Shape-Shifting Peptide Nanomaterials: Surface Asymmetry Enables pH-Dependent Formation and Interconversion of Collagen Tubes and Sheets

Merg, Andrea D.; Touponse, Gavin; Genderen, Eric van; Blum, Thorsten B.; Zuo, Xiaobing; Bazrafshan, Alisina; Siaw, Hew Helen; McCanna, Arthur; Brian Dyer, R.; Salaita, Khalid; Abrahams, Jan Pieter; Conticello, Vincent P.

doi:10.1021/jacs.0c08174

Shape-Shifting Peptide Nanomaterials: Surface Asymmetry Enables pH-Dependent Formation and Interconversion of Collagen Tubes and Sheets

Journal Article · Tue Nov 10 00:00:00 EST 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c08174· OSTI ID:1804482

Merg, Andrea D. ^[1]; Touponse, Gavin ^[1]; Genderen, Eric van ^[2]; Blum, Thorsten B. ^[2]; Zuo, Xiaobing ^[3]; Bazrafshan, Alisina ^[1]; Siaw, Hew Helen ^[1]; McCanna, Arthur ^[1]; ^[1]; ^[1]; Abrahams, Jan Pieter ^[4]; ^[1]

Emory Univ., Atlanta, GA (United States)
Paul Scherrer Inst., Villigen (Switzerland)
Argonne National Lab. (ANL), Argonne, IL (United States)
Paul Scherrer Inst., Villigen (Switzerland); Univ. of Basel (Switzerland)

The fabrication of dynamic, transformable biomaterials that respond to environmental cues represents a significant step forward in the development of synthetic materials that rival their highly functional, natural counterparts. In this work, we describe the design and synthesis of crystalline supramolecular architectures from charge-complementary heteromeric pairs of collagen-mimetic peptides (CMPs). Under appropriate conditions, CMP pairs spontaneously assemble into either 1D ultraporous (pore diameter >100 nm) tubes or 2D bilayer nanosheets due to the structural asymmetry that arises from heteromeric self-association. Crystalline collagen tubes represent a heretofore unobserved morphology of this common biomaterial. In-depth structural characterization from a suite of biophysical methods, including TEM, AFM, high-resolution cryo-EM, and SAXS/WAXS measurements, reveals that the sheet and tube assemblies possess a similar underlying lattice structure. The experimental evidence suggests that the tubular structures are a consequence of the self-scrolling of incipient 2D layers of collagen triple helices and that the scrolling direction determines the formation of two distinct structural isoforms. Furthermore, we show that nanosheets and tubes can spontaneously interconvert through manipulation of the assembly pH and systematic adjustment of the CMP sequence. Altogether, we establish initial guidelines for the construction of dynamically responsive 1D and 2D assemblies that undergo a structurally programmed morphological transition.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1804482

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 47 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Shape-Shifting Peptide Nanomaterials: Surface Asymmetry Enables pH-Dependent Formation and Interconversion of Collagen Tubes and Sheets

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