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1.
J Am Chem Soc ; 146(8): 5108-5117, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38367279

RESUMO

Enzymes are natural catalysts for a wide range of metabolic chemical transformations, including selective hydrolysis, oxidation, and phosphorylation. Herein, we demonstrate a strategy for the encapsulation of enzymes within a highly stable zirconium-based metal-organic framework. UiO-66-F4 was synthesized under mild conditions using an enzyme-compatible amino acid modulator, serine, at a modest temperature in an aqueous solution. Enzyme@UiO-66-F4 biocomposites were then formed by an in situ encapsulation route in which UiO-66-F4 grows around the enzymes and, consequently, provides protection for the enzymes. A range of enzymes, namely, lysozyme, horseradish peroxidase, and amano lipase, were successfully encapsulated within UiO-66-F4. We further demonstrate that the resulting biocomposites are stable under conditions that could denature many enzymes. Horseradish peroxidase encapsulated within UiO-66-F4 maintained its biological activity even after being treated with the proteolytic enzyme pepsin and heated at 60 °C. This strategy expands the toolbox of potential metal-organic frameworks with different topologies or functionalities that can be used as enzyme encapsulation hosts. We also demonstrate that this versatile process of in situ encapsulation of enzymes under mild conditions (i.e., submerged in water and at a modest temperature) can be generalized to encapsulate enzymes of various sizes within UiO-66-F4 while protecting them from harsh conditions (i.e., high temperatures, contact with denaturants or organic solvents).


Assuntos
Estruturas Metalorgânicas , Compostos Organometálicos , Ácidos Ftálicos , Estruturas Metalorgânicas/química , Zircônio/química , Biomimética , Compostos Organometálicos/química , Peroxidase do Rábano Silvestre
2.
Int J Mol Sci ; 24(23)2023 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-38069044

RESUMO

Gintonin, newly extracted from ginseng, is a glycoprotein that acts as an exogenous lysophosphatidic acid (LPA) receptor ligand. This study aimed to demonstrate the in vivo preventive effects of gintonin on gastric damage. ICR mice were randomly assigned to five groups: a normal group (received saline, 0.1 mL/10 g, p.o.); a control group (administered 0.3 M HCl/ethanol, 0.1 mL/10 g, p.o.) or indomethacin (30 mg/kg, p.o.); gintonin at two different doses (50 mg/kg or 100 mg/kg, p.o.) with either 0.3 M HCl/ethanol or indomethacin; and a positive control (Ranitidine, 40 mg/kg, p.o.). After gastric ulcer induction, the gastric tissue was examined to calculate the ulcer index. The expression of gastric damage markers, such as tumor necrosis factor (TNF)-α, cyclooxygenase 2 (COX-2), and LPA2 and LPA5 receptors, were measured by Western blotting. Interleukin-6 (IL-6) and prostaglandin E2 (PGE2) levels were measured by enzyme-linked immunosorbent assay. The platelet endothelial cell adhesion molecule (PECAM-1), Evans blue, and occludin levels in gastric tissues were measured using immunofluorescence analysis. Both HCl/ethanol- and indomethacin-induced gastric ulcers showed increased TNF-α, IL-6, Evans blue permeation, and PECAM-1, and decreased COX-2, PGE2, occludin, and LPA5 receptor expression levels. However, oral administration of gintonin alleviated the gastric ulcer index induced by HCl/ethanol and indomethacin in a dose-dependent manner. Gintonin suppressed TNF-α and IL-6 expression, but increased COX-2 expression and PGE2 levels in mouse gastric tissues. Gintonin intake also increased LPA5 receptor expression in mouse gastric tissues. These results indicate that gintonin can play a role in gastric protection against gastric damage induced by HCl/ethanol or indomethacin.


Assuntos
Indometacina , Úlcera Gástrica , Camundongos , Animais , Indometacina/farmacologia , Úlcera Gástrica/induzido quimicamente , Úlcera Gástrica/tratamento farmacológico , Úlcera Gástrica/patologia , Molécula-1 de Adesão Celular Endotelial a Plaquetas/metabolismo , Ciclo-Oxigenase 2/metabolismo , Fator de Necrose Tumoral alfa/metabolismo , Etanol/farmacologia , Interleucina-6/metabolismo , Dinoprostona/metabolismo , Azul Evans/metabolismo , Ocludina/metabolismo , Camundongos Endogâmicos ICR , Mucosa Gástrica/metabolismo
3.
J Ginseng Res ; 47(5): 672-680, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37720568

RESUMO

Background: Korean Red Ginseng (KRG), the steamed root of Panax ginseng, has pharmacological activities for immunological and neurodegenerative disorders. But, the role of KRGE in multiple sclerosis (MS) remains unclear. Purpose: To determine whether KRG extract (KRGE) could inhibit demyelination in corpus callosum (CC) of cuprizone (CPZ)-induced murine model of MS. Methods: Male adult mice were fed with a standard chow diet or a chow diet supplemented with 0.2% (w/w) CPZ ad libitum for six weeks to induce demyelination while were simultaneously administered with distilled water (DW) alone or KRGE-DW (0.004%, 0.02 and 0.1% of KRGE) by drinking. Results: Administration with KRGE-DW alleviated demyelination and oligodendrocyte degeneration associated with inhibition of infiltration and activation of resident microglia and monocyte-derived macrophages as well as downregulation of proinflammatory mediators in the CC of CPZ-fed mice. KRGE-DW also attenuated the level of infiltration of Th1 and Th17) cells, in line with inhibited mRNA expression of IFN-γ and IL-17, respectively, in the CC. These positive effects of KRGE-DW mitigated behavioral dysfunction based on elevated plus maze and the rotarod tests. Conclusion: The results strongly suggest that KRGE-DW may inhibit CPZ-induced demyelination due to its oligodendroglial protective and anti-inflammatory activities by inhibiting infiltration/activation of immune cells. Thus, KRGE might have potential in therapeutic intervention for MS.

4.
J Ginseng Res ; 47(3): 390-399, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-37252272

RESUMO

Background: Gintonin (GT), a Panax ginseng-derived lysophosphatidic acid receptor (LPAR) ligand, has positive effects in cultured or animal models for Parkinson's disease, Huntington's disease, and so on. However, the potential therapeutic value of GT in treating epilepsy has not yet been reported. Methods: Effects of GT on epileptic seizure (seizure) in kainic acid [KA, 55mg/kg, intraperitoneal (i.p.)]-induced model of mice, excitotoxic (hippocampal) cell death in KA [0.2 µg, intracerebroventricular (i.c.v.)]-induced model of mice, and levels of proinflammatory mediators in lipopolysaccharide (LPS)-induced BV2 cells were investigated. Results: An i.p. injection of KA into mice produced typical seizure. However, it was significantly alleviated by oral administration of GT in a dose-dependent manner. An i.c.v. injection of KA produced typical hippocampal cell death, whereas it was significantly ameliorated by administration of GT, which was related to reduced levels of neuroglial (microglia and astrocyte) activation and proinflammatory cytokines/enzymes expression as well as increased level of the Nrf2-antioxidant response via the upregulation of LPAR 1/3 in the hippocampus. However, these positive effects of GT were neutralized by an i.p. injection of Ki16425, an antagonist of LPA1-3. GT also reduced protein expression level of inducible nitric-oxide synthase, a representative proinflammatory enzyme, in LPS-induced BV2 cells. Treatment with conditioned medium clearly reduced cultured HT-22 cell death. Conclusion: Taken together, these results suggest that GT may suppress KA-induced seizures and excitotoxic events in the hippocampus through its anti-inflammatory and antioxidant activities by activating LPA signaling. Thus, GT has a therapeutic potential to treat epilepsy.

5.
Phytomedicine ; 112: 154569, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36842217

RESUMO

BACKGROUND: Bornyl acetate (BA), a chemical component of essential oil in the Pinus family, has yet to be actively studies in terms of its therapeutic effect on numerous diseases, including autoimmune diseases. PURPOSE: This study aimed to investigate the pharmacological effects and molecular mechanisms of BA on myelin oligodendrocyte glycoprotein (MOG35-55)-induced experimental autoimmune encephalomyelitis (EAE) mice in an animal model of multiple sclerosis (MS), a representative autoimmune disease in central nervous system. METHODS: BA (100, 200, or 400 mg/kg) was orally treated to EAE mice once daily for 30 days after immunization for the behavioral test and for the 16th-18th days for the histopathological and molecular analyses, from the onset stage (8th day) of EAE symptoms. RESULTS: BA mitigated behavioral dysfunction (motor disability) and demyelination in the spinal cord that were associated with the down-regulation of representative pro-inflammatory cytokines (interleukin (IL)-1 beta, IL-6, and tumor necrosis factor-alpha), enzymes (cyclooxygenase-2 and inducible nitric oxide synthase), and chemokines (monocyte chemotactic protein-1, macrophage inflammatory protein-1 alpha, and regulated on activation), and decreased infiltration of microglia (CD11b+/CD45+(low)) and macrophages (CD11b+/CD45+(high)). The anti-inflammatory effect of BA was related to the inhibition of mitogen-activated protein kinases and nuclear factor-kappa B pathways. BA also reduced the recruitment/infiltration rates of CD4+ T, Th1, and Th17 cells into the spinal cords of EAE mice, which was related to reduced blood-spinal cord barrier (BSCB) disruption. CONCLUSION: These findings strongly suggest that BA may alleviate EAE due to its anti-inflammatory and BSCB protective activities. This indicates that BA is a potential therapeutic agent for treating autoimmune demyelinating diseases including MS.


Assuntos
Pessoas com Deficiência , Encefalomielite Autoimune Experimental , Transtornos Motores , Esclerose Múltipla , Fármacos Neuroprotetores , Camundongos , Animais , Humanos , Encefalomielite Autoimune Experimental/tratamento farmacológico , Fármacos Neuroprotetores/farmacologia , Fármacos Neuroprotetores/uso terapêutico , Barreira Hematoencefálica , Transtornos Motores/complicações , Transtornos Motores/tratamento farmacológico , Transtornos Motores/patologia , Esclerose Múltipla/tratamento farmacológico , Anti-Inflamatórios/farmacologia , Anti-Inflamatórios/uso terapêutico
6.
J Am Chem Soc ; 144(28): 12595-12601, 2022 07 20.
Artigo em Inglês | MEDLINE | ID: mdl-35797453

RESUMO

Mechanochemical syntheses of rotaxanes have attracted considerable attention of late because of the superior reaction rates and higher yields associated with their production compared with analogous reactions carried out in solution. Previous investigators, however, have focused on the demonstration of the mechanochemical syntheses of rotaxanes per se, rather than on studying the solid-phase host-guest molecular interplay related to their rapid formation and high yields. In this investigation, we attribute the lower yields of rotaxanes prepared in solution to the limited concentration and a desolvation energy penalty that must be compensated for by host-guest interactions during complexation that precedes the templation leading to rotaxane formation. It follows that, if the desolvation energy can be removed and higher concentrations can be attained, even weak host-guest interactions can drive the complexation of host and guest molecules efficiently. In order to test this hypothesis, we chose two host-guest pairs of permethylated pillar[5]arene/1,6-diaminohexane and permethylated pillar[5]arene/2,2'-(ethylenedioxy)bis(ethylamine) for the simple reason that they exhibit extremely low binding constants (2.7 ± 0.4 M-1 when 1,6-diaminohexane is the guest and <0.1 M-1 when 2,2'-(ethylenedioxy)bis(ethylamine) is the guest in CDCl3; i.e., ostensibly no pseudorotaxane formation is observed). We argue that the amount of pseudorotaxanes formed in the solid state is responsive to mechanical treatments or otherwise and changes in temperature during stoppering reactions. Compared to the amount of pseudorotaxanes that can be obtained in solution, large quantities of pseudorotaxanes are formed in the solid state because of concentration and desolvation effects. This mechanochemical enhancement of pseudorotaxane formation is referred to as a self-correction in the current investigation. Rotaxanes based on permethylated pillar[5]arene/1,6-diaminohexane and permethylated pillar[5]arene/2,2'-(ethylenedioxy)bis(ethylamine) have been synthesized in much higher yields compared to those obtained in solution, aided and abetted by self-correction effects during mechanical treatments and heating at a mild temperature of 50 °C.


Assuntos
Rotaxanos , Etilaminas , Modelos Moleculares , Rotaxanos/química , Temperatura
7.
J Ginseng Res ; 46(3): 337-347, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35233163

RESUMO

Coronavirus disease 2019 (COVID-19) is currently a pandemic caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). COVID-19 are directly associated with hyper-activation of innate immune response that excessively produce pro-inflammatory cytokines and induce cytokine storm, leading to multi-organ-failure and significant morbidity/mortality. Currently, several antiviral drugs such as Paxlovid (nirmatrelvir and ritonavir) and molnupiravir are authorized to treat mild to moderate COVID-19, however, there are still no drugs that can specifically fight against challenges of SARS-CoV-2 variants. Panax ginseng, a medicinal plant widely used for treating various conditions, might be appropriate for this need due to its anti-inflammatory/cytokine/viral activities, fewer side effects, and cost efficiency. To review Panax ginseng and its pharmacologically active-ingredients as potential phytopharmaceuticals for treating cytokine storm of COVID-19, articles that reporting its positive effects on the cytokine production were searched from academic databases. Experimental/clinical evidences for the effectiveness of Panax ginseng and its active-ingredients in preventing or mitigating cytokine storm, especially for the cascade of cytokine storm, suggest that they might be beneficial as an adjunct treatment for cytokine storm of COVID-19. This review may provide a new approach to discover specific medications using Panax ginseng to control cytokine storm of COVID-19.

8.
Langmuir ; 37(26): 7995-8006, 2021 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-34165317

RESUMO

Theoretical and numerical studies were conducted to investigate the transitional interpillar spacing for dual-scale structures, where wetting transition between the Wenzel and Cassie-Baxter states occurs in the primary and secondary pillars. A theoretical formula was derived for the transitional interpillar spacing based on the continuum picture of water. Molecular dynamics (MD) simulations were carried out by varying the interpillar spacing for the primary pillars for single- and dual-scale structures with various pillar heights. The results obtained from the theoretical formula agreed reasonably well with the results obtained from MD simulations, especially when the primary pillar height was relatively high. The transitional interpillar spacing increases as the pillar height and the number of secondary pillars increase. The effect of the secondary pillars on the transitional interpillar spacing was also evaluated using the difference in the grand potentials between the Wenzel and Cassie-Baxter states. These results show that the dual-scale structures increase the transitional interpillar spacing with an increase in the surface hydrophobicity.

9.
Langmuir ; 37(1): 330-338, 2021 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-33356326

RESUMO

The present study investigated the dynamic behavior of a nanosized water droplet on a flat and stepped surface using molecular dynamics simulations. The effects of a wetting gradient associated with the surface and the step height of a stepped surface on the dynamic behavior of the water droplet were considered in this study. The dynamic behaviors of the water droplet were described quantitatively upon analyzing the transient variation of the adhesion energy and the position of the water droplet along with the time required to climb the step. The water droplet moved smoothly along the surface with an increasing wetting gradient. On the other hand, the step obstructed the water droplet from climbing the step as the step height increases. The dynamic behavior of the water droplet depending on the variation of the normalized step height and the differences in adhesion energies between the different surfaces was classified into three types, namely, (1) fully climbing the step, (2) partially climbing the step, and (3) being blocked by the step. In the case in which the water droplet fully climbs the step, the time taken for the water droplet to fully climb the step showed a non-monotonic pattern as the step height increases.

10.
J Am Chem Soc ; 142(5): 2541-2548, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-31895548

RESUMO

Aqueous rechargeable zinc batteries (ZBs) have received considerable attention recently for large-scale energy storage systems in terms of rate performance, cost, and safety. Nevertheless, these ZBs still remain a subject for investigation, as researchers search for cathode materials enabling high performance. Among the various candidate cathode materials for ZBs, quinone compounds stand out as candidates because of their high specific capacity, sustainability, and low cost. Quinone-based cathodes, however, suffer from the critical limitation of undergoing dissolution during battery cycling, leading to a deterioration in battery life. To address this problem, we have introduced a redox-active triangular phenanthrenequinone-based macrocycle (PQ-Δ) with a rigid geometry and layered superstructure. Notably, we have confirmed that Zn2+ ions, together with H2O molecules, can be inserted into the PQ-Δ organic cathode, and, as a consequence, the interfacial resistance between the cathode and electrolytes is decreased effectively. Density functional theory calculations have revealed that the low interfacial resistance can be attributed mainly to decreasing the desolvation energy penalty as a result of the insertion of hydrated Zn2+ ions in the PQ-Δ cathode. The combined effects of the insertion of hydrated Zn2+ ions and the robust triangular structure of PQ-Δ serve to achieve a large reversible capacity of 210 mAh g-1 at a high current density of 150 mA g-1, along with an excellent cycle-life, that is, 99.9% retention after 500 cycles. These findings suggest that the utilization of electron-active organic macrocycles, combined with the low interfacial resistance associated with the solvation of divalent carrier ions, is essential for the overall performance of divalent battery systems.

11.
Adv Mater ; 31(51): e1905048, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31693231

RESUMO

Although being incorporated in commercial lithium-ion batteries for a while, the weight portion of silicon monoxide (SiOx , x ≈ 1) is only less than 10 wt% due to the insufficient cycle life. Along this line, polymeric binders that can assist in maintaining the mechanical integrity and interfacial stability of SiOx electrodes are desired to realize higher contents of SiOx . Herein, a pyrene-poly(acrylic acid) (PAA)-polyrotaxane (PR) supramolecular network is reported as a polymeric binder for SiOx with 100 wt%. The noncovalent functionalization of a carbon coating layer on the SiOx is achieved by using a hydroxylated pyrene derivative via the π-π stacking interaction, which simultaneously enables hydrogen bonding interactions with the PR-PAA network through its hydroxyl moiety. Moreover, the PR's ring sliding while being crosslinked to PAA endows a high elasticity to the entire polymer network, effectively buffering the volume expansion of SiOx and largely mitigating the electrode swelling. Based on these extraordinary physicochemical properties of the pyrene-PAA-PR supramolecular binder, the robust cycling of SiOx electrodes is demonstrated at commercial levels of areal loading in both half-cell and full-cell configurations.

12.
Adv Mater ; 31(29): e1901645, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31148271

RESUMO

Despite their unparalleled theoretical capacity, lithium-metal anodes suffer from well-known indiscriminate dendrite growth and parasitic surface reactions. Conductive scaffolds with lithium uptake capacity are recently highlighted as promising lithium hosts, and carbon nanotubes (CNTs) are an ideal candidate for this purpose because of their capability of percolating a conductive network. However, CNT networks are prone to rupture easily due to a large tensile stress generated during lithium uptake-release cycles. Herein, CNT networks integrated with a polyrotaxane-incorporated poly(acrylic acid) (PRPAA) binder via supramolecular interactions are reported, in which the ring-sliding motion of the polyrotaxanes endows extraordinary stretchability and elasticity to the entire binder network. In comparison to a control sample with inelastic binder (i.e., poly(vinyl alcohol)), the CNT network with PRPAA binder can endure a large stress during repeated lithium uptake-release cycles, thereby enhancing the mechanical integrity of the corresponding electrode over battery cycling. As a result, the PRPAA-incorporated CNT network exhibits substantially improved cyclability in lithium-copper asymmetric cells and full cells paired with olivine-LiFePO4 , indicating that high elasticity enabled by mechanically interlocked molecules such as polyrotaxanes can be a useful concept in advancing lithium-metal batteries.

13.
J Am Chem Soc ; 140(35): 10937-10940, 2018 09 05.
Artigo em Inglês | MEDLINE | ID: mdl-30089358

RESUMO

Conjugated microporous polymers (CMPs) offer a unique structure integrating π-conjugated backbone into a porous network for the simultaneous transport of charges and materials. However, tuning electronic properties of CMPs so far has been limited to an approach of varying the monomers, and the precious metal catalysts are inevitably needed for the C-C coupling reaction. Here, we present a powerful strategy to synthesize CMPs and precisely tune their optical band gap and surface area through metal-free in situ cyclization reaction controlled by the acid strength of acid catalysts. Notably, the optical band gap of CMPs showed a linear relationship with the p Ka of acid catalysts, which provides us with the ability to obtain the desired band gap between 2.07 and 3.35 eV, falling in the range of the visible solar spectrum. Moreover, CMPs exhibited excellent textural properties such as microporosity and high specific surface area.

14.
Chem Soc Rev ; 47(6): 2145-2164, 2018 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-29411809

RESUMO

Silicon (Si) anode is among the most promising candidates for the next-generation high-capacity electrodes in Li-ion batteries owing to its unparalleled theoretical capacity (4200 mA h g-1 for Li4.4Si) that is approximately 10 times higher than that of commercialized graphitic anodes (372 mA h g-1 for LiC6). The battery community has witnessed substantial advances in research on new polymeric binders for silicon anodes mainly due to the shortcomings of conventional binders such as polyvinylidene difluoride (PVDF) to address problems caused by the massive volume change of Si (300%) upon (de)lithiation. Unlike conventional battery electrodes, polymeric binders have been shown to play an active role in silicon anodes to alleviate various capacity decay pathways. While the initial focus in binder research was primarily to maintain the electrode morphology, it has been recently shown that polymeric binders can in fact help to stabilize cracked Si microparticles along with the solid-electrolyte-interphase (SEI) layer, thus substantially improving the electrochemical performance. In this review article, we aim to provide an in-depth analysis and molecular-level design principles of polymeric binders for silicon anodes in terms of their chemical structure, superstructure, and supramolecular interactions to achieve good electrochemical performance. We further highlight that supramolecular chemistry offers practical tools to address challenging problems associated with emerging electrode materials in rechargeable batteries.

15.
Science ; 357(6348): 279-283, 2017 07 21.
Artigo em Inglês | MEDLINE | ID: mdl-28729506

RESUMO

Lithium-ion batteries with ever-increasing energy densities are needed for batteries for advanced devices and all-electric vehicles. Silicon has been highlighted as a promising anode material because of its superior specific capacity. During repeated charge-discharge cycles, silicon undergoes huge volume changes. This limits cycle life via particle pulverization and an unstable electrode-electrolyte interface, especially when the particle sizes are in the micrometer range. We show that the incorporation of 5 weight % polyrotaxane to conventional polyacrylic acid binder imparts extraordinary elasticity to the polymer network originating from the ring sliding motion of polyrotaxane. This binder combination keeps even pulverized silicon particles coalesced without disintegration, enabling stable cycle life for silicon microparticle anodes at commercial-level areal capacities.

16.
ACS Nano ; 9(11): 11317-24, 2015 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-26422642

RESUMO

We report supramolecular cross-linking of polymer binders via dynamic host-guest interactions between hyperbranched ß-cyclodextrin polymer and a dendritic gallic acid cross-linker incorporating six adamantane units for high-capacity silicon anodes. Calorimetric analysis in the solution phase indicates that the given host-guest complexation is a highly spontaneous and enthalpically driven process. These findings are further verified by carrying out gelation experiments in both aqueous and organic media. The dynamic cross-linking process enables intimate silicon-binder interaction, structural stability of electrode film, and controlled electrode-electrolyte interface, yielding enhanced cycling performance. Control experiments using both α, γ-CDp with different cavity sizes and a guest molecule incorporating a single adamantane unit verified that the enhanced cycle life originates from the host-guest interaction between ß-cyclodextrin and adamantane. The impact of the dynamic cross-linking is maximized at an optimal stoichiometry between the two components. Importantly, the present investigation proves that the molecular-level tuning of the host-guest interactions can be translated directly to the cycling performance of silicon anodes.

17.
Adv Mater ; 26(47): 7979-85, 2014 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-25339592

RESUMO

Covalent or Noncovalent? Systematic investigation of polymeric binders incorporating Meldrum's acid reveals most critical binder properties for silicon -anodes in lithium ion batteries, that is self-healing effect facilitated by a series of noncovalent interactions.

18.
J Nanosci Nanotechnol ; 14(5): 3793-6, 2014 May.
Artigo em Inglês | MEDLINE | ID: mdl-24734637

RESUMO

We have fabricated a polymer light-emitting diode (PLED) from the conventional blue-emitting polymer, polyfluorene (PFO), by constructing a multilayer structure with non-metal ion containing water soluble non-conjugated polymer, polyurethane with F- ion (PU:F-), on the top of the PFO. The device with PU:F- layer shows a maximum luminance of 5294 cd/m2 at an applied voltage of 10 V while the one without PU:F- layer shows only 4439 cd/m2 at the same applied voltage. We propose the improvement of device performance with PU:F- layer was due to not only an effective hole blocking at the polymer-polymer interface but also increase of electric field strength with anode after electro-stactic repulsion between electrons from the cathod and anions from the water soluble polymer layer. We will discuss the effect of multilayer polymer structure in PLED in terms of current/voltage characteristics, luminance, and quantum efficiency related with the applied bias.

19.
Nano Lett ; 14(2): 864-70, 2014 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-24417681

RESUMO

Polymeric binders play an important role in electrochemical performance of high-capacity silicon (Si) anodes that usually suffer from severe capacity fading due to unparalleled volume change of Si during cycling. In an effort to find efficient polymeric binders that could mitigate such capacity fading, herein, we introduce polymerized ß-cyclodextrin (ß-CDp) binder for Si nanoparticle anodes. Unlike one-dimensional binders, hyperbranched network structure of ß-CDp presents multidimensional hydrogen-bonding interactions with Si particles and therefore offers robust contacts between both components. Even the Si nanoparticles that lost the original contacts with the binder during cycling recover within the multidimensional binder network, thus creating a self-healing effect. Utilizing these advantageous features, ß-CDp-based Si electrode shows markedly improved cycling performance compared to those of other well-known binder cases, especially when combined with linear polymers at an appropriate ratio to form hybrid binders.


Assuntos
Fontes de Energia Elétrica , Eletrodos , Transferência de Energia , Lítio/química , Silício/química , beta-Ciclodextrinas/química , Desenho de Equipamento , Análise de Falha de Equipamento , Polímeros/química
20.
J Nanosci Nanotechnol ; 12(4): 3214-8, 2012 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-22849091

RESUMO

We modified the surface of a polyvinyl alcohol (PVA) layer by self assembly monolayer technique using a fluorine substituted silane compound (1H,1H,2H,2H-perfluorooctyl-trichlorosilane: FTS) to protect a pentacene thin-film transistor (TFT) from O2 and H2O. Surface modified PVA showed very low surface energy with water contact angle of 106.2 degrees. Surface treatment of PVA layer on pentacene TFT device was done in toluene solvent and we did not observe any damage to the PVA layer or pentacene TFT devices during surface modification process. Pentacene TFT with surface modified PVA passivation layer exhibited very stable TFT operation with almost no field effect mobility drop or threshold voltage shift up to 400 hrs. The performance of unpassivated OTFTs exponentially degraded and almost failed in 290 hrs. We propose that modified PVA layer can be used as a good passivation layer for oxygen and water in OTFT.

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