Supramolecular hydration structure of graphene-based hydrogels: density functional theory, green chemistry and interface application

chemistry Medicinal and pharmaceutical chemistry Nano- and molecular-scale electronics Nano-biomaterials and bioscience Nanomagnetics Nanomaterials, thin films and nanointerfaces Nanomedicine Nanometrology and nanomechanics Nano-optics Nanopatterning, self-assembly and nanofabrication Nanostructures for energy and sensing applications Natural products chemistry Organo main group chemistry Other nanotechnology (unclassified) Other organic chemistry (unclassified) Photochemistry and photovoltaics Physical organic chemistry Supramolecular chemistry Natural hydration shells are discovered to play an essential role in the structure and function of biomolecules (deoxyribonucleic acid, protein and phospholipid membrane). Hydration layers are also important to the structure and property of artificial graphene-based materials. Our recent researches prove that graphene-based hydrogels are supramolecular hydration structures that preserve graphene nanosheets from irreversible stacking via van der Waals forces and π-π interactions. In this manuscript, density functional theory (DFT) and high performance computing (HPC) are used for modeling and calculating van der Waals force between graphene nanosheets in water-intercalated AB bilayer graphene structures. A layer of water molecules significantly decreases the intersheet van der Waals force. Experimentally, a novel hydrogel of graphene oxide – silica gel – zinc hydroxide (GO-SG-ZH) is synthesized to demonstrate the advantages of hydrated hydrogel structure in comparison with dry powder structure. The synthesis of graphene-based hydrogels is a green chemistry approach to attain extraordinary properties of graphene-based nanostructures. Hydration forces in the hydrogel prevent van der Waals stacking and graphene agglomeration. Analytical characterizations exhibited moisture contents, three-dimensional structures, elemental compositions, functional groups and antibacterial activities. Non-stacking state of graphene-based nanosheets in GO-SG-ZH hydrogel was suitable for direct brush painting on polymer substrates, typically polylactide films. GO-SG-ZH coating on polylactide film was antibacterial and stable in aqueous food simulants for one month. In general, supramolecular graphene-based hydrogels are bioinspired hydration structures to advance nanoscale properties and nanotechnology applications.

graphene-based hydrogel; bioinspired hydration; supramolecular structure; density functional theory; antibacterial coating | Format: DOCX | Size: 4.2 MB | Download | When a peer-reviewed version of this preprint is available, this information will be updated in the information box above. If no peer-reviewed version is available, please cite this preprint using the following information: Le, H. N.; Nguyen, D. K.; Dang, M. T.; Nguyen, H. T.; Dao, T. B. T.; Nguyen, T. D.; Ha Thuc, C. N.; Le, V. H. Beilstein Arch. 2025, 20254. doi:10.3762/bxiv.2025.4.v1 Citation data can be downloaded as file using the "Download" button or used for copy/paste from the text window below. Citation data in RIS format can be imported by all major citation management software, including EndNote, ProCite, RefWorks, and Zotero. © 2025 Le et al.; licensee Beilstein-Institut. This is an open access work licensed under the terms of the Beilstein-Institut Open Access License Agreement (https://www.beilstein-archives.org/xiv/terms), which is identical to the Creative Commons Attribution 4.0 International License (https://creativecommons.org/licenses/by/4.0). The reuse of material under this license requires that the author(s), source and license are credited. Third-party material in this work could be subject to other licenses (typically indicated in the credit line), and in this case, users are required to obtain permission from the license holder to reuse the material.