A miscible blended liquid crystalline polymer prepared by Asahi Chemical Industry Co. Ltd. was used to study the effect of temperature on electrorheology. The electrorheological (ER) effect was measured using a rotational viscometer at temperatures between 20 and 60 °C. The polymer showed no yield shear stress under an external electric field, and its ER effect increased with decreasing temperature. We explain the electrorheology of the miscible blended liquid crystalline polymer using our ER mechanism, based on Block’s model. In our mechanism, for an ER fluid to have an appreciable ER effect, its relaxation frequency must be between 100 and 105 Hz and the difference in the dielectric constant must be large below and above the relaxation frequency. The relaxation frequency of the miscible blended liquid crystalline polymer increased with increasing temperature, and the difference in its dielectric constant below and above the relaxation frequency increased with decreasing temperature. These dielectric properties are explained by the Debye theory and account for the electrorheology of the polymer.
A liquid crystalline polysiloxane (LCP), having an ether bond in the spacer between its siloxane main chain and its mesogenic-group side chains, exhibited a very small electrorheological (ER) effect or increase in shear stress upon application of an electric field, but mixtures of the LCP and polydimethylsiloxane (PDMS) exhibited a sharply increasing ER effect with increasing PDMS content throughout the tested range of up to 0.5 of PDMS weight fraction. When phenyl-substituted PDMS (Ph-PDMS) at a weight fraction of 0.3 was used instead of PDMS, however, the ER effect decreased with increasing phenyl content and became nearly undetectable with Ph-PDMS having a phenyl content (ratio of substituted phenyl groups to initial methyl groups) of approximately 15%. DSC analyses showed that the ER effect of the LCP/ PDMS mixtures occurred undiminished throughout a temperature range in which LCP itself is an isotropic liquid in the absence of an applied electric field and suggested that the LC structure of the LCP was maintained even when it was diluted with PDMS in weight fractions of 0.5 or higher, but disrupted when diluted by a 0.3 weight fraction of Ph-PDMS having a 15% phenyl content. Optical microscopic observation of the mixtures of the LCP with a 0.3 weight fraction of PDMS or Ph-PDMS (15% phenyl content) showed that both consisted of uniformly dispersed micron-sized droplets which became elongated in the direction of the applied electric field when it was applied alone but became smaller when both the electric field and shear were applied. These results suggest that the phase separation between the LCP and the dilution oil, as well as the existence and orientation of LC domains, is essential for the generation of a large ER effect.
ABSTRACT:The influence of the molecular structure of homogeneous fluids comprised of liquid crystalline polysiloxanes (LCSs) diluted in polydimethylsiloxane (DMS), on the increase in their viscosity upon application of an electric field (electrorheological effect, or the ER effect) was investigated, particularly in relation to the degree of polysiloxane polymerization, the composition of their mesogenic side chains, and the composition of alkyl spacers inserted between these two components. A large ER effect was observed in LCSs having spacer length of 3 carbons (C3) and diluted with DMS, even though little such effect was observed with no DMS dilution. The ER effect generally increased with increasing DMS dilution and with increasing mesogenic group content, main chain length, and spacer length. At the same time, however, the miscibility of the DMS solvent with the LC polymer decreased, resulting in instability and difficulty in measuring the shear stress at temperatures up to 40ЊC or higher. When spacers containing an ether bond were employed, on the other hand, little or no polymersolvent phase separation occurred, and the ER effect was strong and stable down to temperatures of 30ЊC or lower. With all of the LCSs, the ER effect was observed at temperatures above their isotropic phase transition temperature as measured by DSC.
SYNOPSISLarge increases in shear stress upon application of a 2.0 kV/mm electric field were observed in homogeneous fluids composed of polysiloxane-based liquid crystalline polymers (LCPs) in dimethyl silicone at a shear rate of 200 s-*. The increase was largest (about 3,000 Pa at 50°C) with LCP consisting of a polysiloxane bearing mesogenic groups as side chains. With LCP having the mesogenic groups within the main chain, the maximum increase was about 1,300 Pa at 90°C. It was about 400 Pa at 30°C with LCP having the mesogenic groups at both ends only (biterminal), and several Pa a t 30°C with LCP having the mesogenic group at one end only (monoterminal). The increases were smaller with mesogenic groups of lower positive dielectric anisotropy in the side chain LCP. The side chain, biterminal, and monoterminal LCPs exhibited Newtonian flow in the electric field and shear stress yield at low shear rates in its absence. The complex dynamic modulus and viscosity of the side chain LCP in the electric field showed no dependence on strain at deformation displacements approaching 5", but in its absence were generally strain-dependent, and suggest the strong electrorheological effect of these homogeneous LCP fluids is related to a flexible-chain linkage between their crystalline domains.
Side-chain liquid crystalline polysiloxanes (LCS) diluted with solvents show a large increase in viscosity and a newtonian flow under an electric field. Two types of solvent-diluted LCSs, A and B, are presented and their properties are described in this paper. Type A shows a large temperature-dependent ER effect a quick response of msec. order to an electric field and a dynamic behavior similar to that of a low molecular weight liquid crystal. Type B shows a stable ER effect throughout a wide range of temperatures up to 150°C, a two-step response of shear stress curve upon application of DC electric field and a micron-sized droplets structure which deforms with the electric field. The generation mechanisms of ER effect on the two types were discussed with the data of dynamic and morphological changes, referring those on a low molecular liquid crystal and a particle dispersion type ER fluid.
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