Novel Materials/Technologies for the Adsorption and Removal of Antibiotics from Aqueous Solution

A special issue of Processes (ISSN 2227-9717). This special issue belongs to the section "Environmental and Green Processes".

Deadline for manuscript submissions: closed (31 December 2023) | Viewed by 12516

Special Issue Editors

Institute of Environmental Engineering, School of Earth and Environmental Sciences, Lanzhou University, Lanzhou 730000, China
Interests: wastewater advanced treatment; environmental catalysis; water environment restoration
Special Issues, Collections and Topics in MDPI journals
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
Interests: electrocatalytic oxidation; electrochemical scale removal; electrochemical sterilization; metal oxide electrode
Special Issues, Collections and Topics in MDPI journals
School of Civil Engineering and Architecture, University of Jinan, Jinan 250022, China
Interests: electro biological coupling technology; electrocatalytic oxidation; electro adsorption desalination; emerging contaminants

Special Issue Information

Dear Colleagues,

Today, the overuse and misuse of antibiotics do not only lead to antimicrobial resistance, but also to the pollution of human settlement environments. As a result, water pollution caused by antibiotics is becoming more and more significant. Recently, there has been a number of works showing that antibiotics could be removed from the water environment via novel adsorption or oxidation materials and novel physical/chemical/biological processes. These advancements in antibiotic-removal technology can provide new ideas and references for practical water treatment.

This Special Issue on “Novel Materials/Technologies for the Adsorption and Removal of Antibiotics from Aqueous Solution” seeks high-quality works focusing on the latest novel materials and technologies for the removal of antibiotics from water. Topics include but are not limited to:

  • Novel adsorption materials (ceramic, carbon and/or composites) and performance application;
  • Novel physical/chemical/biological technologies for antibiotic removal;
  • Antibiotic-removal process mechanism, application, and modeling;
  • Traceability and risk assessment for antibiotic contaminants.

Dr. Zhaoyang Wang
Prof. Dr. Hao Xu
Prof. Dr. Yan Feng
Guest Editors

Manuscript Submission Information

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Keywords

  • antibiotics
  • water environment
  • wastewater
  • water body
  • drinking water
  • adsorption
  • removal

Published Papers (9 papers)

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Research

16 pages, 2727 KiB  
Article
Synergetic Adsorption of Dyes in Water by Three-Dimensional Graphene and Manganese Dioxide (PU@RGO@MnO2) Structures for Efficient Wastewater Purification
by Shirong Zong, Jijun Jiang, Guodong Wang, Jin Zhong, Chunlan Tang, Lingxiang Zhou, Fan Yang and Wei Yan
Processes 2024, 12(1), 169; https://doi.org/10.3390/pr12010169 - 10 Jan 2024
Viewed by 477
Abstract
The improper discharge of industrial wastewater causes severe environmental pollution and the textile industry’s dye usage contributes significantly to industrial wastewater pollution. Hence, an effective method for removing the harmful substance methylene blue (MB) from dye wastewater is proposed. This method adopts a [...] Read more.
The improper discharge of industrial wastewater causes severe environmental pollution and the textile industry’s dye usage contributes significantly to industrial wastewater pollution. Hence, an effective method for removing the harmful substance methylene blue (MB) from dye wastewater is proposed. This method adopts a three-dimensional graphene composite material based on manganese dioxide (MnO2), named polyurethane@ reduced graphene oxide@ MnO2 (PU@RGO@MnO2). First, graphene is prepared with hydrazine hydrate as a reducing agent and polyurethane as a framework. MnO2 nanoparticles are synthesized by the reaction of potassium permanganate (KMnO4) with carbon. These nanoparticles are then loaded onto the three-dimensional framework to create the composite material. Finally, adsorption and removal experiments for MB are conducted to compare the performance of the composite material. The results indicate that the graphene based on the polyurethane framework exhibits favorable mechanical properties. The unique three-dimensional lattice structure provides abundant active sites for loading MnO2 nanoparticles, significantly increasing the contact area between the adsorbent and MB solution and thus improving the adsorbent utilization rate (reaching 94%). The nanoparticles synthesized through the reaction of KMnO4 with carbon effectively suppress the agglomeration phenomenon. Additionally, the introduction of dynamic adsorption and dynamic removal modes, aided by a water pump, substantially enhances the adsorption and removal rates, showcasing excellent performance. The research on a multi-porous three-dimensional structure holds significant practical value in water treatment, offering a new research direction for dye wastewater treatment. Full article
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13 pages, 2572 KiB  
Article
Improved Laccase Encapsulation in Copper-Doped Zeolitic Imidazolate Framework-8 for Reactive Black 5 Decolorization
by Shuyu Yu, Yibo Lu, Dandan Du, Rankun Wu, Xiang Ji and Hao Li
Processes 2023, 11(10), 2937; https://doi.org/10.3390/pr11102937 - 10 Oct 2023
Viewed by 798
Abstract
As the largest group of synthetic dyes, azo dyes can pose various health and environmental risks due to their widespread use and challenging degradation. Laccases are efficient green biocatalysts for the degradation of organic pollutants. Herein, we report the in situ packaging of [...] Read more.
As the largest group of synthetic dyes, azo dyes can pose various health and environmental risks due to their widespread use and challenging degradation. Laccases are efficient green biocatalysts for the degradation of organic pollutants. Herein, we report the in situ packaging of laccase in copper-doped zeolitic imidazolate framework-8 (ZIF-8) for the decolorization of reactive black 5, which is a model azo dye. The immobilization support (Cu5/mZIF-8) was obtained via lowering the precursor ratio of ZIF-8 and incorporating copper ions during the synthesis process. Cu5/mZIF-8 were found to be nanospheres with an average diameter of around 150 nm. Laccase encapsulated in Cu5/mZIF-8 showed an activity recovery of 75.6%, which was 2.2 times higher than that of the laccase embedded in ZIF-8. Meanwhile, the immobilized laccase (Lac@Cu5/mZIF-8) showed a higher catalytic activity in organic solvents than that of the free enzyme. In the presence of a mediator, Lac@Cu5/mZIF-8 could remove 95.7% of reactive black 5 in 40 min. After four consecutive cycles, the dye decolorization efficiency declined to 28%. About four transformation products of reactive black 5 were identified via LC-MS analysis, and the potential decolorization mechanism was proposed. The results indicated that the immobilized laccase could be used as an efficient biocatalyst in dye decolorization. Full article
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17 pages, 5604 KiB  
Article
Investigating the Performance and Stability of Fe3O4/Bi2MoO6/g-C3N4 Magnetic Photocatalysts for the Photodegradation of Sulfonamide Antibiotics under Visible Light Irradiation
by Ke Li, Miaomiao Chen, Lei Chen, Wencong Xue, Wenbo Pan and Yanchao Han
Processes 2023, 11(6), 1749; https://doi.org/10.3390/pr11061749 - 08 Jun 2023
Cited by 1 | Viewed by 1222
Abstract
In this study, an Fe3O4/Bi2MoO6/g-C3N4 magnetic composite photocatalyst was synthesized for the visible-light-driven photocatalytic degradation of sulfonamide antibiotics, specifically sulfamerazine (SM1). Characterization techniques, including X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray [...] Read more.
In this study, an Fe3O4/Bi2MoO6/g-C3N4 magnetic composite photocatalyst was synthesized for the visible-light-driven photocatalytic degradation of sulfonamide antibiotics, specifically sulfamerazine (SM1). Characterization techniques, including X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), photoluminescence spectroscopy (PL), UV-vis diffuse reflectance spectra (UV-vis), and the use of a vibrating sample magnetometer (VSM), were employed to analyze the fabricated samples. The composite exhibited efficient visible-light absorption and charge separation, with optimal photocatalytic performance achieved at a pH value of 9.0. The study reveals the importance of solution pH in the degradation process and the potential applicability of the composite for efficient magnetic separation and recycling in photocatalytic processes. The Fe3O4/Bi2MoO6/g-C3N4 magnetic composite photocatalyst demonstrated exceptional stability and recyclability, maintaining a high degradation efficiency of over 87% after five consecutive cycles. An XRD analysis conducted after the cycling tests confirmed that the composite’s composition and chemical structure remained unchanged, further supporting its chemical stability. This investigation offers valuable insights into the photocatalytic degradation of sulfonamide antibiotics using magnetic composite photocatalysts and highlights the potential of the Fe3O4/Bi2MoO6/g-C3N4 composite for practical applications in environmental remediation. Full article
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12 pages, 2881 KiB  
Article
The Methods and Characteristics of the Electrochemical Oxidation Degradation of HMX
by Yishi Qian, Xiaosheng Jing, Wei Yan and Peng Xi
Processes 2023, 11(5), 1344; https://doi.org/10.3390/pr11051344 - 26 Apr 2023
Viewed by 1090
Abstract
Octagon (HMX) is a typical organic pollutant of explosives in the surrounding environments of military factories, and it is widely regarded as a carcinogen which may enter the human body through wastewater and atmospheric exposure, resulting in potential health risks. Therefore, this paper [...] Read more.
Octagon (HMX) is a typical organic pollutant of explosives in the surrounding environments of military factories, and it is widely regarded as a carcinogen which may enter the human body through wastewater and atmospheric exposure, resulting in potential health risks. Therefore, this paper studies the degradation of HMX by electrochemical oxidation. In this study, an electrochemical system was built using a copper plate as the cathode and a Ti/PbO2 electrode as the anode. The effects of various process variables, such as the initial pH value, the current density, and the distance between the electrodes, were investigated in relation to HMX degradation. Following this, performance optimization and intermediate analysis were carried out, along with an estimation of the energy consumption of HMX deterioration in various operating situations. The experimental results in this paper show that when the electrolyte concentration is 0.25 mol/L, the current density is 70 mA/cm2, the electrode spacing is 1.0 cm, and the initial pH is 5.0. Electrochemical oxidation has a better treatment efficiency for pollutants, and the removal rate reaches 81.2%. The findings of kinetic research reveal that the electrochemical oxidation degradation process of HMX follows quasi-first-order kinetics, and protein stress and Deoxyribo Nucleic Acid (DNA) loss stress are significantly different from other stress types throughout the whole degradation process. HMX degradation solution causes damage to protein transcription or expression. However, some genes of oxidative stress are continuously up-regulated, because H2O2 and OH produced by electrochemical oxidation cause a strong response to oxidative stress in cells. The research findings in this report offer crucial guidance and suggestions for the industrialization of HMX wastewater treatment. Full article
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14 pages, 3246 KiB  
Article
Investigating the Effect of Bi2MoO6/g-C3N4 Ratio on Photocatalytic Degradation of Sulfadiazine under Visible Light
by Ke Li, Miaomiao Chen, Lei Chen, Songying Zhao, Wencong Xue and Yanchao Han
Processes 2023, 11(4), 1059; https://doi.org/10.3390/pr11041059 - 31 Mar 2023
Cited by 1 | Viewed by 1417
Abstract
In this study, a series of Bi2MoO6/g-C3N4 composites were prepared through a wet-impregnation method, and their photocatalytic properties were investigated for the degradation of sulfadiazine (SDZ) under visible light irradiation. Physical and chemical characterizations were carried [...] Read more.
In this study, a series of Bi2MoO6/g-C3N4 composites were prepared through a wet-impregnation method, and their photocatalytic properties were investigated for the degradation of sulfadiazine (SDZ) under visible light irradiation. Physical and chemical characterizations were carried out using X-ray diffraction (XRD), scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FT-IR), photoluminescence spectroscopy (PL), UV-vis diffuse reflectance spectra (UV-vis), and electrochemical impedance spectra (EIS). Compared to pure g-C3N4, the introduction of Bi2MoO6 significantly enhanced the visible light responsive photocatalytic activity, with the 1:32 Bi2MoO6/g-C3N4 composite exhibiting the highest photodegradation efficiency towards SDZ under visible light irradiation with a photocatalytic efficiency of 93.88% after 120 min of visible light irradiation. The improved photocatalytic activity can be attributed to the formation of a heterojunction between Bi2MoO6 and g-C3N4, which promotes the transfer of photogenerated electron-hole pairs, thereby elevating its photocatalytic activity. The results suggest that Bi2MoO6/g-C3N4 composites have potential application for the degradation of sulfonamides in aquatic environments. Full article
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14 pages, 4215 KiB  
Article
Synthesis of MRGO@ZIF-7-Based Molecular Imprinted Polymer by Surface Polymerization for the Fast and Selective Removal of Phenolic Endocrine-Disrupting Chemicals from Aqueous Environments
by Ying Li, Yang Li, Zhu Ding, Dong Wan, Zhong Gao, Yu Sun and Ying Liu
Processes 2023, 11(4), 1000; https://doi.org/10.3390/pr11041000 - 25 Mar 2023
Viewed by 1239
Abstract
In this study, Zn(NO3)2·6H2O was selected as the metal source, and ZIF-7-modified magnetic graphene-based matrix materials (MRGO@ZIF-7) were prepared by in situ growth. ZIF-7 modified magnetic graphene-based molecular imprinting complexes (MRGO@ZIF7-MIP) were successfully synthesized by a surface [...] Read more.
In this study, Zn(NO3)2·6H2O was selected as the metal source, and ZIF-7-modified magnetic graphene-based matrix materials (MRGO@ZIF-7) were prepared by in situ growth. ZIF-7 modified magnetic graphene-based molecular imprinting complexes (MRGO@ZIF7-MIP) were successfully synthesized by a surface molecular imprinting technique using bisphenol A (BPA) as the template molecule. The obtained experimental materials were characterized by X-ray diffraction (XRD), Brunner–Emmet–Teller (BET) analysis, scanning electron microscopy (SEM), transmission electron microscopy (TEM), vibrating sample magnetometry (VSM), and X-ray photoelectron spectroscopy (XPS). The proper adsorption and selective recognition ability of the MRGO@ZIF7-MIP were studied by an equilibrium adsorption method. The obtained MRGO@ZIF7-MIP showed significant molecular recognition of bisphenol A (BPA) and good selectivity and reproducibility for BPA in different aqueous environments such as drinking water, river water, and lake water. These properties make this material potentially applicable for the efficient removal of phenolic endocrine disruptors in real water environments. Full article
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14 pages, 3028 KiB  
Article
Synthesis of g-C3N4 Derived from Different Precursors for Photodegradation of Sulfamethazine under Visible Light
by Ke Li, Miaomiao Chen, Lei Chen, Songying Zhao, Wencong Xue, Zixuan Han and Yanchao Han
Processes 2023, 11(2), 528; https://doi.org/10.3390/pr11020528 - 09 Feb 2023
Cited by 10 | Viewed by 2522
Abstract
In this study, a series of g-C3N4 nanosheets were prepared by various thermal oxidative etching times from four different precursors (urea, melamine, dicyandiamide and thiourea). The physicochemical properties of these g-C3N4 nanosheets were analyzed in detail using [...] Read more.
In this study, a series of g-C3N4 nanosheets were prepared by various thermal oxidative etching times from four different precursors (urea, melamine, dicyandiamide and thiourea). The physicochemical properties of these g-C3N4 nanosheets were analyzed in detail using scanning electron microscopy (SEM), X-ray diffraction (XRD), photoluminescence emission spectra, Fourier transform infrared spectroscopy (FTIR), Brunauer–Emmett–Teller (BET) analysis and ultraviolet-visible diffuse reflectance. The results revealed that the g-C3N4 nanosheets obtained a thinner layer thickness and larger specific surface area, with an extension of thermal oxidative etching time. Meanwhile, sulfamethazine (SMZ), one of the most widely used sulfonamides, was used to evaluate the photocatalyst activity of the g-C3N4 nanosheets prepared in this study. Compared to other g-C3N4 nanosheets, urea-derived g-C3N4 nanosheets under 330 min thermal oxidative etching showed the highest photocatalytic activity for SMZ under visible light. In conclusion, our study provides detailed insights into the synthesis and characterization of g-C3N4 nanosheets prepared from various precursors and highlights the importance of thermal oxidative etching time in determining the photocatalytic activity of these materials. Full article
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12 pages, 4693 KiB  
Article
In-Situ Hydrothermal Synthesis of Ag3PO4/g-C3N4 Nanocomposites and Their Photocatalytic Decomposition of Sulfapyridine under Visible Light
by Ke Li, Miaomiao Chen, Lei Chen, Songying Zhao, Wencong Xue, Zixuan Han, Yanchao Han, Fuguo Zhang, Yu Yan and Yanhong Dong
Processes 2023, 11(2), 375; https://doi.org/10.3390/pr11020375 - 25 Jan 2023
Cited by 2 | Viewed by 1335
Abstract
Highly efficient visible-light-driven heterogeneous photocatalyst Ag3PO4/g-C3N4 with different weight ratios from Ag3PO4 to g-C3N4 were synthesized by a facile in situ hydrothermal method and characterized by X-ray diffraction (XRD), scanning [...] Read more.
Highly efficient visible-light-driven heterogeneous photocatalyst Ag3PO4/g-C3N4 with different weight ratios from Ag3PO4 to g-C3N4 were synthesized by a facile in situ hydrothermal method and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectrometry (FTIR), photoluminescence spectra (PL), UV–vis diffuse reflectance spectra (UV-Vis), and electrochemical impedance spectra (EIS). Under visible light irradiation, Ag3PO4/g-C3N4 showed very excellent photocatalytic activity for sulfapyridine (SP) which is one of the widely used sulfonamide antibiotics. When the ratio from Ag3PO4 to g-C3N4 was 1:2, the degradation rate of SP at 120 min was found to be 94.1%, which was superior to that of pure Ag3PO4 and pure g-C3N4. Based on the experimental results, the possible enhanced photocatalytic mechanism of Ag3PO4/g-C3N4 was proposed. Full article
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22 pages, 13283 KiB  
Article
Separation and Removal of Radionuclide Cesium from Water by Biodegradable Magnetic Prussian Blue Nanospheres
by Shanshan Feng, Jie Ni, Xun Cao, Jingshuai Gao, Lu Yang, Wenhao Jia, Feng Chen, Sheng Feng, Yao Zhang and Fang Ma
Processes 2022, 10(12), 2492; https://doi.org/10.3390/pr10122492 - 23 Nov 2022
Cited by 5 | Viewed by 1280
Abstract
As the main component of radioactive wastewater, the cesium ion has seriously endangered the environment and human health. Prussian blue nanoparticles (PB NPs) are used as adsorbents for the purification of cesium-containing wastewater because of their ability to selectively adsorb cesium ions. In [...] Read more.
As the main component of radioactive wastewater, the cesium ion has seriously endangered the environment and human health. Prussian blue nanoparticles (PB NPs) are used as adsorbents for the purification of cesium-containing wastewater because of their ability to selectively adsorb cesium ions. In this work, novel magnetic Prussian blue nanospheres (MPBNs) were developed from polylactic acid nanospheres as a carrier, loaded with Fe3O4 nanoparticles (Fe3O4 NPs) inside and PB NPs outside for the removal of cesium ions with the help of magnetic separation. Meanwhile, the effects on the adsorption efficiency of MPBNs, such as pH, time, temperature and initial concentration of cesium ion solution, were studied. The adsorption isotherms, kinetic models and adsorption thermodynamics were investigated to research the absorption mechanism. The results showed that MPBNs were spherical with a rough surface, and their particle size, iron content and saturation magnetization were 268.2 ± 1.4 nm, 40.01% and 41.71 emu/g, which can be recovered by magnetic separation. At 293 K, MPBNs could reduce the cesium ion solution from 40 mg/L to 4.8 mg/L, and its cesium ion removal rate and adsorption capacity were 82.46% and 16.49 mg/g, respectively. The optimum pH of MPBNs for cesium ion adsorption was 5~9, the adsorption equilibrium time was 60 min, and the maximum adsorption capacity was 17.03 mg/g. In addition, MPBNs were separated rapidly by an external magnetic field, and the adsorption process was an endothermic reaction. The adsorption isotherm and kinetics of MPBNs were in accordance with the Freundlich model and quasi-second-order fitting model, respectively, and the adsorption process of MPBNs was controlled by the diffusion step in particles. Notably, these MPBNs could be effectively separated from water by a magnetic field, facilitating engineering applications in cesium-containing wastewater. Full article
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