Click-Chemistry-Enabled Functionalization of Cellulose Nanocrystals with Single-Stranded DNA for Directed Assembly.

Autor: Bukharina D; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States., Cauffiel K; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States., Killingsworth LM; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States., Brackenridge JA; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States., Poliukhova V; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States., Kim M; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.; Department of Chemical Engineering, Dankook University, Yongin 16890, Republic of Korea., Brower J; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85281, United States.; Biodesign Center for Molecular Design and Biomimetics, Arizona State University, Tempe, Arizona 85251, United States., Bernal-Chanchavac J; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85281, United States.; Biodesign Center for Molecular Design and Biomimetics, Arizona State University, Tempe, Arizona 85251, United States., Stephanopoulos N; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85281, United States.; Biodesign Center for Molecular Design and Biomimetics, Arizona State University, Tempe, Arizona 85251, United States., Tsukruk VV; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.
Jazyk: angličtina
Zdroj: ACS biomaterials science & engineering [ACS Biomater Sci Eng] 2024 Oct 14; Vol. 10 (10), pp. 6155-6166. Date of Electronic Publication: 2024 Sep 11.
DOI: 10.1021/acsbiomaterials.4c01518
Abstrakt: Controlling the self-assembly of cellulose nanocrystals (CNCs) requires precise control over their surface chemistry for the directed assembly of advanced nanocomposites with tailored mechanical, thermal, and optical properties. In this work, in contrast to traditional chemistries, we conducted highly selective click-chemistry functionalization of cellulose nanocrystals with complementary DNA strands via a three-step hybridization-guided process. By grafting terminally functionalized oligonucleotides through copper-free click chemistry, we successfully facilitated the assembly of brushlike DNA-modified CNCs into bundled nanostructures with distinct chiral optical dichroism in thin films. The complexation behavior of grafted DNA chains during the evaporation-driven formation of ultrathin films demonstrates the potential for mediating chiral interactions between the DNA-branched nanocrystals and their assembly into chiral bundles. Furthermore, we discuss the future directions and challenges that include new avenues for the development of functional, responsive, and bioderived nanostructures capable of dynamic reconfiguration via selective complexation, further surface modification strategies, mitigating diverse CNC aggregation, and exploring environmental conditions for the CNC-DNA assembly.
Databáze: MEDLINE