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1.
ACS Omega ; 8(38): 35275-35282, 2023 Sep 26.
Article in English | MEDLINE | ID: mdl-37780022

ABSTRACT

Over the past decade, there has been significant interest in polysiloxane-based dielectric elastomers as promising soft electroactive materials. Nevertheless, the natural low permittivity of polydimethylsiloxane has limited its practical applications. In this study, we have developed silicone rubber/Al@SiO2 composites with a high dielectric constant, low dielectric loss, and high electrical breakdown strength by controlling the shell layer thickness and the content of the core-shell filler. We also investigated the dielectric behavior of the composites. The use of core-shell fillers has increased the Maxwell-Wagner-Sillars (MWS) relaxation process while reducing the dielectric loss of direct current conductance in silicone rubber composites. Moreover, the temperature dependence of the MWS relaxation time in the composites follows the Arrhenius equation. This strategy of increasing the permittivity of silicone composites through core-shell structural fillers can inspire the preparation of other high dielectric constant composites.

2.
ACS Appl Mater Interfaces ; 15(4): 5644-5656, 2023 Feb 01.
Article in English | MEDLINE | ID: mdl-36689682

ABSTRACT

We report a method to construct ordered hierarchical porous structures in carbon nanofiber membranes using poly(ethylene oxide)-block-polydimethylsiloxane bottlebrush block copolymers (BBCPs) as templates. The BBCPs self-assemble into a spherical morphology driven by small-molecule hydrogen bond donors which act as bridges between carbon precursors and templates to promote uniform dispersion of the templates. We successfully obtained flexible, self-supporting, and porous carbon nanofiber membranes (PCNFs) with high porosity. Then, a supercapacitor electrode was independently prepared using PCNFs as an active substance without infiltrating any conductive agents or binders. The PCNFs exhibit excellent performance with a capacitance of 234.1 F g-1 at a current density of 1 A g-1 owing to the abundant hierarchical porous structures and high content of nitrogen and oxygen elements internally. The aqueous symmetric supercapacitor prepared using PCNFs electrodes maintains more than 95% capacitance retention after 55,000 charge-discharge cycles. Furthermore, the capacitance retention reaches up to 67.72% at a current density of 50 A g-1 (compared to 1 A g-1), exhibiting excellent cycling stability and rate capability. Based on the excellent electrochemical performance and flexible self-supporting ability of PCNFs, this work is expected to facilitate the development of flexible displays, flexible sensors, wearable devices, and electrocatalysis.

3.
ACS Appl Mater Interfaces ; 12(51): 57322-57329, 2020 Dec 23.
Article in English | MEDLINE | ID: mdl-33306366

ABSTRACT

We report the self-assembly of amphiphilic polystyrene-block-poly(ethylene oxide) (PS-b-PEO) brush block copolymers (BBCPs) into spherical micelles in an ethanol/water mixture as an efficient templating approach to fabricate mesoporous carbon spheres using polydopamine as a carbon source. Mesopore sizes of up to 25 nm are well controlled and are dependent on the molecular weight (Mw) of the BBCP. Such large pores are difficult to obtain using traditional linear block copolymers templates. Furthermore, bimodal mesoporous carbon spheres with two populations of pore sizes (24.5 and 6.5 nm) are obtained using a BBCP coassembled with a small molecule surfactant (Pluronic F127). An oxygen reduction reaction is used to demonstrate that electrocatalytic performance can be tuned by controlling the carbon sphere morphologies. This work provides a novel and versatile method to fabricate carbon spheres with broadly tunable bimodal pore sizes for potential applications in catalysis, separations, and energy storage.

4.
J Am Chem Soc ; 141(42): 17006-17014, 2019 Oct 23.
Article in English | MEDLINE | ID: mdl-31577903

ABSTRACT

We report the preparation of ordered porous carbon materials with tailored pore sizes selected between 16 and 108 nm using bottlebrush block copolymers (BBCPs) as templates. The nanoporous carbons are prepared via the cooperative assembly of polydimethylsiloxane-block-poly(ethylene oxide) (PDMS-b-PEO) BBCPs with phenol-formaldehyde resin yielding ordered precursor films, followed by carbonization. The assembly of PDMS-b-PEO BBCPs with the resin leads to films exhibiting a spherical morphology (PDMS as the minor domain) with uniform domain sizes between 18 and 150 nm in the bulk. The assembled PDMS sphere diameters scale linearly with BBCPs molecular weights, allowing precise control of domain size. Access to very large ordered domains is an enabling hallmark of BBCPs self-assembly, but reports of well-ordered spherical domains are not common. Carbonization of the ordered precursor films yields nanoporous carbon with uniform and tunable pore size. These nanoporous carbons are shown to exhibit excellent performance as supercapacitor electrodes with capacitance reaching up to 254 F g-1 at a current density of 2 A g-1.

5.
Macromolecules ; 51(6): 2395-2400, 2018 Mar 27.
Article in English | MEDLINE | ID: mdl-29681653

ABSTRACT

Despite a huge variety of methodologies having been proposed to produce photonic structures by self-assembly, the lack of an effective fabrication approach has hindered their practical uses. These approaches are typically limited by the poor control in both optical and mechanical properties. Here we report photonic thermosetting polymeric resins obtained through brush block copolymer (BBCP) self-assembly. We demonstrate that the control of the interplay between order and disorder in the obtained photonic structure offers a powerful tool box for designing the optical appearance of the polymer resins in terms of reflected wavelength and scattering properties. The obtained materials exhibit excellent mechanical properties with hardness up to 172 MPa and Young's modulus over 2.9 GPa, indicating great potential for practical uses as photonic coatings on a variety of surfaces.

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