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

Deadline for manuscript submissions: closed (31 March 2024) | Viewed by 15172

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Dr. Pasquale Iovino

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Department of Biological and Pharmaceutical Environmental Sciences and Technologies (DISTABIF), University of Campania Luigi Vanvitelli, Naples, Italy
Interests: environmental analysis; removal of environmental pollutants; wastewater treatment; environmental chemistry; advanced oxidation processes
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Dear Colleagues,

Environmental pollution, particularly in water, is a significant global concern due to its impact on human health and the ecosystem. The presence of various pollutants in wastewater, such as pharmaceuticals and personal care products, heavy metals, organic compounds, micro- and nanoplastics, surfactants, and pathogens, has resulted in severe consequences, including the contamination of drinking water sources, the destruction of aquatic habitats, and the spread of waterborne diseases.

To address this problem, numerous chemical technologies have been developed for the analysis and removal of pollutants in water, including advanced oxidation processes, membrane filtration, adsorption, and biological treatment, among others. These technologies have demonstrated great potential in effectively removing various types of pollutants from water, either alone or in combination with other methods.

This Special Issue invites original research papers and reviews reporting on recent progress in the development of chemical technologies for environmental analysis and pollution removal in water. The Issue will cover a broad range of topics, including the development of new methods for environmental analysis, the characterization of pollutants in water, the application of advanced oxidation processes, membrane filtration, and new adsorption materials for water treatment, as well as the evaluation of the performance and efficiency of these technologies. Additionally, focused review articles are welcome to examine the state of the art, identify emerging trends, and suggest future directions for developing new applications in this field.

Dr. Pasquale Iovino
Guest Editor

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Molecules is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

advanced oxidation processes
wastewater treatment
adsorbents
emerging technologies
removal of environmental pollutants
analysis techniques
emerging pollutant

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Related Special Issue

Chemical Technologies for Environmental Analysis and Pollution Removal, 2nd Edition in Molecules (1 article)

Published Papers (9 papers)

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14 pages, 14049 KiB

Open AccessArticle

Fabrication of Nitrogen Based Magnetic Conjugated Microporous Polymer for Efficient Extraction of Neonicotinoids in Water Samples

by Zhenzhen Xia, Xinghua Teng, Yuqi Cheng, Yujie Huang, Liwen Zheng, Lei Ji and Leilei Wang

Molecules 2024, 29(10), 2189; https://doi.org/10.3390/molecules29102189 - 8 May 2024

Viewed by 571

Abstract

Facile and sensitive methods for detecting neonicotinoids (NEOs) in aquatic environments are crucial because they are found in extremely low concentrations in complex matrices. Herein, nitrogen-based magnetic conjugated microporous polymers (Fe₃O₄@N-CMP) with quaternary ammonium groups were synthesized for efficient magnetic solid-phase extraction (MSPE) of NEOs from tap water, rainwater, and lake water. Fe₃O₄@N-CMP possessed a suitable specific surface area, extended π-conjugated system, and numerous cationic groups. These properties endow Fe₃O₄@N-CMP with superior extraction efficiency toward NEOs. The excellent adsorption capacity of Fe₃O₄@N-CMP toward NEOs was attributed to its π–π stacking, Lewis acid–base, and electrostatic interactions. The proposed MSPE-HPLC-DAD approach based on Fe₃O₄@N-CMP exhibited a wide linear range (0.1–200 µg/L), low detection limits (0.3–0.5 µg/L), satisfactory precision, and acceptable reproducibility under optimal conditions. In addition, the established method was effectively utilized for the analysis of NEOs in tap water, rainwater, and lake water. Excellent recoveries of NEOs at three spiked levels were in the range of 70.4 to 122.7%, with RSDs less than 10%. This study provides a reliable pretreatment method for monitoring NEOs in environmental water samples. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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Figure 1
SEM images of Fe3O4 (A), Fe3O4@N-CMP (B); TEM images of Fe3O4 (C), and Fe3O4@N-CMP (D). Full article ">Figure 2
(A) FT-IR spectra; (B) N 1s XPS spectra; (C) magnetization curves (the inset shows magnetic separation of Fe3O4@N-CMP; (D) N2 adsorption-desorption isotherm of Fe3O4@N-CMP (inset: pore size distribution curve). Full article ">Figure 3
Optimization of MSPE conditions: (A) Fe3O4@N-CMP amount; (B) extraction time; (C) NaCl concentration; (D) pH; (E) type of elution solvent; (F) elution time (n = 3). Full article ">Figure 4
Reusability of Fe3O4@N-CMP on the extraction of five NEOs. Full article ">Figure 5
HPLC−DAD chromatograms of enriched NEOs from rainwater spiked with 0 (a), 5 (b), 50 (c), and 100 (d) μg/L, respectively. Full article ">Scheme 1
Illustration of the synthesis of Fe3O4@N-CMP and its MSPE procedure. Full article ">

30 pages, 13773 KiB

Open AccessArticle

Influence of Hydrothermal Modification on Adsorptive Performance of Clay Minerals for Malachite Green

by Enwen Wang, Teng Huang, Qian Wu, Lanchun Huang, Desong Kong and Hai Wang

Molecules 2024, 29(9), 1974; https://doi.org/10.3390/molecules29091974 - 25 Apr 2024

Viewed by 655

Abstract

Artificially modified adsorbing materials mainly aim to remedy the disadvantages of natural materials as much as possible. Using clay materials such as rectorite, sodium bentonite and metakaolinite (solid waste material) as base materials, hydrothermally modified and unmodified materials were compared. CM-HT and CM (adsorbing materials) were prepared and used to adsorb and purify wastewater containing malachite green (MG) dye, and the two materials were characterized through methods such as BET, FT-IR, SEM and XRD. Results: (1) The optimal conditions for hydrothermal modification of CM-HT were a temperature of 150 °C, a time of 2 h, and a liquid/solid ratio 1:20. (2) Hydrothermal modification greatly increased the adsorptive effect. The measured maximum adsorption capacity of CM-HT for MG reached 290.45 mg/g (56.92% higher than that of CM). The theoretical maximum capacity was 625.15 mg/g (186.15% higher than that of CM). (3) Because Al-OH and Si-O-Al groups were reserved in unmodified clay mineral adsorbing materials with good adsorbing activity, after hydrothermal modification, the crystal structure of the clay became loosened along the direction of the c axis, and the interlayer space increased to partially exchange interlayer metal cations connected to the bottom oxygen, giving CM-HT higher electronegativity and creating more crystal defects and chemically active adsorbing sites for high-performance adsorption. (4) Chemical adsorption was the primary way by which CM-HT adsorbed cationic dye, while physical adsorption caused by developed pore canal was secondary. The adsorption reaction occurred spontaneously. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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17 pages, 1762 KiB

Open AccessArticle

A Study on the Adsorption of Rhodamine B onto Adsorbents Prepared from Low-Carbon Fossils: Kinetic, Isotherm, and Thermodynamic Analyses

by Aleksandra Bazan-Wozniak, Aleksandra Jędrzejczak, Robert Wolski, Sławomir Kaczmarek, Agnieszka Nosal-Wiercińska, Judyta Cielecka-Piontek, Sultan Yagmur-Kabas and Robert Pietrzak

Molecules 2024, 29(6), 1412; https://doi.org/10.3390/molecules29061412 - 21 Mar 2024

Cited by 1 | Viewed by 1307

Abstract

The aim of this study was to obtain a series of activated carbon samples by the chemical activation of low-rank coal. The precursor was impregnated with a NaOH solution. Activated carbons were characterized by determining their textural parameters and content of surface oxygen functional groups and by using an elemental analysis. The carbons were tested as potential adsorbents for the removal of liquid pollutants represented by rhodamine B. The effectiveness of rhodamine B removal from water solutions depended on the initial concentration of the dye, the mass of rhodamine B, and the pH and temperature of the reaction. The isotherm examination followed the Langmuir isotherm model. The maximum adsorption capacity of the rhodamine B was 119 mg/g. The kinetic investigation favored the pseudo-second-order model, indicating a chemisorption mechanism. The thermodynamic assessment indicated spontaneous and endothermic adsorption, with decreased randomness at the solid–liquid interface. The experiment revealed that a 0.1 M HCl solution was the most effective regenerative agent. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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18 pages, 1575 KiB

Open AccessArticle

Enhanced Sorption Performance of Natural Zeolites Modified with pH-Fractionated Humic Acids for the Removal of Methylene Blue from Water

by Stefano Salvestrini, Jean Debord and Jean-Claude Bollinger

Molecules 2023, 28(20), 7083; https://doi.org/10.3390/molecules28207083 - 14 Oct 2023

Cited by 1 | Viewed by 1052

Abstract

This work explores the effect of humic acids (HA) fractionation on the sorption ability of a natural zeolite (NYT)—HA adduct. HA were extracted from compost, fractionated via the pH fractionation method, and characterized via UV-Vis spectroscopy and gel permeation chromatography. The HA samples were immobilized onto NYT via thermal treatment. The resulting adducts (NYT-HA) were tested for their ability to remove methylene blue (MB) from an aqueous solution. It was found that the sorption performance of NYT-HA strongly depends on the chemical characteristics of humic acids. Sorption capacity increased with the molecular weight and hydrophobicity degree of the HA fractions. Hydrophobic and π–π interactions are likely the primary mechanisms by which MB interacts with HA. The sorption kinetic data conform to the pseudo-second-order model. The Freundlich isotherm model adequately described the sorption equilibrium and revealed that the uptake of MB onto NYT-HA is endothermic in nature. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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High-pressure gel permeation chromatograms of extracted HA samples: (A) unfractionated HA; (B) fraction of HA soluble at pH 3; (C) fraction of HA insoluble at pH 3 and dissolved at pH 5; (D) residual fraction of HA insoluble at pH 5 and dissolved at pH 7. Full article ">Figure 2
Dependence of the MB aqueous concentration on time in the presence of NYT; C0 = initial MB concentration in the liquid phase; T = 20 °C. The curves in the figure were obtained via non-linear regression of the data using the Vermeulen model. Full article ">Figure 3
Comparison of the sorption kinetics regarding the sorption of MB onto various sorbents. Initial concentration of MB = 11.9 mg L−1; T = 20 °C. The curves in the figure were obtained via nonlinear regression analysis using the PSO model, with the exception of the NYT data set modelled using the Vermeulen equation. Full article ">Figure 4
Sorption isotherms regarding the sorption of MB onto various sorbents. T = 20 °C. The curves in the figure were obtained via nonlinear regression analysis using the Freundlich model, with the exception of NYT data set modelled using the Langmuir equation. Full article ">Figure 5
Sorption isotherms regarding the sorption of MB onto NYT-HA7 at various temperatures. The curves in the figure were obtained via non-linear regression analysis using the Freundlich isotherm model. Full article ">Figure 6
Plot of 1/n against 1/T for the estimation of the standard sorption enthalpy (<math display="inline"><semantics> <mrow> <mi mathvariant="sans-serif">Δ</mi> <mi>H</mi> <mo>°</mo> </mrow> </semantics></math>) and the standard sorption entropy (<math display="inline"><semantics> <mrow> <mi mathvariant="sans-serif">Δ</mi> <mi>S</mi> <mo>°</mo> </mrow> </semantics></math>). Full article ">

15 pages, 1087 KiB

Open AccessArticle

Identification of the Contamination Sources by PCBs Using Multivariate Analyses: The Case Study of the Annaba Bay (Algeria) Basin

by Soumeya Khaled-Khodja, Hassen Cheraitia, Karima Rouibah, Hana Ferkous, Gaël Durand, Semia Cherif, Gamal A. El-Hiti, Krishna Kumar Yadav, Alessandro Erto and Yacine Benguerba

Molecules 2023, 28(19), 6841; https://doi.org/10.3390/molecules28196841 - 28 Sep 2023

Cited by 1 | Viewed by 1262

Abstract

Persistent Organic Pollutants (POPs), particularly the indicator polychlorinated biphenyls (PCBs), were first quantified in water and sediments of two wadis, Boujemaâ and Seybouse, as well as in the effluents from a fertilizer and phytosanitary production industrial plant (Fertial). Since these contaminated discharges end in Annaba Bay (Algeria) in the Mediterranean Sea, with a significant level of contamination, all the potential sources should be identified. In this work, this task is conducted by a multivariate analysis. Liquid–liquid extraction and gas chromatography/mass spectrometry (GC–MS) methods were applied to quantify seven PCB congeners, usually taken as indicators of contamination. The sum of the PCB concentrations in the sediments ranged from 1 to 6.4 μg/kg dw (dry weight) and up to 0.027 μg/L in waters. Principal component analysis (PCA) and hierarchical cluster analysis (HCA) were used for the multivariate analysis, indicating that the main sources of PCB emissions in the bay are urban/domestic and agricultural/industrial. The outfalls that mostly contribute to the pollution of the gulf are the Boujemaâ wadi, followed by the Seybouse wadi, and finally by the Fertial cluster and more precisely the annex basin of the plant. Although referring to a specific site of local importance, the work aims to present a procedure and a methodological analysis that can be potentially applicable to further case studies all over the world. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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14 pages, 4808 KiB

Open AccessArticle

Removal of Hexamethyldisiloxane via a Novel Hydrophobic (3–Aminopropyl)Trimethoxysilane-Modified Activated Porous Carbon

by Siqi Lv, Yingrun Wang, Yanhui Zheng and Zichuan Ma

Molecules 2023, 28(18), 6493; https://doi.org/10.3390/molecules28186493 - 7 Sep 2023

Viewed by 1251

Abstract

Volatile methyl siloxanes (VMS) must be removed because the formation of silica in the combustion process seriously affects the resource utilization of biogas. Herein, a series of APTMS ((3–aminopropyl)trimethoxysilane)-modified activated porous carbon (APC) adsorbents (named APTMS@APC) were prepared for VMS efficient removal. The as-prepared adsorbents were characterized using SEM, FTIR, Raman, X-ray diffraction analyses, and N₂ adsorption/desorption. The results showed that the surface modification with APTMS enhanced the hydrophobicity of APC with the water contact angle increasing from 74.3° (hydrophilic) to 127.1° (hydrophobic), and meanwhile improved its texture properties with the S_BET increasing from 981 to 1274 m² g⁻¹. The maximum breakthrough adsorption capacity of APTMS@APC for hexamethyldisiloxane (L2, model pollutant) was 360.1 mg g⁻¹. Effects of an inlet L2 concentration (31.04–83.82 mg L⁻¹) and a bed temperature (0–50 °C) on the removal of L2 were investigated. Meanwhile, after five adsorption–desorption cycles, the APTMS@APC demonstrated a superior cycling performance. This indicated that the hydrophobic APTMS@APC has a great significance to remove VMS. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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20 pages, 4503 KiB

Open AccessArticle

Experimental and Theoretical Estimations of Atrazine’s Adsorption in Mangosteen-Peel-Derived Nanoporous Carbons

by Juan Matos, Claudia P. Amézquita-Marroquín, Johan D. Lozano, Jhon Zapata-Rivera, Liliana Giraldo, Po S. Poon and Juan C. Moreno-Piraján

Molecules 2023, 28(13), 5268; https://doi.org/10.3390/molecules28135268 - 7 Jul 2023

Cited by 1 | Viewed by 1209

Abstract

Nanoporous carbons were prepared via chemical and physical activation from mangosteen-peel-derived chars. The removal of atrazine was studied due to the bifunctionality of the N groups. Pseudo-first-order, pseudo-second-order, and intraparticle pore diffusion kinetic models were analyzed. Adsorption isotherms were also analyzed according to the Langmuir and Freundlich models. The obtained results were compared against two commercially activated carbons with comparable surface chemistry and porosimetry. The highest uptake was found for carbons with higher content of basic surface groups. The role of the oxygen-containing groups in the removal of atrazine was estimated experimentally using the surface density. The results were compared with the adsorption energy of atrazine theoretically estimated on pristine and functionalized graphene with different oxygen groups using periodic DFT methods. The energy of adsorption followed the same trend observed experimentally, namely the more basic the pH, the more favored the adsorption of atrazine. Micropores played an important role in the uptake of atrazine at low concentrations, but the presence of mesoporous was also required to inhibit the pore mass diffusion limitations. The present work contributes to the understanding of the interactions between triazine-based pollutants and the surface functional groups on nanoporous carbons in the liquid–solid interface. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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Figure 1
(a) N2 adsorption–desorption isotherms at −196 °C; (b) pore size distributions. The figure inset shows the cumulative pore volume on the activated carbons. Full article ">Figure 2
SEM images of the homemade carbons: (a) MPB-CO2; (b) MPB-P50. Full article ">Figure 3
Evolution of pH of activated carbons as a function of contact time. Full article ">Figure 4
Kinetics of atrazine adsorption (qt) as a function of the initial concentration: (a) ACM; (b) ACPC; (c) MPB-CO2; (d) MPB-P50. Full article ">Figure 5
Adsorption isotherms of atrazine: (a) ACM; (b) ACPC; (c) MPB-CO2; (d) MPB-P50. Full article ">Figure 6
Optimized geometries of adsorbed systems in 1/1 monolayer using one atrazine molecule on a 5 × 5 graphene surface unit cell. O, N, Cl, and H atoms correspond to red, blue, green, and grey spheres, respectively. Full article ">Figure 7
DOS (black line) and projected DOS on the pristine GPristine graphene (green line) and atrazine (blue line) with the PBE functional. Full article ">Figure 8
Schematic model for the atrazine adsorption on porous carbons: (a) low ATZ concentration. (b) high ATZ concentration. Full article ">

17 pages, 3190 KiB

Open AccessArticle

Untreated Opuntia ficus indica for the Efficient Adsorption of Ni(II), Pb(II), Cu(II) and Cd(II) Ions from Water

by Marcella Barbera, Serena Indelicato, David Bongiorno, Valentina Censi, Filippo Saiano and Daniela Piazzese

Molecules 2023, 28(9), 3953; https://doi.org/10.3390/molecules28093953 - 8 May 2023

Cited by 3 | Viewed by 1986

Abstract

The raw cladode of Opuntia ficus indica (OFI) was evaluated as a sustainable biosorbent for the removal of heavy metals (Ni, Pb, Cu, and Cd) from aqueous solutions. The functional groups of OFI were identified by employing DRIFT-FTIR and CP-MAS-NMR techniques before and after contact with the ions in an aqueous media, showing a rearrangement of the biomass structure due to the complexation between the metal and the functional groups. The adsorption process was studied in both single- and multi-component systems under batch conditions at different pHs (4.0, 5.0, and 6.0), different metal concentrations, and different biomass amounts. The results show that the raw OFI had a removal capacity at room temperature of over 80% for all metals studied after only 30 min of contact time, indicating a rapid adsorption process. Biosorption kinetics were successfully fitted by the pseudo-second-order equation, while Freundlich correctly modelled the biosorption data at equilibrium. The results of this work highlight the potential use of the untreated cladode of OFI as an economical and environmentally friendly biosorbent for the removal of heavy metals from the contaminated aqueous solution. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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Figure 1
DRIFT spectra of OFI biomass. Full article ">Figure 2
DRIFT spectra of biomass before and after the contact with single- and multi-component ion solutions at pH 5. The violet line is the spectrum of the raw biomass; the blue line is the spectrum of the biomass in contact with the multi-component solution; and the pink, orange, red, and green lines are the spectra of the biomass in contact with solutions of Pb, Cu, Cd, and Ni, respectively. Full article ">Figure 3
CP-NMR-MAS spectra of biomass before (blue line) and after contact with multi-elemental ion solution (red line). Full article ">Figure 4
Sorption isotherm for a single-component system at 25 °C. Full article ">Figure 5
The effect of contact time on OFI adsorption capacity in water solution at pHs 4.0, 5.0, and 6.0. Full article ">Figure 6
Adsorption efficiency of biomass (0.1 mg) in single- (<bold>a</bold>,<bold>c</bold>) and multi-component (<bold>b</bold>,<bold>d</bold>) solutions as a function of metal concentrations after a contact time of 30 min. (<bold>a</bold>,<bold>b</bold>) are the results obtained at pH 4.0 and (<bold>c</bold>,<bold>d</bold>) at pH 5.0. Full article ">

Review

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24 pages, 2417 KiB

Open AccessReview

Application of Electrochemical Oxidation for Water and Wastewater Treatment: An Overview

by Mohammad Saleh Najafinejad, Simeone Chianese, Angelo Fenti, Pasquale Iovino and Dino Musmarra

Molecules 2023, 28(10), 4208; https://doi.org/10.3390/molecules28104208 - 20 May 2023

Cited by 21 | Viewed by 5152

Abstract

In recent years, the discharge of various emerging pollutants, chemicals, and dyes in water and wastewater has represented one of the prominent human problems. Since water pollution is directly related to human health, highly resistant and emerging compounds in aquatic environments will pose many potential risks to the health of all living beings. Therefore, water pollution is a very acute problem that has constantly increased in recent years with the expansion of various industries. Consequently, choosing efficient and innovative wastewater treatment methods to remove contaminants is crucial. Among advanced oxidation processes, electrochemical oxidation (EO) is the most common and effective method for removing persistent pollutants from municipal and industrial wastewater. However, despite the great progress in using EO to treat real wastewater, there are still many gaps. This is due to the lack of comprehensive information on the operating parameters which affect the process and its operating costs. In this paper, among various scientific articles, the impact of operational parameters on the EO performances, a comparison between different electrochemical reactor configurations, and a report on general mechanisms of electrochemical oxidation of organic pollutants have been reported. Moreover, an evaluation of cost analysis and energy consumption requirements have also been discussed. Finally, the combination process between EO and photocatalysis (PC), called photoelectrocatalysis (PEC), has been discussed and reviewed briefly. This article shows that there is a direct relationship between important operating parameters with the amount of costs and the final removal efficiency of emerging pollutants. Optimal operating conditions can be achieved by paying special attention to reactor design, which can lead to higher efficiency and more efficient treatment. The rapid development of EO for removing emerging pollutants from impacted water and its combination with other green methods can result in more efficient approaches to face the pressing water pollution challenge. PEC proved to be a promising pollutants degradation technology, in which renewable energy sources can be adopted as a primer to perform an environmentally friendly water treatment. Full article

(This article belongs to the Special Issue Chemical Technologies for Environmental Analysis and Pollution Removal)

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