3D Printing of Supramolecular Polymer Hydrogels with Hierarchical Structure

Sather, Nicholas A.; Sai, Hiroaki; Sasselli, Ivan R.; Sato, Kohei; Ji, Wei; Synatschke, Christopher V.; Zambrotta, Ryan T.; Edelbrock, John F.; Kohlmeyer, Ryan R.; Hardin, James O.; Berrigan, John Daniel; Durstock, Michael F.; Mirau, Peter; Stupp, Samuel I.

doi:10.1002/smll.202005743

Title: 3D Printing of Supramolecular Polymer Hydrogels with Hierarchical Structure

Journal Article · Fri Jan 15 00:00:00 EST 2021 · Small

DOI:https://doi.org/10.1002/smll.202005743· OSTI ID:1823087

^[1];

^[2];

^[2]; Zambrotta, Ryan T. ^[3];

^[3]; Kohlmeyer, Ryan R. ^[4];

^[4]; Berrigan, John Daniel ^[5]; Durstock, Michael F. ^[5];

^[5];

^[1]

Northwestern Univ., Evanston, IL (United States); Northwestern Univ., Chicago, IL (United States)
Northwestern Univ., Chicago, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Wright Patterson Air Force Base, Dayton, OH (United States); UES, Inc., Dayton, OH (United States)
Wright Patterson Air Force Base, Dayton, OH (United States)

Liquid crystalline hydrogels are an attractive class of soft materials to direct charge transport, mechanical actuation, and cell migration. When such systems contain supramolecular polymers, it is possible in principle to easily shear align nanoscale structures and create bulk anisotropic properties. However, reproducibly fabricating and patterning aligned supramolecular domains in 3D hydrogels remains a challenge using conventional fabrication techniques. Here, a method is reported for 3D printing of ionically crosslinked liquid crystalline hydrogels from aqueous supramolecular polymer inks. Using a combination of experimental techniques and molecular dynamics simulations, it is found that pH and salt concentration govern intermolecular interactions among the self-assembled structures where lower charge densities on the supramolecular polymers and higher charge screening from the electrolyte result in higher viscosity inks. Enhanced hierarchical interactions among assemblies in high viscosity inks increase the printability and ultimately lead to greater nanoscale alignment in extruded macroscopic filaments when using small nozzle diameters and fast print speeds. The use of this approach is demonstrated to create materials with anisotropic ionic and electronic charge transport as well as scaffolds that trigger the macroscopic alignment of cells due to the synergy of supramolecular self-assembly and additive manufacturing.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0000989; AC02‐06CH11357

OSTI ID:: 1823087

Alternate ID(s):: OSTI ID: 1804819; OSTI ID: 1846607

Journal Information:: Small, Vol. 17, Issue 5; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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99 GENERAL AND MISCELLANEOUS
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77 NANOSCIENCE AND NANOTECHNOLOGY

Title: 3D Printing of Supramolecular Polymer Hydrogels with Hierarchical Structure

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