Abstract
An ability to develop sequence-defined synthetic polymers that both mimic lipid amphiphilicity for self-assembly of highly stable membrane-mimetic 2D nanomaterials and exhibit protein-like functionality would revolutionize the development of biomimetic membranes. Here we report the assembly of lipid-like peptoids into highly stable, crystalline, free-standing and self-repairing membrane-mimetic 2D nanomaterials through a facile crystallization process. Both experimental and molecular dynamics simulation results show that peptoids assemble into membranes through an anisotropic formation process. We further demonstrated the use of peptoid membranes as a robust platform to incorporate and pattern functional objects through large side-chain diversity and/or co-crystallization approaches. Similar to lipid membranes, peptoid membranes exhibit changes in thickness upon exposure to external stimuli; they can coat surfaces in single layers and self-repair. We anticipate that this new class of membrane-mimetic 2D nanomaterials will provide a robust matrix for development of biomimetic membranes tailored to specific applications.
Highlights
IntroductionBecause peptoids lack backbone hydrogen bonds, which simplifies tuning interpeptoid and peptoid-surface interactions exclusively through side-chain chemistry, they offer unique opportunity for achieving sequence-specific molecular recognition[7,10] and controlling self-assembly[11,12,13,14,15]
Berkeley, California 94720, USA. * These authors contributed to this work. w Present address: Department of Biochemistry and Molecular Biology, University of Texas Medical Branch, Galveston, Texas 77555, USA
Because cell membranes are a great source of inspiration in biotechnology and nanotechnology, many efforts have been made to create synthetic, membrane-mimetic 2D nanomaterials assembled from lipids, or synthetic analogues of lipids[3,4,5]
Summary
Because peptoids lack backbone hydrogen bonds, which simplifies tuning interpeptoid and peptoid-surface interactions exclusively through side-chain chemistry, they offer unique opportunity for achieving sequence-specific molecular recognition[7,10] and controlling self-assembly[11,12,13,14,15]. All these features make peptoids highly attractive as synthetic analogues of lipids for self-assembly of membrane-mimetic 2D materials. We report the first example of self-assembling highly stable and self-repairing membrane-mimetic 2D nanomaterials by designing lipid-like sequence-defined peptoids
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