Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures

Merg, Andrea D.; van Genderen, Eric; Bazrafshan, Alisina; Su, Hanquan; Zuo, Xiaobing; Touponse, Gavin; Blum, Thorsten B.; Salaita, Khalid; Abrahams, Jan Pieter; Conticello, Vincent P.

doi:10.1021/jacs.9b09335

Title: Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures

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Abstract

Engineering free-standing 2D nanomaterials with compositional, spatial, and functional control across size regimes from the nano- to mesoscale represents a significant challenge. Herein, we demonstrate a straightforward strategy for the thermodynamically controlled fabrication of multicomponent sectored nanosheets in which each sector can be chemically and spatially addressed independently and orthogonally. Collagen triple helices, comprising collagen-mimetic peptides (CMPs), are employed as molecularly programmable crystallizable units. Modulating their thermodynamic stability affords the controlled synthesis of 2D core-shell nanostructures via thermally driven heteroepitaxial growth. Structural information, gathered from SAXS and cryo-TEM, reveals that the distinct peptide domains maintain their intrinsic lattice structure and illuminates various mechanisms employed by CMP triple helices to alleviate the elastic strain associated with the interfacial lattice mismatch. Finally, we demonstrate that different sectors of the sheet surface can be selectively functionalized using bioorthogonal conjugation chemistry. Altogether, we establish a robust platform for constructing multifunctional 2D nanoarchitectures in which one can systematically program their compositional, spatial, and functional properties, which is a significant step toward their deployment into functional nanoscale devices.

Authors:

^[1]; van Genderen, Eric ^[2]; Bazrafshan, Alisina ^[1]; Su, Hanquan ^[1]; Zuo, Xiaobing ^[3]; Touponse, Gavin ^[1]; Blum, Thorsten B. ^[2];

^[1]; Abrahams, Jan Pieter ^[4];

^[1]

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

Publication Date:: 2019-12-04

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

OSTI Identifier:: 1608800

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 141; Journal Issue: 51; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2D nanoarchitectonics; biomaterials; collagen-mimetic peptides; peptide nanosheets; seeded growth; self-assembly

Citation Formats


                    Merg, Andrea D., van Genderen, Eric, Bazrafshan, Alisina, Su, Hanquan, Zuo, Xiaobing, Touponse, Gavin, Blum, Thorsten B., Salaita, Khalid, Abrahams, Jan Pieter, and Conticello, Vincent P.. Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures.  United States: N. p., 2019. 
Web.  https://doi.org/10.1021/jacs.9b09335.

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                    Merg, Andrea D., van Genderen, Eric, Bazrafshan, Alisina, Su, Hanquan, Zuo, Xiaobing, Touponse, Gavin, Blum, Thorsten B., Salaita, Khalid, Abrahams, Jan Pieter, & Conticello, Vincent P.. Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures.  United States.  https://doi.org/10.1021/jacs.9b09335

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                    Merg, Andrea D., van Genderen, Eric, Bazrafshan, Alisina, Su, Hanquan, Zuo, Xiaobing, Touponse, Gavin, Blum, Thorsten B., Salaita, Khalid, Abrahams, Jan Pieter, and Conticello, Vincent P.. Wed .  
"Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures".  United States.  https://doi.org/10.1021/jacs.9b09335.  https://www.osti.gov/servlets/purl/1608800.

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@article{osti_1608800,

  title        = {Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core–Shell Nanostructures},

  author       = {Merg, Andrea D. and van Genderen, Eric and Bazrafshan, Alisina and Su, Hanquan and Zuo, Xiaobing and Touponse, Gavin and Blum, Thorsten B. and Salaita, Khalid and Abrahams, Jan Pieter and Conticello, Vincent P.},

  abstractNote = {Engineering free-standing 2D nanomaterials with compositional, spatial, and functional control across size regimes from the nano- to mesoscale represents a significant challenge. Herein, we demonstrate a straightforward strategy for the thermodynamically controlled fabrication of multicomponent sectored nanosheets in which each sector can be chemically and spatially addressed independently and orthogonally. Collagen triple helices, comprising collagen-mimetic peptides (CMPs), are employed as molecularly programmable crystallizable units. Modulating their thermodynamic stability affords the controlled synthesis of 2D core-shell nanostructures via thermally driven heteroepitaxial growth. Structural information, gathered from SAXS and cryo-TEM, reveals that the distinct peptide domains maintain their intrinsic lattice structure and illuminates various mechanisms employed by CMP triple helices to alleviate the elastic strain associated with the interfacial lattice mismatch. Finally, we demonstrate that different sectors of the sheet surface can be selectively functionalized using bioorthogonal conjugation chemistry. Altogether, we establish a robust platform for constructing multifunctional 2D nanoarchitectures in which one can systematically program their compositional, spatial, and functional properties, which is a significant step toward their deployment into functional nanoscale devices.},

  doi          = {10.1021/jacs.9b09335},

  journal      = {Journal of the American Chemical Society},

  number       = 51,

  volume       = 141,

  place        = {United States},

  year         = {2019},

  month        = {12}

}

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