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      Disordered protein-graphene oxide co-assembly and supramolecular biofabrication of functional fluidic devices

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          Abstract

          Supramolecular chemistry offers an exciting opportunity to assemble materials with molecular precision. However, there remains an unmet need to turn molecular self-assembly into functional materials and devices. Harnessing the inherent properties of both disordered proteins and graphene oxide (GO), we report a disordered protein-GO co-assembling system that through a diffusion-reaction process and disorder-to-order transitions generates hierarchically organized materials that exhibit high stability and access to non-equilibrium on demand. We use experimental approaches and molecular dynamics simulations to describe the underlying molecular mechanism of formation and establish key rules for its design and regulation. Through rapid prototyping techniques, we demonstrate the system’s capacity to be controlled with spatio-temporal precision into well-defined capillary-like fluidic microstructures with a high level of biocompatibility and, importantly, the capacity to withstand flow. Our study presents an innovative approach to transform rational supramolecular design into functional engineering with potential widespread use in microfluidic systems and organ-on-a-chip platforms.

          Abstract

          Self-organising systems have huge potential in device design and fabrication; however, demonstrations of this are limited. Here, the authors report on a combination of disordered proteins and graphene oxide which allows spatio-temporal patterning and demonstrate the fabrication of microfluidic devices.

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          Graphene oxide sheets at interfaces.

          Graphite oxide sheet, now called graphene oxide (GO), is the product of chemical exfoliation of graphite and has been known for more than a century. GO has been largely viewed as hydrophilic, presumably due to its excellent colloidal stability in water. Here we report that GO is an amphiphile with hydrophilic edges and a more hydrophobic basal plane. GO can act like a surfactant, as measured by its ability to adsorb on interfaces and lower the surface or interfacial tension. Since the degree of ionization of the edge -COOH groups is affected by pH, GO's amphiphilicity can be tuned by pH. In addition, size-dependent amphiphilicity of GO sheets is observed. Since each GO sheet is a single molecule as well as a colloidal particle, the molecule-colloid duality makes it behave like both a molecular and a colloidal surfactant. For example, GO is capable of creating highly stable Pickering emulsions of organic solvents like solid particles. It can also act as a molecular dispersing agent to process insoluble materials such as graphite and carbon nanotubes in water. The ease of its conversion to chemically modified graphene could enable new opportunities in solution processing of functional materials.
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            Transient assembly of active materials fueled by a chemical reaction.

            Fuel-driven self-assembly of actin filaments and microtubules is a key component of cellular organization. Continuous energy supply maintains these transient biomolecular assemblies far from thermodynamic equilibrium, unlike typical synthetic systems that spontaneously assemble at thermodynamic equilibrium. Here, we report the transient self-assembly of synthetic molecules into active materials, driven by the consumption of a chemical fuel. In these materials, reaction rates and fuel levels, instead of equilibrium composition, determine properties such as lifetime, stiffness, and self-regeneration capability. Fibers exhibit strongly nonlinear behavior including stochastic collapse and simultaneous growth and shrinkage, reminiscent of microtubule dynamics.
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              Toxicity of graphene-family nanoparticles: a general review of the origins and mechanisms

              Due to their unique physicochemical properties, graphene-family nanomaterials (GFNs) are widely used in many fields, especially in biomedical applications. Currently, many studies have investigated the biocompatibility and toxicity of GFNs in vivo and in intro. Generally, GFNs may exert different degrees of toxicity in animals or cell models by following with different administration routes and penetrating through physiological barriers, subsequently being distributed in tissues or located in cells, eventually being excreted out of the bodies. This review collects studies on the toxic effects of GFNs in several organs and cell models. We also point out that various factors determine the toxicity of GFNs including the lateral size, surface structure, functionalization, charge, impurities, aggregations, and corona effect ect. In addition, several typical mechanisms underlying GFN toxicity have been revealed, for instance, physical destruction, oxidative stress, DNA damage, inflammatory response, apoptosis, autophagy, and necrosis. In these mechanisms, (toll-like receptors-) TLR-, transforming growth factor β- (TGF-β-) and tumor necrosis factor-alpha (TNF-α) dependent-pathways are involved in the signalling pathway network, and oxidative stress plays a crucial role in these pathways. In this review, we summarize the available information on regulating factors and the mechanisms of GFNs toxicity, and propose some challenges and suggestions for further investigations of GFNs, with the aim of completing the toxicology mechanisms, and providing suggestions to improve the biological safety of GFNs and facilitate their wide application.
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                Author and article information

                Contributors
                a.mata@nottingham.ac.uk
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                4 March 2020
                4 March 2020
                2020
                : 11
                : 1182
                Affiliations
                [1 ]ISNI 0000 0001 2171 1133, GRID grid.4868.2, Institute of Bioengineering, , Queen Mary University of London, ; London, E1 4NS UK
                [2 ]ISNI 0000 0001 2171 1133, GRID grid.4868.2, School of Engineering and Materials Science, , Queen Mary University of London, ; London, E1 4NS UK
                [3 ]ISNI 0000 0004 1936 8868, GRID grid.4563.4, School of Pharmacy, , University of Nottingham, ; NG7 2RD Nottingham, UK
                [4 ]ISNI 0000 0004 1936 8868, GRID grid.4563.4, Department of Chemical and Environmental Engineering, , University of Nottingham, ; NG7 2RD Nottingham, UK
                [5 ]ISNI 0000 0004 1936 8868, GRID grid.4563.4, Biodiscovery Institute, , University of Nottingham, ; NG7 2RD Nottingham, UK
                [6 ]ISNI 0000 0004 1937 0351, GRID grid.11696.39, Laboratory of Bio-inspired, Bionic, Nano, Meta Materials & Mechanics, , Università di Trento, ; via Mesiano, 77, I-38123 Trento, Italy
                [7 ]ISNI 0000 0004 1757 3729, GRID grid.5395.a, Research Center‘E. Piaggio’ & Dipartimento di Ingegneria dell’Informazione, , University of Pisa, Largo Lucio Lazzarino, ; 256126 Pisa, Italy
                [8 ]ISNI 0000 0004 1936 9297, GRID grid.5491.9, Bone and Joint Research Group, Centre for Human Development, Stem Cells and Regeneration, Institute of Developmental Sciences, , University of Southampton, ; Southampton, SO16 6YD UK
                [9 ]ISNI 0000 0004 0517 6080, GRID grid.18999.30, Department of Physical Chemistry, , V. N. Karazin Kharkiv National University, Svobody Sq. 4, ; Kharkiv, 61022 Ukraine
                [10 ]ISNI 0000 0001 0742 9289, GRID grid.417687.b, United Kingdom Atomic Energy Authority, , Culham Science Centre, ; Abingdon, OX14 3DB UK
                [11 ]ISNI 0000 0004 1936 8403, GRID grid.9909.9, The Astbury Biostructure Laboratory, Astbury Centre for Structural Molecular Biology, Faculty of Biological Sciences, , University of Leeds, ; Leeds, UK
                [12 ]ISNI 0000 0004 0376 4727, GRID grid.7273.1, Systems Analytics Research Institute, Department of Mathematics, , Aston University, ; Birmingham, B4 7ET UK
                [13 ]ISNI 0000 0001 2286 5329, GRID grid.5239.d, BIOFORGE Group, , University of Valladolid, CIBER-BBN, ; 47011 Valladolid, Spain
                [14 ]KET Labs, Edoardo Amaldi Foundation, Via del Politecnico snc, 00133 Rome, Italy
                [15 ]ISNI 0000 0004 1936 9297, GRID grid.5491.9, Present Address: Mathematical Sciences, , University of Southampton, ; Southampton SO17 1BJ, UK
                [16 ]ISNI 0000 0004 1937 0351, GRID grid.11696.39, Present Address: C3A - Center Agriculture Food Environment, , University of Trento/Fondazione Edmund Mach, Via Edmund Mach, 1 - 38010, ; San Michele allʼAdige (TN), Italy
                Author information
                http://orcid.org/0000-0002-3955-6474
                http://orcid.org/0000-0003-0392-9205
                http://orcid.org/0000-0002-2346-0507
                http://orcid.org/0000-0002-7348-9578
                http://orcid.org/0000-0002-1648-0833
                http://orcid.org/0000-0003-0785-9582
                http://orcid.org/0000-0002-4254-8854
                http://orcid.org/0000-0003-0773-2100
                http://orcid.org/0000-0001-9005-9919
                http://orcid.org/0000-0001-5995-6726
                http://orcid.org/0000-0002-9414-9994
                http://orcid.org/0000-0002-5470-1844
                http://orcid.org/0000-0003-2136-2396
                Article
                14716
                10.1038/s41467-020-14716-z
                7055247
                32132534
                f423db81-d83a-4c9f-a45b-3c9bc239de34
                © The Author(s) 2020

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 13 November 2019
                : 24 January 2020
                Funding
                Funded by: ERC Starting Grant (STROFUNSCAFF) The Marie Curie Integration Grant FP7-PEOPLE-2013-CIG (BIOMORPH) UK Regenerative Medicine Platform (UKRMP2)
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                © The Author(s) 2020

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                biomaterials - proteins,graphene,mechanical and structural properties and devices

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