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Liquid-liquid crystalline phase separation in biological filamentous colloids: nucleation, growth and order-order transitions of cholesteric tactoids.

ABSTRACT: The process of liquid-liquid crystalline phase separation (LLCPS) in filamentous colloids is at the very core of multiple biological, physical and technological processes of broad significance. However, the complete theoretical understanding of the process is still missing. LLCPS involves the nucleation, growth and up-concentration of anisotropic droplets from a continuous isotropic phase, until a state of equilibrium is reached. Herein, by combining the thermodynamic extremum principle with the Onsager theory, we describe the nucleation and growth of liquid crystalline droplets, and the evolution of their size and concentration during phase separation, eventually leading to a multitude of order-order phase transitions. Furthermore, a decreasing pitch behaviour can be predicted using this combined theory during tactoid growth, already observed experimentally but not yet explained by present theories. The results of this study are compared with the experimental data of cholesteric pitch, observed in three different systems of biological chiral liquid crystals. These findings give an important framework for predicting the formation, growth and phase behaviour of biological filamentous colloids undergoing LLCPS, advancing our understanding of liquid-liquid phase separation and self-assembly mechanisms in biological systems, and provide a valuable rationale for developing nanomaterials and applications in nanotechnology.

SUBMITTER: Azzari P

PROVIDER: S-EPMC8279111 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:To prevent greenhouse emissions into the atmosphere, separations like CO2/CH4 and CO2/N2 from natural gas, biogas, and flue gasses are crucial. Polymer membranes gained a key role in gas separations over the past decades, but these polymers are often not organized at a molecular level, which results in a trade-off between permeability and selectivity. In this work, the effect of molecular order and orientation in liquid crystals (LCs) polymer membranes for gas permeation is demonstrated. Using the self-assembly of polymerizable LCs to prepare membranes ensures control over the supramolecular organization and alignment of the building blocks at a molecular level. Robust freestanding LC membranes were fabricated that have various, distinct morphologies (isotropic, nematic cybotactic, and smectic C) and alignment (planar and homeotropic), while using the same chemical composition. Single gas permeation data show that the permeability decreases with increasing molecular order while the ideal gas selectivity of He and CO2 over N2 increases tremendously (36-fold for He/N2 and 21-fold for CO2/N2) when going from randomly ordered to the highly ordered smectic C morphology. The calculated diffusion coefficients showed a 10-fold decrease when going from randomly ordered membranes to ordered smectic C membranes. It is proposed that with increasing molecular order, the free volume elements in the membrane become smaller, which hinders gasses with larger kinetic diameters (Ar, N2) more than gasses with smaller kinetic diameters (He, CO2), inducing selectivity. Comparison of gas sorption and permeation performances of planar and homeotropic aligned smectic C membranes shows the effect of molecular orientation by a 3-fold decrease of the diffusion coefficient of homeotropic aligned smectic C membranes resulting in a diminished gas permeation and increased ideal gas selectivities. These results strongly highlight the importance of molecular order and orientation in LC polymer membranes for gas separation.

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Liquid-liquid crystalline phase separation in biological filamentous colloids: nucleation, growth and order-order transitions of cholesteric tactoids.

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