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1.
Small ; 20(27): e2312091, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38308418

RESUMO

Grafted biopolymer binders are demonstrated to improve the processability and cycling stability of the silicon (Si) nanoparticle anodes. However, there is little systematical exploration regarding the relationship between grafting density and performance of grafted binder for Si anodes, especially when Si particles exceed the critical breaking size. Herein, a series of guar gum grafted polyacrylamide (GP) binders with different grafting densities are designed and prepared to determine the optimal grafting density for maximizing the electrochemical performance of Si submicroparticle (SiSMP) anodes. Among various GP binders, GP5 with recommended grafting density demonstrates the strongest adhesion strength, best mechanical properties, and highest intrinsic ionic conductivity. These characteristics enable the SiSMP electrodes to sustain the electrode integrity and accelerate lithium-ion transport kinetics during cycling, resulting in high capacity and stable cyclability. The superior role of GP5 binder in enabling robust structure and stable interface of SiSMP electrodes is revealed through the PeakForce atomic force microscopy and in situ differential electrochemical mass spectrometry. Furthermore, the stable cyclabilities of high-loading SiSMP@GP5 electrode with ultralow GP5 content (1 wt%) at high areal capacity as well as the good cyclability of Ah-level LiNi0.8Co0.1Mn0.1O2/SiSMP@GP5 pouch cell strongly confirms the practical viability of the GP5 binder.

2.
Macromol Rapid Commun ; 45(8): e2300674, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38234077

RESUMO

Defined, branched polymer architectures with low dispersity and architectural purity are of great interest to polymer science but are challenging to synthesize. Besides star and comb, especially the pom-pom topology is of interest as it is the simplest topology with exactly two branching points. Most synthetic approaches to a pom-pom topology reported a lack of full control and variability over one of the three topological parameters, the backbone or arm molecular weight and arm number. A new, elegant, fast, and scalable synthetic route without the need for post-polymerization modification (PPM) or purification steps during the synthesis to a pom-pom and a broad variety of topologies made from styrene and dienes is reported, with potential application to barbwire, bottlebrush, miktoarm star, Janus type polymers, or multi-graft copolymers. The key is to inset short poly(2-vinyl-pyridine) blocks (<2 mol% in the branched product) into the backbone as branching points. Carb anions can react at the C6 carbon of the pyridine ring, grafting the arms onto the backbone. Since the synthetic route to polystyrene pom-poms has only two steps and is free of PPM or purification, large amounts of up to 300 g of defined pom-pom structures can be synthesized in one batch.


Assuntos
Ânions , Polimerização , Poliestirenos , Poliestirenos/química , Ânions/química , Estrutura Molecular , Polímeros/química , Polímeros/síntese química , Polivinil/química , Polivinil/síntese química
3.
Chemistry ; 23(54): 13337-13341, 2017 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-28816377

RESUMO

Polymer brushes are for the first time used to induce the synthesis of metal-organic frameworks (MOFs). The semi-fixed polymer chains provide a confined environment, which allows a mild growth of MOFs in between polymer chains to give surface-attached spherical MOF nanoparticles, in contrast to the larger MOF cubes/plates formed simultaneously in solution. Polymer brushes bearing carboxylate acid functionalities are indispensable for the formation of surface bound MOFs, while no MOF nanoparticles are observed on neutral polymer brushes. Characterization of the resultant MOF/polymer brushes hybrid film indicates the formation of crystalline MOF structure. The dimension of surface-attached MOFs can be fine-tuned from 20 nm to 1.4 µm simply by varying the structural parameter of polymer brushes and the nucleation duration. The method is not only applicable to the synthesis of MOF-5 and MIL-125, but shows great potential for the preparation of other surface-attached MOFs.

4.
Small ; 11(38): 5097-104, 2015 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-26237680

RESUMO

Understanding the growth behavior of nanocrystals (NCs), especially when heteroatoms are introduced, is very important for the optimization of doping (or alloying) and optoelectronic performances. Here, it is reported on the observation of alloying-facilitated self-assembly of MgZnO NCs and the underlying mechanism of alloying concentration-dependent surface grafting. Using the developed one-pot thermolysis of Zn and Mg organic salts with the help of oleylamine (OAm) and oleic acid (OA), the Mg ions can be introduced into the ZnO lattice without phase separation with concentrations as high as 20%. Interestingly, with the increase of Mg alloying concentration, the morphologies of the products transform from monodispersed NCs to nanoflowers, and then nanobouquet superstructures, which have quasi-monocrystal features and obey the oriented attachment rules. According to the analyses of surface functional groups, a mechanism involving concentration-dependent surface grafting is proposed for such alloying-facilitated self-assembly.

5.
J Phys Condens Matter ; 36(50)2024 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-39312954

RESUMO

We investigate the dynamics of comb-like polymer translocation through a nanochannel using three-dimensional Langevin dynamics simulations based on a coarse-grained chain model. A comprehensive set of simulations are performed to examine the effects of system parameters such as the grafting densityρof the side chains, the polymer chain length, the nanochannel dimensions, and the magnitude of the pulling force on the translocation dynamics. For a given polymer chain length, keeping the backbone length is constant while varyingρ, we have found that the dependence of the mean translocation time⟨τ⟩onρis non-monotonic, with a maximum translocation time for a specificρat which the translocation is the slowest. The simulation results also show that⟨τ⟩is not significantly affected by the channel width above a certain radius, while the comb-like polymer translocation is hindered by a narrower channel due to increased interactions between the chain monomers and the channel. In addition,⟨τ⟩increases linearly with the nanochannel length. A linear scaling relationship between the mean translocation time⟨τ⟩and the chain lengthNof polymer is obtained,⟨τ⟩∼N. Similarly, the dependence of⟨τ⟩on the backbone chain sizeNbbhas a quasi-linear dependence,⟨τ⟩∼Nbb. On the other hand, the translocation velocityvfollows a power-law relationship with the polymer chain lengthNasv∼N-1. The mean translocation time also shows an inverse linear relationship with the magnitude of the pulling forceF,⟨τ⟩∼F-1. The power-law relationships discovered in this study contribute to the fundamental understanding of the comb polymer translocation dynamics and to establishing a framework for further investigations in this field.

6.
Int J Pharm ; 646: 123476, 2023 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-37805148

RESUMO

Polymer lung surfactant (PLS) is a polyethylene glycol (PEG)-brushed block copolymer micelle designed for pulmonary surfactant replacement therapy. Saccharides (e.g., sucrose and (2-hydroxypropyl)-ß-cyclodextrin) and water-soluble polymers (e.g., PEG), common excipients for lyophilization, were found to severely impair the surface activity of lyophilized PLS. To investigate the feasibility of excipient-free lyophilization of PLS, we studied the effects of both PLS material parameters and lyophilization operating parameters on the redispersibility and surface availability of reconstituted PLS, all without relying on excipients. We found that the redispersibility was improved by three factors; a faster cooling rate during the freezing stage reduced freezing stress; a higher PEG grafting density enhanced dissipating effects; and the absence of hydrophobic endgroups in the PEG block further prevented micelle aggregation. Consequently, the surface availability of PLS increased, enabling the micelle monolayer at the air/water interface to achieve a surface tension below 10 mN/m, which is a key pharmaceutical function of PLS. Moreover, the lyophilized micelles in powder form could be easily dispersed on water surfaces without the need for reconstitution, which opens up the possibility of inhalation delivery, a more patient-friendly administration method compared to instillation. The successful excipient-free lyophilization unlocks the potential of PLS for addressing acute respiratory distress syndrome (ARDS) and other pulmonary dysfunctions.


Assuntos
Micelas , Surfactantes Pulmonares , Humanos , Excipientes/química , Polímeros/química , Polietilenoglicóis/química , Tensoativos/química , Liofilização/métodos , Água , Pulmão
7.
ACS Appl Mater Interfaces ; 15(48): 56181-56191, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38010839

RESUMO

Due to the flexibility and versatility of the layered crystal structure of layered double hydroxides (LDHs), they have shown great potential in various fields. However, LDH nanosheets (LDH-NSs) are easy to agglomerate, leading to the problem of accumulation, which hinders their further application. Accordingly, once LDHs are combined with solvent-free nanofluids (SFNs), the advantages of LDHs and SFNs could be combined to achieve an extraordinary performance. However, the stacked structure of traditional LDHs is not conducive to the exposure of hydroxyl functional groups, and hydroxyl sites are key to the conversion of LDHs to SFNs. Therefore, in this work, nanoflower-like LDHs (NFLs) with abundant exposed hydroxyl groups were prepared and combined with organic oligomers to achieve a solid-to-liquid transition. The formation mechanism of NFLs and the grafting mechanism of OS-PEA on their surface were identified. The prepared NFL-F3 still has good fluidity and dispersion stability in different solvents after storage for 100 days. The high-saturated grafting density on the surface of NFLs increased the steric hindrance effect of the nanoparticles, thereby improving the dispersion stability and reducing the viscosity of NFL-F3. Notably, the CO2 sorption performance of NFL-F3 is significantly improved, which is attributed to the voids between polymers, physical sorption, and good fluidity caused by high-saturation grafting on the surface of NFL-F3. Finally, by combining the sorption behavior and model fitting, it was confirmed that the physical effect was dominant in CO2 sorption by the NFL-F, which saved energy for the sorption-desorption process of its industrial application. Moreover, NFL-F3 has a good CO2/N2 separation performance and cycle stability. We envision that this general strategy will open up new insights into the construction of innovative low-viscosity LDH-based SFNs with high CO2 capacity and facilitate CO2/N2 selectivity and offer new directions for LDH utilizations.

8.
Matter ; 5(12): 4502-4512, 2022 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-36569514

RESUMO

Slippery surfaces are sought after due to their wide range of applications in self-cleaning, drag reduction, fouling-resistance, enhanced condensation, biomedical implants etc. Recently, non-textured, all-solid, slippery surfaces have gained significant attention because of their advantages over super-repellent surfaces and lubricant-infused surfaces. Currently, almost all non-textured, all-solid, slippery surfaces are hydrophobic. In this work, we elucidate the systematic design of non-textured, all-solid, slippery hydrophilic (SLIC) surfaces by covalently grafting polyethylene glycol (PEG) brushes to smooth substrates. Furthermore, we postulate a plateau in slipperiness above a critical grafting density, which occurs when the tethered brush size is equal to the inter-tether distance. Our SLIC surfaces demonstrate exceptional performance in condensation and fouling-resistance compared to non-slippery hydrophilic surfaces and slippery hydrophobic surfaces. Based on these results, SLIC surfaces constitute an emerging class of surfaces with the potential to benefit multiple technological landscapes ranging from thermofluidics to biofluidics.

9.
Eng Life Sci ; 21(6): 392-404, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34140850

RESUMO

The formation of a stable spatial arrangement of protein A ligands is a great challenge for the development of high-capacity polymer-grafted protein A adsorbents due to the complexity in interplay between coupled ligands and polymer chain. In this work, carboxymethyl dextrans (CMDs) with different molecular weight were introduced to provide stable spatial ligand arrangement in CMD-grafted protein A gels to improve IgG adsorption. The result showed that coupling of protein A ligand in CMD-grafted layer had no marked influence on pore size and dextran layers coupled with the ligands were stable in experimental range of salt concentrations. The result of IgG adsorption revealed that carboxymethyl dextran T10, a short CMD, was more suitable as a scaffold for the synthesis of high-capacity protein A gels. Moreover, the maximal adsorption capacity for IgG was obtained to be 96.4 mg/g gel at ionic capacities of 300-350 mmol/L and a ligand density of 15.2 mg/g gel. Dynamic binding capacity for IgG exhibited a higher capacity utilization in CMD-grafted protein A gels than non-grafted protein A gel. The research presented a tactics to establish a stable dextran layer coupled with protein A ligands and demonstrated its importance to improve binding capacity for IgG.

10.
ACS Appl Mater Interfaces ; 13(8): 10349-10358, 2021 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-33600166

RESUMO

Design of the crowding of chains tethered at the faces of ß-sheet nanocrystals self-assembled from ß-alanine trimers grafted on polyisobutylene (PIB) rubber tailors nanocrystal size and thus the elastic matrix morphology, thereby altering the material's macroscopic elastic properties. Results from transmission electron microscopy, small-angle X-ray scattering, and small-angle neutron scattering characterizations of the morphology demonstrate that increasing the density of chain tethering at the crystalline nanodomain/matrix interface can sharply limit the nanodomain growth in the direction of hydrogen bonding in the crystals. The nanocrystal size, in turn, impacts the gradient in chain stretching away from the crystal surface and the macroscopic volume fraction of unperturbed chains. Nanocomposite mechanical and dynamic mechanical properties at low degrees of deformation are related to the structural hierarchy resulting from the control of interfacial tethering density.


Assuntos
Proteínas Imobilizadas/química , Nanopartículas/química , Oligopeptídeos/química , Polienos/química , Polímeros/química , Propriedades de Superfície
11.
Colloids Surf B Biointerfaces ; 199: 111517, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33352490

RESUMO

An excellent blood-compatible polymer, poly(2-methoxyethyl acrylate) (PMEA), exhibits nanometer-scale phase-separated structures at the interface with water or phosphate-buffered saline (PBS), and fibrinogen adsorption is suppressed, especially on the water-rich region. To understand the correlation between the interfacial structure based on the grafting density of PMEA and blood compatibility, grafted PMEA (gPMEA) surfaces with controlled density were prepared by immobilizing thiol-terminated PMEA on a gold substrate. The amount of adsorbed fibrinogen and the number of adhered platelets on gPMEAs decreased first with the increasing grafting density (σ), but increased after showed minimum at σ of approximately 0.11 chains/nm2. The interfacial structures of the gPMEA/PBS interface changed with grafting density, and the maximum area of water-rich region was obtained at σ = 0.11. The water contact angle at σ = 0.11 is smaller than that at the other grafting density. These results revealed that hydration to the polymer is very effective to suppress the platelet adhesion and water-rich region shows excellent blood compatibility on gPMEA surfaces. This work clearly indicated that the density of PMEA affects the interfacial structure and plays an important role in the blood compatibility of the material.


Assuntos
Materiais Biocompatíveis , Polímeros , Acrilatos , Adsorção , Materiais Biocompatíveis/farmacologia , Adesividade Plaquetária , Propriedades de Superfície
12.
Polymers (Basel) ; 12(8)2020 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-32722595

RESUMO

In order to study the influences of amino silane coupling agents with different grafting densities on the surface of nano silica on the thermomechanical properties of cross-linked epoxy resin, the molecular dynamics method was used to establish an amorphous model and calculate the mechanical properties, glass transition temperature, mean square displacement, hydrogen bond, binding energy, and radial distribution function of the composite models in this paper. The results are as follows: with the increase of the grafting density of an amino silane coupling agent on the surface of nano silica particles, the mechanical properties and glass transition temperature of epoxy resin showed a trend of increasing first and then decreasing. When the grafting ratio was 9%, the mechanical properties and glass transition temperature of the epoxy resin were the largest, and the glass transition temperature was increased by 41 K. At the same time, it was found that the higher the grafting ratio, the lower the chain movement ability, but the higher the binding energy. Besides, the binding energy between the nanoparticles of the grafted silane coupling agent and epoxy resin was negatively correlated with the temperature. By analyzing the hydrogen bond and radial distribution function, the results showed that the improvement of the grafted silane coupling agent on the surface of the nanoparticle to the thermomechanical properties of the epoxy resin was related to the OH···O and NH···O hydrogen bonds. The analysis results indicated that the proper grafting density should be selected based on the established model size, selected nanoparticle diameter, and epoxy resin materials in order to better improve the thermomechanical properties of the epoxy resin.

13.
Polymers (Basel) ; 12(8)2020 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-32824574

RESUMO

The behavior of nanogels in suspension can be dramatically affected by the grafting of a canopy of end-tethered polymer chains. The architecture of the interfacial layer, defined by the grafting density and length of the polymer chains, is a crucial parameter in defining the conformation and influencing the dynamics of the grafted chains. However, the influence of this architecture when the core substrate is itself soft and mobile is complex; the dynamics of the core influences the dynamics of the tethered chains, and, conversely, the dynamics of the tethered chains can influence the dynamics of the core. Here, poly(styrene) (PS) particles were functionalized with poly(methyl acrylate) (PMA) chains and swollen in a common solvent. NMR relaxation reveals that the confinement influences the mobility of the grafted chain more prominently for densely grafted short chains. The correlation time associated with the relaxation of the PMA increased by more than 20% when the grafting density increased for short chains, but for less than 10% for long chains. This phenomenon is likely due to the steric hindrance created by the close proximity to the rigid core and of the neighboring chains. More interestingly, a thick layer of a densely grafted PMA canopy efficiently increases the local mobility of the PS cores, with a reduction of the correlation time of more than 30%. These results suggest an interplay between the dynamics of the core and the dynamics of the canopy.

14.
Materials (Basel) ; 13(22)2020 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-33202639

RESUMO

Reversible deactivation radical polymerizations with reduced amount of organometallic catalyst are currently a field of interest of many applications. One of the very promising techniques is photoinduced atom transfer radical polymerization (photo-ATRP) that is mainly studied for copper catalysts in the solution. Recently, advantageous iron-catalyzed photo-ATRP (photo-Fe-ATRP) compatible with high demanding biological applications was presented. In response to that, we developed surface-initiated photo-Fe-ATRP (SI-photo-Fe-ATRP) that was used for facile synthesis of poly(methyl methacrylate) brushes with the presence of only 200 ppm of FeBr3/tetrabutylammonium bromide catalyst (FeBr3/TBABr) under visible light irradiation (wavelength: 450 nm). The kinetics of both SI-photo-Fe-ATRP and photo-Fe-ATRP in solution were compared and followed by 1H NMR, atomic force microscopy (AFM) and gel permeation chromatography (GPC). Brush grafting densities were determined using two methodologies. The influence of the sacrificial initiator on the kinetics of brush growth was studied. It was found that SI-photo-Fe-ATRP could be effectively controlled even without any sacrificial initiators thanks to in situ production of ATRP initiator in solution as a result of reaction between the monomer and Br radicals generated in photoreduction of FeBr3/TBABr. The optimized and simplified reaction setup allowed synthesis of very thick (up to 110 nm) PMMA brushes at room temperature, under visible light with only 200 ppm of iron-based catalyst. The same reaction conditions, but with the presence of sacrificial initiator, enabled formation of much thinner layers (18 nm).

15.
Polymers (Basel) ; 12(9)2020 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-32846926

RESUMO

Thermoresponsive poly(glycidyl ether) brushes can be grafted to applied tissue culture substrates and used for the fabrication of primary human cell sheets. The self-assembly of such brushes is achieved via the directed physical adsorption and subsequent UV immobilization of block copolymers equipped with a short, photo-reactive benzophenone-based anchor block. Depending on the chemistry and hydrophobicity of the benzophenone anchor, we demonstrate that such block copolymers exhibit distinct thermoresponsive properties and aggregation behaviors in water. Independent on the block copolymer composition, we developed a versatile grafting-to process which allows the fabrication of poly(glycidyl ether) brushes on various tissue culture substrates from dilute aqueous-ethanolic solution. The viability of this process crucially depends on the chemistry and hydrophobicity of, both, benzophenone-based anchor block and substrate material. Utilizing these insights, we were able to manufacture thermoresponsive poly(glycidyl ether) brushes on moderately hydrophobic polystyrene and polycarbonate as well as on rather hydrophilic polyethylene terephthalate and tissue culture-treated polystyrene substrates. We further show that the temperature-dependent switchability of the brush coatings is not only dependent on the cloud point temperature of the block copolymers, but also markedly governed by the hydrophobicity of the surface-bound benzophenone anchor and the subjacent substrate material. Our findings demonstrate that the design of amphiphilic thermoresponsive block copolymers is crucial for their phase transition characteristics in solution and on surfaces.

16.
Int J Biol Macromol ; 128: 885-892, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-30711563

RESUMO

Side chain modification of collagen provides an attractive way to enhance their structure and functions, which is highly desirable for the development of promising biomaterials. However, the impact of structural change of side chains on the intrinsic self-assembly property of collagen was always ignored. Here, a series of acrylic acid-grafted-collagen (AA-g-Col) with different grafting density were prepared to explore the impact of side chain structural variation on the self-assembly of collagen. The results showed that excessive grafting density would weaken or even disappear the self-assembly property of AA-g-Col, but only affects the triple helix to a minor extent. Compared to pristine collagen, the mechanical property and cytocompatibility of AA-g-Col based matrices also deteriorated, along with the increase of grafting density. Therefore, this work contributed a new insight into the importance of grafting density for the study of modified collagen, which would be helpful for the design of optimized formulate collagen-based hybrid materials with both additional novel functions and tissue-mimicking fibrillary structures.


Assuntos
Acrilatos/química , Materiais Biocompatíveis/química , Colágeno/química , Animais , Materiais Biocompatíveis/farmacologia , Colágeno/farmacologia , Hidrogéis/química , Teste de Materiais , Fenômenos Mecânicos , Camundongos , Modelos Moleculares , Células NIH 3T3 , Conformação Proteica
17.
J Colloid Interface Sci ; 541: 150-162, 2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-30685610

RESUMO

Alkylated graphene oxide (GO)/reduced graphene oxide (rGO) are prepared by covalent interaction with octadecyltrichlorosilane (OTCS) and octadecyltriethoxysilane (OTES). The variable oxygen functionalities in the GO/rGO and hydrolysis rate of octadecylsilanes having different leaving groups viz. trichloro and triethoxy found to govern the grafting density of octadecyl chains on the GO and rGO. FTIR, XPS, and TGA results revealed a higher grafting of octadecyl chains in the GO-OTCS, whereas the rGO-OTES exhibited minimum grafting. The van der Waals interaction between the octadecyl chain of alkylated GO/rGO and octadecenyl chains of polyol ester makes alkylated GO/rGO dispersible in the polyol lube base oil. The dispersion stability is collectively driven by grafting density of octadecyl chains and presence of oxygen functionalities in the GO/rGO. Tribological properties in terms of the coefficient of friction and wear scar diameter revealed a good correlation with the structure of alkylated GO/rGO and their dispersion stability in the polyol lube base oil. Raman analysis of the worn surface revealed the sheared-induced deposition of a graphene-based tribo-thin film, which reduced the friction and protected the tribo-interfaces against the wear.

18.
Cell Surf ; 52019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31179402

RESUMO

The roles of the thicknesses and grafting densities of the surface biopolymers of four multi-drug resistant (MDR) Escherichia coli bacterial strains that varied in their biofilm formation in controlling cellular elasticities after exposure to ampicillin were investigated using atomic force microscopy. Exposure to ampicillin was carried out at minimum inhibitory concentrations for different duration times. Our results indicated that the four strains resisted ampicillin through variable mechanisms. Strain A5 did not change its cellular properties upon exposure to ampicillin and as such resisted ampicillin through dormancy. Strain H5 increased its biopolymer brush thickness, adhesion and biofilm formation and kept its roughness, surface area and cell elasticity unchanged upon exposure to ampicillin. As such, this strain likely limits the diffusion of ampicillin by forming strong biofilms. At three hours' exposure to ampicillin, strains D4 and A9 increased their roughness, surface areas, biofilm formation, and brush thicknesses and decreased their elasticities. Therefore, at short exposure times to ampicillin, these strains resisted ampicillin through forming strong biofilms that impede ampicillin diffusion. At eight hours' exposure to ampicillin, strains D4 and A9 collapsed their biopolymers, increased their apparent grafting densities and increased their cellular elasticities. Therefore, at long exposure times to ampicillin, cells utilized their higher rigidity to reduce the diffusion of ampicillin into the cells. The findings of this study clearly point to the potential of using the nanoscale characterization of MDR bacterial properties as a means to monitor cell modifications that enhance "phenotypic antibiotic resistance".

19.
Adv Mater ; 30(21): e1706321, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29512237

RESUMO

Well-defined polymer strands covalently tethered onto solid substrates determine the properties of the resulting functional interface. Herein, the current approaches to determine quantitative grafting densities are assessed. Based on a brief introduction into the key theories describing polymer brush regimes, a user's guide is provided to estimating maximum chain coverage and-importantly-examine the most frequently employed approaches for determining grafting densities, i.e., dry thickness measurements, gravimetric assessment, and swelling experiments. An estimation of the reliability of these determination methods is provided via carefully evaluating their assumptions and assessing the stability of the underpinning equations. A practical access guide for comparatively and quantitatively evaluating the reliability of a given approach is thus provided, enabling the field to critically judge experimentally determined grafting densities and to avoid the reporting of grafting densities that fall outside the physically realistic parameter space. The assessment is concluded with a perspective on the development of advanced approaches for determination of grafting density, in particular, on single-chain methodologies.

20.
ACS Appl Mater Interfaces ; 10(4): 3470-3478, 2018 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-29300451

RESUMO

Although significant progress has been made in improving cycling performance of silicon-based electrodes, few studies have been performed on the architecture effect on polymer binder performance for lithium-ion batteries. A systematic study on the relationship between polymer architectures and binder performance is especially useful in designing synthetic polymer binders. Herein, a graft block copolymer with readily tunable architecture parameters is synthesized and tested as the polymer binder for the high-mass loading silicon (15 wt %)/graphite (73 wt %) composite electrode (active materials >2.5 mg/cm2). With the same chemical composition and functional group ratio, the graft block copolymer reveals improved cycling performance in both capacity retention (495 mAh/g vs 356 mAh/g at 100th cycle) and Coulombic efficiency (90.3% vs 88.1% at first cycle) than the physical mixing of glycol chitosan (GC) and lithium polyacrylate (LiPAA). Galvanostatic results also demonstrate the significant impacts of different architecture parameters of graft copolymers, including grafting density and side chain length, on their ultimate binder performance. By simply changing the side chain length of GC-g-LiPAA, the retaining delithiation capacity after 100 cycles varies from 347 mAh/g to 495 mAh/g.

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