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1.
Water Environ Res ; 96(2): e10984, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38298030

RESUMEN

In this study, a highly efficient peroxymonosulfate (PMS) activator, ZnO/ZnMn2 O4 , was synthesized using a simple one-step hydrothermal method. The resulting bimetallic oxide catalyst demonstrated a homogenous and high-purity composition, showcasing synergistic catalytic activity in activating PMS for degrading 2, 4-dichlorophenol (2, 4-DCP) in aqueous solution. This catalytic performance surpassed that of individual ZnO, Mn2 O3 , and ZnMn2 O4 metal materials. Under the optimized conditions, the removal efficiency of 2, 4-DCP reached approximately 86% within 60 min, and the catalytic ability remained almost constant even after four cycles of recycling. The developed degradation system proved effective in degrading other azo-dye pollutants. Certain inorganic anions such as HPO4 - , HCO3 - , and NO3 - significantly inhibited the degradation of 2, 4-DCP, while Cl- and SO4 2- did not exhibit such interference. Results from electrochemical experiments indicated that the electron transfer ability of ZnO/ZnMn2 O4 surpassed that of individual metals, and electron transfer occurred between ZnO/ZnMn2 O4 and the oxidant. The primary active radicals responsible for degrading 2, 4-DCP were identified as SO4 •- , OH• and O2 •- , generated through the oxidation and reduction of PMS catalyzed by Zn (II) and Mn (III). Furthermore, X-ray photoelectron spectroscopy (XPS) analysis of the fresh and used catalysts revealed that the exceptional electron transfer ability of ZnO facilitated the valence transfer of Mn (III) and the transfer of electrons to the catalyst's oxygen surface, thus enhancing the catalytic efficiency. The analysis of radicals and intermediates indicates that the two main pathways for degrading 2, 4-DCP involve hydroxylation and radical attack on its aromatic ring. PRACTITIONER POINTS: A bimetallic ZnO/ZnMn2 O4 catalyst was synthesized and characterized. ZnO/ZnMn2 O4 can synergistically activate PMS to degrade 2, 4-DCP compared with single metal oxide. Three primary active radicals, O2 •- , • OH, and SO4 •- , were generated to promote the degradation. ZnO promoted electron transfer among the three species of Mn to facilitate oxidizing pollutants. Hydroxylation and radical attack on the aromatic ring of 2, 4-DCP are the two degradation pathways.


Asunto(s)
Contaminantes Ambientales , Óxido de Zinc , Peróxidos/química , Óxidos , Fenoles , Oxígeno , Catálisis
2.
Int J Biol Macromol ; 223(Pt A): 1083-1093, 2022 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-36372101

RESUMEN

Fucoidan (FU) is a natural sulfated polysaccharide with certain biological activity and has been shown to be an excellent nano-delivery material. In this study, ferulic acid (FA)-loaded FU nanoparticles (FA/FU NPs) were prepared and their nephroprotective mechanism was investigated. With a particle size of 158.6 ± 4.5 nm, FA/FU NPs increased the antioxidant activity of FA in vitro, possibly related to the increased dispersity of FA. In vitro results demonstrated that FA/FU NPs significantly protected human renal proximal tubule (HK-2) cells from cisplatin-induced damage, possibly by suppressing cisplatin-induced DNA damage and activating the cGAS-STING pathway. Furthermore, in vivo experiments confirmed that FA/FU NPs protected mice from cisplatin-induced acute kidney injury (AKI). Mechanistic studies confirmed that FA/FU NPs exerted nephroprotective effects by reducing MDA activity and increasing GSH and SOD activity. Our results demonstrated the potential of FU for delivering poorly soluble drug FA and protecting against cisplatin-induced AKI.


Asunto(s)
Lesión Renal Aguda , Nanopartículas , Ratones , Humanos , Animales , Cisplatino/efectos adversos , Ácidos Cumáricos/farmacología , Lesión Renal Aguda/inducido químicamente , Lesión Renal Aguda/tratamiento farmacológico , Polisacáridos/efectos adversos
3.
Glycoconj J ; 38(5): 551-560, 2021 10.
Artículo en Inglés | MEDLINE | ID: mdl-34515908

RESUMEN

Methylene blue (MB) is one of the most common cationic dyes to detect heparin. As the sulfate residue presented in heparin was the main contributor to bind with MB, the UV performance of the MB with selectively desulfated heparin derivatives was investigated. It was found that the sulfate residue in different heparin analogues did not show the equal ability to attract MB binding. The stoichiometry of sulfate with MB among the heparin and derivatives was verified as a non-constant number. For the two selectively desulfated heparin derivatives: sulfate elimination at 6-O (6-OdeS) and N-acetylated heparin (N-deS-Acetyl), the MB to sulfate ratios were significantly higher than for heparin. For the not fully diminished sulfate at 2-O heparin derivative (2-OdeS), the MB-SO3- ratio of 2-OdeS was between 6-OdeS, N-deS-Acetlyl and heparin. Although in a distinct sulfation position, the MB-SO3- ratio of 6-OdeS and N-deS-Acetyl was almost equal, which agreed with the comparable total desulfation degree between 6-OdeS and N-deS-Acetyl. In addition, compared to heparin groups, the non-desulfated gs-HP showed no significantly different MB-SO3- ratio with heparin. The above results demonstrated that compared with the sulfate location and glycan composition of heparin, the content of sulfate was the most essential factor for the MB binding.


Asunto(s)
Anticoagulantes/química , Inhibidores Enzimáticos/química , Heparina/química , Azul de Metileno/química , Sulfatos/química , Enlace de Hidrógeno , Concentración de Iones de Hidrógeno , Estructura Molecular
4.
Biotechnol Prog ; 36(1): e2901, 2020 01.
Artículo en Inglés | MEDLINE | ID: mdl-31465150

RESUMEN

ε-Caprolactone (ε-CL) has attracted a great deal of attention and a high product concentration is of great significance for reducing production cost. The optimization of ε-CL synthesis through chemoenzymatic Baeyer-Villiger oxidation mediated by immobilized Trichosporon laibacchii lipase was studied using response surface methodology (RSM). The yield of ε-CL was 98.06% with about 1.2 M ε-CL concentration that has a substantial increase mainly due to both better stability of the cross-linked immobilized lipase used and the optimum reaction conditions in which the concentration of cyclohexanone was 1.22 M, the molar ratio of cyclohexanone:urea hydrogen peroxide (UHP) was 1:1.3, and the reaction temperature was 56.5°C. Based on our experimental results, it can be safely concluded that there are three reactions in this reaction system, not just two reactions, in which the third reaction is that the acetic acid formed reacts with UHP to form peracetic acid in situ catalyzed by the immobilized lipase. A quadratic polynomial model based on RSM experimental results was developed and the R2 value of the equation is 0.9988, indicating that model can predict the experimental results with high precision. The experimental results also show that the molar ratio of cyclohexanone to UHP has very significant impact on the yield of ε-CL (p < .0006).


Asunto(s)
Caproatos/metabolismo , Ciclohexanonas/metabolismo , Lactonas/metabolismo , Lipasa/metabolismo , Basidiomycota/enzimología , Biocatálisis , Caproatos/química , Ciclohexanonas/química , Enzimas Inmovilizadas/metabolismo , Lactonas/química , Estructura Molecular , Oxidación-Reducción , Propiedades de Superficie
5.
Drug Dev Ind Pharm ; 46(1): 42-49, 2020 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-31794271

RESUMEN

The number of Parkinson's disease (PD) patients with the advanced phase and motor fluctuations is increasing. The objective of this study is developing levodopa/benzylhydrazine orally disintegrating tablets (L/B ODTs), which would provide greater convenience and ease of use than conventional tablets for these patients. In the present study, the L/B ODTs were developed successfully with an optimized formulation using response surface methodology (RSM). The direct compression technology was employed for the preparation of L/B ODTs. Considerably shorter disintegration time and faster dissolution profile were obtained under the optimum formulation with microcrystalline cellulose 25.7%, cross-polyvinylpyrrolidone 6.22% and Sodium carboxymethyl starch 5.36%. The content uniformity (%) of levodopa and benzylhydrazine was 50 ± 1.4% and 14.25 ± 0.6%, respectively. Thickness, friability, hardness and wetting time were 2.8 ± 0.05 mm, 0.46 ± 0.21%, 5.42 ± 1.1 kp and 31.2 ± 2.1 s, respectively, and all of data well comply with the General Principles of the Chinese Pharmacopeia. Mannitol of 22% in formulation could bring a pleasant taste: sweet, cool and refreshing. Almost all the volunteers felt that the ODTs had good taste, no roughness, and no gritty feeling, indicating that the ODTs prepared had good palatability, so patients will have good compliance when taking medicine.


Asunto(s)
Antiparkinsonianos/administración & dosificación , Excipientes/química , Hidrazinas/administración & dosificación , Levodopa/administración & dosificación , Administración Oral , Adulto , Antiparkinsonianos/química , Celulosa/química , Química Farmacéutica , Combinación de Medicamentos , Liberación de Fármacos , Femenino , Humanos , Hidrazinas/química , Levodopa/química , Masculino , Povidona/química , Almidón/análogos & derivados , Almidón/química , Comprimidos , Gusto , Tecnología Farmacéutica , Adulto Joven
6.
Eng Life Sci ; 19(11): 805-814, 2019 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-32624973

RESUMEN

To reach the excellent yield as well as environmental friendliness, an efficient one-pot process for the synthesis of 2-methyl-3-n-butylaminoyl-1,4-benzoquinone, a mitomycin-like compound by the domino reaction of 2-methyl-1,4-hydroquinone and butylamine using laccase/lipase as co-catalysts, has been developed. In this present study, the process proposed here was further improved by optimizing the relevant factors using the response surface methodology based on Box-Benkhen Design. The optimum condition that afforded the highest yield (98%) of 2-methyl-3-n-butylaminoyl-1,4-benzoquinone was obtained as follows: molar ratio of amines to hydroquinones 1.16:1, activity ratio of laccase to lipase 1.14:2, and reaction temperature 38.9°C. The results obtained indicate that this process may be useful as a green alternative method for higher yield production of mitomycin analogs.

7.
J Biotechnol ; 281: 74-80, 2018 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-29908204

RESUMEN

A novel method to synthesize poly(ε-caprolactone) (PCL) through a three-step, lipase-mediated chemo-enzymatic reaction from cyclohexanone using an immobilized lipase from Trichosporon laibacchii (T. laibacchii) CBS5791 was developed. The immobilized preparation with 1280 U· g-1 used here was obtained by a method of purification and in situ immobilization where the crude intracellular lipase (cell homogenate) was subjected to partial purification by an aqueous two-phase system (ATPS) consisting of 12% (w/w) polyethylene glycol (PEG) 4000 and 13% (w/w) potassium phosphate (K2HPO4) and then in situ immobilization directly on diatomite from the top PEG-rich phase of ATPS. In this multi-step process, the ε-caprolactone (ε-CL) produced by lipase-mediated one-pot two-step chemo-enzymatic oxidation of cyclohexanone was directly subjected to in situ ring-opening polymerization (ROP) started by adding highly hydrophobic solvents. It is necessary to note that ε-CL synthesis and its subsequent ROP were catalyzed by the same lipase. The impact of various reaction parameters, e.g., solvent, cyclohexanone: hydrogen peroxide molar ratio, hydrogen peroxide forms and reaction temperature were investigated. Toluene was selected as a preferred solvent due to supporting the highest molecular weight (Mn = 2168) and moderate ε-CL conversion (65.42%). Through the optimization of reaction conditions, PCL was produced with a Mn of 2283 at 50 °C for 24 h. These results reveal that this lipase-mediated direct ring-opening polymerization of in situ formed ε-CL is an alternative route to the conventional synthesis of PCL.


Asunto(s)
Caproatos/química , Ciclohexanonas/química , Enzimas Inmovilizadas/química , Proteínas Fúngicas/química , Lactonas/química , Lipasa/química , Catálisis , Oxidación-Reducción , Polimerizacion , Solventes/química , Trichosporon/enzimología
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