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1.
Chemosphere ; 358: 142136, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38692363

RESUMEN

The soil-water interface is replete with photic biofilm and iron minerals; however, the potential of how iron minerals promote biotic nitrate removal is still unknown. This study investigates the physiological and ecological responses of photic biofilm to hematite (Fe2O3), in order to explore a practically feasible approach for in-situ nitrate removal. The nitrate removal by photic biofilm was significantly higher in the presence of Fe2O3 (92.5%) compared to the control (82.8%). Results show that the presence of Fe2O3 changed the microbial community composition of the photic biofilm, facilitates the thriving of Magnetospirillum and Pseudomonas, and promotes the growth of photic biofilm represented by the extracellular polymeric substance (EPS) and the content of chlorophyll. The presence of Fe2O3 also induces oxidative stress (•O2-) in the photic biofilm, which was demonstrated by electron spin resonance spectrometry. However, the photic biofilm could improve the EPS productivity to prevent the entrance of Fe2O3 to cells in the biofilm matrix and mitigate oxidative stress. The Fe2O3 then promoted the relative abundance of Magnetospirillum and Pseudomonas and the activity of nitrate reductase, which accelerates nitrate reduction by the photic biofilm. This study provides an insight into the interaction between iron minerals and photic biofilm and demonstrates the possibility of combining biotic and abiotic methods to improve the in-situ nitrate removal rate.


Asunto(s)
Biopelículas , Compuestos Férricos , Nitratos , Compuestos Férricos/metabolismo , Compuestos Férricos/química , Nitratos/metabolismo , Estrés Oxidativo , Pseudomonas/fisiología , Pseudomonas/metabolismo
2.
Anal Chim Acta ; 1306: 342598, 2024 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-38692791

RESUMEN

BACKGROUND: Carbon-based nanozymes have recently received enormous concern, however, there is still a huge challenge for inexpensive and large-scale synthesis of magnetic carbon-based "Two-in-One" mimics with both peroxidase (POD)-like and laccase-like activities, especially their potential applications in multi-mode sensing of antibiotics and neurotransmitters in biofluids. Although some progresses have been made in this field, the feasibility of biomass-derived carbon materials with both POD-like and laccase-like activities by polyatomic doping strategy is still unclear. In addition, multi-mode sensing platform can provide a more reliable result because of the self-validation, self-correction and mutual agreement. Nevertheless, the use of magnetic carbon-based nanozyme sensors for the multi-mode detection of antibiotics and neurotransmitters have not been investigated. RESULTS: We herein report a shrimp shell-derived N, O-codoped porous carbon confined magnetic CuFe2O4 nanosphere with outstanding laccase-like and POD-like activities for triple-mode sensing of antibiotic d-penicillamine (D-PA) and chloramphenicol (CPL), as well as colorimetric detection of neurotransmitters in biofluids. The magnetic CuFe2O4/N, O-codoped porous carbon (MCNPC) armored mimetics was successfully fabricated using a combined in-situ coordination and high-temperature crystallization method. The synthesized MCNPC composite with superior POD-like activity can be used for colorimetric/temperature/smartphone-based triple-mode detection of D-PA and CPL in goat serum. Importantly, the MCNPC nanozyme can also be used for colorimetric analysis of dopamine and epinephrine in human urine. SIGNIFICANCE: This work not only offered a novel strategy to large-scale, cheap synthesize magnetic carbon-based "Two-in-One" armored mimetics, but also established the highly sensitive and selective platforms for triple-mode monitoring D-PA and CPL, as well as colorimetric analysis of neurotransmitters in biofluids without any tanglesome sample pretreatment.


Asunto(s)
Antibacterianos , Carbono , Cobre , Neurotransmisores , Carbono/química , Antibacterianos/análisis , Antibacterianos/orina , Antibacterianos/sangre , Neurotransmisores/orina , Neurotransmisores/análisis , Neurotransmisores/sangre , Porosidad , Cobre/química , Humanos , Nanosferas/química , Colorimetría/métodos , Compuestos Férricos/química , Materiales Biomiméticos/química , Animales , Técnicas Biosensibles/métodos , Cloranfenicol/análisis , Cloranfenicol/orina , Límite de Detección
3.
J Environ Sci (China) ; 144: 159-171, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38802228

RESUMEN

Dissolved organic matter (DOM) is a heterogeneous pool of compounds and exhibits diverse adsorption characteristics with or without phosphorous (P) competition. The impacts of these factors on the burial and mobilization of organic carbon and P in aquatic ecosystems remain uncertain. In this study, an algae-derived DOM (ADOM) and a commercially available humic acid (HA) with distinct compositions were assessed for their adsorption behaviors onto iron (oxy)hydroxides (FeOx), both in the absence and presence of phosphate. ADOM contained less aromatics but more protein-like and highly unsaturated structures with oxygen compounds (HUSO) than HA. The adsorption capacity of FeOx was significantly greater for ADOM than for HA. Protein-like and HUSO compounds in ADOM and humic-like compounds and macromolecular aromatics in HA were preferentially adsorbed by FeOx. Moreover, ADOM demonstrated a stronger inhibitory effect on phosphate adsorption than HA. This observation suggests that the substantial release of autochthonous ADOM by algae could elevate internal P loading and pose challenges for the restoration of restore eutrophic lakes. The presence of phosphate suppressed the adsorption of protein-like compounds in ADOM onto FeOx, resulting in an increase in the relative abundance of protein-like compounds and a decrease in the relative abundance of humic-like compounds in post-adsorption ADOM. In contrast, phosphate exhibited no discernible impact on the compositional fractionation of HA. Collectively, our results show the source-composition characters of DOM influence the immobilization of both DOM and P in aquatic ecosystems through adsorption processes. The preferential adsorption of proteinaceous compounds within ADOM and aromatics within HA highlights the potential for the attachment with FeOx to diminish the original source-specific signatures of DOM, thereby contributing to the shared DOM characteristics observed across diverse aquatic environments.


Asunto(s)
Carbono , Compuestos Férricos , Sustancias Húmicas , Lagos , Fosfatos , Fósforo , Contaminantes Químicos del Agua , Adsorción , Fósforo/química , Lagos/química , Fosfatos/química , Sustancias Húmicas/análisis , Contaminantes Químicos del Agua/química , Carbono/química , Compuestos Férricos/química , Modelos Químicos
4.
Sci Rep ; 14(1): 12368, 2024 05 29.
Artículo en Inglés | MEDLINE | ID: mdl-38811671

RESUMEN

Iron, a crucial micronutrient, is an integral element of biotic vitality. The scarcity of iron in the soil creates agronomic challenges and has a detrimental impact on crop vigour and chlorophyll formation. Utilizing iron oxide nanoparticles (IONPs) via nanopriming emerges as an innovative method to enhance agricultural efficiency and crop health. The objective of this study was to synthesize biogenic IONPs from Glycyrrhiza glabra (G. glabra) plant extract using green chemistry and to evaluate their nanopriming effects on rice seed iron levels and growth. The synthesized IONPs were analyzed using UV-Vis spectroscopy, Fourier-transform infrared spectroscopy (FTIR), Scanning electron microscope (SEM), Transmission electron microscopy (TEM), and Energy-dispersive X-ray (EDX) techniques. The UV-Vis peak at 280 nm revealed the formation of IONPs. SEM and TEM showed that the nanoparticles were spherical and had an average diameter of 23.8 nm. Nanopriming resulted in a substantial enhancement in growth, as seen by a 9.25% and 22.8% increase in shoot lengths for the 50 ppm and 100 ppm treatments, respectively. The yield metrics showed a positive correlation with the concentrations of IONPs. The 1000-grain weight and spike length observed a maximum increase of 193.75% and 97.73%, respectively, at the highest concentration of IONPs. The study indicates that G. glabra synthesized IONPs as a nanopriming agent significantly increased rice seeds' growth and iron content. This suggests that there is a relationship between the dosage of IONPs and their potential for improving agricultural biofortification.


Asunto(s)
Biofortificación , Glycyrrhiza , Oryza , Semillas , Oryza/crecimiento & desarrollo , Oryza/metabolismo , Semillas/crecimiento & desarrollo , Semillas/metabolismo , Semillas/química , Glycyrrhiza/química , Glycyrrhiza/crecimiento & desarrollo , Glycyrrhiza/metabolismo , Extractos Vegetales/química , Nanopartículas Magnéticas de Óxido de Hierro/química , Tecnología Química Verde/métodos , Hierro/metabolismo , Hierro/química , Compuestos Férricos/química , Espectroscopía Infrarroja por Transformada de Fourier
5.
Luminescence ; 39(5): e4758, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38712530

RESUMEN

The ability of heterogeneous photocatalysis to effectively remove organic pollutants from wastewater has shown great promise as a tool for environmental remediation. Pure zinc ferrites (ZnFe2O4) and magnesium-doped zinc ferrites (Mg@ZnFe2O4) with variable percentages of Mg (0.5, 1, 3, 5, 7, and 9 mol%) were synthesized via hydrothermal route and their photocatalytic activity was checked against methylene blue (MB) taken as a model dye. FTIR, XPS, BET, PL, XRD, TEM, and UV-Vis spectroscopy were used for the identification and morphological characterization of the prepared nanoparticles (NPs) and nanocomposites (NCs). The 7% Mg@ZnFe2O4 NPs demonstrated excellent degradation against MB under sunlight. The 7% Mg@ZnFe2O4 NPs were integrated with diverse contents (10, 50, 30, and 70 wt.%) of S@g-C3N4 to develop NCs with better activity. When the NCs were tested to degrade MB dye, it was revealed that the 7%Mg@ZnFe2O4/S@g-C3N4 NCs were more effective at utilizing solar energy than the other NPs and NCs. The synergistic effect of the interface formed between Mg@ZnFe2O4 and S@g-C3N4 was primarily responsible for the boosted photocatalytic capability of the NCs. The fabricated NCs may function as an effective new photocatalyst to remove organic dyes from wastewater.


Asunto(s)
Compuestos Férricos , Azul de Metileno , Compuestos de Nitrógeno , Energía Solar , Contaminantes Químicos del Agua , Zinc , Catálisis , Contaminantes Químicos del Agua/química , Compuestos Férricos/química , Azul de Metileno/química , Zinc/química , Magnesio/química , Fotólisis , Procesos Fotoquímicos , Colorantes/química , Nanocompuestos/química , Grafito/química , Aguas Residuales/química , Nitrilos/química
6.
Int J Mol Sci ; 25(9)2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38732166

RESUMEN

This current study assessed the impacts of morphology adjustment of perovskite BiFeO3 (BFO) on the construction and photocatalytic activity of P-infused g-C3N4/U-BiFeO3 (U-BFO/PCN) heterostructured composite photocatalysts. Favorable formation of U-BFO/PCN composites was attained via urea-aided morphology-controlled hydrothermal synthesis of BFO followed by solvosonication-mediated fusion with already synthesized P-g-C3N4 to form U-BFO/PCN composites. The prepared bare and composite photocatalysts' morphological, textural, structural, optical, and photocatalytic performance were meticulously examined through various analytical characterization techniques and photodegradation of aqueous rhodamine B (RhB). Ellipsoids and flakes morphological structures were obtained for U-BFO and BFO, and their effects on the successful fabrication of the heterojunctions were also established. The U-BFO/PCN composite exhibits 99.2% efficiency within 20 min of visible-light irradiation, surpassing BFO/PCN (88.5%), PCN (66.8%), and U-BFO (26.1%). The pseudo-first-order kinetics of U-BFO/PCN composites is 2.41 × 10-1 min-1, equivalent to 2.2 times, 57 times, and 4.3 times of BFO/PCN (1.08 × 10-1 min-1), U-BFO, (4.20 × 10-3 min-1), and PCN, (5.60 × 10-2 min-1), respectively. The recyclability test demonstrates an outstanding photostability for U-BFO/PCN after four cyclic runs. This improved photocatalytic activity exhibited by the composites can be attributed to enhanced visible-light utilization and additional accessible active sites due to surface and electronic band modification of CN via P-doping and effective charge separation achieved via successful composites formation.


Asunto(s)
Bismuto , Fotólisis , Rodaminas , Catálisis , Bismuto/química , Rodaminas/química , Luz , Compuestos Férricos/química , Compuestos de Nitrógeno/química , Titanio/química , Procesos Fotoquímicos , Nitrilos/química , Cinética , Grafito , Óxidos , Compuestos de Calcio
7.
Chemosphere ; 358: 142158, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38697561

RESUMEN

A novel dual Photo-Fenton photocatalyst Fe2O3-Fe-CN with excellent Fe(III)/Fe(II) conversion efficiency and trace metal ion leaching rate has been fabricated by in-situ deposition of α-Fe2O3 quantum dots on ultrathin porous Fe-doped carbon nitride (Fe-CN) nanosheets. The iron species in Fe-CN and α-Fe2O3 QDs constitute a mutually reinforcing dual Photo-Fenton effect. The 4% Fe2O3-Fe-CN showed superior performance with kobs values 8.60 and 4.80 folders greater than pure CN and Fe-CN, respectively. The synergistic effect between α-Fe2O3 QDs and the ultrathin porous structure of Fe-CN is the primary reason for the outstanding catalytic performance exhibited by α-Fe2O3/Fe-CN. On one hand, the ultrathin porous structure of Fe-CN promotes the rapid transfer of photogenerated electrons. On the other hand, the efficient photogenerated charge separation at the α-Fe2O3/Fe-CN interface enables more photogenerated electrons to participate in the Fe3+/Fe2+ conversion and H2O2 activation. The trapping experiments demonstrate that •OH and •O2- are the primary active species in TC degradation. This work presents novel insights into the design of efficient heterogeneous Fenton catalysts for practical applications.


Asunto(s)
Compuestos Férricos , Peróxido de Hidrógeno , Hierro , Puntos Cuánticos , Catálisis , Compuestos Férricos/química , Hierro/química , Peróxido de Hidrógeno/química , Puntos Cuánticos/química , Procesos Fotoquímicos , Nitrilos/química , Porosidad , Grafito , Compuestos de Nitrógeno
8.
Sci Total Environ ; 931: 172945, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38703849

RESUMEN

The coagulation process has a high potential as a treatment method that can handle pathogenic viruses including emerging enveloped viruses in drinking water treatment process which can lower infection risk through drinking water consumption. In this study, a surrogate enveloped virus, bacteriophage Փ6, and surrogate non-enveloped viruses, including bacteriophage MS-2, T4, ՓX174, were used to evaluate removal efficiencies and mechanisms by the conventional coagulation process with alum, poly­aluminum chloride, and ferric chloride at pH 5, 7, and 9 in turbid water. Also, treatability of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), a recent virus of global concern by coagulation was evaluated as SARS-CoV-2 can presence in drinking water sources. It was observed that an increase in the coagulant dose enhanced the removal efficiency of turbidity and viruses, and the condition that provided the highest removal efficiency of enveloped and non-enveloped viruses was 50 mg/L of coagulants at pH 5. In addition, the coagulation process was more effective for enveloped virus removal than for the non-enveloped viruses, and it demonstrated reduction of SARS-CoV-2 Omicron BA.2 over 0.83-log with alum. According to culture- and molecular-based assays (qPCR and CDDP-qPCR), the virus removal mechanisms were floc adsorption and coagulant inactivation. Through inactivation with coagulants, coagulants caused capsid destruction, followed by genome damage in non-enveloped viruses; however, damage to a lipid envelope is suggested to contribute to a great extend for enveloped virus inactivation. We demonstrated that conventional coagulation is a promising method for controlling emerging and re-emerging viruses in drinking water.


Asunto(s)
SARS-CoV-2 , Purificación del Agua , Purificación del Agua/métodos , SARS-CoV-2/fisiología , COVID-19 , Agua Potable/virología , Agua Potable/química , Compuestos de Alumbre , Microbiología del Agua , Betacoronavirus/fisiología , Floculación , Compuestos de Aluminio , Compuestos Férricos/química
9.
Environ Sci Technol ; 58(20): 8955-8965, 2024 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-38718175

RESUMEN

The development of Fe-based catalysts for the selective catalytic reduction of NOx by NH3 (NH3-SCR of NOx) has garnered significant attention due to their exceptional SO2 resistance. However, the influence of different sulfur-containing species (e.g., ferric sulfates and ammonium sulfates) on the NH3-SCR activity of Fe-based catalysts as well as its dependence on exposed crystal facets of Fe2O3 has not been revealed. This work disclosed that nanorod-like α-Fe2O3 (Fe2O3-NR) predominantly exposing (110) facet performed better than nanosheet-like α-Fe2O3 (Fe2O3-NS) predominantly exposing (001) facet in NH3-SCR reaction, due to the advantages of Fe2O3-NR in redox properties and surface acidity. Furthermore, the results of the SO2/H2O resistance test at a critical temperature of 250 °C, catalytic performance evaluations on Fe2O3-NR and Fe2O3-NS sulfated by SO2 + O2 or deposited with NH4HSO4 (ABS), and systematic characterization revealed that the reactivity of ammonium sulfates on Fe2O3 catalysts to NO(+O2) contributed to their improved catalytic performance, while ferric sulfates showed enhancing and inhibiting effects on NH3-SCR activity on Fe2O3-NR and Fe2O3-NS, respectively; despite this, Fe2O3-NR showed higher affinity for SO2 + O2. This work set a milestone in understanding the NH3-SCR reaction on Fe2O3 catalysts in the presence of SO2 from the aspect of crystal facet engineering.


Asunto(s)
Amoníaco , Catálisis , Amoníaco/química , Dióxido de Azufre/química , Compuestos Férricos/química , Oxidación-Reducción
10.
Sci Rep ; 14(1): 11400, 2024 05 18.
Artículo en Inglés | MEDLINE | ID: mdl-38762571

RESUMEN

The current study developed an innovative design for the production of smart multifunctional core-double shell superparamagnetic nanoparticles (NPs) with a focus on the development of a pH-responsive drug delivery system tailored for the controlled release of Phenytoin, accompanied by real-time monitoring capabilities. In this regard, the ultra-small superparamagnetic iron oxide@silica NPs (IO@Si MNPs) were synthesized and then coated with a layer of gelatin containing Phenytoin as an antiepileptic drug. The precise saturation magnetization value for the resultant NPs was established at 26 emu g-1. The polymeric shell showed a pH-sensitive behavior with the capacity to regulate the release of encapsulated drug under neutral pH conditions, simultaneously, releasing more amount of the drug in a simulated tumorous-epileptic acidic condition. The NPs showed an average size of 41.04 nm, which is in the desired size range facilitating entry through the blood-brain barrier. The values of drug loading and encapsulation efficiency were determined to be 2.01 and 10.05%, respectively. Moreover, kinetic studies revealed a Fickian diffusion process of Phenytoin release, and diffusional exponent values based on the Korsmeyer-Peppas equation were achieved at pH 7.4 and pH 6.3. The synthesized NPs did not show any cytotoxicity. Consequently, this new design offers a faster release of PHT at the site of a tumor in response to a change in pH, which is essential to prevent epileptic attacks.


Asunto(s)
Anticonvulsivantes , Sistemas de Liberación de Medicamentos , Gelatina , Fenitoína , Dióxido de Silicio , Gelatina/química , Anticonvulsivantes/química , Anticonvulsivantes/administración & dosificación , Dióxido de Silicio/química , Concentración de Iones de Hidrógeno , Fenitoína/química , Fenitoína/administración & dosificación , Sistemas de Liberación de Medicamentos/métodos , Humanos , Compuestos Férricos/química , Liberación de Fármacos , Portadores de Fármacos/química , Nanopartículas Magnéticas de Óxido de Hierro/química , Nanopartículas de Magnetita/química , Nanopartículas/química , Tamaño de la Partícula
11.
Environ Monit Assess ; 196(6): 569, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38777943

RESUMEN

Nanomaterials are widely employed in wastewater treatment, among which nanoferrites and their composites hold significant prominence. This study adopts a green approach to synthesize zinc ferrite nanoparticles, subsequently integrating them with polyaniline (PANI) to fabricate the ZnFe2O4-PANI nanocomposite. Characterization of the prepared ZnFe2O4-PANI nanocomposite was conducted using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR) and scanning electron microscopic (SEM) techniques. Using Scherrer's equation, the crystallite size of the synthesized zinc ferrite nanoparticles was found to be 17.67 nm. SEM micrographs of the ZnFe2O4-PANI nanocomposite revealed that in situ polymerization of ZnFe2O4 with polyaniline transforms the amorphous surface morphology of the polymer into a homogeneous nanoparticle structure. The adsorption of crystal violet (CV) dye onto the surface of the ZnFe2O4-PANI nanocomposite depends on pH, adsorbent dosage, temperature, concentration levels and duration. The Langmuir adsorption model fitted the data well, indicating adherence to a pseudo-second-order kinetic pattern. Thermodynamic values ΔG°, ΔH° and ΔS° indicated that the adsorption process occurred spontaneously. Advantages and disadvantages of the technique have also been highlighted. Mechanism of adsorption is discussed. From the obtained results, it is evident that the ZnFe2O4-PANI nanocomposite holds promise as a sorbent for the removal of dye from wastewater.


Asunto(s)
Compuestos de Anilina , Compuestos Férricos , Violeta de Genciana , Nanocompuestos , Contaminantes Químicos del Agua , Zinc , Compuestos de Anilina/química , Violeta de Genciana/química , Nanocompuestos/química , Contaminantes Químicos del Agua/química , Compuestos Férricos/química , Zinc/química , Adsorción , Eliminación de Residuos Líquidos/métodos , Cinética , Purificación del Agua/métodos
12.
Environ Monit Assess ; 196(6): 576, 2024 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-38789652

RESUMEN

Phosphorus pollution poses a significant challenge in addressing water contamination. The coagulant is one of the effective methods to remove phosphorus from wastewater. Abundant Al and Fe oxides in sludge residue make it have great potential to synthesize water treatment coagulants. However, the utilization of sludge residue for preparation of coagulant was seldom investigated. In this study, we fabricated a novel coagulant, polyaluminum ferric chloride (SM-PAC), using sludge residue as a raw material through acid leaching and polymerization processes. Characterization results confirm that the parameters of SM-PAC meet the specifications outlined in the national standard (GB/T 22627-2022). We investigated the effects of pH, dosage, initial phosphorus concentration, and contact time on the removal efficiency of SM-PAC. As anticipated, the prepared SM-PAC exhibited a significant efficacy in removing phosphorus, meeting the discharge standards set for municipal sewage. Furthermore, the adsorption kinetics analysis suggests that the predominant mode of phosphorus adsorption on SM-PAC is chemical adsorption. Furthermore, the SM-PAC was employed in the actual wastewater treatment plant and exhibited excellent efficiency in phosphorus removal. The utilization of SM-PAC can not only effectively address the issue of sludge disposal but also achieve the goal of "treating waste with waste." It is expected that the proposed method of reusing sludge residue as a resource can provide a sustainable way to synthesize a coagulant for phosphorus removal.


Asunto(s)
Fósforo , Reciclaje , Aguas del Alcantarillado , Eliminación de Residuos Líquidos , Contaminantes Químicos del Agua , Fósforo/análisis , Fósforo/química , Aguas del Alcantarillado/química , Eliminación de Residuos Líquidos/métodos , Contaminantes Químicos del Agua/análisis , Contaminantes Químicos del Agua/química , Reciclaje/métodos , Adsorción , Compuestos Férricos/química , Aguas Residuales/química
13.
Inorg Chem ; 63(21): 9907-9918, 2024 May 27.
Artículo en Inglés | MEDLINE | ID: mdl-38754069

RESUMEN

Nitrobindins (Nbs) are all-ß-barrel heme proteins present along the evolutionary ladder. They display a highly solvent-exposed ferric heme group with the iron atom being coordinated by the proximal His residue and a water molecule at the distal position. Ferric nitrobindins (Nb(III)) play a role in the conversion of toxic peroxynitrite (ONOO-) to harmless nitrate, with the value of the second-order rate constant being similar to those of most heme proteins. The value of the second-order rate constant of Nbs increases as the pH decreases; this suggests that Nb(III) preferentially reacts with peroxynitrous acid (ONOOH), although ONOO- is more nucleophilic. In this work, we shed light on the molecular basis of the ONOO- and ONOOH reactivity of ferric Mycobacterium tuberculosis Nb (Mt-Nb(III)) by dissecting the ligand migration toward the active site, the water molecule release, and the ligand binding process by computer simulations. Classical molecular dynamics simulations were performed by employing a steered molecular dynamics approach and the Jarzynski equality to obtain ligand migration free energy profiles for both ONOO- and ONOOH. Our results indicate that ONOO- and ONOOH migration is almost unhindered, consistent with the exposed metal center of Mt-Nb(III). To further analyze the ligand binding process, we computed potential energy profiles for the displacement of the Fe(III)-coordinated water molecule using a hybrid QM/MM scheme at the DFT level and a nudged elastic band approach. These results indicate that ONOO- exhibits a much larger barrier for ligand displacement than ONOOH, suggesting that water displacement is assisted by protonation of the leaving group by the incoming ONOOH.


Asunto(s)
Simulación de Dinámica Molecular , Mycobacterium tuberculosis , Ácido Peroxinitroso , Ácido Peroxinitroso/química , Ácido Peroxinitroso/metabolismo , Mycobacterium tuberculosis/química , Hemoproteínas/química , Hemoproteínas/metabolismo , Compuestos Férricos/química , Compuestos Férricos/metabolismo , Termodinámica
14.
Bioresour Technol ; 402: 130844, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38754560

RESUMEN

In this study, a novel magnetic Ni-Fe2O3-C catalyst combined with electromagnetic induction heating in biomass steam gasification was proposed to enhance H2 production. Better catalytic performance for H2 production was observed with the Ni-Fe2O3-C catalyst under induction heating, resulting in an increase in H2 yield from 735.1 to 2271.2 mL/g-biomass (a 209.1 % enhancement). SEM, TGA and XRD analysis demonstrated a significant decrease in coking deposition, caking, and particle agglomeration of the Ni-Fe2O3-C catalyst under induction heating, while maintaining more active sites. Importantly, the benefits of induction heating were also applicable to different magnetic catalysts like Ni-Al2O3-C, Ni-ZrO2-C, and Ni-MgO-C. Experimental results revealed a logarithmic correlation between the increase in H2 yields due to induction heating and the magnetic saturation (Ms) of the catalysts. The Ni-Fe2O3-C catalyst, with a high Ms of 50.9 emu/g, showed the highest catalytic activity for H2 production under induction heating in this study.


Asunto(s)
Biomasa , Compuestos Férricos , Hidrógeno , Níquel , Vapor , Catálisis , Hidrógeno/química , Níquel/química , Compuestos Férricos/química , Calor , Calefacción , Difracción de Rayos X , Fenómenos Electromagnéticos
15.
J Biol Inorg Chem ; 29(3): 291-301, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38722396

RESUMEN

In addition to its primary oxygen-atom-transfer function, cysteamine dioxygenase (ADO) exhibits a relatively understudied anaerobic disproportionation reaction (ADO-Fe(III)-SR → ADO-Fe(II) + ½ RSSR) with its native substrates. Inspired by ADO disproportionation reactivity, we employ [Fe(tacn)Cl3] (tacn = 1,4,7-triazacyclononane) as a precursor for generating Fe(III)-thiolate model complexes in buffered aqueous media. A series of Fe(III)-thiolate model complexes are generated in situ using aqueous [Fe(tacn)Cl3] and thiol-containing ligands cysteamine, penicillamine, mercaptopropionate, cysteine, cysteine methyl ester, N-acetylcysteine, and N-acetylcysteine methyl ester. We observe trends in UV-Vis and electron paramagnetic resonance (EPR) spectra, disproportionation rate constants, and cathodic peak potentials as a function of thiol ligand. These trends will be useful in rationalizing substrate-dependent Fe(III)-thiolate disproportionation reactions in metalloenzymes.


Asunto(s)
Compuestos Férricos , Compuestos de Sulfhidrilo , Cinética , Compuestos de Sulfhidrilo/química , Concentración de Iones de Hidrógeno , Compuestos Férricos/química , Compuestos Férricos/metabolismo , Espectroscopía de Resonancia por Spin del Electrón , Dioxigenasas/metabolismo , Dioxigenasas/química , Técnicas Electroquímicas
16.
Iran Biomed J ; 28(2&3): 71-81, 2024 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-38770844

RESUMEN

Background: Bioreductive processes are quite potent, effective and affordable for the synthesis of green NPs, as compared to the physical and chemical methods. The present study aimed to evaluate the bactericidal, antioxidative and anticancer activity of FeONPs derived from the turmeric rhizome (Curcuma amada) using ferric chloride as a precursor. Methods: With focusing on the manufacture of FeONPs via green approach, we characterized the NPs using FTIR, FT-Vis, DLS, and UV-Vis spectroscopy. The produced particles were tested for antibacterial, antioxidant, and anticancer properties. The synthesized NPs were also examined using the MDA-MB-231 human epithelial breast cancer cell line and NCI-60 cancer cell lines. Results: The antioxidant activity of TR-FeONPs was concentration-dependent. The scavenging activity of TR-FeONPs was 76.09% at a concentration of 140 µg/ml. Using different concentrations of TR-FeONPs in the MTT assay against the MDA-MB-231 cell line indicated a reduction of less than 50% in cell viability at 125 µg/ml. Moreover, TR-FeONPs exhibited an effective bactericidal property. The gTR-FeONPs synthesized bioreductively were found to be effective in renal cancer, UO-31 cell line, with GI50 value of 66.64%. Conclusion: Our study showcases a sustainable method based on green chemistry principles to produce FeONPs utilizing turmeric rhizome. We anticipate that the FeONPs produced through this biosynthesis process could serve as a promising drug delivery system in cancer treatment and as an effective antimicrobial agent against various diseases.


Asunto(s)
Antibacterianos , Antioxidantes , Tecnología Química Verde , Antibacterianos/farmacología , Antioxidantes/farmacología , Humanos , Nanopartículas Magnéticas de Óxido de Hierro/química , Pruebas de Sensibilidad Microbiana , Animales , Compuestos Férricos/farmacología , Compuestos Férricos/química
17.
Nanotechnology ; 35(32)2024 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-38701766

RESUMEN

One of the global challenges for living things is to provide pollution and harmful microbes-free environment. In this study, magnetically retrievable spinel-structured manganese zinc ferrite (Mn0.5Zn0.5Fe2O4) (MZF) was synthesized by a facile solvothermal method. Further, the MZF with different weight percentages (10 wt%, 50 wt%, and 80 wt%) were supported on reduced graphene oxide (rGO). The phase purity and morphology of MZF and MZF/rGO nanocomposite were confirmed by x-ray diffraction technique and scanning electron microscopy, respectively. The Fourier transform infrared spectroscopy, Raman, UV-visible spectroscopy, and thermogravimetric analyses of the as-synthesized nanocomposites were examined for the detection of various chemical groups, band gap, and thermal properties, respectively. The MZF/rGO nanocomposite exhibited significant antibacterial and antifungal activity againstEggerthella lenta, Enterococcus faecalis, Klebsiella pneumonia, Pseudomonas aeruginosa,andCandida albicanscompared to bare MZF and rGO. The high surface area of rGO plays a crucible role in antimicrobial analysis. Additionally, the antibacterial and antifungal activity is compared by synthesizing various metal ferrites such as MnFe2O4, ZnFe2O4, and Fe3O4. The 50 wt% MZF/rGO nanocomposite exhibits significantly high antibacterial activity. However, 10 wt% MZF/rGO nanocomposite shows good antifungal activity than Fe3O4, MnFe2O4, ZnFe2O4, MnZnFe2O4, 50 wt%, and 80 wt% MZF/rGO nanocomposites. These findings suggest that the prepared ferrite nanocomposites hold promise for microbial inhibition.


Asunto(s)
Bacterias , Compuestos Férricos , Hongos , Grafito , Nanocompuestos , Grafito/química , Grafito/farmacología , Compuestos Férricos/química , Compuestos Férricos/farmacología , Nanocompuestos/química , Hongos/efectos de los fármacos , Bacterias/efectos de los fármacos , Pruebas de Sensibilidad Microbiana , Antibacterianos/farmacología , Antibacterianos/química , Antiinfecciosos/farmacología , Antiinfecciosos/química , Antifúngicos/farmacología , Antifúngicos/química , Zinc/química , Zinc/farmacología , Óxido de Aluminio , Óxido de Magnesio
18.
Bioresour Technol ; 402: 130775, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38701984

RESUMEN

Acidification recovery in anaerobic digestion of food waste is challenging. This study explored its in-situ recovery using a co-substrate of food waste and waste activated sludge. Fe3O4 and bentonite were used as conductor and carrier, respectively, to enhance AD performance under severe acidification. The application of Fe3O4-bentonite resulted in a 152% increase in cumulative methane in the Fe3O4-bentonite 10 digester, demonstrating its effectiveness in restoring the acidified AD system. In acidified systems, bentonite enhanced the diversity and richness of microbial communities due to its buffering capacity. The excessive non-conductive polysaccharides excreted by bacteria in extracellular polymeric substances reduced the possibility of electron transfer by Fe3O4. However, in the synergistic application of Fe3O4 and bentonite, this resistance was alleviated, increasing the possibility of direct interspecies electron transfer, and accelerating the consumption of volatile fatty acids. This approach of integrating carrier and conductive materials is significant for in-situ restoration of acidified systems.


Asunto(s)
Bentonita , Metano , Aguas del Alcantarillado , Bentonita/química , Anaerobiosis , Metano/metabolismo , Concentración de Iones de Hidrógeno , Alimentos , Ácidos Grasos Volátiles , Reactores Biológicos , Ácidos/química , Residuos , Compuestos Férricos/química , Alimento Perdido y Desperdiciado
19.
Biosens Bioelectron ; 258: 116358, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38718634

RESUMEN

Wearable sensors for sweat glucose monitoring are gaining massive interest as a patient-friendly and non-invasive way to manage diabetes. The present work offers an alternative on-body method employing an all-printed flexible electrochemical sensor to quantify the amount of glucose in human sweat. The working electrode of the glucose sensor was printed using a custom-formulated ink containing multi-walled carbon nanotube (MWCNT), poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOPT: PSS), and iron (II, III) oxide (Fe3O4) nanoparticles. This novel ink composition has good conductivity, enhanced catalytic activity, and excellent selectivity. The working electrode was modified using Prussian blue (PB) nanoparticles and glucose oxidase enzyme (GOx). The sensor displayed a linear chronoamperometric response to glucose from 1 µM to 400 µM, with a precise detection limit of ∼0.38 µM and an impressive sensitivity of ∼4.495 µAµM-1cm-2. The sensor stored at 4 °C exhibited excellent stability over 60 days, high selectivity, and greater reproducibility. The glucose detection via the standard addition method in human sweat samples acquired a high recovery rate of 96.0-98.6%. Examining human sweat during physical activity also attested to the biosensor's real-time viability. The results also show an impressive correlation between glucose levels obtained from a commercial blood glucose meter and sweat glucose concentrations. Remarkably, the present results outperform previously published printed glucose sensors in terms of detection range, low cost, ease of manufacturing, stability, selectivity, and wearability.


Asunto(s)
Técnicas Biosensibles , Glucosa Oxidasa , Glucosa , Límite de Detección , Nanocompuestos , Nanotubos de Carbono , Sudor , Dispositivos Electrónicos Vestibles , Humanos , Técnicas Biosensibles/instrumentación , Nanotubos de Carbono/química , Sudor/química , Nanocompuestos/química , Glucosa/análisis , Glucosa Oxidasa/química , Tinta , Técnicas Electroquímicas , Compuestos Férricos/química , Ferrocianuros/química , Polímeros/química , Reproducibilidad de los Resultados , Compuestos Bicíclicos Heterocíclicos con Puentes/química , Poliestirenos
20.
Molecules ; 29(10)2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38792172

RESUMEN

Pyrethroid pesticides (PYRs) have found widespread application in agriculture for the protection of fruit and vegetable crops. Nonetheless, excessive usage or improper application may allow the residues to exceed the safe limits and pose a threat to consumer safety. Thus, there is an urgent need to develop efficient technologies for the elimination or trace detection of PYRs from vegetables. Here, a simple and efficient magnetic solid-phase extraction (MSPE) strategy was developed for the simultaneous purification and enrichment of five PYRs in vegetables, employing the magnetic covalent organic framework nanomaterial COF-SiO2@Fe3O4 as an adsorbent. COF-SiO2@Fe3O4 was prepared by a straightforward solvothermal method, using Fe3O4 as a magnetic core and benzidine and 3,3,5,5-tetraaldehyde biphenyl as the two building units. COF-SiO2@Fe3O4 could effectively capture the targeted PYRs by virtue of its abundant π-electron system and hydroxyl groups. The impact of various experimental parameters on the extraction efficiency was investigated to optimize the MSPE conditions, including the adsorbent amount, extraction time, elution solvent type and elution time. Subsequently, method validation was conducted under the optimal conditions in conjunction with gas chromatography-mass spectrometry (GC-MS). Within the range of 5.00-100 µg·kg-1 (1.00-100 µg·kg-1 for bifenthrin and 2.5-100 µg·kg-1 for fenpropathrin), the five PYRs exhibited a strong linear relationship, with determination coefficients ranging from 0.9990 to 0.9997. The limits of detection (LODs) were 0.3-1.5 µg·kg-1, and the limits of quantification (LOQs) were 0.9-4.5 µg·kg-1. The recoveries were 80.2-116.7% with relative standard deviations (RSDs) below 7.0%. Finally, COF-SiO2@Fe3O4, NH2-SiO2@Fe3O4 and Fe3O4 were compared as MSPE adsorbents for PYRs. The results indicated that COF-SiO2@Fe3O4 was an efficient and rapid selective adsorbent for PYRs. This method holds promise for the determination of PYRs in real samples.


Asunto(s)
Plaguicidas , Piretrinas , Dióxido de Silicio , Extracción en Fase Sólida , Verduras , Extracción en Fase Sólida/métodos , Dióxido de Silicio/química , Verduras/química , Piretrinas/aislamiento & purificación , Piretrinas/análisis , Piretrinas/química , Plaguicidas/aislamiento & purificación , Plaguicidas/química , Plaguicidas/análisis , Cromatografía de Gases y Espectrometría de Masas , Adsorción , Contaminación de Alimentos/análisis , Límite de Detección , Residuos de Plaguicidas/análisis , Residuos de Plaguicidas/aislamiento & purificación , Compuestos Férricos/química , Cobalto
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