Journal article
Shape-Shifting Peptide Nanomaterials: Surface Asymmetry Enables pH-Dependent Formation and Interconversion of Collagen Tubes and Sheets.
- Merg AD Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- Touponse G Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- Genderen EV Paul Scherrer Institut, CH-5232 Villigen, Switzerland.
- Blum TB Paul Scherrer Institut, CH-5232 Villigen, Switzerland.
- Zuo X X-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.
- Bazrafshan A Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- Siaw HMH Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- McCanna A The Robert P. Apkarian Integrated Electron Microscopy Core, Emory University, Atlanta, Georgia 30322, United States.
- Brian Dyer R Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- Salaita K Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- Abrahams JP Paul Scherrer Institut, CH-5232 Villigen, Switzerland.
- Conticello VP Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.
- 2020-11-10
Published in:
- Journal of the American Chemical Society. - 2020
English
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. Here, 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.
- Language
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- English
- Open access status
- closed
- Identifiers
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- DOI 10.1021/jacs.0c08174
- PMID 33170675
- Persistent URL
- https://sonar.ch/global/documents/231714
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