Superstructured Biomaterials Formed by Exchange Dynamics and Host–Guest Interactions in Supramolecular Polymers

Alexandra N. Edelbrock; Tristan D. Clemons; Stacey M. Chin; Joshua J.W. Roan; Eric P. Bruckner; Zaida Álvarez; Jack F. Edelbrock; Kristen S. Wek; Samuel I. Stupp

doi:10.1002/advs.202004042

Superstructured Biomaterials Formed by Exchange Dynamics and Host–Guest Interactions in Supramolecular Polymers

Alexandra N. Edelbrock, Tristan D. Clemons, Stacey M. Chin, Joshua J.W. Roan, Eric P. Bruckner, Zaida Álvarez, Jack F. Edelbrock, Kristen S. Wek, Samuel I. Stupp^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

41 Scopus citations

Abstract

Dynamic and reversible assembly of molecules is ubiquitous in the hierarchical superstructures of living systems and plays a key role in cellular functions. Recent work from the laboratory reported on the reversible formation of such superstructures in systems of peptide amphiphiles conjugated to oligonucleotides and electrostatically complimentary peptide sequences. Here, a supramolecular system is reported upon where exchange dynamics and host–guest interactions between β-cyclodextrin and adamantane on peptide amphiphiles lead to superstructure formation. Superstructure formation with bundled nanoribbons generates a mechanically robust hydrogel with a highly porous architecture that can be 3D printed. Functionalization of the porous superstructured material with a biological signal results in a matrix with significant in vitro bioactivity toward neurons that could be used as a supramolecular model to design novel biomaterials.

Original language	English (US)
Article number	2004042
Journal	Advanced Science
Volume	8
Issue number	8
DOIs	https://doi.org/10.1002/advs.202004042
State	Published - Apr 21 2021

Funding

This work was supported by the Center for Regenerative Nanomedicine at the Simpson Querrey Institute at Northwestern. A.N.E., S.M.C., and K.S.W. received graduate research fellowships through the National Science Foundation (DGE‐1842165). T.D.C. acknowledges funding support from an American Australian Association Fellowship. J.J.W.R. was supported by the Northwestern University Department of Materials Science and Engineering Meister Research Grant. E.P.B was supported by the Department of Defense (DoD), Army Research Office, through the National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. Z.A. received postdoctoral support from the Paralyzed Veterans of America (PVA) Research Foundation, grant #PVA17_RF_0008. J. F. E. would like to acknowledge the Northwestern University Medical Scientist Training Program (T32GM008152). The authors are grateful to the following core facilities at Northwestern University: Peptide Synthesis Core and the Analytical BioNanotechnology Equipment Core both at the Simpson Querrey Institute. These facilities have support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS ‐ 1542205). The Simpson Querrey Institute, Northwestern University Office for Research, U.S. Army Research Office, and the U.S. Army Medical Research and Material Command have also provided funding to develop this facility. Imaging work was performed at the Northwestern University Center for Advanced Microscopy and CD measurements were performed at the Northwestern University Keck Biophysics facility. Both of these facilities were generously supported by an NCI Cancer Center Support Grant (P30 CA060553) awarded to the Robert H Lurie Comprehensive Cancer Center. Electron Microscopy experiments were performed at the Electron Probe Instrumentation Center (EPIC) and the BioCryo facility of Northwestern University's NUANCE Center which have both received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205); the MRSEC program (NSF DMR‐1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. NMR and FTIR characterization in this work made use of IMSERC at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). Portions of this work were performed at the DuPont‐Northwestern‐Dow Collaborative Access Team (DND‐CAT) located at Sector 5 of the Advanced Photon Source (APS). DND‐CAT was supported by Northwestern University, The Dow Chemical Company, and DuPont de Nemours, Inc. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. The authors also thank Prof. Liam Palmer, Dr. Nick Sather, Dr Hiroaki Sai, and Hussain Sangji for helpful discussions and invaluable advice. The authors would also like to thank Mark Seniw for his design of Cinema 4D schematic drawings in the manuscript.

Keywords

3D printing
adamantane
biomaterials
cyclodextrin
host–guest
peptide amphiphile
superstructure

ASJC Scopus subject areas

General Engineering
General Physics and Astronomy
General Chemical Engineering
General Materials Science
Biochemistry, Genetics and Molecular Biology (miscellaneous)
Medicine (miscellaneous)

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10.1002/advs.202004042

Cite this

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title = "Superstructured Biomaterials Formed by Exchange Dynamics and Host–Guest Interactions in Supramolecular Polymers",

abstract = "Dynamic and reversible assembly of molecules is ubiquitous in the hierarchical superstructures of living systems and plays a key role in cellular functions. Recent work from the laboratory reported on the reversible formation of such superstructures in systems of peptide amphiphiles conjugated to oligonucleotides and electrostatically complimentary peptide sequences. Here, a supramolecular system is reported upon where exchange dynamics and host–guest interactions between β-cyclodextrin and adamantane on peptide amphiphiles lead to superstructure formation. Superstructure formation with bundled nanoribbons generates a mechanically robust hydrogel with a highly porous architecture that can be 3D printed. Functionalization of the porous superstructured material with a biological signal results in a matrix with significant in vitro bioactivity toward neurons that could be used as a supramolecular model to design novel biomaterials.",

keywords = "3D printing, adamantane, biomaterials, cyclodextrin, host–guest, peptide amphiphile, superstructure",

author = "Edelbrock, {Alexandra N.} and Clemons, {Tristan D.} and Chin, {Stacey M.} and Roan, {Joshua J.W.} and Bruckner, {Eric P.} and Zaida {\'A}lvarez and Edelbrock, {Jack F.} and Wek, {Kristen S.} and Stupp, {Samuel I.}",

note = "Funding Information: This work was supported by the Center for Regenerative Nanomedicine at the Simpson Querrey Institute at Northwestern. A.N.E., S.M.C., and K.S.W. received graduate research fellowships through the National Science Foundation (DGE‐1842165). T.D.C. acknowledges funding support from an American Australian Association Fellowship. J.J.W.R. was supported by the Northwestern University Department of Materials Science and Engineering Meister Research Grant. E.P.B was supported by the Department of Defense (DoD), Army Research Office, through the National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. Z.A. received postdoctoral support from the Paralyzed Veterans of America (PVA) Research Foundation, grant #PVA17_RF_0008. J. F. E. would like to acknowledge the Northwestern University Medical Scientist Training Program (T32GM008152). The authors are grateful to the following core facilities at Northwestern University: Peptide Synthesis Core and the Analytical BioNanotechnology Equipment Core both at the Simpson Querrey Institute. These facilities have support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS ‐ 1542205). The Simpson Querrey Institute, Northwestern University Office for Research, U.S. Army Research Office, and the U.S. Army Medical Research and Material Command have also provided funding to develop this facility. Imaging work was performed at the Northwestern University Center for Advanced Microscopy and CD measurements were performed at the Northwestern University Keck Biophysics facility. Both of these facilities were generously supported by an NCI Cancer Center Support Grant (P30 CA060553) awarded to the Robert H Lurie Comprehensive Cancer Center. Electron Microscopy experiments were performed at the Electron Probe Instrumentation Center (EPIC) and the BioCryo facility of Northwestern University's NUANCE Center which have both received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205); the MRSEC program (NSF DMR‐1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. NMR and FTIR characterization in this work made use of IMSERC at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). Portions of this work were performed at the DuPont‐Northwestern‐Dow Collaborative Access Team (DND‐CAT) located at Sector 5 of the Advanced Photon Source (APS). DND‐CAT was supported by Northwestern University, The Dow Chemical Company, and DuPont de Nemours, Inc. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. The authors also thank Prof. Liam Palmer, Dr. Nick Sather, Dr Hiroaki Sai, and Hussain Sangji for helpful discussions and invaluable advice. The authors would also like to thank Mark Seniw for his design of Cinema 4D schematic drawings in the manuscript. Publisher Copyright: {\textcopyright} 2021 The Authors. Advanced Science published by Wiley-VCH GmbH",

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doi = "10.1002/advs.202004042",

language = "English (US)",

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T1 - Superstructured Biomaterials Formed by Exchange Dynamics and Host–Guest Interactions in Supramolecular Polymers

AU - Edelbrock, Alexandra N.

AU - Clemons, Tristan D.

AU - Chin, Stacey M.

AU - Roan, Joshua J.W.

AU - Bruckner, Eric P.

AU - Álvarez, Zaida

AU - Edelbrock, Jack F.

AU - Wek, Kristen S.

AU - Stupp, Samuel I.

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Superstructured Biomaterials Formed by Exchange Dynamics and Host–Guest Interactions in Supramolecular Polymers

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