ZnO semiconductors to be replaced with the harmless, non-toxic, and more powerful nanocomposites as photocatalysts. Not only because of their higher efficiency as compared to the bulk semiconductors, but also because of the presence of biomolecules that can add up to the pollutant removal efficiency, which has been already confirmed in many researches. However, despite the fact that the application of heterogeneous photocatalysis together with green nanotechnology is absolutely the future in water purification, there are some challenges which have to be overcome. The exact effects of the biomolecules obtained from plants in the synthesis of nanoparticles, as well as in the photocatalytic processes, are not exactly known and require further investigation. Furthermore, heterogeneous photocatalysis is a well-known and commonly examined process; however, its practical use outside the laboratory is expensive and difficult. Thus, it has to be simplified and improved in order to be available for everyone. The aim of our review is to suggest and prove that using these bio-inspired compounds it is possible to reduce human footprint in the nature. Full article
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