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1.
J Hazard Mater ; 477: 135366, 2024 Jul 28.
Article de Anglais | MEDLINE | ID: mdl-39088943

RÉSUMÉ

Deoxynivalenol-3-glucoside (D3G), the masked form of the important mycotoxin deoxynivalenol (DON), displays potential toxicity but is difficult to control owing to the lack of rapid detection methods. Herein, an innovative molecularly imprinted polymer (MIP)-based electrochemical sensor was developed for the rapid detection of D3G. MIP, an efficient recognition element for D3G, was electropolymerized using o-phenylenediamine based on a surface functional monomer-directing strategy for the first time. CeO2, which contains both Ce3+ and Ce4+ oxidation states, was introduced as a nanozyme to catalyze H2O2 reduction, while Mn doping generated more oxygen vacancies and considerably improved the catalytic activity. Mn-CeO2 also served as a promising substrate material because of its large surface area and excellent conductivity. Under optimal conditions, a good linear relationship was observed for D3G detection over the concentration range of 0.01-50 ng/mL. The proposed sensor could detect D3G down to 0.003 ng/mL with excellent selectivity, even distinguishing its precursor DON in complex samples. The sensor exhibited acceptable stability with high reproducibility and accuracy, and could successfully determine D3G in grain samples. To the best of our knowledge, this is the first electrochemical sensing platform for rapid D3G detection that can easily be expanded to other masked mycotoxins.

2.
Article de Anglais | MEDLINE | ID: mdl-39091093

RÉSUMÉ

Rare-earth doped CeO2 materials find extensive application in high-temperature energy conversion devices such as solid oxide fuel cells and electrolyzers. However, understanding the complex relationship between structural and electrical properties, particularly concerning rare-earth ionic size and content, remains a subject of ongoing debate, with conflicting published results. In this study, we have conducted comprehensive long-range and local order structural characterization of Ce1-xLnxO2-x/2 samples (x ≤ 0.6; Ln = La, Nd, Sm, Gd, and Yb) using X-ray and neutron powder diffraction, Raman spectroscopy, and electron diffraction. The increase in the rare-earth dopant content leads to a progressive phase transformation from a disordered fluorite structure to a C-type ordered superstructure, accompanied by reduced ionic conductivity. Samples with low dopant content (x = 0.2) exhibit higher ionic conductivity in Gd3+ and Sm3+ series due to lower lattice cell distortion. Conversely, highly doped samples (x = 0.6) exhibit superior conductivity for larger rare-earth dopant cations. Thermogravimetric analysis confirms increased water uptake and proton conductivity with increasing dopant concentration, while the electronic conductivity remains relatively unaffected, resulting in reduced ionic transport numbers. These findings offer insights into the relationship between transport properties and defect-induced local distortions in rare-earth doped CeO2, suggesting the potential for developing new functional materials with mixed ionic oxide, proton, and electronic conductivity for high-temperature energy systems.

3.
Talanta ; 279: 126603, 2024 Jul 22.
Article de Anglais | MEDLINE | ID: mdl-39053355

RÉSUMÉ

Enzyme catalytic cascade reactions based on peroxidase nanozymes and natural enzymes have aroused extensive attention in analytical fields. However, a majority of peroxidase nanozymes perform well only in acidic environments, resulting in their optimal pH mismatch with a neutral pH of natural enzymes, further restricting their application in biochemical sensing. Herein, Mn-doped CeO2 (Mn/CeO2) performing enhanced peroxidase-like activity at neutral conditions was prepared via a facile and feasible strategy. An effective enzyme cascade catalysis system via integrating glucose oxidase (GOx) with Mn/CeO2 was developed for one-pot detection of glucose in serum at neutral conditions. Using one-pot multistep catalytic reactions, this work provided a detection platform that allows for faster detection and easier operations than traditional methods. Under optimized conditions, our assay performed a sensitive detection of glucose ranging from 2.0 µΜ to 300 µΜ and a low detection limit of 0.279 µΜ. Notably, favorable analytical outcomes for glucose detection in serum samples were obtained, exhibiting potential applications in clinical diagnosis.

4.
ACS Sens ; 2024 Jul 23.
Article de Anglais | MEDLINE | ID: mdl-39042863

RÉSUMÉ

Detecting and distinguishing between hazardous gases with similar odors by using conventional sensor technology for safeguarding human health and ensuring food safety are significant challenges. Bulky, costly, and power-hungry devices, such as that used for gas chromatography-mass spectrometry (GC-MS), are widely employed for gas sensing. Using a single chemiresistive semiconductor or electric nose (e-nose) gas sensor to achieve this objective is difficult, mainly because of its selectivity issue. Thus, there is a need to develop new materials with tunable and versatile sensing characteristics. Phase engineering of two-dimensional materials to better utilize their physiochemical properties has attracted considerable attention. Here, we show that MoSe2 phase-transition/CeO2 composites can be effectively used to distinguish ammonia (NH3) and triethylamine (TEA) at room temperature. The phase transition of nanocomposite samples from semimetallic (1T) to semiconducting (2H) prepared at different synthesis temperatures is confirmed via X-ray photoelectron spectroscopy (XPS). A composite sensor in which the 2H phase of MoSe2 is predominant lacks discrimination capability and is less responsive to NH3 and TEA. An MoSe2/CeO2 composite sensor with a higher 1T phase content exhibits high selectivity for NH3, whereas one with a higher 2H phase content (2H > 1T) shows more selective behavior toward TEA. For example, for 50% relative humidity, the MoSe2/CeO2 sensor's signal changes from the baseline by 45% and 58% for 1 ppm of NH3 and TEA, respectively, indicating a low limit of detection (LOD) of 70 and 160 ppb, respectively. The composites' superior sensing characteristics are mainly attributed to their large specific surface area, their numerous active sites, presence of defects, and the n-n type heterojunction between MoSe2 and CeO2. The sensing mechanism is elucidated using Raman spectroscopy, XPS, and GC-MS results. Their phase-transition characteristics render MoSe2/CeO2 sensors promising for use in distributed, low-cost, and room-temperature sensor networks, and they offer new opportunities for the development of integrated advanced smart sensing technologies for environmental and healthcare.

5.
Nanomaterials (Basel) ; 14(13)2024 Jun 27.
Article de Anglais | MEDLINE | ID: mdl-38998708

RÉSUMÉ

In the current study, the synthesis of hydroxyapatite-ceria (HAP-CeO2) scaffolds is attempted through a bioinspired chemical approach. The utilized colloidal CeO2 suspension presents antifungal activity against the Aspergillus flavus and Aspergillus fumigatus species at concentrations higher than 86.1 ppm. Three different series of the composite HAP-CeO2 suspensions are produced, which are differentiated based on the precursor suspension to which the CeO2 suspension is added and by whether this addition takes place before or after the formation of the hydroxyapatite phase. Each of the series consists of three suspensions, in which the pure ceria weight reaches 4, 5, and 10% (by mass) of the produced hydroxyapatite, respectively. The characterization showed that the 2S series's specimens present the greater alteration towards their viscoelastic properties. Furthermore, the 2S series's sample with 4% CeO2 presents the best mechanical response. This is due to the growth of needle-like HAP crystals during lyophilization, which-when oriented perpendicular to the direction of stress application-enhance the resistance of the sample to deformation. The 2S series's scaffolds had an average pore size equal to 100 µm and minimum open porosity 89.5% while simultaneously presented the lowest dissolution rate in phosphate buffered saline.

6.
Molecules ; 29(13)2024 Jun 21.
Article de Anglais | MEDLINE | ID: mdl-38998900

RÉSUMÉ

The electrocatalytic carbon dioxide (CO2) reduction reaction (CO2RR) is extensively regarded as a promising strategy to reach carbon neutralization. Copper sulfide (CuS) has been widely studied for its ability to produce C1 products with high selectivity. However, challenges still remain owing to the poor selectivity of formate. Here, a Bi/CeO2/CuS composite was synthesized using a simple solvothermal method. Bi/CeO2-decorated CuS possessed high formate selectivity, with the Faraday efficiency and current density reaching 88% and 17 mA cm-2, respectively, in an H-cell. The Bi/CeO2/CuS structure significantly reduces the energy barrier formed by OCHO*, resulting in the high activity and selectivity of the CO2 conversion to formate. Ce4+ readily undergoes reduction to Ce3+, allowing the formation of a conductive network of Ce4+/Ce3+. This network facilitates electron transfer, stabilizes the Cu+ species, and enhances the adsorption and activation of CO2. Furthermore, sulfur catalyzes the OCHO* transformation to formate. This work describes a highly efficient catalyst for CO2 to formate, which will aid in catalyst design for CO2RR to target products.

7.
Molecules ; 29(13)2024 Jun 23.
Article de Anglais | MEDLINE | ID: mdl-38998939

RÉSUMÉ

In this paper, four heteroleptic Ce(III) complexes, including Ce(thd)3-phen (thd = 2,2,6,6-tetramethyl-3,5-heptanedione, phen = 1, 10-phenanthroline (1), Ce(thd)3-MEDA (MEDA = N-Methylethylenediamine (2), Ce(thd)3-MOMA (MOMA = N-(2-Methoxyethyl)methylamine (3), and Ce(thd)3-DMDE (DMDE = N,N″-dimethyl ethanol amine (4), were synthesized and characterized with 1H-NMR, elemental analysis, and X-ray single-crystal diffraction. The thermogravimetric analysis and vapor pressure results indicated that the complexing ability of a nitrogen-containing bidentate ligand with a cerium ion was stronger than that of a mixed oxygen-nitrogen-containing bidentate ligand. Complex 2 was selected as an ALD precursor to deposit a CeO2 film on a SiO2/Si (100) wafer. The self-limited deposition results demonstrated that complex 2 was a potential ALD precursor.

8.
Biosens Bioelectron ; 262: 116553, 2024 Oct 15.
Article de Anglais | MEDLINE | ID: mdl-39018977

RÉSUMÉ

A spatial-resolved and self-calibrated photoelectrochemical (PEC) biosensor has been fabricated by a multifunctional CeO2/CdS heterostructure, achieving portable and sensitive detection of carcinoembryonic antigen (CEA) using a homemade 3D printing device. The CeO2/CdS heterostructure with matched band structure is prepared to construct the dual-photoelectrodes to improve the PEC response of CeO2. In particular, as the photoactive nanomaterial, the CeO2 also plays the role of peroxidase mimetic nanozymes. Therefore, the catalytic performance of CeO2 with different morphologies (e.g., nano-cubes, nano-rods and nano-octahedra) have been studied, and CeO2 nano-cubes (c-CeO2) achieve the optimal catalytic activity. Upon introducing CEA, the sandwich-type immunocomplex is formed in the microplate using GOx-AuNPs-labeled second antibody as detection antibody. As a result, H2O2 can be produced from the catalytic oxidization of glucose substrate by GOx, which is further catalyzed by CeO2 to form •OH, thus in situ etching CdS and decreasing the photocurrents. The self-calibration is achieved by the dual-channel photoelectrodes on the homemade 3D printing device to obtain the photocurrents ratio, thus effectively normalizing the fluctuations of external factors to enhance the accuracy. This integrated biosensor with a detection limit as low as 0.057 ng mL-1 provides a promising way for ultrasensitive immunoassay in clinic application in complex environments.


Sujet(s)
Techniques de biocapteur , Composés du cadmium , Antigène carcinoembryonnaire , Cérium , Techniques électrochimiques , Impression tridimensionnelle , Sulfures , Techniques de biocapteur/instrumentation , Cérium/composition chimique , Dosage immunologique/instrumentation , Dosage immunologique/méthodes , Antigène carcinoembryonnaire/sang , Composés du cadmium/composition chimique , Sulfures/composition chimique , Humains , Limite de détection , Or/composition chimique , Anticorps immobilisés/composition chimique , Nanoparticules métalliques/composition chimique
9.
Sci Rep ; 14(1): 15693, 2024 Jul 08.
Article de Anglais | MEDLINE | ID: mdl-38977834

RÉSUMÉ

To mitigate the decrease in mechanical performance of Sn58Bi/Cu solder joints resulting from electromigration-induced damage. The CeO2 nanoparticles were incorporated into Sn58Bi solder by a melt-casting method, and their effects on the microstructure and properties of Sn58Bi/Cu solder joints under electromigration were investigated. The study results demonstrate that the addition of 0.125 ~ 0.5 wt% CeO2 nanoparticles refines the eutectic microstructure of Sn58Bi solder alloy. At an addition amount of 0.5 wt%, the composite solder alloy exhibits the maximum tensile strength of 68.9 MPa, which is 37% higher than that of the base solder. CeO2 nanoparticle-reinforced Sn58Bi solder can achieve excellent solderbility with Cu substrates and the joints can significantly inhibit the growth of the anodic Bi-rich layer, which is responsible for electromigration. With the extension of current stressing time, Bi-rich and Sn-rich layer are respectively formed on the anode and cathode in the joints. The intermetallic compound (IMC) layer grows asymmetrically, transitioning from a fan-shaped morphology to a flattened structure at the anode and to a thickened mountain-like morphology at the cathode. Adding the CeO2 nanoparticles helps to mitigate the decrease in mechanical performance caused by electromigration damage during current application to some extent. Over the current stressing period of 288 ~ 480 h, the fracture position shifts from the anodic IMC/Bi-rich interface to the cathodic Sn-rich/IMC interface. The fracture mechanism transitions from a brittle fracture characterized by plate-like cleavage to a ductile-brittle mixed fracture with fine dimples and cleavage.

10.
J Environ Manage ; 366: 121890, 2024 Jul 18.
Article de Anglais | MEDLINE | ID: mdl-39029170

RÉSUMÉ

In today's world, the development of an efficient water treatment strategy requires a prospective approach for the production of active and stable photocatalysts. The construction of heterojunctions with different semiconductors is a promising procedure for improving photocatalytic performances. In the present research, binary CeO2-x/BiCrO3 photocatalysts were synthesized using a hydrothermal route preceded by a calcination step. The CeO2-x/BiCrO3 (15%) photocatalyst proved its unique performance of 29.3, 11.4, 11.7, and 23.0 times better than CeO2 for photodegradation of respectively tetracycline hydrochloride (TCH), metronidazole (MET), azithromycin (AZM), and cephalexin (CPN), as antibiotic pollutants, upon visible light. The effective photocatalytic ability, which was caused by the impressive suppression of charge carriers, can be understood by the developed S-scheme mechanism. Moreover, the lower resistance of CeO2-x/BiCrO3 (15%) compared to CeO2, CeO2-x, and BiCrO3 against the charges transfer was another confirmation for boosted photocatalytic performance of the CeO2-x/BiCrO3 (15%) nanocomposite. Ultimately, the boosted activity, repeated utilization for five runs, and biocompatibility confirmation of the purified solution through pinto bean cultivation exhibited that CeO2-x/BiCrO3 photocatalysts could have the promising capability for detoxification of polluted water.

11.
Int J Mol Sci ; 25(14)2024 Jul 10.
Article de Anglais | MEDLINE | ID: mdl-39062829

RÉSUMÉ

Inspired by our finding that metallic Ni particles could be uniformly distributed on a reduced CeO2 surface and stabilized on Ce3+ sites, we suppose a possible improvement in the activity and selectivity of the MgNi/SiO2 vegetable oil hydrogenation catalyst by increasing the surface metal Ni availability via modification by ceria. The proposed approach involved the addition of a CeO2 modifier to the SiO2 carrier and as a catalyst component. Evaluation of the structure, reducibility, and surface and electronic states of the CeO2-doped MgNi/SiO2 catalyst was performed by means of the Powder X-ray diffraction (PXRD), Scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), and X-ray photoelectron spectroscopy (XPS) combined with High-resolution transmission electron microscopy (HRTEM), Temperature-programmed reduction with hydrogen (H2-TPR), and H2-chemisortion techniques. So far, no studies related to this approach of designing Ni/SiO2 catalysts for the partial hydrogenation of vegetable oil have been reported. The added ceria impact was elucidated by comparing fatty acid compositions obtained by the catalysts at an iodine value of 80. In summary, tuning the hydrogenation performance of Ni-based catalysts can be achieved by structural reconstruction using 1 wt.% CeO2. The introduction mode changed the selectivity towards C18:1-cis and C18:0 fatty acids by applying ceria as a carrier modifier, while hydrogenation activity was improved upon ceria operation as the catalyst dopant.


Sujet(s)
Cérium , Nickel , Huiles végétales , Silice , Cérium/composition chimique , Catalyse , Silice/composition chimique , Hydrogénation , Nickel/composition chimique , Huiles végétales/composition chimique , Diffraction des rayons X
12.
J Colloid Interface Sci ; 674: 778-790, 2024 Jun 18.
Article de Anglais | MEDLINE | ID: mdl-38955009

RÉSUMÉ

The CO preferential oxidation reaction (CO-PROX) is an effective strategy to remove residual poisonous CO in proton exchange membrane fuel cells, in which oxygen vacancies play a critical role in CO adsorption and activation. Herein, a series of CuO/CeO2 catalysts derived from Ce-MOFs precursors were synthesized using different organic ligands via the hydrothermal method and the CO-PROX performance was investigated. The CuO/CeO2-135 catalyst derived from homophthalic tricarboxylic acid (1,3,5-H3BTC) exhibited superior catalytic performance with 100 % CO conversion at a relatively low temperature (T100% = 100 °C), with a wide reaction temperature range and excellent stability. The superior catalytic properties were attributed to the structural improvements provided by the 1,3,5-H3BTC precursors and the promotional effects of oxygen vacancies. Additionally, in-situ Raman spectroscopy was performed to verify the dynamic roles of oxygen vacancies for CO adsorption and activation, while in-situ DRIFTS analysis revealed key intermediates in the CO-PROX reaction, shedding light on the mechanistic aspects of the catalytic process. This work not only demonstrates insights into the effective CuO/CeO2 catalysts for CO preferential oxidation, but also provides a feasible way to synthesize MOF-derived catalysts.

13.
ChemSusChem ; : e202400681, 2024 Jul 31.
Article de Anglais | MEDLINE | ID: mdl-39083347

RÉSUMÉ

Transition metal-doped ceria (M-CeO2) catalysts (M = Fe, Co, Ni and Cu) with multiple loadings were experimentally investigated for reverse water gas shift (RWGS) reaction. Density functional theory (DFT) calculations were performed to benchmark the properties that impact catalytic activity of CO2 reduction. Temperature-programmed desorption (TPD) was conducted to study the CO2 binding strength on doped CeO2 surfaces; the trend of the energy along increasing metal loading agrees with the DFT calculations. Notably, CO2 dissociative adsorption energy and oxygen vacancy (OV) formation energy are key descriptors obtained from both DFT and experiments, which can be used to evaluate catalytic performance. Results show the effectiveness of transition metal doping in enhancing CO2 adsorption and reducibility of the surfaces, with Fe showing particularly promising results, i.e., CO2 conversion higher than 56% at 600 °C and 100% selectivity to CO. Cu exhibits 100% selectivity to CO but low CO2 conversion, while Co and Ni showed notable ability of methanation, particularly at high loadings. This study finds that an effective CeO2 based RWGS catalyst corresponds to OV sites that have low OV formation energies for surface reduction, and moderate CO2 adsorption energies for strong interaction with the surface to promote C-O bond scission.

14.
Small ; : e2403517, 2024 Jul 24.
Article de Anglais | MEDLINE | ID: mdl-39045902

RÉSUMÉ

The cyclization of 3-hydroxy alkynes and the carboxylation of terminal alkynes both with CO2 are two attractive strategies to simultaneously reduce CO2 emission and produce value-added chemicals. Herein, the differential activation of alkynes over atomically precise Ag nanoclusters (NCs) supported on Metal-organic framework-derived highly-open mesoporous CeO2 (HM-CeO2) by reserving or removing their surface captopril ligands is reported. The ligand-capped Ag NCs possess electron-rich Ag atoms as efficient π-activation catalytic sites in cyclization reactions, while the naked Ag NCs possess partial positive-charged Ag atoms as perfect σ-activation catalytic sites in carboxylation reactions. Impressively, via coupling with HM-CeO2 featuring abundant basic sites and quick mass transfer, the ligand-capped Ag NCs afford 97.9% yield of 4,4-dimethyl-5-methylidene-1,3-dioxolan-2-one for the cyclization of 2-methyl-3-butyn-2-ol with CO2, which is 4.5 times that of the naked Ag NCs (21.7%), while the naked Ag NCs achieve 98.5% yield of n-butyl 2-alkynoate for the carboxylation of phenylacetylene with CO2, which is 15.6 times that of ligand-capped Ag NCs (6.3%). Density functional theory calculations reveal the ligand-capped Ag NCs can effectively activate alkynyl carbonate ions for the intramolecular ring closing in cyclization reaction, while the naked Ag NCs are highly affiliative in stabilizing terminal alkynyl anions for the insertion of CO2 in carboxylation reaction.

15.
Environ Sci Pollut Res Int ; 31(35): 48103-48121, 2024 Jul.
Article de Anglais | MEDLINE | ID: mdl-39017869

RÉSUMÉ

We have adopted a novel CeO2/Bi2MoO6/g-C3N4-based ternary nanocomposite that was synthesized via hydrothermal technique. The physiochemical characterization of as-prepared samples was examined through various analytical techniques such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy TEM, photoluminescent spectra (PL), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), and ultraviolet diffuse reflectance spectroscopy (UV-DRS) technique. In addition, the photocatalytic performance was carried out by degradation of Rhodamine B dye under visible light irradiation using this nanocatalyst. The ternary nanocomposite achieved 94% of the degradation efficiency within 100 min which is higher than the pristine and binary composites under the predetermined condition pH = 7, Rhodamine B dye = 5 mg/L, and catalyst concentration = 150 mg/L. The experimental synergetic effect of CeO2/Bi2MoO6/g-C3N4 ternary nanocomposite has been ascribed to the interfacial charge carrier migration between CeO2, Bi2MoO6, and g-C3N4. The optical absorption range of CeO2/Bi2MoO6/g-C3N4 ternary nanocomposite was enhanced, and the band gap was reduced up to 2.2 eV. In addition, scavenger trapping experiment proves that the super oxide anions (O2-.) and photogenerated holes are the major active species. The reusability and stability experiment proved the CeO2/Bi2MoO6/g-C3N4 ternary nanocomposite keeps good durability during the photocatalytic degradation process after the five successive cycles. Furthermore, based on the results, the charge carrier transfer photocatalytic mechanism was also discussed. This CeO2/Bi2MoO6/g-C3N4 ternary nanocomposite may offer the cheapest material and extend the great opportunity for clean and environmental remediation approach under the visible light irradiation.


Sujet(s)
Cérium , Rhodamines , Rhodamines/composition chimique , Cérium/composition chimique , Catalyse , Nanosphères/composition chimique , Bismuth/composition chimique , Polluants environnementaux/composition chimique , Nanocomposites/composition chimique , Molybdène/composition chimique
16.
Molecules ; 29(11)2024 Jun 04.
Article de Anglais | MEDLINE | ID: mdl-38893519

RÉSUMÉ

Nitrite is one of the most common nitrogenous compounds, which is not only an important indicator of aquaculture water but also widely used as a food additive. Its potential toxicity poses a huge threat to aquatic products and human health. Therefore, it is important to develop a convenient and rapid sensor for the high-efficient onsite detection of nitrite. In this work, a novel electrochemical sensor was developed for the qualitative and quantitative analysis of nitrite. The developed nitrite electrochemical detection system is easily applied in onsite detection. The electrochemical working electrode was constructed based on the combination of Ag-CeO2 and conductive carbon paste (CPE) with excellent electrocatalysis activity and rapid electron transfer ability. By the application of the developed system and under the optimal conditions, the linear range was from 40.0 µM to 500.0 µM, and the detection limit was reduced to 4.3 µM. The recovery was between 92.1% and 108.1%, and the relative standard deviations (RSDs) were 0.49%~9.31%. The sensor exhibited superior reproducibility, high stability sensitivity, and anti-interference ability, confirming its effectiveness for nitrite analysis. Finally, the developed electrochemical sensor was successfully applied to detect nitrite in beverages and aquaculture water samples, indicating that this approach has great potential in onsite food testing and environmental monitoring.


Sujet(s)
Aquaculture , Boissons , Cérium , Techniques électrochimiques , Nitrites , Nitrites/analyse , Techniques électrochimiques/méthodes , Cérium/composition chimique , Boissons/analyse , Argent/composition chimique , Limite de détection , Polluants chimiques de l'eau/analyse , Électrodes , Reproductibilité des résultats , Eau/composition chimique , Eau/analyse
17.
J Hazard Mater ; 474: 134829, 2024 Aug 05.
Article de Anglais | MEDLINE | ID: mdl-38865924

RÉSUMÉ

Selective catalytic oxidation of the hazardous DMF exhaust gas presents a significant challenge in balancing oxidation activity and products selectivity (CO, NOx, N2, etc.). It is found that Cu/H-MOR demonstrates superior performance for DMF oxidation compared to CuO on other supports (γ-Al2O3, HY, ZSM-5) in terms of product selectivity and stability. The geometric and electronic structures of CuO active sites in Cu/H-MOR have been regulated by CeO2 promoter, leading to an increase in the ratio of active CuO (highly dispersed CuO and Cu+ specie). As a result, the oxidation activity and stability of the Cu/H-MOR catalyst were enhanced for DMF selective catalytic oxidation. However, excessive CuO or CeO2 content led to decreased N2 selectivity due to over-high oxidation activity. It is also revealed that Ce3+ species, active CuO species, and surface acid sites play a critical role in internal selective catalytic reduction reaction during DMF oxidation. The 10Cu-Ce/H-MOR (1/4) catalyst exhibited both high oxidation activity and internal selective catalytic reduction activity due to its abundance of active CuO specie as well as Ce3+ species and surface acid sites. Consequently, the 10Cu-Ce/H-MOR (1/4) catalyst demonstrated the widest temperature window for DMF oxidation with high N2 selectivity. These findings emphasize the importance of surface active sites modification for DMF selective catalytic oxidation.

18.
Nanomaterials (Basel) ; 14(12)2024 Jun 07.
Article de Anglais | MEDLINE | ID: mdl-38921871

RÉSUMÉ

Self-made agglomerated nanometer CeO2-Y2O3-ZrO2 (CYSZ) powders for plasma spray-physical vapor deposition (PS-PVD) were prepared by spray-drying, followed by calcination treatment at four different temperatures (600 °C, 700 °C, 800 °C, 900 °C). The physical properties, microstructure, and phase composition of the calcined powders were investigated using a laser particle size analyzer, scanning electron microscopy (SEM), and X-ray diffraction (XRD). The results showed that compared to the agglomerated powders obtained through spray-drying, the particle size of the agglomerated powders changed with increasing calcination temperature, accompanied by an increase in the self-bonding force of the agglomerated powder particles. The proper calcination temperature improved the sprayability of the powders. Additionally, with the increase in the calcination temperature, a transformation from the m-phase to the t-phase occurred in the powder, with Ce4+ partially entering the Zr lattice to form the t-Zr0.84Ce0.16O2 phase, which facilitated the suppression of the m-phase and improved the high-temperature phase stability. It was also found that the PS-PVD coatings prepared using the aforementioned powders exhibited coarser columnar structures with increasing powder calcination temperature.

19.
Int J Biol Macromol ; 272(Pt 2): 132935, 2024 Jun.
Article de Anglais | MEDLINE | ID: mdl-38844279

RÉSUMÉ

Currently, the treatment of diabetic wounds in clinical practice is still unsatisfactory due to the risks of oxidative damage and bacterial infection during the healing process. An optimal wound dressing should exhibit robust capabilities in scavenging reactive oxygen species (ROS) and combatting bacterial growth. In this study, we utilized borax as a crosslinker and prepared a pH/glucose dual-responsive composite hydrogel based on poly(vinyl alcohol) (PVA), sodium alginate (SA), and tannic acid (TA). This hydrogel, loaded with cerium dioxide, serves as an effective ROS scavenger, promoting wound closure by reducing the level of ROS in the wound area. Additionally, the hydrogel can release the antibacterial drug ofloxacin in response to the low pH and high glucose microenvironment in infected wounds. Results from skin defect model in diabetic mice demonstrated this ROS-scavenging and antibacterial hydrogel can suppress inflammation and accelerate wound healing. In summary, our work provides a new perspective on a local and stimulus-responsive drug delivery strategy for treating diabetic wounds.


Sujet(s)
Antibactériens , Diabète expérimental , Glucose , Hydrogels , Espèces réactives de l'oxygène , Cicatrisation de plaie , Animaux , Cicatrisation de plaie/effets des médicaments et des substances chimiques , Antibactériens/pharmacologie , Antibactériens/composition chimique , Espèces réactives de l'oxygène/métabolisme , Souris , Concentration en ions d'hydrogène , Hydrogels/composition chimique , Hydrogels/pharmacologie , Diabète expérimental/traitement médicamenteux , Diabète expérimental/complications , Alginates/composition chimique , Alginates/pharmacologie , Tanins/composition chimique , Tanins/pharmacologie , Poly(alcool vinylique)/composition chimique , Cérium/composition chimique , Cérium/pharmacologie , Mâle
20.
Chemosphere ; 361: 142576, 2024 Aug.
Article de Anglais | MEDLINE | ID: mdl-38852628

RÉSUMÉ

Photocatalytic degradation stands as a promising method for eliminating gas-phase pollutants, with the efficiency largely hinging on the capture of photogenerated electrons by oxygen. In this work, we synthesized a porous CeO2 single crystal cube with abundant oxygen vacancies as photocatalyst, employing urea as a pore-forming agent and for gas-phase formaldehyde degradation. Compared with the CeO2 cubes without pores, the porous ones were superior in specific surface area, akin to conventional CeO2 nanoparticles. The photocatalytic degradation for gas-phase formaldehyde on porous CeO2 cubes was significantly accelerated, of which degradation rate is 3.3 times and 2.1 times that of CeO2 cubes without pores and CeO2 nanoparticles, respectively. Photoelectric tests and DFT calculations revealed that this enhancement stemmed from facilitated oxygen adsorption due to pronounced oxygen vacancies. Consequently, the capture of photoelectrons by oxygen was promoted and its recombination with holes was suppressed, along with an accelerated generation of curial free radicals such as ·OH. This work reveals the pivotal role of surface oxygen vacancies in promoting adsorbed oxygen, proposing a viable strategy to enhance the photocatalytic degradation efficiency for gas-phase pollutants.


Sujet(s)
Cérium , Formaldéhyde , Oxygène , Formaldéhyde/composition chimique , Cérium/composition chimique , Oxygène/composition chimique , Adsorption , Porosité , Catalyse , Gaz/composition chimique , Polluants atmosphériques/composition chimique
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