title: Self-assembled hydrogels utilizing polymer-nanoparticle interactions.
abstract: Mouldable hydrogels that flow on applied stress and rapidly self-heal are increasingly utilized as they afford minimally invasive delivery and conformal application. Here we report a new paradigm for the fabrication of self-assembled hydrogels with shear-thinning and self-healing properties employing rationally engineered polymer-nanoparticle (NP) interactions. Biopolymer derivatives are linked together by selective adsorption to NPs. The transient and reversible interactions between biopolymers and NPs enable flow under applied shear stress, followed by rapid self-healing when the stress is relaxed. We develop a physical description of polymer-NP gel formation that is utilized to design biocompatible gels for drug delivery. Owing to the hierarchical structure of the gel, both hydrophilic and hydrophobic drugs can be entrapped and delivered with differential release profiles, both in vitro and in vivo. The work introduces a facile and generalizable class of mouldable hydrogels amenable to a range of biomedical and industrial applications.
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Eric A
authors.initials: EA
authors.lastname: Appel
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Mark W
authors.initials: MW
authors.lastname: Tibbitt
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Matthew J
authors.initials: MJ
authors.lastname: Webber
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Bradley A
authors.initials: BA
authors.lastname: Mattix
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Omid
authors.initials: O
authors.lastname: Veiseh
authors.affiliation: Department of Chemical Engineering, David H. Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Room 76-661, 500 Main Street, Cambridge, Massachusetts 02139, USA.
authors.forename: Robert
authors.initials: R
authors.lastname: Langer
mesh_terms: D000327:Adsorption; D000818:Animals; D001704:Biopolymers / Q000737:chemistry*; D020285:Cryoelectron Microscopy; D016503:Drug Delivery Systems; D020100:Hydrogels / Q000737:chemistry*; D057927:Hydrophobic and Hydrophilic Interactions; D065347:Hypromellose Derivatives / Q000737:chemistry; D009682:Magnetic Resonance Spectroscopy; D008297:Male; D008422:Materials Testing; D051379:Mice; D008810:Mice, Inbred C57BL; D053758:Nanoparticles / Q000737:chemistry*; D011108:Polymers / Q000737:chemistry; D011137:Polystyrenes / Q000737:chemistry; D012212:Rheology
chemical_list: D001704:Biopolymers; D020100:Hydrogels; D011108:Polymers; D011137:Polystyrenes; D065347:Hypromellose Derivatives