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1.
Microsc Res Tech ; 87(10): 2355-2370, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38798148

RESUMEN

The preparation of ethylenediaminetetraacetic acid (EDTA) functionalized pine needles biochar (EDTA@BC) as a low-cost active adsorbent and its effectiveness in removing Ni(II) from aqueous solution at various conditions is reported in this paper. First, alkali activation was selected to render the pine needle biochar with an excellent porous structure and increased concentration of hydroxyl groups to facilitate grafting. Subsequently, a simple method was utilized to graft EDTA onto the biochar. The prepared EDTA@BC was characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and energy dispersive x-ray spectrometry (EDX). Batch adsorption studies were conducted to assess the impact of various parameters such as solution pH, adsorbent dosage, adsorbate volume, and shaking time on the removal efficiency of Ni(II). At pH 6, 100 mg dosage, 4 mL of adsorbate volume, and 10 min of shaking time, the maximum removal efficiency of Ni(II) was observed to be 89%. EDTA@BC showed reasonable sorption performance still after the third cycle of regeneration. The effect of interfering ions such as Pb, Cr, Cu, and Hg was evaluated, resulting a decrease of 69%, 78%, 76%, and 68%, respectively, in its sorption capacity. The Langmuir model provided a better fit for Ni(II) in the concentration range of 0.1-2000 ppm under optimized conditions, with qmax of 46.69 ± 1.031 mg/g and KL of 0.001, compared with the Freundlich isotherm, which yielded n = 0.234 and χ2 = 2.7899, Temkin isotherm (R2 = 0.9520), and Redlich-Peterson isotherm (R2 = 0.9725). The removal of Ni(II) by EDTA@BC was found to be the pseudo-second-order kinetics. Thermodynamic studies indicated adsorption process to be endothermic and nonspontaneous. Hence, a sustainable valorized bio-material (EDTA@BC) is prepared having better sorption efficiency of Ni(II) from aqueous solution with possible wide applicability. RESEARCH HIGHLIGHTS: New EDTA functionalized indigenous pine needles biochar (EDTA@BC) was prepared. This low-cost active adsorbent found effective in removing Ni(II) from aqueous solution. FTIR, SEM, and EDX proved synthesis and uptake of Ni(II) from aqueous solution. Ni(II) removal, regeneration, interfering and adsorption studies were performed by UV-Vis spectroscopy.


Asunto(s)
Carbón Orgánico , Ácido Edético , Níquel , Pinus , Contaminantes Químicos del Agua , Purificación del Agua , Carbón Orgánico/química , Ácido Edético/química , Níquel/química , Adsorción , Pinus/química , Purificación del Agua/métodos , Concentración de Iones de Hidrógeno , Espectroscopía Infrarroja por Transformada de Fourier , Microscopía Electrónica de Rastreo , Cinética , Hojas de la Planta/química
2.
Angew Chem Int Ed Engl ; 63(30): e202404386, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-38720177

RESUMEN

Based on the electron-withdrawing effect of the Pt(bpy)Cl2 molecule, a simple post-modification amide reaction was firstly used to graft it onto the surface of NH2-MIL-125, which performed as a highly efficient electron acceptor that induced the conversion of the photoinduced charge migration pathway from internal BDC→TiOx migration to external BDC→PtNx migration, significantly improving the efficiency of photoinduced electron transfer and separation. Furthermore, precisely regulating over the first coordination sphere of Pt single atoms was achieved using further post-modification with additional bipyridine to investigate the effect of Pt-Nx coordination numbers on reaction activity. The as-synthesized NML-PtN2 exhibited superior photocatalytic hydrogen evolution activity of 7.608 mmol g-1 h-1, a remarkable improvement of 225 and 2.26 times compared to pristine NH2-MIL-125 and NML-PtN4, respectively. In addition, the superior apparent quantum yield of 4.01 % (390 nm) and turnover frequency of 190.3 h-1 (0.78 wt % Pt SA; 129 times compared to Pt nanoparticles/NML) revealed the high solar utilization efficiency and hydrogen evolution activity of the material. And macroscopic color changes caused by the transition of carrier migration paths was first observed. It holds profound significance for the design of MOF-Molecule catalysts with efficient charge carrier separation and precise regulation of single-atom coordination sphere.

3.
Environ Res ; 239(Pt 1): 117346, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37821069

RESUMEN

A commercialized and widely applied nanofiltration membrane, NF90, was in-situ modified through a surface grafting modification method by using 3-sulfopropyl methacrylate potassium salt and initiators. The effects of water electrical conductivity (EC) and fouling types on membrane separation efficiency were examined before and after membrane modification. Results reveal that both the pristine membrane (PTM) and surface grafting modification membrane (SGMM) had a declining permeate flux and salt (NaCl) removal efficiency but an increasing trend of pharmaceuticals and personal care products (PPCPs) removal with increasing water EC from 250 to 10,000 µs cm-1. However, SGMM exhibited a slightly declining permeate flux but 13%-17% and 1%-42% higher rejection of salt and PPCPs, respectively, compared with PTM, due to electrostatic repulsion and size exclusion provided by the grafted polymer. After sodium alginate (SA) and humic acid (HA) fouling, SGMM had 17%-26% and 16%-32% higher salt rejection and 1%-12% and 1%-51% greater PPCP removal, respectively, compared with PTM due to the additional steric barrier layer contributed by the foulants. The successful grafting and increasing hydrophilicity of the SGMM were confirmed by contact angle analysis, which was beneficial for mitigating membrane fouling. Overall, the proposed in-situ surface grafting modification of NF90 can considerably mitigate organic and biological fouling while raising the rejection of salt and PPCPs at different background water EC, which is beneficial for practical applications in producing clean and high quality water for consumers.


Asunto(s)
Polímeros , Cloruro de Sodio , Membranas , Conductividad Eléctrica , Agua
4.
Molecules ; 28(15)2023 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-37570632

RESUMEN

Molecular engineering is a unique methodology to take advantage of the electrochemical characteristics of materials that are used in energy-harvesting devices. Particularly in triboelectric nanogenerator (TENG) studies, molecular grafting on dielectric metal oxide surfaces can be regarded as a feasible way to alter the surface charge density that directly affects the charge potential of triboelectric layers. Herein, we develop a feasible methodology to synthesize organic-inorganic hybrid structures with tunable triboelectric features. Different types of self-assembled monolayers (SAMs) with electron-donating and withdrawing groups have been used to modify metal oxide (MO) surfaces and to modify their charge density on the surface. All the synthetic routes for hybrid material production have been clearly shown and the formation of covalent bonds on the MO's surface has been confirmed by XPS. The obtained hybrid structures were applied as dopants to distinct polymer matrices with various ratios and fiberization processes were carried out to the prepare opposite triboelectric layers. The formation of the fibers was analyzed by SEM, while their surface morphology and physicochemical features have been measured by AFM and a drop shape analyzer. The triboelectric charge potential of each layer after doping and their contribution to the TENG device's parameters have been investigated. For each triboelectric layer, the best-performing tribopositive and tribonegative material combination was separately determined and then these opposite layers were used to fabricate TENG with the highest efficiency. A comparison of the device parameters with the reference indicated that the best tribopositive material gave rise to a 40% increase in the output voltage and produced 231 V, whereas the best tribonegative one led to a 33.3% rise in voltage and generated 220 V. In addition, the best device collected ~83% more charge than the reference device and came up with 250 V that corresponds to 51.5% performance enhancement. This approach paved the way by addressing the issue of how molecular engineering can be used to manipulate the triboelectric features of the same materials.

5.
Small Methods ; : e2300247, 2023 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-37357558

RESUMEN

Current hydrophilic modification strategies improve the antifouling ability of membranes but fail to completely eliminate the fouling of emulsified oil droplets with a wide size distribution. Constructing membranes with superior anti-oil-fouling ability to resist various oil droplets especially at high permeation fluxes is challenging. Here, the fabrication of a zero-oil-fouling membrane by grafting considerably high coverage of zwitterionic polymer and building defect-free hydration defense barrier on the surface is reported. A uniform layer of protocatechuic acid with COOH as abundant as existing in every molecule is stably deposited on the membrane so as to provide sufficient reactive sites and achieve dense grafting of the zwitterionic polymer. The coverage of zwitterionic polymer on the membrane plays a crucial role in promoting the antifouling ability to emulsified oil droplets. The poly(vinylidene fluoride) membrane with 93% coverage of the zwitterionic polymer exhibits zero oil fouling when separating multitudinous oil-in-water emulsions with ≈0% flux decline, ≈100% flux recovery, and a high water flux of ≈800 L m-2 h-1 bar-1 . This membrane outperforms almost all of the reported membranes in terms of the comprehensive antifouling performance. This work provides a feasible route for manufacturing super-antifouling membranes toward oil/water separation application.

6.
Small ; 19(44): e2303251, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37376823

RESUMEN

In this paper, strong hydrophilic poly(ionic liquid)s (PILs) are selectively grafted on different positions (mesoporous channels and outer surface) of mesoporous silica via thiol-ene click chemical reaction. The purposes of selective grafting are on the one hand, to explore the differences of adsorption and transportation of water molecules in mesoporous channels and on the outer surface, and on the other hand, to combine the two approaches (intra-pore grafting and external surface grafting) to reasonably design SiO2 @PILs low humidity sensing film with synergetic function to achieve high sensitivity. The results of low relativehumidity (RH) sensing test show that the sensing performance of humidity sensor based on mesoporous silica grafted with PILs in the channels is better than that of humidity sensor based on mesoporous silica grafted with PILs on the outer surface. Compared with water molecules transport single channel, the construction of dual-channel water transport significantly improves the sensitivity of the low humidity sensor, and the response of the sensor is up to 4112% in the range of 7-33% RH. Moreover, the existence of micropores and the formation of dual-channel water transport affect the adsorption/desorption behaviors of the sensor under different humidity ranges, especially below 11% RH.

7.
Molecules ; 28(5)2023 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-36903468

RESUMEN

Efficient and selective extractions of precious and critical metal ions such as Au(III) and Pd(II) were investigated using zirconia nanoparticles surface modified with different organic mono- and di-carbamoyl phosphonic acid ligands. The modification is made on the surface of commercial ZrO2 that is dispersed in aqueous suspension and was achieved by optimizing the Bronsted acid-base reaction in ethanol/H2O solution (1:2), resulting in inorganic-organic systems of ZrO2-Ln (Ln: organic carbamoyl phosphonic acid ligand). The presence, binding, amount, and stability of the organic ligand on the surface of zirconia nanoparticles were confirmed by different characterizations such as TGA, BET, ATR-FTIR, and 31P-NMR. Characterizations showed that all the prepared modified zirconia had a similar specific surface area (50 m2.g-1) and the same amount of ligand on the zirconia surface in a 1:50 molar ratio. ATR-FTIR and 31P-NMR data were used to elucidate the most favorable binding mode. Batch adsorption results showed that (i) ZrO2 surface modified with di-carbamoyl phosphonic acid ligands had the highest adsorption efficiency to extract metals than mono-carbamoyl ligands, and (ii) higher hydrophobicity of the ligand led to better adsorption efficiency. The surface-modified ZrO2 with di-N,N-butyl carbamoyl pentyl phosphonic acid ligand (ZrO2-L6) showed promising stability, efficiency, and reusability in industrial applications for selective gold recovery. In terms of thermodynamic and kinetic adsorption data, ZrO2-L6 fits the Langmuir adsorption model and pseudo-second-order kinetic model for the adsorption of Au(III) with maximum experimental adsorption capacity qmax = 6.4 mg.g-1.

8.
J Biomater Sci Polym Ed ; 34(10): 1382-1397, 2023 08.
Artículo en Inglés | MEDLINE | ID: mdl-36617532

RESUMEN

Thermoplastic polyurethane (TPU) membrane has super physical-mechanical properties and biocompatibility, but the surface is inert and lack of active groups which limit its application in cell culture. Silk sericin (SS) can improve cell adhesion, proliferation, growth and metabolism. In this paper, SS was grafted onto the surface of TPU membrane by -NH2 bridge to build a high efficiency cell culture membrane. The FT-IR spectrum results indicated SS was grafted by chemical bond. According to the SEM and AFM results, we found that the grafting of SS reduced the water contact angle by 43.31% and increased the surface roughness by about four times. When TPU-SS was used for HepG2 cell culture, the cell adhesion rate of TPU-SS was significantly higher than that of the general TCPS cell culture plate, and the cell proliferation rate was close to that of TCPS. FDA/EB staining showed that HepG2 cells remained a better cellular growth behavior. HepG2 cells had higher cell vitality including the albumin secretion and the intracellular total protein synthesis. Grafting SS maintained the stability of cell and significantly decreased the cytotoxicity by decreased LDH release. In conclusion, SS grafting is beneficial to cell culture in vitro, and provides a key material for bioartificial liver culture system.


Asunto(s)
Poliuretanos , Sericinas , Poliuretanos/química , Sericinas/farmacología , Adhesión Celular , Espectroscopía Infrarroja por Transformada de Fourier , Técnicas de Cultivo de Célula
9.
Nanotechnology ; 34(6)2022 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-36347019

RESUMEN

The surface-supported silver nanoparticles have been studied and applied in various applications. Many unique nanostructures have been introduced into this field to improve the functionalities of the surfaces depending on application purposes. We created featured silver nano-array surfaces by utilizing the solvent-mediated phase transition on the surface grafted with poly (acrylic) acids polymer chains and taking advantage of the low temperature of argon gas discharged plasma as a reducing agent. The applied solvents and grafted polymer chain densities affected the phase transition and thus determined the outcome of surface nano-array patterns. However, the total loaded silver ions on the surface affected silver nano-array structures at the sub-micron levels. The featured silver patterned surfaces made in the optimal conditions present a favorable surface-enhanced Raman spectroscopy enhancement as well as recyclability for detection re-usage. This novel method prepares tunable silver nanopatterned surfaces and provides a new approach to various potential applications.

10.
ACS Appl Bio Mater ; 5(12): 5645-5656, 2022 12 19.
Artículo en Inglés | MEDLINE | ID: mdl-36446396

RESUMEN

A hernia is a pathological condition caused by a defect or opening in the muscle wall, which leads to organs pushing through the opening or defect. Hernia recurrence, seroma, persistent pain, tissue adhesions, and wound infection are common complications following hernia repair surgery. Infection after hernia mesh implantation is the third major complication leading to hernia recurrence. In order to reduce the incidence of late infections, we developed a polypropylene mesh with antibacterial properties. In this study, knitted polypropylene meshes were exposed to radio-frequency plasma to activate their surfaces. The antibacterial monomer diallyldimethylammonium chloride (DADMAC) was then grafted onto the mesh surface using pentaerythritol tetraacrylate as the cross-linker since it is able to engage all four functional groups to form a high-density cross-linked network. The subsequent antibacterial performance showed a 2.9 log reduction toward Staphylococcus aureus and a 0.9 log reduction for Escherichia coli.


Asunto(s)
Hernia Ventral , Mallas Quirúrgicas , Humanos , Mallas Quirúrgicas/efectos adversos , Polipropilenos , Hernia Ventral/tratamiento farmacológico , Antibacterianos/farmacología
11.
J Environ Manage ; 324: 116306, 2022 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-36166864

RESUMEN

This study concerns the fabrication of CTAB- and N,N-dimethyltetradecylamine-grafted zirconia and evaluation of their ability to adsorb vanadium ions. The effectiveness of ZrO2 functionalization and the different nature of the modifiers used were confirmed by differences in the porosity (ZrO2: SBET = 347 m2/g; ZrO2-CTAB: SBET = 375 m2/g, ZrO2-NH+: SBET = 155 m2/g), types of functional groups, and isoelectric points (the ZrO2 and CTAB-modified samples have IEPs = 3.8 and 3.9, ZrO2-NH+ has IEP = 7.1) of the prepared adsorbents. The designed materials were tested in batch adsorption experiments involving the removal of vanadium ions from model wastewaters at various process parameters, among which pH proved to be the most important. Based on equilibrium and kinetic evaluations, it was proved that the sorption of V(V) ions followed pseudo-second-order and intraparticle diffusion models, and the data were better fitted to the Langmuir model, suggesting the following order of the sorbents in terms of favorability for V(V) ion adsorption: ZrO2-NH+ > ZrO2 > ZrO2-CTAB. The estimated maximum monolayer capacity of ZrO2-NH+ for V(V) (87.72 mg/g) was the highest among the tested materials. Additionally, it was confirmed that adsorption of V(V) ions onto synthesized materials is a heterogeneous, exothermic, and spontaneous reaction, as evidenced by the calculated values of thermodynamic parameters. The key goals included the transfer of experimental findings obtained using model solutions to the adsorption of V(V) ions from solutions arising from the leaching process of spent catalysts. The highest adsorption efficiencies of 70.8% and 47.5% were recorded for the ZrO2-NH+ material in acidic solution; this may be related to the protonization of -NH+ groups, which favors the sorption of V(V) ions. Based on desorption tests as well as the results of infrared and X-ray photoelectron spectroscopy, irrespective of the process conditions, the physical nature of the adsorbent/adsorbate interaction was confirmed.


Asunto(s)
Aguas Residuales , Contaminantes Químicos del Agua , Aguas Residuales/química , Vanadio , Contaminantes Químicos del Agua/química , Cetrimonio , Concentración de Iones de Hidrógeno , Adsorción , Iones , Cinética , Termodinámica
12.
Macromol Biosci ; 22(11): e2200200, 2022 11.
Artículo en Inglés | MEDLINE | ID: mdl-35789095

RESUMEN

The grafting of zwitterionic molecules onto solid surfaces is an important tool for decreasing the unwanted adsorption of biomolecules, such as proteins, bacteria, and cells. This has been achieved through various approaches, such as zwitterionic monolayer/multilayer formation, surface-initiated polymerization of zwitterionic monomers, and grafting of presynthesized zwitterionic polymers. Recently, a coordination-driven approach to grafting zwitterionic polymers onto solid surfaces has been discovered to be an effective method because of its versatility and robustness. However, the bacterial adhesion resistance of zwitterionic polymer grafting has been explored using only one molecular weight, and the non-biofouling performance against other fouling organisms has remained unexamined. In this study, the characteristics of coordination-driven surface zwitteration are systematically investigated. Sulfobetaine (SB) polymers with three different molecular weights are synthesized and employed for surface grafting. Polydopamine is used as a surface primer, and SB polymers are grafted onto the surfaces via the formation of metal-mediated coordinate bonds. The effect of molecular weight on the grafting efficiency and non-biofouling performance is investigated via protein adsorption and marine diatom adhesion assays. The SB polymer with a high molecular weight is found to be crucial for achieving strong resistance to protein adsorption and marine fouling.


Asunto(s)
Betaína , Polímeros , Peso Molecular , Polímeros/química , Polimerizacion , Betaína/química , Propiedades de Superficie
13.
Membranes (Basel) ; 12(2)2022 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-35207070

RESUMEN

The implementation of membrane surface modification to enhance the performance of membrane-based separation has become a favored strategy due to its promise to address the trade-off between water permeability and salt rejection as well as to improve the durability of the membranes. Tremendous work has been committed to modifying polymeric membranes through physical approaches such as surface coating and ontology doping, as well as chemical approaches such as surface grafting to introduce various functional groups to the membrane. In the context of liquid separation membranes applied for desalination and water and wastewater treatment, biomolecules have gained increasing attention as membrane-modifying agents due to their intriguing structural properties and chemical functionalities. Biomolecules, especially carbohydrates and proteins, exhibit attractive features, including high surface hydrophilicity and zwitterionic and antimicrobial properties that are desired for liquid separation membranes. In this review, we provide an overview of the recent developments in biomolecule-enabled liquid separation membranes. The roles and potentials of some commonly explored biomolecules in heightening the performance of polymeric membranes are discussed. With the advancements in material synthesis and the need to answer the call for more sustainable materials, biomolecules could serve as attractive alternatives for the development of high-performance composite membranes.

14.
Chem Rec ; 22(7): e202100320, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35189025

RESUMEN

Oily wastewater has become one of the leading causes of environmental pollution. A massive quantity of oily wastewater is released from industries, oil spills, and routine activities, endangering the ecosystem's sustainability. Due to the enormous negative impact, researchers put strenuous efforts into developing a sustainable solution to treat oily wastewater. Microfiltration/ultrafiltration membranes are considered an efficient solution to treat oily wastewater due to their low cost, small footprint, facile operation, and high separation efficiencies. However, membranes severely fouled during the separation process due to oil's adsorption and cake layer formation, which shortens the membranes' life. This review has critically discussed the microfiltration/ultrafiltration membrane synthesizing methods and their emulsion's separation performance. In the end, key challenges and their possible solutions are highlighted to provide future direction to synthesize next-generation membranes.


Asunto(s)
Ultrafiltración , Purificación del Agua , Ecosistema , Emulsiones , Membranas Artificiales , Aceites , Ultrafiltración/métodos , Aguas Residuales , Purificación del Agua/métodos
15.
Anal Chim Acta ; 1192: 339374, 2022 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-35057961

RESUMEN

Driven by the urgent need for the determination of trace level triphenyl phosphate (TPhP) present in environment, a simple, rapid and ultrasensitive sensor has been fabricated for detection of TPhP by directly measuring transmembrane current. The transmembrane containing artificial nanochannel named polyethylene terephthalate (PET) nanochannel membrane is designed to be grafted by TPhP molecularly imprinted polymers (TPhP-MIPs) on its outer surface and inner surface of nanochannel. After the fabricated membrane banded TPhP, the transmembrane current decreased. The rate of current change is linearly proportional to the logarithm value of TPhP concentrations in the range of 0.001 ng mL-1 -800 ng mL-1. Meanwhile, the limit of detection (LOD) was 0.0003 ng mL-1. This LOD value is much lower than most results acquired by using chromatography-mass spectrometry and electrochemistry (EC) sensor based on the functionalization of electrode, whereas the cost of our fabricated EC sensor is much lower. The newly developed sensor is suitable for real-time or field detection of TPhP. The interference of analogs and non-analogs with similar structure of TPhP can be effectively avoided. The sensor not only exhibits high selectivity for TPhP, but also shows ultrasensitive assay for measuring TPhP in real environmental water.


Asunto(s)
Impresión Molecular , Técnicas Electroquímicas , Electrodos , Organofosfatos
16.
Molecules ; 26(20)2021 Oct 13.
Artículo en Inglés | MEDLINE | ID: mdl-34684747

RESUMEN

While the sonochemical grafting of molecules on silicon hydride surface to form stable Si-C bond via hydrosilylation has been previously described, the susceptibility towards nucleophilic functional groups during the sonochemical reaction process remains unclear. In this work, a competitive study between a well-established thermal reaction and sonochemical reaction of nucleophilic molecules (cyclopropylamine and 3-Butyn-1-ol) was performed on p-type silicon hydride (111) surfaces. The nature of surface grafting from these reactions was examined through contact angle measurements, X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM). Cyclopropylamine, being a sensitive radical clock, did not experience any ring-opening events. This suggested that either the Si-H may not have undergone homolysis as reported previously under sonochemical reaction or that the interaction to the surface hydride via a lone-pair electron coordination bond was reversible during the process. On the other hand, silicon back-bond breakage and subsequent surface roughening were observed for 3-Butyn-1-ol at high-temperature grafting (≈150 °C). Interestingly, the sonochemical reaction did not produce appreciable topographical changes to surfaces at the nano scale and the further XPS analysis may suggest Si-C formation. This indicated that while a sonochemical reaction may be indifferent towards nucleophilic groups, the surface was more reactive towards unsaturated carbons. To the best of the author's knowledge, this is the first attempt at elucidating the underlying reactivity mechanisms of nucleophilic groups and unsaturated carbon bonds during sonochemical reaction of silicon hydride surfaces.

17.
Colloids Surf B Biointerfaces ; 208: 112119, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34571469

RESUMEN

Tunable multi-responsive mesoporous silica nanoparticles were prepared by post-condensation/surface modification of MCM-41 nanoparticles. Surface grafting of a poly(N,N-dimethylaminoethyl methacrylate)-based polymer containing disulfide bonds was achieved by a click reaction. Chemical modification, morphological characteristics, and textural properties of the nanoparticles were studied using multiple characterization techniques such as Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, transmission electron microscopy, small-angle X-ray scattering, and nitrogen adsorption/desorption behavior. The nanoparticles retained the meso-structural integrity of MCM41 and particle size < 100 nm after grafting with the polymer. The pH and redox-responsive behavior of the nanoparticles were also studied. The nanoparticles possess excellent drug-loading capacity owing to their large surface area and 'closed gate' mechanism of the grafted polymer chains. The release profile of doxorubicin at two different pH (7.4 and 5.5) and in the presence of dithiothreitol showed a dual response behavior. The nano drug carrier device exhibited efficient intracellular uptake in cancer cells with suitable cytotoxicity and pharmacokinetic behavior, and may therefore be considered a good candidate for cancer therapy.


Asunto(s)
Portadores de Fármacos , Nanopartículas , Doxorrubicina/farmacología , Liberación de Fármacos , Porosidad , Dióxido de Silicio
18.
Environ Sci Pollut Res Int ; 28(46): 66287-66302, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34331654

RESUMEN

In the past 10 years, the treatment and restoration of soil and water bodies contaminated by mercury and other heavy metals have received unprecedented attention and support from China's environmental protection authorities. The search for low-cost and high-efficiency adsorbents has become one of the research hotspots in this field. In this paper, a simple and environment-friendly method was used to graft 3-mercaptopropyl trimethoxysilane on the surface of palygorskite. The synthesized mercaptofunctionalized palygorskite (M-PAL) was characterized by XRD, FT-IR, BET and SEM-EDS, respectively, and its adsorption conditions, adsorption models and thermodynamic parameters for Hg2+ were systematically investigated. The experimental results indicated that the saturated adsorption capacity of Hg2+ on the M-PAL could reach 203.4 mg·g-1, within 120 min at pH 4 and 298 K. By analyzing the experimental data of adsorption kinetics and thermodynamics, it was found that the adsorption process of Hg2+ conformed to the pseudo-second-order kinetic model, which belonged to chemical adsorption of the rate-controlled step; the Langmuir model better described the adsorption isotherm. The thermodynamic parameters obtained (ΔH=29.95 kJ·mol-1, ΔS=103.09 J·mol-1·K-1 and ΔG<0) show that the whole process is a spontaneous endothermic process. When the concentration of Na+, K+, Ca2+, Mg2+, Cl-, NO3-, H2C2O4 and C6H8O7 was 200 times that of Hg2+, although these organic acids had a slightly greater effect on the adsorption of Hg2+ on mercaptofunctionalized palygorskite than inorganic ions, the adsorption capacity remained above 185 mg·g-1. The adsorption products could be still stable in simulated acid rain with pH 3, 4, 5, 6, 7 and oxalic acid solution with concentration of 1, 2, 3, 4 and 5 mmol·L-1, and the desorption rates were about 3%. Through XPS analysis, the specific coordination of Hg2+ with the S atom on the surface of M-PAL was confirmed.


Asunto(s)
Mercurio , Contaminantes Químicos del Agua , Purificación del Agua , Adsorción , Concentración de Iones de Hidrógeno , Cinética , Compuestos de Magnesio , Compuestos de Silicona , Espectroscopía Infrarroja por Transformada de Fourier , Termodinámica , Contaminantes Químicos del Agua/análisis
19.
Carbohydr Polym ; 262: 117972, 2021 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-33838788

RESUMEN

In order to improve the anti-inflammatory activity of chitosan oligosaccharide (COS), chitosan oligosaccharide graft citronellol derivatives (COS-g-Cit1-3) were successfully synthesized via grafting citronellol (Cit) onto COS backbone. The degrees of substitution (DS) of COS-g-Cit1-3 were 0.165, 0.199 and 0.182, respectively. The structure of COS-g-Cit1-3 was confirmed by UV-vis, FT-IR, 1H NMR and elemental analysis. The in vivo anti-inflammatory activity evaluation results displayed that COS-g-Cit1-3 drastically reduced the paw swelling, and the oedema inhibitions were 22.58 %, 29.03 % and 25.81 %, respectively. The results indicated that the anti-inflammatory effects of COS-g-Cit1-3 were significantly higher than COS and COS-g-Cit2 exhibited the highest anti-inflammatory ability. The results also presented that COS-g-Cit1-3 reduced the expression levels of TNF-α by promoting the secretion of IL-4 and IL-10. Moreover, western blot analysis data proved that COS-g-Cit1-3 inactivated the NF-κB signaling pathway via inhibiting the phosphorylation of p65, IKBα and IKKß.


Asunto(s)
Monoterpenos Acíclicos/química , Monoterpenos Acíclicos/farmacología , Antiinflamatorios/química , Antiinflamatorios/farmacología , Quitosano/química , Oligosacáridos/química , Animales , Edema/tratamiento farmacológico , Edema/patología , Femenino , Espectroscopía de Resonancia Magnética/métodos , Masculino , Ratones , FN-kappa B/metabolismo , Ratas , Ratas Sprague-Dawley , Transducción de Señal/efectos de los fármacos , Espectroscopía Infrarroja por Transformada de Fourier/métodos , Factor de Necrosis Tumoral alfa/metabolismo
20.
Nanomaterials (Basel) ; 11(4)2021 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-33917895

RESUMEN

This study focuses on the preparation of innovative nanocomposite materials based on surface modification of commercial nano-ZrO2 optimized from Brønsted acid-base surface reactions. This surface modification was carried out by direct grafting of suitable phosphonic acids bearing a vinylic or phenylic substituent in aqueous solution. Different loading quantities of the anchoring organophosphorus compounds were applied for each materials synthesis. The resulting nanohybrids were thoroughly characterized by infrared spectroscopy (DRIFT), solid-state nuclear magnetic resonance (NMR), nitrogen adsorption-desorption (BET), thermogravimetric analysis (TG), and X-ray photoelectron spectroscopy (XPS), demonstrating the reliability and efficient tunability of the surface functionalization based on the starting Zr/P ratio. Our nanocomposite materials exhibited a high specific surface area as well as complex porosity networks with well-defined meso-pore. The as-prepared materials were investigated for the adsorption of a mixture of 16 polycyclic aromatic hydrocarbons (PAHs) at 200 ng·mL-1 in an aqueous solution. Adsorption kinetics experiments of each individual material were carried out on the prepared PAHs standard solution for a contact time of up to 6 h. Pretreatments of the adsorption test samples were performed by solid-phase extraction (SPE), and the resulting samples were analyzed using an ultrasensitive GC-orbitrap-MS system. The pseudo-first-order and the pseudo-second-order models were used to determine the kinetic data. The adsorption kinetics were best described and fitted by the pseudo-second-order kinetic model. The correlation between the nature of the substituent (vinylic or phenylic) and the parameters characterizing the adsorption process were found. In addition, an increase of PAHs adsorption rates with phosphonic acid loading was observed.

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