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1.
Chemosphere ; 240: 124921, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31726593

RESUMO

The interplay of phenolic molecules with 3d transition metals, such as Fe and Cu, and their oxide surfaces, provide important fingerprints for environmental burdens associated with thermal recycling of e-waste and subsequent generation of notorious dioxins compounds and phenoxy-type Environmental Persistent Free Radicals (EPFRs). DRIFTS and EPR measurements established a strong interaction of the phenol molecule with transition metal oxides via synthesis of phenolic- and catecholic-type EPFRs intermediates. In this contribution, we comparatively examined the dissociative adsorption of a phenol molecule, as the simplest model for phenolic-type compounds, on Cu and Fe surfaces and their partially oxidized configurations through accurate density functional theory (DFT) studies. The underlying aim is to elucidate the specific underpinning mechanism forming phenoxy- or phenolate-type EFPRs. Simulated results show that, the phenol molecule undergoes fission of its hydroxyl's O-H bond via accessible activation energies. These values are lower by 46.5-74.1% when compared with the analogous gas phase value. Physisorbed molecules of phenol incur very low binding energies in the range of -2.1 to -5.5 over clean Cu/Fe and their oxides surfaces. Molecular attributes based on charge transfer and geometrical features are in accord with the very weak interaction in physisorbed states. Thermo-kinetic parameters established over the temperature region of 300 and 1000 K, exhibit a lower activation energy for scission of phenolic's O-H bonds over the oxide surfaces in reference to their pure surfaces (24.7 and 43.0 kcal mol-1vs 38.4 and 47.0 kcal mol-1).


Assuntos
Radicais Livres/química , Fenol/química , Fenóis/química , Adsorção , Catecóis , Dioxinas , Radical Hidroxila , Oxirredução , Óxidos/química , Temperatura Ambiente , Elementos de Transição
2.
Chemosphere ; 239: 124686, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31494321

RESUMO

Oxidative degradation of aniline in aqueous solution was performed by the sono-activated peroxydisulfate coupled with PbO process, wherein a dramatic synergistic effect was found. Experiments were carried out in the batch-wise mode to investigate the influence of various operation parameters on the sonocatalytic behavior, such as ultrasonic power intensity, peroxydisulfate anion concentrations and PbO dosages. According to the scavenging effect of ethanol, methanol and tert-butyl alcohol, the principal oxidizing agents were presumed to be sulfate radicals descended from peroxydisulfate anions, activated via ultrasound or sonocatalysis of PbO. Based on the results attained from gas chromatograph-mass spectrometer, it was hypothesized that aniline was initially oxidized into iminobenzene radicals, followed with formation of nitrosobenzene, p-benzoquinonimine and nitrobenzene respectively. Condensation of nitrosobenzene with aniline generated azobenzene. Phenol was detected as one of degradation intermediates, which was sequentially converted into hydroquinone and p-benzoquinone.


Assuntos
Compostos de Anilina/química , Chumbo/química , Óxidos/química , Fenol/química , Sulfatos/química , Compostos Azo/síntese química , Benzoquinonas/síntese química , Etanol/metabolismo , Cromatografia Gasosa-Espectrometria de Massas , Hidroquinonas/síntese química , Metanol/metabolismo , Nitrobenzenos/síntese química , Compostos Nitrosos/síntese química , Oxidantes , Oxirredução , Semicondutores , Ondas Ultrassônicas , terc-Butil Álcool/metabolismo
3.
Chemosphere ; 239: 124745, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31521939

RESUMO

A novel three dimensional MnO2 modified biochar-based porous hydrogel (MBCG) was fabricated to overcome the low sorption capacity and difficulty in solid-liquid separation of biochar (BC) for Cd(II) and Pb(II) removal. BC was initially modified by a rapid redox reaction between KMnO4 and Mn(II) acetate, and then incorporated into a polyacrylamide gel network via a rapid and facile free-radical polymerization. A foaming method was deliberately introduced during the fabrication to establish interpenetrated porous structure inside the network. Various characterizations were employed to examine the morphology, porous structures, chemical compositions, and mechanical properties of the samples. Adsorption performance of MBCG on Cd(II) and Pb(II) (isotherms and kinetics) as well as its desorption and reusability were also investigated. The results indicated that MnO2 modified biochars (MBC) were successfully introduced and homogeneously distributed in the porous bulk hydrogel, endowing MBCG with more uniform pore structure, excellent thermostability, remarkable mechanic strength, and superior adsorption performance. The maximum Langmuir adsorption capacity on Cd(II) and Pb(II) is 84.76 and 70.90 mg g-1, respectively, which is comparable or even larger than that of MBC. More importantly, MBCG can be rapidly separated and easily regenerated with an excellent reusability, which could retain 92.1% and 80.5% of the initial adsorption capacities of Cd(II) and Pb(II) after five cycles. These new insights make MBCG an ideal candidate in practical applications in water treatment and soil remediation contaminated with various heavy metals.


Assuntos
Cádmio/isolamento & purificação , Carvão Vegetal/química , Hidrogéis/química , Chumbo/isolamento & purificação , Compostos de Manganês/química , Óxidos/química , Resinas Acrílicas/química , Adsorção , Cádmio/química , Poluentes Ambientais/química , Poluentes Ambientais/isolamento & purificação , Chumbo/química , Microscopia Eletrônica de Varredura , Microscopia Eletrônica de Transmissão , Polimerização , Porosidade , Impressão Tridimensional , Espectroscopia de Infravermelho com Transformada de Fourier , Termogravimetria
4.
Chemosphere ; 239: 124763, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31526989

RESUMO

Nonredox metal ions have been widely recognized to be important in a wide range of biological and chemical oxidations as Lewis acids (LA). However, the role of LA in peroxymonosulfate (PMS) activation for wastewater treatment has not been considered until now. This study shows that oxidizing power of PMS can be promoted after binding nonredox metal ions such as Ca2+ as LA, leading to the easier reduction of the oxidant to radicals and substantial enhancement of dye degradation by employing manganese oxides OMS-2 as model catalysts. Increased with Lewis acidity of the metal ion, the rate of PMS decomposition enhanced linearly, while the dye degradation rate first increased and then declined due to the formation of a larger amount of dioxygen. The interactions between Ca2+ and PMS were further investigated by Raman, cyclic voltammetry and XPS; and the detailed mechanism of PMS activation was proposed. The performance of Ca2++OMS-2/PMS system under different conditions was also studied. The findings indicate the importance of LA in PMS activation reaction and their role must be considered in other transition metal oxides/PMS systems. It will be also helpful to design new and highly active catalysts for the reactions.


Assuntos
Ácidos de Lewis/química , Compostos de Manganês/química , Óxidos/química , Peróxidos/química , Poluentes Químicos da Água/química , Cálcio/química , Catálise , Corantes/química , Oxidantes/química , Oxirredução , Soluções , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química
5.
J Colloid Interface Sci ; 559: 313-323, 2020 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-31675662

RESUMO

Antibiotic resistance is a common phenomenon observed during treatment with antibacterials. Use of nanozymes, especially those with synergistic enzyme-like activities, as antibacterials could overcome this problem, but their synthesis is limited by their high cost and/or complex production process. Herein, vanadium oxide nanodots (VOxNDs) were prepared via a one-step bottom-up ethanol-thermal method using vanadium trichloride as the precursor. VOxNDs alone possess bienzyme mimics of peroxidase and oxidase. Accordingly, highly efficient antibacterials against drug-resistant bacteria can be obtained through synergistic catalysis; the oxidase-like activity decomposes O2 to generate superoxide anion radical (O2-) and hydroxyl radicals (OH), and the intrinsic peroxidase-like activity can further induce the production of OH from external H2O2. Consequently, H2O2 concentration could decrease up to four magnitude orders with VOxNDs to achieve an antibacterial efficacy similar to that of H2O2 alone. Wound healing in vivo further confirms the high antibacterial efficiency, good biocompatibility, and application potential of the synergistic antibacterial system due to the "nano" structure of VOxNDs. The method of synthesis of nanodot antibacterials described in this paper is inexpensive, and the results of this study reveal the multi-enzymatic synergism of nanozymes.


Assuntos
Antibacterianos/química , Nanopartículas Metálicas/química , Óxidos/química , Compostos de Vanádio/química , Cicatrização/efeitos dos fármacos , Animais , Materiais Biocompatíveis/química , Materiais Biomiméticos/química , Catálise , Sobrevivência Celular/efeitos dos fármacos , Farmacorresistência Bacteriana/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Células HeLa , Células Endoteliais da Veia Umbilical Humana , Humanos , Peróxido de Hidrogênio/química , Radical Hidroxila/química , Peroxidases/metabolismo , Ratos Sprague-Dawley , Staphylococcus aureus/efeitos dos fármacos
6.
J Environ Sci (China) ; 87: 60-70, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31791518

RESUMO

The performance of Ce-OMS-2 catalysts was improved by tuning the fill percentage in the hydrothermal synthesis process to increase the oxygen vacancy density. The Ce-OMS-2 samples were prepared with different fill percentages by means of a hydrothermal approach (i.e. 80%, 70%, 50% and 30%). Ce-OMS-2 with 80% fill percentage (Ce-OMS-2-80%) showed ozone conversion of 97%, and a lifetime experiment carried out for more than 20 days showed that the activity of the catalyst still remained satisfactorily high (91%). For Ce-OMS-2-80%, Mn ions in the framework as well as K ions in the tunnel sites were replaced by Ce4+, while for the others only Mn ions were replaced. O2-TPD and H2-TPR measurements proved that the Ce-OMS-2-80% catalyst possessed the greatest number of mobile surface oxygen species. XPS and XAFS showed that increasing the fill percentage can reduce the AOS of Mn and augment the amount of oxygen vacancies. The active sites, which accelerate the elimination of O3, can be enriched by increasing the oxygen vacancies. These findings indicate that increasing ozone removal can be achieved by tuning the fill percentage in the hydrothermal synthesis process.


Assuntos
Modelos Químicos , Ozônio/química , Catálise , Manganês/química , Óxidos/química , Oxigênio
7.
J Colloid Interface Sci ; 558: 137-144, 2020 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-31586733

RESUMO

Platinum oxide (PtOx) nanoparticles (NPs) have been shown to possess anticancer activity by releasing ionic Pt species under biological conditions. However, the dissolution kinetics and the changes in the chemical state of Pt during PtOx dissolution have not yet been studied. To fill this gap, we prepared a composite (designated as PtOx@MMT-2) containing PtOx NPs on hollow mesoporous silica nanospheres and studied the dissolution of the material in different biorelevant media. We found that the release of Pt was retarded due to the adsorption of biomolecules on PtOx NPs during the degradation of host silica. The biomolecules adsorption also lowered the accessibility of PtOx NPs, resulting in the reduced catalase-like activity of the NPs. In line with the results, the cytotoxicity of PtOx@MMT-2, which was positively correlated to the amount of Pt uptake, was reduced by biomolecules adsorption. Our findings should be applicable to other metal (oxide) NPs under biological conditions and may provide implications for the design of nanomaterials for practical therapeutic applications.


Assuntos
Materiais Biocompatíveis/química , Nanopartículas/química , Óxidos/química , Platina/química , Dióxido de Silício/química , Adsorção , Materiais Biocompatíveis/farmacologia , Sobrevivência Celular/efeitos dos fármacos , Células HeLa , Humanos , Nanopartículas/uso terapêutico , Solubilidade
8.
Chem Commun (Camb) ; 55(87): 13100-13103, 2019 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-31612179

RESUMO

Using the steady state and time resolved NIR emission and specific chemical trapping techniques, we show for the first time that metal halide perovskite quantum dots can effectively generate singlet oxygen with a quantum yield of up to 0.34, the highest among nano semiconductor/nano metal singlet oxygen photosensitizers. The mechanism is concluded to be due to energy transfer from triplet excitons to molecular oxygen.


Assuntos
Compostos de Cálcio/química , Hidrocarbonetos Halogenados/química , Compostos Organometálicos/química , Óxidos/química , Fármacos Fotossensibilizantes/química , Pontos Quânticos/química , Oxigênio Singlete/química , Titânio/química , Raios Infravermelhos , Tamanho da Partícula , Propriedades de Superfície
9.
Chem Commun (Camb) ; 55(89): 13366-13369, 2019 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-31631205

RESUMO

A target-triggered, self-powered strategy for in situ monitoring of intracellular microRNAs was fabricated via a versatile DNAzyme-MnO2 nanosystem, which integrates delivery, quenching, target recognition, self-supply of cofactors and signal amplification all in one.


Assuntos
Sobrevivência Celular , DNA Catalítico/química , Compostos de Manganês/química , MicroRNAs/análise , Nanopartículas/química , Imagem Óptica , Óxidos/química , Linhagem Celular Tumoral , DNA Catalítico/metabolismo , Células HeLa , Humanos , Células MCF-7 , Compostos de Manganês/metabolismo , Nanopartículas/metabolismo , Óxidos/metabolismo
10.
Chemosphere ; 235: 1189-1196, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31561310

RESUMO

A high oxygen evolution potential (2.6V) and conductivity of Ti/TiO2 NTs/Ta2O5-PbO2 anode was fabricated by mixed metal oxide. A well-aligned TiO2 nanotubes was successfully prepared by using 1-butyl-3-methylimidazolium tetrafluoroborate as the electrolyte. The surface structure of anodes were characterized by scanning electron microscope, X-ray diffraction and energy dispersive X-ray spectroscopy. During the electrochemical degradation experiments, the effects of different anodes, current density, initial pH value and concentration were discussed. The results showed that co-doped Ta2O5 coating is an effective method to improve the surface morphology and the electrochemical characterization of Ti/TiO2 NTs/PbO2. At the initial pH value of 3 and current density of 12 mA cm-2, the removal rates of Acid Orange 7 and total organic carbon with Ti/TiO2 NTs/Ta2O5-PbO2 anode were almost 100% and 98.3%. Comparing with Ti/PbO2 anode at the same charge consumption (3 A h L-1), the instantaneous current efficiency of the Ti/TiO2 NTs/Ta2O5-PbO2 anode and Ti/TiO2 NTs/PbO2 anode increased by 40.0% and 27.1%, respectively. The highest rate of k.OH on Ti/TiO2 NTs/Ta2O5-PbO2 anode was 12.4 µmol (L min)-1. The organic dyes are oxidized into CO2 and H2O by .OH radical. The reaction process and mechanism during the electrochemical degradation were discussed.


Assuntos
Corantes/química , Técnicas Eletroquímicas/métodos , Nanotubos/química , Titânio/química , Compostos Azo , Benzenossulfonatos , Eletrodos , Oxirredução , Óxidos/química
11.
Braz Oral Res ; 33: e042, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31508725

RESUMO

This study evaluated the cytotoxicity and biocompatibility of a new bioceramic endodontic sealer (i.e., Sealer Plus BC) in comparison with those of MTA Fillapex and AH Plus. L929 fibroblasts were cultured and Alamar Blue was used to evaluate cell viability of diluted extracts (1:50, 1:100, and 1:200) from each sealer at 24 h. Polyethylene tubes that were filled with material or empty (as a control) were implanted in the subcutaneous tissue of rats. The rats were killed after 7 and 30 d (n = 8), and the tubes were removed for histological analysis. Parametric data was analyzed using a one-way ANOVA test, and nonparametric data was analyzed via the Kruskal-Wallis test followed by the Dunn test (p < 0.05). A reduction in cell viability was observed in the extracts that were more diluted for Sealer Plus BC when compared to that of Control and AH Plus (p < 0.05). However, the 1:50 dilution of the Sealer Plus BC was similar to that of the Control (p > 0.05). Conversely, more diluted extracts of MTA Fillapex (1:200) and AH Plus (1:100 and 1:200) were similar to the Control (p > 0.05). Histological analysis performed at 7 d did not indicate any significant difference between tissue response for all materials, and the fibrous capsule was thick (p > 0.05). At 30 d, Sealer Plus BC was similar to the Control (p > 0.05) and MTA Fillapex and AH Plus exhibited greater inflammation than the Control (p < 0.05). The fibrous capsule was thin for the Control and for most specimens of Sealer Plus BC and AH Plus. Thus, Sealer Plus BC is biocompatible when compared to MTA Fillapex and AH Plus, and it is less cytotoxic when less-diluted extracts are used.


Assuntos
Cimentos para Ossos/química , Hidróxido de Cálcio/química , Cerâmica/química , Materiais Restauradores do Canal Radicular/química , Compostos de Alumínio/química , Animais , Materiais Biocompatíveis , Cimentos para Ossos/farmacologia , Cimentos para Ossos/toxicidade , Compostos de Cálcio/química , Hidróxido de Cálcio/farmacologia , Hidróxido de Cálcio/toxicidade , Sobrevivência Celular/efeitos dos fármacos , Células Cultivadas/efeitos dos fármacos , Combinação de Medicamentos , Resinas Epóxi/química , Fibroblastos/efeitos dos fármacos , Técnicas In Vitro , Inflamação , Masculino , Teste de Materiais , Óxidos/química , Ratos Wistar , Materiais Restauradores do Canal Radicular/toxicidade , Silicatos/química , Tela Subcutânea/patologia
12.
J Appl Oral Sci ; 27: e20180556, 2019 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-31508791

RESUMO

OBJECTIVE: To evaluate the effect of ultrasonic and sonic activation on physicochemical properties of AH Plus, MTA Fillapex, ADSeal, GuttaFlow Bioseal, and GuttaFlow 2 sealers. METHODOLOGY: Three experimental groups were formed: no activation (NA), ultrasonic activation (UA), and sonic activation (SA). The sealers were manipulated according to the manufacturers' instructions. A 3-mL syringe was adapted to receive 1 mL of sealer. Activation was performed with a 20/.01 ultrasonic insert (20 s/1W) in the UA group. A size 35.04 sonic tip was used (20 s/10,000 cycles/min-1) in the SA group. The molds for physicochemical analysis were filled and evaluated according to ANSI/ADA specification no. 57: setting time (ST), flow (FL), dimensional change (DC), solubility (SB), and radiopacity (RD). Statistical analysis was performed by Kruskal-Wallis, one-way ANOVA, and Tukey's tests (P<0.05). RESULTS: Regarding ST, only AH Plus and GuttaFlow 2 in the NA group met the ANSI/ADA standards. All FL values were greater than 20 mm in diameter, as determined by ANSI/ADA. The tested sealers and protocols did not comply with the ANSI/ADA standards for DC. As for SB, only MTA Fillapex, regardless of the activation protocol, did not follow the ANSI/ADA standards. All of the investigated sealers, regardless of the activation protocol, presented radiographic density higher than 3 mm Al, as proposed by ANSI/ADA. CONCLUSIONS: UA and SA promoted changes in the physicochemical properties of the evaluated root canal sealers, mainly in ST and F. Thus, it is important to evaluate the physicochemical properties of endodontic sealers associated with activation techniques prior to clinical application in order to determine whether the properties follow the parameters set by ANSI/ADA, ensuring safety and quality of root canal filling.


Assuntos
Compostos de Alumínio/química , Compostos de Cálcio/química , Dimetilpolisiloxanos/química , Resinas Epóxi/química , Guta-Percha/química , Óxidos/química , Materiais Restauradores do Canal Radicular/química , Silicatos/química , Ondas Ultrassônicas , Análise de Variância , Combinação de Medicamentos , Teste de Materiais , Valores de Referência , Reprodutibilidade dos Testes , Solubilidade , Estatísticas não Paramétricas , Propriedades de Superfície , Fatores de Tempo
13.
J Environ Sci (China) ; 85: 168-176, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31471023

RESUMO

Cadmium (Cd) and arsenic (As) are two of the most toxic elements. However, the chemical behaviors of these two elements are different, making it challenging to utilize a single adsorbent with high adsorption capacity for both Cd(II) and As(V) removal. To solve this problem, we synthesized HA/Fe-Mn oxides-loaded biochar (HFMB), a novel ternary material, to perform this task, wherein scanning electron microscopy (SEM) combined with EDS (SEM-EDS) was used to characterize its morphological and physicochemical properties. The maximum adsorption capacity of HFMB was 67.11 mg/g for Cd(II) and 35.59 mg/g for As(V), which is much higher compared to pristine biochar (11.06 mg/g, 0 mg/g for Cd(II) and As(V), respectively). The adsorption characteristics were investigated by adsorption kinetics and the effects of the ionic strength and pH of solutions. X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FT-IR) revealed that chelation and deposition were the adsorption mechanisms that bound Cd(II) to HFMB, while ligand exchange was the adsorption mechanism that bound As(V).


Assuntos
Arsênico/química , Cádmio/química , Poluentes Ambientais/química , Carvão Vegetal , Óxidos/química
15.
J Photochem Photobiol B ; 198: 111579, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31401316

RESUMO

The sol-gel/ultrasonically rout produced the novel MnS2-SiO2 nano-hetero-photocatalysts with the various ratio of MnS2. Prepared nano-catalyst were investigated in the photo-degradation of methylene blue under UV light illumination. Structural and optical attributes of as-prepared nano-catalysts were evaluated by X-ray diffraction and photoelectron spectroscopy. The morphological were studied by scanning electron microscopy-EDS, and dynamic light scattering. The diffuse reflectance spectroscopy was applied to examine the band gap energy. The Eg values of SiO2, MnS2-SiO2-0, MnS2-SiO2-1, and MnS2-SiO2-2 nanocomposites are 6.51, 3.85, 3.17, and 2.67 eV, respectively. The particle size of the SiO2 and MnS2-SiO2-1 nanocomposites were 100.0, and 65.0 nm, respectively. The crystallite size values of MnS2-SiO2-1 were 52.21 nm, and 2.9 eV, respectively. MnS2-SiO2 nano-photocatalyst was recognized as the optimum sample by degrading 96.1% of methylene blue from water. Moreover, the influence of pH of the solution, and contact time as decisive factors on the photo-degradation activity were investigated in this project. The optimum data for pH and time were found 9 and 60 min, respectively. The photo-degradation capacity of MnS2-SiO2-2 is improved (96.1%) due to the low band gap was found from UV-vis DRS. The antimicrobial data of MnS2-SiO2 were studied and demonstrated that the MnS2-SiO2 has fungicidal and bactericidal attributes.


Assuntos
Anti-Infecciosos/química , Antioxidantes/química , Compostos de Manganês/química , Nanocompostos/química , Óxidos/química , Dióxido de Silício/química , Raios Ultravioleta , Anti-Infecciosos/síntese química , Anti-Infecciosos/farmacologia , Antioxidantes/síntese química , Catálise , Escherichia coli/efeitos dos fármacos , Fungos/efeitos dos fármacos , Concentração de Íons de Hidrogênio , Azul de Metileno/química , Tamanho da Partícula , Streptococcus pyogenes/efeitos dos fármacos
16.
Mar Pollut Bull ; 146: 366-376, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31426169

RESUMO

Solid-phase speciation and porewater chemistry measured by the diffusive gradients in thin films (DGT) technique were used to understand the diagenesis of sulfur (S), iron (Fe), and phosphorus (P) in sediments of Jiaozhou Bay (China), which has been impacted by multiple anthropogenic perturbations. Despite water eutrophication, sediments of the bay are low in organic carbon and sulfide, but high in unsulfidized Fe(II). Dissimilatory iron reduction (DIR) prevails in sediments of the bay, and there is no evidence for responses of S and Fe diagenesis to the water eutrophication, which is largely attributable to unique depositional and diagenetic regimes in association with multiple anthropogenic perturbations. Good coupling of porewater Fe2+ and P in the porewaters suggests that P mobilization is driven mainly by DIR. Low Fe2+/P ratios in porewaters imply that oxidative regeneration of Fe oxides within the upper sediments is incapable of efficiently scavenging upward diffusing P.


Assuntos
Sedimentos Geológicos/química , Ferro/química , Fósforo/química , Enxofre/química , Baías , Isótopos de Carbono/análise , China , Monitoramento Ambiental/métodos , Eutrofização , Sedimentos Geológicos/análise , Ferro/análise , Nitrogênio/análise , Oxirredução , Óxidos/análise , Óxidos/química , Fósforo/análise , Água do Mar/química , Sulfetos/análise , Sulfetos/química , Enxofre/análise , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/química
17.
J Phys Chem Lett ; 10(18): 5343-5350, 2019 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-31452370

RESUMO

In this work, a sensitive deep ultraviolet (DUV) light photodetector based on inorganic and lead-free Cs3Cu2I5 crystalline film derived by a solution method was reported. Optoelectronic characterization revealed that the perovskite device exhibited nearly no sensitivity to visible illumination with wavelength of 405 nm but exhibited pronounced sensitivity to both DUV and UV light illumination with response speeds of 26.2/49.9 ms for rise/fall time. The Ilight/Idark ratio could reach 127. What is more, the responsivity and specific detectivity were calculated to be 64.9 mA W-1 and 6.9 × 1011 Jones, respectively. In addition, the device could keep its photoresponsivity after storage in air environment for a month. It is also found that the capability of Cs3Cu2I5 crystalline film device can readily record still DUV image with acceptable resolution. The above results confirm that the DUV photodetector may hold great potential for future DUV optoelectronic device and systems.


Assuntos
Compostos de Cálcio/química , Césio/química , Cobre/química , Desenho de Equipamento/instrumentação , Iodetos/química , Óxidos/química , Titânio/química , Cristalização , Técnicas Eletroquímicas/métodos , Cinética , Membranas Artificiais , Processos Fotoquímicos , Fenômenos Físicos , Propriedades de Superfície , Termodinâmica , Raios Ultravioleta
18.
Bioelectrochemistry ; 130: 107347, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31437809

RESUMO

A multifunctional nanocomposite theranostic system is constructed of manganese oxide (Mn3O4) nanoparticles (NPs), as a tumor diagnostic agent, in conjunction with polyacrylic acid (PAA), as a pH-sensitive drug delivery agent, and methotrexate (MTX), as a model of targeting agent and anticancer drug. Physicochemical characteristics of the Mn3O4@PAA/MTX system is studied in detail by several techniques, including X-ray and Auger photoelectron spectroscopy, Fourier transform infrared spectroscopy, X-ray diffraction, field-emission scanning electron microscopy, transmission electron microscopy, and electrochemical methods. The system performance is studied based on (i) in-vitro MRI measurements to support efficiency of the Mn3O4@PAA NPs as a diagnostic agent, (ii) drug release performance of the Mn3O4@PAA/MTX NPs at pHs of 5.4 and 7.4 through in-vitro method to evaluate application of the NPs as pH-sensitive nanocarriers for MTX, and (iii) impedance spectroscopy measurements to show Mn3O4@PAA/MTX NPs affinity for capturing of cancer cells. The results show that (i) Mn3O4@PAA NPs can be used as a contrast agent in MRI measurements (r1 ≅ 6.5 mM-1 s-1), (ii) the MTX, loaded on Mn3O4@PAA NPs, is released faster and more efficient at pH 5.4 than 7.4, and (iii) the GC-Mn3O4@PAA/MTX electrode system captures the 4T1 cells 3.32 times larger than L929 cells.


Assuntos
Resinas Acrílicas/química , Antineoplásicos/administração & dosagem , Preparações de Ação Retardada/química , Compostos de Manganês/química , Metotrexato/administração & dosagem , Nanopartículas/química , Óxidos/química , Animais , Antineoplásicos/farmacocinética , Antineoplásicos/farmacologia , Neoplasias da Mama/diagnóstico por imagem , Neoplasias da Mama/tratamento farmacológico , Linhagem Celular Tumoral , Meios de Contraste/química , Liberação Controlada de Fármacos , Feminino , Concentração de Íons de Hidrogênio , Imagem por Ressonância Magnética , Metotrexato/farmacocinética , Metotrexato/farmacologia , Camundongos , Nanomedicina Teranóstica
19.
J Food Sci ; 84(9): 2507-2519, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31432530

RESUMO

Metal oxide coated multilayered polymeric pouches provide a suitable alternative to foil-based packaging for shelf-stable products with extended shelf-life. The barrier performance of these films depends upon the integrity of the metal oxide coating which can develop defects as a result of thermal processing and improper handling. In this work, we developed a methodology to visually identify these defects using an oxygen-sensitive model gel system. Four pouches with different metal oxide coatings: MOA (Coated PET), MOB (SiOx -coated PET), MOC (Overlayer-AlOx -Organic-coated PET), MOD (Overlayer-SiOx -coated PET) were filled with water and retort-processed for 30 and 40 min at 121 °C. After processing, the pouches were cut open, dried and subsequently filled with a gel containing methylene blue that changes color in the presence of oxygen. The pouches were then stored at 23 and 40 °C for 180 and 90 days, respectively. Defects were identified by observing the localized color change from yellow to blue in the packaged gel. These observations were confirmed through measurement of oxygen and water vapor transmission rates, as well as SEM and CLSM analyses. The MOC pouches showed the least change in barrier properties after thermal processing. This was due to crosslinking in the organic coating and protection provided by the overlayer. The melting enthalpy of all films increased significantly (P < 0.05) after sterilization. This may increase the brittleness of the substrates after processing. Findings may be used to improve the barrier performance of metal oxide coated polymeric films intended for food packaging applications. PRACTICAL APPLICATION: In this study, we developed a methylene blue-based, oxygen-sensitive model gel system to identify defects in metal oxide coated polymeric structures induced by thermal processing and mechanical stresses. We also performed a comprehensive analysis of these defects through CLSM and SEM. The gel system and methodology developed may be useful in the design and development of high barrier metal oxide coated films.


Assuntos
Técnicas de Química Analítica/métodos , Embalagem de Alimentos/instrumentação , Géis/química , Metais/química , Oxigênio/química , Polímeros/química , Cor , Óxidos/química , Vapor/análise
20.
J Enzyme Inhib Med Chem ; 34(1): 1465-1473, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31411081

RESUMO

In this investigation, we studied a family of compounds with an oxathiazolidine-4-one-2,2-dioxide skeleton and their amide synthetic precursors as new anticonvulsant drugs. The cyclic structures were synthesized using a three-step protocol that include solvent-free reactions and microwave-assisted heating. The compounds were tested in vivo through maximal electroshock seizure test in mice. All the structures showed activity at the lower doses tested (30 mg/Kg) and no signs of neurotoxicity were detected. Compound encoded as 1g displayed strong anticonvulsant effects in comparison with known anticonvulsants (ED50 = 29 mg/Kg). First approximations about the mechanisms of action of the cyclic structures were proposed by docking simulations and in vitro assays against sodium channels (patch clamp methods).


Assuntos
Anticonvulsivantes/química , Anticonvulsivantes/farmacologia , Desenho de Drogas , Imidas/química , Imidas/farmacologia , Tiazóis/química , Animais , Anticonvulsivantes/administração & dosagem , Anticonvulsivantes/síntese química , Espectroscopia de Ressonância Magnética Nuclear de Carbono-13 , Relação Dose-Resposta a Droga , Células HEK293 , Humanos , Imidas/síntese química , Masculino , Camundongos , Canal de Sódio Disparado por Voltagem NAV1.1/efeitos dos fármacos , Óxidos/química , Técnicas de Patch-Clamp , Espectroscopia de Prótons por Ressonância Magnética
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