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1.
Environ Res ; 246: 118564, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38417658

ABSTRACT

Metal-organic frameworks (MOFs) have shown great prospects in wastewater remediation. However, the easy aggregation, difficult separation and inferior reusability greatly limit their large-scale application. Herein, we proposed a facile, green and low-cost strategy to construct robust and stable MOF-based hydrogel beads (Fe-BTC-HBs) in a gram scale, and employed them to remove antibiotics from wastewater. As a result, the Fe-BTC-HBs demonstrated outstanding adsorption capacity for both ofloxacin (OFL) and tetracycline (TC) (281.17 mg/g for OFL and 223.60 mg/g for TC) under a near-neutral environment. The main adsorption mechanisms of OFL and TC were hydrogen bonding and π-π stacking interaction. Owing to its macroscopic granule and stable structure, Fe-BTC-HBs can be separated rapidly from wastewater after capturing antibiotics, and more than 85% adsorption capacity still remained after six cycles, while the powdered Fe-BTC only showed less than 6% recovery efficiency with massive weight loss (around 92%). In real industrial effluent, the adsorption performance of Fe-BTC-HBs toward two antibiotics exhibited negligible decreases (2.9% for OFL and 2.2% for TC) compared with that in corresponding solutions. Furthermore, Fe-BTC-HBs also had appealing economic and environmental benefit. Overall, the macro-manufactured MOF beads have the promising potential for the large-scale wastewater treatment.


Subject(s)
Metal-Organic Frameworks , Water Pollutants, Chemical , Anti-Bacterial Agents/chemistry , Wastewater , Water Pollutants, Chemical/chemistry , Tetracycline , Adsorption , Kinetics
2.
J Environ Manage ; 354: 120312, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38340667

ABSTRACT

The increased use of antibiotics by humans for various purposes has left the environment polluted. Antibiotic pollution remediation is challenging because antibiotics exist in trace amounts and only highly sensitive detection techniques could be used to quantify them. Nevertheless, their trace quantity is not a hindrance to their transfer along the food chain, causing sensitization and the development of antibiotic resistance. Despite an increase in the literature on antibiotic pollution and the development and transfer of antibiotic-resistant genes (ARGs), little attention has been given to the behavior of antibiotics at the soil-solution interface and how this affects antibiotic adsorption-desorption interactions and subsequent uptake and transformation by plants. Thus, this review critically examines the interactions and possible degradation mechanisms of antibiotics in soil and the link between antibiotic soil-solution chemistry and uptake by plants. Also, different factors influencing antibiotic mobility in soil and the transfer of ARGs from one organism to another were considered. The mechanistic and critical analyses revealed that: (a) the charge characteristics of antibiotics at the soil-root interface determine whether they are adsorbed to soil or taken up by plants; (b) antibiotics that avoid soil colloids and reach soil pore water can be absorbed by plant roots, but their translocation to the stem and leaves depends on the ionic state of the molecule; (c) few studies have explored how plants adapt to antibiotic pollution and the transformation of antibiotics in plants; and (d) the persistence of antibiotics in cropland soils can be influenced by the content of soil organic matter, coexisting ions, and fertilization practices. Future research should focus on the soil/solution-antibiotic-plant interactions to reveal detailed mechanisms of antibiotic transformation by plants and whether plant-transformed antibiotics could be of environmental risk.


Subject(s)
Anti-Bacterial Agents , Soil Pollutants , Humans , Anti-Bacterial Agents/metabolism , Soil , Soil Pollutants/chemistry , Plants/metabolism , Environmental Pollution/analysis
3.
Small ; 19(26): e2301200, 2023 06.
Article in English | MEDLINE | ID: mdl-36942696

ABSTRACT

Techniques beyond crystal engineering are critical for manufacturing covalent organic frameworks (COFs) and to explore them for advanced applications. However, COFs are normally obtained as insoluble, unmeltable, and thus nonprocessible microcrystalline powders. Therefore, it is a significant challenge to implement COFs into larger architectures and structural control on different length scales. Herein, a facile strategy is presented to prepare flexible COF nanofiber membranes by in-situ growth of COFs on polyacrylonitrile (PAN) nanofiber substrates via a reversible polycondensation-termination approach. The obtained PAN@COF nanofiber membranes with vertically aligned COF nanoplates combine a large functional surface with efficient mass transport, thus making it a promising adsorbent, for example, for water purification. The antibiotic pollutant ofloxacin (OFX) is removed from water with a superior absorption capacity of ≈236 mg g-1 and removal efficiency as high as 98%. The here presented in-situ growth of COFs on nanofiber membranes can be extended to various Schiff base-derived COF materials with different compositions, providing a highly efficient way to construct flexible COF-based membranes for several applications.


Subject(s)
Metal-Organic Frameworks , Nanofibers , Anti-Bacterial Agents , Adsorption , Commerce
4.
Mar Pollut Bull ; 205: 116576, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38875969

ABSTRACT

The objective of this study was to determine microplastic-antibiotic interaction by examining how heat-activated persulfate decomposed polyamide adsorbed antibiotics and explored the environmental consequences of treated water. Sulfate radicals roughened the microplastic surfaces, significantly enhancing the adsorption capacity of polyamide. The kinetic and isotherm studies provided confirmation that electrostatic interactions were the primary mechanisms, with a minor contribution from H-bonding, highlighting that antibiotic adsorption was prone to occur, especially on the aged surface. Thermodynamic data indicated that the process was spontaneous and exothermic. The results showed significant negative effects of treated water on seed germination, copepod survival, and cell lines at only a higher concentration, due to a decrease in pH and the potential presence of polymer degradates. Our findings revealed the significant impact of decomposed polyamide on the antibiotic adsorption and offered insight into the potential harm that microplastic-treated water might cause to aquatic and marine ecosystems.


Subject(s)
Anti-Bacterial Agents , Microplastics , Water Pollutants, Chemical , Water Pollutants, Chemical/toxicity , Adsorption , Anti-Bacterial Agents/chemistry , Microplastics/toxicity , Hot Temperature , Animals , Sulfates/chemistry
5.
Article in English | MEDLINE | ID: mdl-38528220

ABSTRACT

Emerging contaminants are diverse ecotoxic materials requiring unique treatment for removal. Asphaltenes are environmentally hazardous carbon-rich solid waste product of the petroleum industry. In the current work, asphaltene-derived activated carbon (AC) was loaded with silver (Ag/AC) and used to remove amoxicillin (AMX) and tetracycline (TC) from aqueous phase. The prepared Ag/AC was characterised using FESEM, FTIR, XRD and surface area analysis. The FESEM micrographs confirmed the spherical silver nanoparticle-laden porous AC, and the BET surface area was found to be 213 m2/g. Batch adsorption studies were performed, and the equilibrium data were fit into adsorption isotherm and kinetic models. The Ag/AC exhibited superior monolayer adsorption capacity of 1012 mg/g and 770 mg/g for AMX and TC, respectively. The continuous column studies were also performed to evaluate the breakthrough parameters. Furthermore, the antimicrobial activity of the adsorbent was evaluated using zone of inhibition studies. Ag/AC was found to have an 8-mm-diameter zone of microbial inhibition. The obtained results showed that Ag/AC was a promising material for the removal of antibiotics and inhibition of resistance-developed mutated microbes in effluent water.

6.
Environ Pollut ; 360: 124588, 2024 Nov 01.
Article in English | MEDLINE | ID: mdl-39033844

ABSTRACT

Antibiotics present in human urine pose significant challenges for the use of urine-based fertilizers in agriculture. This study introduces a novel two-stage approach utilizing distinct biochar types to mitigate this concern. Initially, a modified biochar selectively adsorbed azithromycin (AZ), ciprofloxacin (CPX), sulfamethoxazole (SMX), trimethoprim (TMP), and tetracycline (TC) from human urine. Subsequently, a separate pristine biochar was employed to capture nutrients. Biochar, derived from sewage sludge and pyrolyzed at 550 and 700 °C, was modified using dimethyl sulfoxide, deep eutectic solvent, and ionic liquid to enhance antibiotic removal in the first stage. The modifications introduced hydrophilic functional groups (-OH/-COOH), which favor antibiotic adsorption. Adsorption kinetics followed the pseudo-second-order model, with the Langmuir isotherm model best describing the adsorption data. The maximum adsorption capacities for AZ, CPX, SMX, TMP, and TC after the modification were 196.08, 263.16, 81.30, 370.37, and 833.33 µg/g, respectively. Pristine biochar exhibited a superior ammonia adsorption capacity compared to the modified biochar. Hydrogen bonding, electrostatic attraction, and chemisorption drove antibiotic adsorption on the modified biochar. Regeneration efficiency declined due to solvent accumulation and potential byproduct formation on the biochar surface (<30% removal capacity after three cycles). This study presents innovative biochar modification strategies for selective antibiotic adsorption, laying the groundwork for environmentally friendly urine-based fertilizers in agriculture.


Subject(s)
Anti-Bacterial Agents , Charcoal , Deep Eutectic Solvents , Dimethyl Sulfoxide , Ionic Liquids , Charcoal/chemistry , Adsorption , Humans , Ionic Liquids/chemistry , Anti-Bacterial Agents/urine , Anti-Bacterial Agents/chemistry , Dimethyl Sulfoxide/chemistry , Deep Eutectic Solvents/chemistry , Sulfamethoxazole/urine , Sulfamethoxazole/chemistry , Water Pollutants, Chemical/chemistry , Trimethoprim/urine , Trimethoprim/chemistry , Ciprofloxacin/urine , Ciprofloxacin/chemistry , Tetracycline/chemistry , Tetracycline/urine , Azithromycin/chemistry , Azithromycin/urine , Fertilizers , Kinetics
7.
J Colloid Interface Sci ; 639: 59-67, 2023 Jun.
Article in English | MEDLINE | ID: mdl-36804793

ABSTRACT

Highly effective removal of antibiotics from aqueous solution is of importance while still faces challenge. Herein, we report a novel metal-organic framework (MOF) adsorbent, MOF-808-SIPA (SIPA, 5-sulfoisophthalic acid), constructed via post-synthesis exchange strategy. On the basis, dual active groups including sulfonic acid and carboxyl groups are successfully introduced. The novel MOF-808-SIPA exhibits a high adsorption capacity of 287.1 mg g-1 for moxifloxacin hydrochloride (MOX·HCl), superior to that (174.6 mg g-1) of the pristine MOF-808-AA (AA, acetic acid). Besides, MOF-808-SIPA shows rapid adsorption equilibrium of âˆ¼ 30 min, strong anti-interference ability from pH and inorganic ions, and feasible regeneration. The superiority renders MOF-808-SIPA a potential adsorbent for MOX removal. Density function theory (DFT) calculation and experiment confirm that H-bond interaction contributes largely to the excellent adsorption in MOF-808-SIPA. Our work provides a guideline for designing high-efficiency MOF-based adsorbent.

8.
Int J Biol Macromol ; 235: 123826, 2023 Apr 30.
Article in English | MEDLINE | ID: mdl-36828094

ABSTRACT

Tetracycline (TC) antibiotic-related water pollution directly threatens human health and ecosystems. Here, a zinc ferrite/chitosan-curdlan (ZNF/CHT-CRD) magnetic composite was prepared via a co-precipitation method to be used as a novel, green adsorbent for TC removal from water. Benefiting from a multitude of functional groups, CRD was first crosslinked with CHT and then magnetized with ZNF to provide an easy separation from the solution with an external magnetic force. The successful synthesis and magnetization of the composite were verified with different characterization techniques. The effect of solution pH and composite dosage was carefully evaluated. The optimum solution pH and composite dosage were 6 and 0.65 g/L, respectively, with complete TC removal. The adsorption process by the magnetic composite followed the pseudo-first-order kinetics and Langmuir isotherm models. The maximum adsorption capacity determined from the Langmuir model was 371.42 mg/g at 328 K. Thermodynamic parameters indicated endothermic and spontaneous adsorption. Meanwhile, the composite could be readily separated from the aqueous solution thanks to its magnetic property. Then, it was regenerated with acetone and ethanol to be reused for five more successive cycles. Interestingly, the prepared adsorbent was highly stable and performant in removing TC, maintaining approximately 90 % of its first-cycle adsorption capacity. The adsorption mechanism was primarily attributed to electrostatic and hydrogen bonding attractions. Overall, the currently developed adsorbent could be a more favorable, efficient, and cost-effective candidate than other magnetic chitosan-based composites. These features make it applicable for treating water contaminated with various pharmaceutical pollutants with high separation efficiency and easy recovery under successive adsorption-desorption cycles.


Subject(s)
Chitosan , Water Pollutants, Chemical , Water Purification , Humans , Zinc , Chitosan/chemistry , Adsorption , Water/chemistry , Ecosystem , Anti-Bacterial Agents , Pharmaceutical Preparations , Tetracyclines , Water Pollutants, Chemical/chemistry , Kinetics , Hydrogen-Ion Concentration , Water Purification/methods
9.
Antibiotics (Basel) ; 11(9)2022 Sep 16.
Article in English | MEDLINE | ID: mdl-36140040

ABSTRACT

Excessive antibiotic use in veterinary applications has resulted in water contamination and potentially poses a serious threat to aquatic environments and human health. The objective of the current study was to quantify carbonized leonardite (cLND) adsorption capabilities to remove sulfamethoxazole (SMX)- and enrofloxacin (ENR)-contaminated water and to determine the microbial activity of ENR residuals on cLND following adsorption. The cLND samples prepared at 450 °C and 850 °C (cLND450 and cLND550, respectively) were evaluated for structural and physical characteristics and adsorption capabilities based on adsorption kinetics and isotherm studies. The low pyrolysis temperature of cLND resulted in a heterogeneous surface that was abundant in both hydrophobic and hydrophilic functional groups. SMX and ENR adsorption were best described using a pseudo-second-order rate expression. The SMX and ENR adsorption equilibrium data on cLND450 and cLND550 revealed their better compliance with a Langmuir isotherm than with four other models based on 2.3-fold higher values of qmENR than qmSMX. Under the presence of the environmental interference, the electrostatic interaction was the main contributing factor to the adsorption capability. Microbial activity experiments based on the growth of Staphylococcus aureus ATCC 25923 revealed that cLND could successfully adsorb and subsequently retain the adsorbed antibiotic on the cLND surface. This study demonstrated the potential of cLND550 as a suitable low-cost adsorbent for the highly efficient removal of antibiotics from water.

10.
Antibiotics (Basel) ; 10(2)2021 Feb 15.
Article in English | MEDLINE | ID: mdl-33672037

ABSTRACT

Antibiotics used in agriculture may reach the environment and stimulate the development and dissemination of antibiotic resistance in the soil microbiome. However, the scope of this phenomenon and the link to soil properties needs to be elucidated. This study compared the short-term effects of a range of gentamicin concentrations on the microbiome and resistome of bacterial enrichments and microcosms of an agricultural soil using a metagenomic approach. Gentamicin impact on bacterial biomass was roughly estimated by the number of 16SrRNA gene copies. In addition, the soil microbiome and resistome response to gentamicin pollution was evaluated by 16SrRNA gene and metagenomic sequencing, respectively. Finally, gentamicin bioavailability in soil was determined. While gentamicin pollution at the scale of µg/g strongly influenced the bacterial communities in soil enrichments, concentrations up to 1 mg/g were strongly adsorbed onto soil particles and did not cause significant changes in the microbiome and resistome of soil microcosms. This study demonstrates the differences between the response of bacterial communities to antibiotic pollution in enriched media and in their environmental matrix, and exposes the limitations of culture-based studies in antibiotic-resistance surveillance. Furthermore, establishing links between the effects of antibiotic pollution and soil properties is needed.

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