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1.
ACS Appl Mater Interfaces ; 16(21): 27694-27704, 2024 May 29.
Article in English | MEDLINE | ID: mdl-38747638

ABSTRACT

To achieve multifunctional properties using nanocomposites, selectively locating nanofillers in specific areas by tailoring a mixture of two immiscible polymers has been widely investigated. Forming a phase-separated structure from entirely miscible molecules is rarely reported, and the related mechanisms to govern the formation of assemblies from molecules have not been fully resolved. In this work, a novel method and the underlying mechanism to fabricate self-assembling, bicontinuous, biphasic structures with localized domains made up of amine-functionalized graphene nanoplatelets are presented, involving the tailoring of compositions in a liquid processable multicomponent epoxy blend. Kinetics studies were carried out to investigate the differences in reactivity of various epoxy-hardener pairs. Molecular dynamics simulations and in situ optical photothermal infrared spectroscopy measurements revealed the trajectories of different components during the early stages of polymerization, supporting the migration (phase behavior) of each component during the curing process. Confirmed by the phase structure and the correlated chemical maps down to the submicrometer level, it is believed that the bicontinuous phase separation is driven by the change of the miscibility between various building blocks forming during polymerization, leading to the formation of nanofiller domains. The proposed morphology evolution mechanism is based on combining solubility parameter calculations with kinetics studies, and preliminary experiments are performed to validate the applicability of the mechanism of selectively locating nanofillers in the phase-separated structure. This provides a simple yet sophisticated engineering model and a roadmap to a mechanism for fabricating phase-separated structures with nanofiller domains in nanocomposite films.

2.
Anal Chem ; 94(34): 11848-11855, 2022 Aug 30.
Article in English | MEDLINE | ID: mdl-35972471

ABSTRACT

By incorporating 1-(2-aminoethyl)piperazine (AEPIP) into a commercial epoxy blend, a bicontinuous microstructure is produced with the selective localization of amine-functionalized graphene nanoplatelets (A-GNPs). This cured blend underwent self-assembly, and the morphology and topology were observed via spectral imaging techniques. As the selective localization of nanofillers in thermoset blends is rarely achieved, and the mechanism remains largely unknown, the optical photothermal infrared (O-PTIR) spectroscopy technique was employed to identify the compositions of microdomains. The A-GNP tends to be located in the region containing higher concentrations of both secondary amine and secondary alcohol; additionally, the phase morphology was found to be influenced by the amine concentration. With the addition of AEPIP, the size of the graphene domains becomes smaller and secondary phase separation is detected within the graphene domain evidenced by the chemical contrast shown in the high-resolution chemical map. The corresponding chemical mapping clearly shows that this phenomenon was mainly induced by the chemical contrast in related regions. The findings reported here provide new insight into a complicated, self-assembled nanofiller domain formed in a multicomponent epoxy blend, demonstrating the potential of O-PTIR as a powerful and useful approach for assessing the mechanism of selectively locating nanofillers in the phase structure of complex thermoset systems.

3.
Materials (Basel) ; 13(7)2020 Mar 27.
Article in English | MEDLINE | ID: mdl-32230820

ABSTRACT

In order to increase the material throughput of aligned discontinuous fibre composites using technologies such as HiPerDiF, stability of the carbon fibres in an aqueous solution needs to be achieved. Subsequently, a range of surfactants, typically employed to disperse carbon-based materials, have been assessed to determine the most appropriate for use in this regard. The optimum stability of the discontinuous fibres was observed when using the anionic surfactant, sodium dodecylbenzene sulphonate, which was superior to a range of other non-ionic and anionic surfactants, and single-fibre fragmentation demonstrated that the employment of sodium dodecylbenzene sulphonate did not affect the interfacial adhesion between fibres. Rheometry was used to complement the study, to understand the potential mechanisms of the improved stability of discontinuous fibres in aqueous suspension, and it led to the understanding that the increased viscosity was a significant factor. For the shear rates employed, fibre deformation was neither expected nor observed.

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