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      Bio-transformation of Graphene Oxide in Lung Fluids Significantly Enhances Its Photothermal Efficacy

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          Abstract

          Rationale: Graphene oxide (GO) has shown great promises in biomedical applications, such as drug delivery and thermotherapeutics, owing to its extraordinary physicochemical properties. Nonetheless, current biomedical applications of GO materials are premised on the basis of predesigned functions, and little consideration has been given to the influence of bio-transformation in the physiological environment on the physicochemical properties and predesigned functionalities of these materials. Hence, it is crucial to uncover the possible influence on GO's physicochemical properties and predesigned functionalities for better applications.

          Methods: Bio-transformed GOs were characterized by X-ray diffraction (XRD) spectra, Raman spectra, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared transmission (FT-IR) spectra. The morphologies of various GO materials were assessed via transmission electron microscopy (TEM), scanning electron microscopy (SEM) and atomic force microscopy (AFM) images. The photothermal (PTT) performance of different GO materials in vitro and in vivo were measured using 808 nm laser at a power density of 2 W/cm 2. The PTT efficacy was determined using transplanted 4T1 cells-derived breast tumors in mice.

          Results: Bio-transformation of GO in the lung (a main target organ for GO to localize in vivo) can induce dramatic changes to its physicochemical properties and morphology, and consequently, its performances in biomedical applications. Specifically, GO underwent significant reduction in two simulated lung fluids, Gamble's solution and artificial lysosomal fluid (ALF), as evidenced by the increase of C/O ratio (the ratio of C content to O content) relative to pristine GO. Bio-transformation also altered GO's morphology, characterized by sheet folding and wrinkle formation. Intriguingly, bio-transformation elevated the PTT performance of GO in vitro, and this elevation further facilitated PTT-based tumor-killing efficacy in tumor cells in vitro and in a mouse model with transplanted tumors. Bio-transformation also compromised the interaction between drug with GO, leading to reduced drug adsorption, as tested using doxorubicin (DOX).

          Conclusions: Transformation in Gamble's solution and ALF resulted in varied degrees of improved performances of GO, due to the differential effects on GO's physicochemical properties. Our findings unveiled an overlooked impact of GO bio-transformation, and unearthed a favorable trait of GO materials in thermotherapeutics and drug delivery in the lung microenvironment.

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          Most cited references37

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          Supramolecular chemistry on water-soluble carbon nanotubes for drug loading and delivery.

          We show that large surface areas exist for supramolecular chemistry on single-walled carbon nanotubes (SWNTs) prefunctionalized noncovalently or covalently by common surfactant or acid-oxidation routes. Water-soluble SWNTs with poly(ethylene glycol) (PEG) functionalization via these routes allow for surprisingly high degrees of pi-stacking of aromatic molecules, including a cancer drug (doxorubicin) with ultrahigh loading capacity, a widely used fluorescence molecule (fluorescein), and combinations of molecules. Binding of molecules to nanotubes and their release can be controlled by varying the pH. The strength of pi-stacking of aromatic molecules is dependent on nanotube diameter, leading to a method for controlling the release rate of molecules from SWNTs by using nanotube materials with suitable diameter. This work introduces the concept of "functionalization partitioning" of SWNTs, i.e., imparting multiple chemical species, such as PEG, drugs, and fluorescent tags, with different functionalities onto the surface of the same nanotube. Such chemical partitioning should open up new opportunities in chemical, biological, and medical applications of novel nanomaterials.
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            Nano-Graphene Oxide for Cellular Imaging and Drug Delivery

            Two-dimensional graphene offers interesting electronic, thermal and mechanical properties that are currently explored for advanced electronics, membranes and composites. Here we synthesize and explore the biological application of nano-graphene oxide NGO, single-layer graphene oxide sheets down to a few nanometers in lateral width. We develop functionalization chemistry to impart solubility and compatibility of NGO in biological environments. We obtain size separated pegylated NGO sheets that are soluble in buffers and serum without agglomeration. The NGO sheets are found to be photoluminescent in the visible and infrared regions. The intrinsic photoluminescence of NGO is used for live cell imaging in the near-infrared with little background. We found that simple physisorption via pi-stacking can be used for loading doxorubicin, a widely used cancer drug onto NGO functionalized with antibody for selective cancer cell killing in vitro. Owing to the small size, intrinsic optical properties, large specific surface area,low cost, and useful non-covalent interactions with aromatic drug molecules, NGO is a promising new material for biological and medical applications.
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              High-Efficiency Loading and Controlled Release of Doxorubicin Hydrochloride on Graphene Oxide

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                Author and article information

                Journal
                Nanotheranostics
                Nanotheranostics
                ntno
                Nanotheranostics
                Ivyspring International Publisher (Sydney )
                2206-7418
                2018
                20 May 2018
                : 2
                : 3
                : 222-232
                Affiliations
                [1 ]Key Laboratory of High Magnetic Field and Ion Beam Physical Biology, Hefei Institutes of Physical Science, Chinese Academy of Sciences; Anhui Province Key Laboratory of Environmental Toxicology and Pollution Control Technology, Hefei, Anhui 230031, China.
                [2 ]State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
                [3 ]College of Environmental Science and Engineering, Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Nankai University, Tianjin 300350, China.
                [4 ]University of Chinese Academy of Sciences, Beijing 100049, China.
                [5 ]Institute for Medical Engineering and Science, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
                Author notes
                ✉ Corresponding authors: E-mail: chenwei@ 123456nankai.edu.cn and sjliu@ 123456rcees.ac.cn

                #These authors contributed equally to this work.

                Competing Interests: The authors have declared that no competing interest exists.

                Article
                ntnov02p0222
                10.7150/ntno.25719
                5984285
                29868347
                bd0ff771-dbca-4eea-bab5-4bfba0970dd1
                © Ivyspring International Publisher

                This is an open access article distributed under the terms of the Creative Commons Attribution (CC BY-NC) license ( https://creativecommons.org/licenses/by-nc/4.0/). See http://ivyspring.com/terms for full terms and conditions.

                History
                : 1 March 2018
                : 7 May 2018
                Categories
                Research Paper

                graphene oxide,bio-transformation,simulated lung fluids,physicochemical properties,functionality

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