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Title: Highly stable and self-repairing membrane-mimetic 2D nanomaterials assembled from lipid-like peptoids

Two-dimensional (2D) materials with molecular-scale thickness have attracted increasing interest for separation, electronic, catalytic, optical, energy and biomedical applications. Although extensive research on 2D materials, such as graphene and graphene oxide, has been performed in recent years, progress is limited on self-assembly of 2D materials from sequence-specific macromolecules, especially from synthetic sequences that could exhibit lipid-like self-assembly of bilayer sheets and mimic membrane proteins for functions. The creation of such new class of materials could enable development of highly stable biomimetic membranes that exhibit cell-membrane-like molecular transport with exceptional selectively and high transport rates. Here we demonstrate self-assembly of lipid-like 12-mer peptoids into extremely stable, crystalline, flexible and free-standing 2D membrane materials. As with cell membranes, upon exposure to external stimuli, these materials exhibit changes in thickness, varying from 3.5 nm to 5.6 nm. We find that self-assembly occurs through a facile crystallization process, in which inter-peptoid hydrogen bonds and enhanced hydrophobic interactions drive the formation of a highly-ordered structure. Molecular simulation confirms this is the energetically favored structure. Displaying functional groups at arbitrary locations of membrane-forming peptoids produces membranes with similar structures. This research further shows that single-layer membranes can be coated onto substrate surfaces. Moreover, membranes with mechanically-inducedmore » defects can self-repair. Given that peptoids are sequence-specific and exhibit protein-like molecular recognition with enhanced stability, we anticipate our membranes to be a robust platform tailored to specific applications.« less
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [4] ;  [1] ;  [5] ;  [1] ;  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Division of Physical Sciences
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Division of Physical Sciences; East China Normal Univ. (ECNU), Shanghai (China). School of Chemistry and Molecular Engineering
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Division of Physical Sciences; Linyi Univ., Linyi (China). College of Chemistry and Chemical Engineering
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Division of Physical Sciences; Xiangtan Univ., Xiantan (China). Inst. of Rheology Mechanics
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Publication Date:
OSTI Identifier:
1267592
Report Number(s):
PNNL-SA--112006
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC05-76RL01830; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English