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Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials

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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Green Materials".

Deadline for manuscript submissions: closed (20 February 2025) | Viewed by 12512

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Dr. Marin Senila

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INCDO-INOE 2000, Research Institute for Analytical Instrumentation Cluj-Napoca, Ploiesti, Romania
Interests: trace elements analysis in environmental samples using advanced analytical techniques; miniaturized spectrometric instrumentation; passive sampling using the diffusive gradients in thin-films (DGT) technique; development and validation of spectrometric methods for environmental applications; elements bioavailability in soil and water; materials characterization using spectrometric techniques
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Dear Colleagues,

The topic of the Special Issue is devoted to the newest research trends in the field of environmental treatment techniques using zeolites and other adsorbent materials.

Natural zeolites and their modified forms, synthetic zeolites, and other adsorbent materials have received considerable attention in environmental remediation due to their remarkable physical and chemical properties. Water treatment with the aid of zeolites and adsorbent materials is one of the oldest applications; however, at the same time, there are many perspectives related to its future developments. One of the most promising soil remediation techniques is in situ stabilization using adsorbing amendments to incorporate and immobilize heavy metals to reduce their bioavailability and transfer to the biota. Zeolites and other adsorbent materials have potential in the purification and separation of gases based on their ability to act as molecular sieves. All these applications are based on porous characteristics which provide them with high adsorption capacities and ion exchangers properties.

The articles presented in this Special Issue of Materials will cover various topics ranging from reports on the zeolites and other porous materials’ characterization, modifications and synthesis and their applications in wastewater treatment, soil remediation, and purification and separation of gases.

Dr. Marin Senila
Guest Editor

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Keywords

zeolites and porous adsorbents
environmental protection and remediation
physico-chemical characterization of porous adsorbents
modification of natural zeolites
synthesis of zeolites
wastewater treatment
soil remediation via in situ stabilization
gas separation/purification using zeolites and other porous adsorbents

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Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials (2nd Edition) in Materials

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30 pages, 6811 KiB

Open AccessArticle

Efficacious Removal of Cd²⁺ and Pb²⁺ Ions from Wastewater Using a Novel Fe₃O₄/SiO₂/PANI-SDBS Nanocomposite

by Mahmoud M. Youssif and Marek Wojnicki

Materials 2025, 18(9), 2083; https://doi.org/10.3390/ma18092083 - 1 May 2025

Viewed by 179

Abstract

The current work synthesizes and characterizes a new Fe₃O₄/SiO₂/PANI-SDBS nanocomposite designed as an efficient adsorbent for the removal of Cd²⁺ and Pb²⁺ ions from contaminated water. The process includes the polymerization of aniline on the Fe₃O₄/SiO₂ nanocomposite in the presence of SDBS. The Fe₃O₄/SiO₂/PANI-SDBS nanocomposite was characterized by using a variety of techniques, including FT-IR, XRD, TEM, SEM, BET, TGA, zeta potential measurements, and particle size distribution analysis, to evaluate its magnetic, structural, and surface properties. For the elimination of both Cd²⁺ and Pb²⁺ ions, ideal adsorption parameters were examined, including pH, adsorbent dose, and contact duration. The solution medium’s optimal pH for achieving the highest effectiveness of elimination for both metal ions was decided to be 7.0. The Fe₃O₄/SiO₂/PANI-SDBS adsorbent demonstrated high adsorption capacities for both Pb²⁺ (72.20 mg g⁻¹) and Cd²⁺ (67.84 mg g⁻¹) at pH 7, with corresponding removal efficiencies of over 94.10% and 77.47%, respectively. This efficiency is attributed to the composite’s large specific surface area and the strong binding affinity of its PANI and SDBS functional groups toward heavy metal ions. Multilayer adsorption on heterogeneous surfaces was shown by isotherm analysis that matched the Freundlich model and adsorption kinetic investigations that showed strong conformance with pseudo-second order for both metal ions. The thermodynamic study proves endothermic and spontaneous process for the removal of metal ions. Furthermore, the adsorbent may be readily recovered from solution thanks to the magnetic core, and regeneration by acid treatment enables reusability with consistent adsorption efficiency across several cycles, making it a cost-effective and sustainable option for continuous water purification processes. Its high adsorption capacity and reusability also make it suitable for use in emergency-response situations, such as the rapid cleanup of wastewater. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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14 pages, 2007 KiB

Open AccessArticle

The Role of Organic Materials in Shaping the Content of Trace Elements in Iron-Contaminated Soil

by Mirosław Wyszkowski and Natalia Kordala

Materials 2025, 18(7), 1522; https://doi.org/10.3390/ma18071522 - 28 Mar 2025

Viewed by 306

Abstract

Iron contamination negatively affects how plants grow and develop, and it has an analogous influence on the health of other organisms. The use of different types of organic soil amendments can be a strategy to reduce the effects of excess iron stress and limit its assimilation by plants. The aim of this experiment was to investigate the possibility of using organic material in the form of humic acids (HAs) to reduce the influence of iron contamination on the content of trace elements (TEs) in the soil. The content of iron in the soil increased linearly (by 14%) as more iron was added. The addition of humic acids to the soil also promoted an increase in soil Fe content (by 12%) in comparison to the series without HAs. The highest dose of iron resulted in a decrease in Cd (by 49%), Pb (by 29%), Cr (by 13%), and Zn (by 10%) and an increase in Mn (by 6%), Cu (by 16%), and Co (by 33%) in the soil in comparison to the object without Fe. However, the first dose of iron increased the lead content, and the first and second dose of Fe also increased the Zn content in the soil. The nickel content in the soil also increased to 500 mg Fe kg⁻¹ of soil. Thereafter, a decline was observed in the nickel content. The addition of organic material had a different influence on the content of individual TEs in the iron-contaminated soils. The most evident constraining impact of HAs pertained to the level of Cd (reducing it by 14%) and Zn in the soil (only for two of its doses). The content of other TEs in the soil after the addition of organic material was found to be higher than in the series without HAs. This was especially evident for elements such as cobalt (Co) and lead (Pb). Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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14 pages, 4386 KiB

Open AccessArticle

Enhanced Cement Foam Composite with Biochar for Eriochrome Black T Dye Removal

by Mohammed Ettahar Boussalah, Malika Medjahdi, Sofiane Guella and Dominique Baillis

Materials 2025, 18(5), 1158; https://doi.org/10.3390/ma18051158 - 5 Mar 2025

Viewed by 614

Abstract

Cement-based foam composites have gained attention as innovative and high-performing adsorbents for wastewater treatment due to their lightweight, porous, and structurally robust properties. This study investigates the adsorption of Eriochrome Black T dye onto biochar-modified cement foam, providing a cost-effective solution for industrial wastewater management. The integration of biochar into cement foam enhances its surface area and adsorption capabilities while maintaining structural stability and tunable porosity. The composites were characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and energy-dispersive X-ray spectroscopy to verify quality and functionality. The adsorption process adhered to the Freundlich isotherm model (R² = 0.967), indicating multilayer adsorption, with a maximum capacity of 13.33 mg/g under optimal conditions. Kinetic studies showed a pseudo-first-order fit (R² = 0.981), while thermodynamic analysis revealed a spontaneous and endothermic process, with ΔH° = 28.84 KJ/mol and ΔG° values ranging from −0.457 to −2.36 KJ/mol. These results demonstrate the composite’s exceptional efficiency and scalability, making it a sustainable and practical option for removing persistent dyes such as Eriochrome Black T. This work contributes significantly to the advancement of environmentally friendly wastewater treatment technologies. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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16 pages, 4359 KiB

Open AccessArticle

The Adsorption of Arsenate and Arsenite Ions on Oxidic Substrates Prepared with a Variable-Charge Lithological Material

by Xinyao Ren, Enju Wang, Fernando Millán, José G. Prato, Marin Senilă, Andrés Eduardo Márquez Chacón, Luisa Carolina González, Guido P. Santillán Lima and Carla Silva Padilla

Materials 2024, 17(22), 5544; https://doi.org/10.3390/ma17225544 - 13 Nov 2024

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Abstract

The adsorption of As(V) and As(III) (0.01–1 mM) on a calcined oxidic lithologic material substrate with pH-dependent surface variable charges, chemically modifiable, was investigated. The substrate was prepared via thermal treatment using a natural lithologic material rich in amphoteric oxides of Fe, Al, Mn and Ti. The calcined substrate was treated with acid media (HCl 0.1) to homogenize the positive charge density on the oxide surface via oxide protonation so that anion adsorption would be favored. A batch experiment was performed on the acid-treated substrate (activated) and non-activated substrate. L-type isotherms were obtained, which fit the Freundlich model. Isotherm constants showed that there was a greater affinity between the activated substrate and As(V) (K = 10.58) compared to As(III) (K = 5.45). The adsorption capacity of the activated substrate was two times greater than that of the non-activated substrate, As(V) (K_act = 10.58 and K_noact = 5.45) vs. As(III) (K_act = 5.45 y K_noact = 2.44), which was due to the greater positive charge density on the activated surface, created by the protonation of the surface oxides. Protons were liberated during the adsorption reaction (As(V): 2.17 × 10⁻³ and As(III): 0.96 × 10⁻³ mmol/mL). The forms H₂AsO₄⁻ and H₃AsO₃ deprotonated when adsorbed by the surface groups

M - O H_{2}^{+}

(M: Fe, Al). Kinetic data showed a second-order process for As(V) adsorption and a first-order process for As(III) adsorption. The adsorption rate on the activated substrate was two times greater compared with the non-activated substrate: As(V) (k_act = 3.78 × 10⁻⁵ L/mg·min and k_noact = 2.16 × 10⁻⁵ L/mg·min) vs. As(III) (k_act = 0.055 h⁻¹ and k_noact = 0.027 h⁻¹). The tested substrate is potentially useful as a low-cost natural material for arsenic removal from contaminated water. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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23 pages, 3251 KiB

Open AccessArticle

Regeneration and Single Stage Batch Adsorber Design for Efficient Basic Blue-41 Dye Removal by Porous Clay Heterostructures Prepared from Al13 Montmorillonite and Pillared Derivatives

by Saheed A. Popoola, Hmoud Al Dmour, Rawan Al-Faze, Mohd Gulfam Alam, Souad Rakass, Hicham Oudghiri Hassani and Fethi Kooli

Materials 2024, 17(20), 4948; https://doi.org/10.3390/ma17204948 - 10 Oct 2024

Cited by 1 | Viewed by 1151

Abstract

Porous clay heterostructures are a hybrid precursor between the pillaring process and organoclays. In this study, the organoclay was substituted by an aluminium intercalated species clay or pillared alumina clays. A porous clay heterostructure was successfully achieved from an aluminium intercalated species clay, due to the easy exchange of the aluminium species by the cosurfactant and silica species. However, using alumina pillared clays, the porous clay heterostructures were not formed; the alumina species were strongly attached to clay sheets which made difficult their exchange with cosurfactant molecules. In this case, the silica species were polymerized and decorated the surface of the used materials as indicated by different characterization techniques. The specific surface area of the porous clay heterostructure material reached 880 m²/g, and total pore volume of 0.258 cc/g, while the decorated silica alumina pillared clays exhibited lower specific surface area values of 244–440 m²/g and total pore volume of 0.315 to 0.157 cc/g. The potential of the synthesized materials was evaluated as a basic blue-41 dye removal agent. Porous clay heterostructure material has a removal capacity of 279 mg/g; while the other materials exhibited lower removal capacities between 75 mg/g and 165 mg/g. The used regeneration method was related to the acidity of the studied materials. The acidity of the materials possessed an impact on the adopted regeneration procedure in this study, the removal efficiency was maintained at 80% of the original performance after three successive regeneration cycles for the porous clay heterostructure. The Langmuir isotherm characteristics were used to propose a single-stage batch design. Porous clay heterostructures with a higher removal capacity resulted in a decrease in the quantities needed to achieve the target removal percentage of the BB-41 dye from an aqueous solution. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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30 pages, 6440 KiB

Open AccessArticle

Mercury Ion Selective Adsorption from Aqueous Solution Using Amino-Functionalized Magnetic Fe₂O₃/SiO₂ Nanocomposite

by Mahmoud M. Youssif, Heba G. El-Attar, Stanisław Małecki, Grzegorz Włoch, Maciej Czapkiewicz, Kamil Kornaus and Marek Wojnicki

Materials 2024, 17(17), 4254; https://doi.org/10.3390/ma17174254 - 28 Aug 2024

Cited by 2 | Viewed by 1528

Abstract

This study focuses on the development of new amino-functionalized magnetic Fe₂O₃/SiO₂ nanocomposites with varying silicate shell ratios (1:0.5, 1:1, and 1:2) for the efficient elimination of Hg²⁺ ions found in solutions. The Fe₂O₃/SiO₂–NH₂ adsorbents were characterized for their structural, surface, and magnetic properties using various techniques, including Fourier transform infrared spectrum (FT-IR), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), Braunauer–Emmett–Teller (BET), thermogravimetric analysis (TGA), zeta-potential, and particle size measurement. We investigated the adsorption circumstances, such as pH, dosage of the adsorbent, and duration of adsorption. The pH value that yielded the best results was determined to be 5.0. The Fe₂O₃/SiO₂–NH₂ adsorbent with a silicate ratio of (1:2) exhibited the largest amount of adsorption capacity of 152.03 mg g⁻¹. This can be attributed to its significantly large specific surface area of 100.1 m² g⁻¹, which surpasses that of other adsorbents. The adsorbent with amino functionalization demonstrated a strong affinity for Hg²⁺ ions due to the chemical interactions between the metal ions and the amino groups on the surface. The analysis of adsorption kinetics demonstrated that the adsorption outcomes adhere to the pseudo-second-order kinetic model. The study of adsorption isotherms revealed that the adsorption followed the Langmuir model, indicating that the adsorption of Hg²⁺ ions with the adsorbent occurred as a monomolecular layer adsorption process. Furthermore, the thermodynamic analyses revealed that the adsorption of Hg²⁺ ions using the adsorbent was characterized by a spontaneous and endothermic process. Additionally, the adsorbent has the ability to selectively extract mercury ions from a complex mixture of ions. The Fe₂O₃/SiO₂–NH₂ nanocomposite, which is loaded with metal, can be easily recovered from a water solution due to its magnetic properties. Moreover, it can be regenerated effortlessly through acid treatment. This study highlights the potential use of amino-functionalized Fe₂O₃/SiO₂ magnetic nanoparticles as a highly efficient, reusable adsorbent for the removal of mercury ions from contaminated wastewater. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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15 pages, 3112 KiB

Open AccessArticle

Polyurethane Foam and Algae-Based Activated Carbon Biocomposites for Oil Spill Remediation

by Lokmane Abdelkaddous Baidar, Malika Medjahdi, Badra Mahida, Belaid Mechab and Dominique Baillis

Materials 2024, 17(16), 4137; https://doi.org/10.3390/ma17164137 - 21 Aug 2024

Cited by 1 | Viewed by 1215

Abstract

This study investigates the incorporation of algae-based activated carbon into polyurethane foam to improve a biocomposite for gasoil sorption. The biocomposites were thoroughly analyzed using various techniques to examine the properties of both the blank foam and the algae activated carbon foam with a carbon content of 4.41 mass% and particle diameter of 500 µm. These techniques included Scanning Electron Microscopy (SEM), thermogravimetric analysis (TGA), and density analysis. The TGA analysis revealed that the biocomposites had an impact on the onset temperature (T_onset) of the foams. Higher concentrations of the biocomposites resulted in a decrease in T_onset from approximately 310 °C in the blank foam (PUF0) to 300 °C in the composite (PUF3B). The final residue percentage also decreased from around 20% in PUF0 to 10% in PUF3B. Density analysis showed that the apparent density of the foam increased from 0.016 g/cm³ in the blank foam to 0.020 g/cm³ in the biocomposite (PUF3B), while the real density slightly decreased from 0.092 g/cm³ to 0.076 g/cm³, indicating a reduction in overall porosity from 82.5% to 74.4%. All foams that were modified showed an increase in their ability to absorb gasoil in a PUF/gasoil/water system. The optimized biocomposite (PUF1B), with 1.14 mass% of 500 µm algae carbon, displayed the highest sorption capacity, starting at approximately 50 g/g at 1.5 h and increasing to 53 g/g over 72 h. The analysis of adsorption kinetics revealed that by utilizing adsorption isotherms, particularly the Langmuir isotherm, a more accurate fit to the data was achieved. This allowed for the prediction of the maximum gasoil adsorption capacity. This study aims to further develop, analyze, and utilize biocomposites made from algae-based activated carbon and polyurethane. These materials offer a sustainable and environmentally friendly approach to cleaning up oil spills. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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19 pages, 5255 KiB

Open AccessArticle

Development of a Novel Cyclodextrin–Chitosan Polymer for an Efficient Removal of Pharmaceutical Contaminants in Aqueous Solution

by Fadila Oughlis-Hammache, Mohamed Skiba, Lamia Moulahcene, Nicolas Milon, Frédéric Bounoure and Malika Lahiani-Skiba

Materials 2024, 17(14), 3594; https://doi.org/10.3390/ma17143594 - 21 Jul 2024

Cited by 1 | Viewed by 1322

Abstract

A novel polymer synthesized by grafting three cyclodextrins onto chitosan was characterized and evaluated for its potential to adsorb two pharmaceutical residues: ibuprofen and progesterone. The influence of various operational parameters, including contact time, initial molecule concentration, pH, ionic strength, and temperature, was investigated. The synthesized polymer exhibits an amorphous and porous structure with a remarkable swelling capacity of 9.5 mmol/g. It demonstrates remarkable adsorption capacities for progesterone and ibuprofen, reaching 90% and 75%, respectively. Kinetic studies reveal that the adsorption of both molecules follows a pseudo-second-order model. A DSC analysis elucidated the adsorption mechanism, which is governed by the formation of inclusion complexes and electrostatic interactions within the polymer network. The polymer’s regeneration after 23 cycles demonstrates its sustainable adsorption efficiency. The combination of chitosan with three cyclodextrins opens up promising new avenues for water treatment and the removal of specific pollutants. This approach significantly improves the material’s selectivity towards target pollutants, offering a significant advantage in pollution remediation applications. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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23 pages, 9451 KiB

Open AccessArticle

Odors Adsorption in Zeolites Including Natural Clinoptilolite: Theoretical and Experimental Studies

by Izabela Czekaj and Natalia Sobuś

Materials 2024, 17(13), 3088; https://doi.org/10.3390/ma17133088 - 24 Jun 2024

Cited by 1 | Viewed by 1562

Abstract

This publication presents the results of combined theoretical and experimental research for the potential use of natural clinoptilolite zeolite (CLI) as an odor-adsorbing material. In this study of adsorption capacity, CLI of various granulation was used and its modifications were made by ion exchange using Sn and Fe metals to check whether the presence of metals as potential active centers does not lead to catalytic processes and may lead to enhanced absorption of odorous substances through their adsorption on the created metallic forms. Additionally, in order to increase the specific surface area, modifications were made in the form of hierarchization in an acidic environment using hydrochloric acid to also create the hydrogen form of zeolite and thus also check how the material behaves as an adsorbent. To compare the effect of CLI as a sorption material, synthetic zeolite MFI was also used—as a sodium form and after the introduction of metals (Sn, Fe). The above materials were subjected to adsorption measurements using odorous substances (including acetaldehyde, dimethylamine, pentanoic acid and octanoic acid). Based on the measurements performed, the most advantageous material that traps odorants is a natural material—clinoptilolite. Depending on the faction, its ability varies for different compounds. In the case of acetaldehyde, an effective material is clinoptilolite with a grain size of up to 2 mm. In the case of carboxylic acids, it is material after hierarchization with a fraction of 3–4 mm. In the case of theoretical calculations, information was obtained to show that metallic centers are more stable above oxygen, which is associated with the skeletal aluminum in clinoptilolite. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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14 pages, 6576 KiB

Open AccessArticle

Green Synthesis and Efficient Adsorption: Na-X Zeolite vs. C/Mn/SiO₂ Composite for Heavy Metals Removal

by Magdalena Medykowska, Małgorzata Wiśniewska, Katarzyna Szewczuk-Karpisz, Mariia Galaburda, Olena Oranska and Rafał Panek

Materials 2024, 17(4), 954; https://doi.org/10.3390/ma17040954 - 19 Feb 2024

Cited by 2 | Viewed by 1539

Abstract

The studies aimed to test the adsorption capacity of two silica-enriched porous materials, synthetic Na-X zeolite and Mn-containing carbon composite, towards Pb(II) and Zn(II) ions in single and mixed systems and in the presence of diclofenac (DCF) and (or) poly(acrylic acid) (PAA). The synthetic zeolite was characterized by a well-developed surface area of 728 m²/g and a pore diameter of 1.73 nm, while the carbon composite exhibited 268 m²/g and 7.37 nm, respectively. Na-X was found to be more efficient than the carbon composite (75–212 mg/g) in adsorbing heavy metal ions in both single and bimetallic systems (322–333 mg/g). In turn, the C/Mn/SiO₂ composite was more effective in removing Pb(II) ions from the systems that simultaneously contained DCF or PAA (480 and 476 mg/g, respectively). The Na-X zeolite demonstrated the greatest stability in all the systems studied. The highest stability was observed in the DCF + Pb(II) mixture, in contrast to the carbon composites where the stability was much lower. To evaluate the possibility of regeneration of the solids, HCl proved to be the best desorbent for heavy metal ions (efficiency of 99%). In general, both adsorbents offer promising potential for solving environmental problems. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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Review

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22 pages, 2345 KiB

Open AccessReview

Composites Based on Natural Zeolites and Green Materials for the Immobilization of Toxic Elements in Contaminated Soils: A Review

by Marin Senila and Oana Cadar

Materials 2024, 17(23), 5977; https://doi.org/10.3390/ma17235977 - 6 Dec 2024

Viewed by 1212

Abstract

Soil contamination by toxic elements is a global problem, and the remediation of contaminated soils requires complex and time-consuming technology. Conventional methods of soil remediation are often inapplicable, so an intensive search is underway for innovative and environmentally friendly ways to clean up ecosystems. The use of amendments that stabilize the toxic elements in soil by reducing their mobility and bioavailability is one of the simplest and most cost-effective ways to remediate soil. This paper provides a summary of studies related to the use of composites based on natural zeolites and green materials for the immobilization of toxic elements in contaminated soils and highlights positive examples of returning land to agricultural use. The published literature on natural zeolites and their composites has shown that combinations of zeolite with biochar, chitosan and other clay minerals have beneficial synergistic effects on toxic element immobilization and soil quality. The effects of zeolite properties, different combinations, application rates, or incubation periods on toxic elements immobilization were tested in laboratory scale or field experiments, whereas the mobility of toxic elements in soil was evaluated by chemical extractions of toxic elements transferred to the plants. This review highlights the excellent potential of natural zeolites to be used as single or combined sustainable green materials to solve environmental pollution problems related to the presence of toxic elements. Full article

(This article belongs to the Special Issue Recent Advances in the Environmental Remediation Using Zeolites and Other Adsorbent Materials)

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