Premium
3D Printing of Supramolecular Polymer Hydrogels with Hierarchical Structure
Author(s) -
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.
Publication year - 2021
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202005743
Subject(s) - self healing hydrogels , materials science , supramolecular chemistry , nanotechnology , supramolecular polymers , polymer , fabrication , nanoscopic scale , electrolyte , viscosity , ionic bonding , supramolecular assembly , chemical engineering , polymer chemistry , composite material , crystallography , ion , chemistry , crystal structure , electrode , organic chemistry , medicine , alternative medicine , pathology , engineering
Abstract 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.