Super-swelled lyotropic single crystals

Kim, Hojun; Song, Ziyuan; Leal, Cecilia

doi:10.1073/pnas.1710774114

Super-swelled lyotropic single crystals

Journal Article · Mon Sep 25 00:00:00 EDT 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1710774114· OSTI ID:1405023

^[1]; Song, Ziyuan ^[1]; Leal, Cecilia ^[1]

Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)

Lipids self-assemble into diverse supramolecular structures that exhibit thermotropic and/or lyotropic behavior. Lyotropic mesophases, where membranes conform to periodic minimal surfaces dividing two nonpenetrating aqueous subspaces, are arguably one of the most intriguing phases of lipid materials. Traditional 3D bicontinuous cubic lipid materials appear as a polycrystal of varying degrees of order. When exposed to water, the properties of the molecular building blocks of the membrane determine specific swelling limits setting the lattice dimensions at about 15 nm. This limited swelling severely impairs their application as delivery vehicles of large drugs or as matrices for guiding protein crystallization. We report the discovery of self-assembly strategies leading to the emergence of lipid bicontinuous single crystals with unprecedented swelling capacity. Here, the conventional strategy to increase unit cell size is tweaking membrane composition to include charged building blocks, a process to achieve electrostatic-driven swelling. In this paper, we demonstrate that controlling self-assembly external conditions when coupled to membrane composition yields 3D bicontinuous cubic phases that swell up to lattice dimensions of 68 nm. Importantly, and contrary to what is perceived for soft lyotropic materials in general, the self-assembly methodology enables the development of large super-swelled monocrystals. Utilizing small-angle X-ray scattering and cryoelectron microscopy, we underpin three crucial factors dictating the stabilization of super-swelled lipid bicontinuous cubic single crystals: (i) organic solvent drying speed, (ii) membrane charge density, and (iii) polyethylene glycol-conjugated lipids amount.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Inst. of Health

OSTI ID:: 1405023

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 41 Vol. 114; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Design of ultra-swollen lipidic mesophases for the crystallization of membrane proteins with large extracellular domains Zabara, Alexandru; Chong, Josephine T. Y.; Martiel, Isabelle ETH Zurich https://doi.org/10.3929/ethz-b-000242161	text	January 2018
Nanostructured Lipid-Based Films for Substrate-Mediated Applications in Biotechnology Kang, Minjee; Tuteja, Mohit; Centrone, Andrea Advanced Functional Materials, Vol. 28, Issue 9 https://doi.org/10.1002/adfm.201704356	journal	January 2018
Cubosomes: The Next Generation of Smart Lipid Nanoparticles? Barriga, Hanna M. G.; Holme, Margaret N.; Stevens, Molly M. Angewandte Chemie International Edition, Vol. 58, Issue 10 https://doi.org/10.1002/anie.201804067	journal	March 2019
Design of ultra-swollen lipidic mesophases for the crystallization of membrane proteins with large extracellular domains Zabara, Alexandru; Chong, Josephine Tse Yin; Martiel, Isabelle Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-02996-5	journal	February 2018
The structural fate of lipid nanoparticles in the extracellular matrix Bandara, Sarith R.; Molley, Thomas G.; Kim, Hojun Materials Horizons, Vol. 7, Issue 1 https://doi.org/10.1039/c9mh00835g	journal	January 2020
Lipid-based liquid crystalline films and solutions for the delivery of cargo to cells Porras-Gomez, Marilyn; Leal, Cecilia Liquid Crystals Reviews, Vol. 7, Issue 2 https://doi.org/10.1080/21680396.2019.1666752	journal	July 2019
Double diamond phase in pear-shaped nanoparticle systems with hard sphere solvent Schönhöfer, Philipp W. A.; Cleaver, Douglas J.; Schröder-Turk, Gerd E. Journal of Physics D: Applied Physics, Vol. 51, Issue 46 https://doi.org/10.1088/1361-6463/aae229	journal	October 2018
Cubosomes: the next generation of smart lipid nanoparticles? Barriga, H. M. G.; Holme, M. N.; Stevens, M. M. Zenodo https://doi.org/10.5281/zenodo.1406159	text	January 2018
Cubosomes: the next generation of smart lipid nanoparticles? Barriga, H. M. G.; Holme, M. N.; Stevens, M. M. Zenodo https://doi.org/10.5281/zenodo.1406160	text	January 2018

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