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

IF 5.4 2区医学 Q2 MATERIALS SCIENCE, BIOMATERIALS ACS Biomaterials Science & Engineering Pub Date : 2024-09-11 DOI:10.1021/acsbiomaterials.4c01518

Daria Bukharina, Katherine Cauffiel, Laura Mae Killingsworth, Justin A. Brackenridge, Valeriia Poliukhova, Minkyu Kim, Justin Brower, Julio Bernal-Chanchavac, Nicholas Stephanopoulos, Vladimir V. Tsukruk

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Abstract

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.

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用单链 DNA 对纤维素纳米晶体进行单击化学功能化，实现定向组装

要控制纤维素纳米晶体（CNC）的自组装，就必须精确控制其表面化学成分，以便定向组装出具有定制机械、热和光学特性的先进纳米复合材料。在这项工作中，与传统的化学方法不同，我们通过三步杂交引导过程，用互补 DNA 链对纤维素纳米晶体进行了高选择性的点击化学功能化。通过无铜点击化学将末端功能化的寡核苷酸接枝，我们成功地将DNA修饰的刷状纳米纤维素组装成具有独特手性光学二色性的薄膜束状纳米结构。在蒸发驱动的超薄薄膜形成过程中，接枝 DNA 链的复合行为证明了 DNA 支化纳米晶体之间的手性相互作用及其组装成手性束的潜力。此外，我们还讨论了未来的发展方向和挑战，包括通过选择性复合、进一步的表面改性策略、减轻不同 CNC 的聚集以及探索 CNC-DNA 组装的环境条件，开发能够动态重构的功能性、响应性和生物源纳米结构的新途径。

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来源期刊

ACS Biomaterials Science & Engineering Materials Science-Biomaterials

CiteScore

10.30

自引率

3.40%

发文量

413

期刊介绍： ACS Biomaterials Science & Engineering is the leading journal in the field of biomaterials, serving as an international forum for publishing cutting-edge research and innovative ideas on a broad range of topics: Applications and Health – implantable tissues and devices, prosthesis, health risks, toxicology Bio-interactions and Bio-compatibility – material-biology interactions, chemical/morphological/structural communication, mechanobiology, signaling and biological responses, immuno-engineering, calcification, coatings, corrosion and degradation of biomaterials and devices, biophysical regulation of cell functions Characterization, Synthesis, and Modification – new biomaterials, bioinspired and biomimetic approaches to biomaterials, exploiting structural hierarchy and architectural control, combinatorial strategies for biomaterials discovery, genetic biomaterials design, synthetic biology, new composite systems, bionics, polymer synthesis Controlled Release and Delivery Systems – biomaterial-based drug and gene delivery, bio-responsive delivery of regulatory molecules, pharmaceutical engineering Healthcare Advances – clinical translation, regulatory issues, patient safety, emerging trends Imaging and Diagnostics – imaging agents and probes, theranostics, biosensors, monitoring Manufacturing and Technology – 3D printing, inks, organ-on-a-chip, bioreactor/perfusion systems, microdevices, BioMEMS, optics and electronics interfaces with biomaterials, systems integration Modeling and Informatics Tools – scaling methods to guide biomaterial design, predictive algorithms for structure-function, biomechanics, integrating bioinformatics with biomaterials discovery, metabolomics in the context of biomaterials Tissue Engineering and Regenerative Medicine – basic and applied studies, cell therapies, scaffolds, vascularization, bioartificial organs, transplantation and functionality, cellular agriculture