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Controlling the Self-Assembly of Synthetic Metal-Coordinating Coiled-Coil Peptides

Scheib, Kimberly A. (2019) Controlling the Self-Assembly of Synthetic Metal-Coordinating Coiled-Coil Peptides. Master's Thesis, University of Pittsburgh. (Unpublished)

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A distinct gap between the fields of peptide-based supramolecular assemblies and metal-organic frameworks (MOFs) exists. Despite recent efforts to explore this area of materials, many metal-directed peptide-based assemblies remain unpredictable, necessitating deeper study to establish robust design principles with which functional materials may be built. The profound unpredictability is not surprising, since peptide-based building blocks are more complex than others which have achieved success in organic and inorganic materials chemistry. The present study attempts to expand and solidify basic design rules for self-assembling metal-directed peptide-based architectures by first exerting control over the assembly of a serendipitously discovered supramolecular lattice. Recent published work has shown coiled-coil peptides containing one or more unnatural solvent-exposed terpyridine (Tpy) side chains can self-assemble to form supramolecular networks in the presence of copper (II) ion. Unexpected was the involvement of glutamic acid (Glu) side chains in the coordination motif (Tpy-Cu2+-Glu). Here, we seek to exert better control over these materials through systematic placement of both Tpy and Glu residues. Results are presented for six designed sequences, including one that manifests a hexagonal net rare in the materials literature. Collectively, these results demonstrate the power of harnessing peptide folding and metal coordination as driving forces for the formation of predictable supramolecular architectures.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Scheib, Kimberly A.kas350@pitt.edukas350
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairHorne, W. Sethhorne@pitt.eduhorne0000-0003-2927-1739
Committee MemberChong, Lillian T.ltchong@pitt.edultchong0000-0002-0590-483X
Committee MemberWeber, Stephen G.sweber@pitt.edusweber0000-0002-7970-2632
Date: 25 June 2019
Date Type: Publication
Defense Date: 8 April 2019
Approval Date: 25 June 2019
Submission Date: 11 April 2019
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Number of Pages: 92
Institution: University of Pittsburgh
Schools and Programs: Dietrich School of Arts and Sciences > Chemistry
Degree: MS - Master of Science
Thesis Type: Master's Thesis
Refereed: Yes
Uncontrolled Keywords: Metal-driven, self-assembly, supramolecular, assembly, peptide, de novo, metal-coordinating, terpyridine, glutamic acid, glutamate, copper, copper (II), x-ray, diffraction, crystallography, materials, nanomaterials, coiled-coil, helical, backbone, hydrophobic, core, oligomerization, oligomer state, hexagonal, lattice, net, packed, open, control, rational design, horne, scheib, tavenor, metal-binding, metal-coordination, crystal structure
Date Deposited: 25 Jun 2019 21:12
Last Modified: 25 Jun 2019 21:12


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