Supramolecular and Hybrid Bonding Polymers

Stupp, Samuel I.; Clemons, Tristan D.; Carrow, James K.; Sai, Hiroaki; Palmer, Liam C.

doi:10.1002/ijch.202000005

Cited by 18 publications

(20 citation statements)

References 42 publications

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“…[5,6] The non-covalent bonds enable transient complexation among molecules of interest, thus allowing reversible and dynamic functionality in the hierarchical structures of living matter. [7] The ability to emulate this dynamic hierarchical self-assembly in synthetic systems has proven to be challenging, especially to trigger the reversible assembly of molecules.…”

Section: Introductionmentioning

confidence: 99%

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

Edelbrock¹,

Clemons

Chin

et al. 2021

Advanced Science

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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 -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.

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Section: Introductionmentioning

confidence: 99%

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

Edelbrock¹,

Clemons

Chin

et al. 2021

Advanced Science

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“… 11 − 14 These PA fibers have been used in a number of exciting applications, while at the same time, the fundamental understanding of their structure–property relationship has been crucial to progress. 15 …”

Section: Introductionmentioning

confidence: 99%

Exploring the Potential of Benzene-1,3,5-tricarboxamide Supramolecular Polymers as Biomaterials

et al. 2020

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The fast dynamics occurring in natural processes increases the difficulty of creating biomaterials capable of mimicking Nature. Within synthetic biomaterials, water-soluble supramolecular polymers show great potential in mimicking the dynamic behavior of these natural processes. In particular, benzene-1,3,5-tricaboxamide (BTA)-based supramolecular polymers have shown to be highly dynamic through the exchange of monomers within and between fibers, but their suitability as biomaterials has not been yet explored. Herein we systematically study the interactions of BTA supramolecular polymers bearing either tetraethylene glycol or mannose units at the periphery with different biological entities. When BTA fibers were incubated with bovine serum albumin (BSA), the protein conformation was only affected by the fibers containing tetraethylene glycol at the periphery (BTA-OEG 4 ). Coarse-grained molecular simulations showed that BSA interacted with BTA-OEG 4 fibers rather than with BTA-OEG 4 monomers that are present in solution or that may exchange out of the fibers. Microscopy studies revealed that, in the presence of BSA, BTA-OEG 4 retained their fiber conformation although their length was slightly shortened. When further incubated with fetal bovine serum (FBS), both long and short fibers were visualized in solution. Nevertheless, in the hydrogel state, the rheological properties were remarkably preserved. Further studies on the cellular compatibility of all the BTA assemblies and mixtures thereof were performed in four different cell lines. A low cytotoxic effect at most concentrations was observed, confirming the suitability of utilizing functional BTA supramolecular polymers as dynamic biomaterials.

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“…An example is skeletal muscle where supramolecular polymers of actin and myosin are linked to the giant protein covalent polymer known as titin to make-up the highly aligned structure of the sarcomere. We believe there is great promise in the combination of supramolecular and covalent polymers, and termed these systems in an earlier publication as hybrid bonding polymers [37] . In recent publications we also demonstrated the functional value of hybrid bonding polymers aiming at the development of robotic soft materials [ 34 , 35 ].…”

Section: Discussionmentioning

confidence: 99%

“…The partial replacement is in fact extremely important in order to create materials that combine the robustness of covalent polymers with dynamics and order of supramolecular polymers. We referred earlier to these systems as “hybrid bonding polymers” which chemically integrate covalent and supramolecular polymers [37] . Supramolecular polymers are definitely attractive as biomaterials in areas such as regenerative medicine and drug delivery since bioactive supramolecular scaffolds and drug vehicles could be designed to biodegrade rapidly after their function has been performed [ 4 , 38 ].…”

Section: Introductionmentioning

confidence: 99%

Design of materials with supramolecular polymers

Clemons

Stupp

2020

Progress in Polymer Science

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One hundred years ago Hermann Staudinger was strongly criticized by his scientific peers for his macromolecular hypothesis, but today it is hard to imagine a world without polymers. His hypothesis described polymers as macromolecules composed of large numbers of structural units connected by covalent bonds. In the 1990s the concept of supramolecular polymers emerged in the scientific literature as discrete entities of large molar mass comparable to that of classical polymers but built through non-covalent bonds among monomers. Supramolecular polymers exist in biological systems, and potentially blend the physical properties of covalent polymers with unique features such as high degrees of internal order within the polymeric structure, defined shapes, and novel dynamics. This trend article provides a summary of seminal contributions in supramolecular polymerization and provides recent examples from the Stupp laboratory to demonstrate the potential applications of an exciting class of materials composed fully or partially of supramolecular polymers. In closing, we provide our perspective on future opportunities provided by this field at the onset of a second century of polymers. It is our objective here to demonstrate that this second century could be as prosperous, if not more so, than the preceding one.

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Supramolecular and Hybrid Bonding Polymers

Cited by 18 publications

References 42 publications

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

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

Exploring the Potential of Benzene-1,3,5-tricarboxamide Supramolecular Polymers as Biomaterials

Design of materials with supramolecular polymers

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