@article{01a61989860540f2bfd2d176e294757e,
title = "3D-Printed Hydrogel Composites for Predictive Temporal (4D) Cellular Organizations and Patterned Biogenic Mineralization",
abstract = "Materials chemistries for hydrogel scaffolds that are capable of programming temporal (4D) attributes of cellular decision-making in supported 3D microcultures are described. The scaffolds are fabricated using direct-ink writing (DIW)—a 3D-printing technique using extrusion to pattern scaffolds at biologically relevant diameters (≤ 100 µm). Herein, DIW is exploited to variously incorporate a rheological nanoclay, Laponite XLG (LAP), into 2-hydroxyethyl methacrylate (HEMA)-based hydrogels—printing the LAP–HEMA (LH) composites as functional modifiers within otherwise unmodified 2D and 3D HEMA microstructures. The nanoclay-modified domains, when tested as thin films, require no activating (e.g., protein) treatments to promote robust growth compliances that direct the spatial attachment of fibroblast (3T3) and preosteoblast (E1) cells, fostering for the latter a capacity to direct long-term osteodifferentiation. Cell-to-gel interfacial morphologies and cellular motility are analyzed with spatial light interference microscopy (SLIM). Through combination of HEMA and LH gels, high-resolution DIW of a nanocomposite ink (UniH) that translates organizationally dynamic attributes seen with 2D gels into dentition-mimetic 3D scaffolds is demonstrated. These analyses confirm that the underlying materials chemistry and geometry of hydrogel nanocomposites are capable of directing cellular attachment and temporal development within 3D microcultures—a useful material system for the 4D patterning of hydrogel scaffolds.",
keywords = "3D printing, biomineralization, cellular biocompliance, direct ink write 4D printing, hydrogel nanocomposites",
author = "McCracken, {Joselle M.} and Rauzan, {Brittany M.} and Kjellman, {Jacob C.E.} and Kandel, {Mikhail E.} and Liu, {Yu Hao} and Adina Badea and Miller, {Lou Ann} and Rogers, {Simon A.} and Gabriel Popescu and Nuzzo, {Ralph G.}",
note = "Funding Information: The authors graciously acknowledge Dr. Debbie Cassout for her expertise, assistance, and advice to prepare microsectioned samples from 3D nanocomposite scaffolds. The authors also thank Dr. Elizabeth A. Driskell for her knowledge and explanation of different cell behaviors in natural organ systems and Dr. David J. Wetzel for his SEM imaging of cell-loaded bead arrays. The authors thank Dr. Kathleen A. Walsh for her AFM scan measurements and image postprocessing. The authors thank Dr. Leilei Yin for his assistance with micro-CT imaging. The authors also thank Prof. Jennifer A. Lewis for her foundational contributions regarding the principles underlying DIW and Dr. A. Sydney Gladman for her instrumental advice for setting up the DIW system. This material was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DE-FG02-07ER46471 through the Frederick Seitz Materials Research Laboratory at the University of Illinois at Urbana–Champaign. J.M.M. developed the principal objectives of the research, conceived of, organized, and implemented the experimental plan, constructed the figures, and wrote the manuscript. J.M.M. performed all cellular experiments, data analysis, and was the lead researcher on all 3D-printing protocols. B.M.R. conceived of and implemented the rheological modifier to enable small diameter printing and performed rheological and XRD measurements. J.C.E.K., with assistance from J.M.M., developed the UniH ink composition. M.E.K. conducted SLIM experiments. Y.H.L. designed the original microloop scaffold array pattern. A.B. contributed parallel procedural knowledge for LAP-related protocols. L.A.M. prepared samples and collected images from TEM. S.A.R. was a principal resource for rheological measurements and analysis. G.P. was a principal resource for SLIM analyses. R.G.N. developed and organized the central guiding principles and foundational approaches for the project overall and the manuscript specifically. All authors contributed to discussion and evaluation of results. Publisher Copyright: {\textcopyright} 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",
year = "2019",
month = jan,
day = "10",
doi = "10.1002/adhm.201800788",
language = "English (US)",
volume = "8",
journal = "Advanced healthcare materials",
issn = "2192-2640",
publisher = "John Wiley & Sons, Ltd.",
number = "1",
}