Computational and Experimental Determination of the Properties, Structure, and Stability of Peptoid Nanosheets and Nanotubes

Zhao, Mingfei; Zhang, Shuai; Zheng, Renyu; Alamdari, Sarah; Mundy, Christopher J.; Pfaendtner, Jim; Pozzo, Lilo D.; Chen, Chun-Long; De Yoreo, James J.; Ferguson, Andrew L.

doi:10.1021/acs.biomac.3c00107

Computational and Experimental Determination of the Properties, Structure, and Stability of Peptoid Nanosheets and Nanotubes

Journal Article · Thu May 04 00:00:00 EDT 2023 · Biomacromolecules

DOI:https://doi.org/10.1021/acs.biomac.3c00107· OSTI ID:1993122

^[1]; ^[2]; Zheng, Renyu ^[2]; ^[3]; ^[4]; ^[2]; ^[3]; ^[4]; ^[4]; ^[5]

University of Chicago, IL (United States); University of Chicago
University of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
University of Washington, Seattle, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); University of Washington, Seattle, WA (United States)
University of Chicago, IL (United States)

Peptoids (N-substituted glycines) are a group of highly controllable peptidomimetic polymers. Amphiphilic diblock peptoids have been engineered to assemble crystalline nanospheres, nanofibrils, nanosheets, and nanotubes with biochemical, biomedical, and bioengineering applications. The mechanical properties of peptoid nanoaggregates and their relationship to the emergent self-assembled morphologies have been relatively unexplored and are critical for the rational design of peptoid nanomaterials. In this work, we consider a family of amphiphilic diblock peptoids consisting of a prototypical tube-former (Nbrpm6Nc6, a NH₂-capped hydrophobic block of six N-((4-bromophenyl)methyl)glycine residues conjugated to a polar NH₃(CH₂)₅CO tail), a prototypical sheet-former (Nbrpe6Nc6, where the hydrophobic block comprises six N-((4-bromophenyl)ethyl)glycine residues), and an intermediate sequence that forms mixed structures ((NbrpeNbrpm)3Nc6). We combine all-atom molecular dynamics simulations and atomic force microscopy to determine the mechanical properties of the self-assembled 2D crystalline nanosheets and relate these properties to the observed self-assembled morphologies. We find good agreement between our computational predictions and experimental measurements of Young’s modulus of crystalline nanosheets. A computational analysis of the bending modulus along the two axes of the planar crystalline nanosheets reveals bending to be more favorable along the axis in which the peptoids stack by interdigitation of the side chains compared to that in which they form columnar crystals with π-stacked side chains. Here, we construct molecular models of nanotubes of the Nbrpm6Nc6 tube-forming peptoid and predict a stability optimum in good agreement with experimental measurements. A theoretical model of nanotube stability suggests that this optimum is a free energy minimum corresponding to a “Goldilocks” tube radius at which capillary wave fluctuations in the tube wall are minimized.

View Accepted Manuscript (DOE)

Research Organization:: University of Washington, Seattle, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019288

OSTI ID:: 1993122

Journal Information:: Biomacromolecules, Journal Name: Biomacromolecules Journal Issue: 6 Vol. 24; ISSN 1525-7797

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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