Combination of Surface Charge and Size Controls the Cellular Uptake of Functionalized Graphene Sheets

Tu, Zhaoxu; Achazi, Katharina; Schulz, Andrea; Mülhaupt, Rolf; Thierbach, Steffen; Rühl, E.; Adeli, Mohsen; Haag, Rainer

doi:10.1002/adfm.201701837

Cited by 105 publications

(119 citation statements)

References 59 publications

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“…[35,36] Furthermore, sharp edges, basal plane, and mobility of GO flakes have been reported to modulate the antibacterial role of GO. [38] RNA possesses the capability to encode structural and functional informations, facilitating potential strategies for therapy and diagnostics. [35] Cellular uptake of GO can also be enhanced by employing nanometric GO.…”

Section: Lateral Sizementioning

confidence: 99%

“…In contrast, cellular uptake efficiency of the counterpart material with a negative surface charge is strongly modulated by lateral size. [38] RNA possesses the capability to encode structural and functional informations, facilitating potential strategies for therapy and diagnostics. [39] In this context, GO could be utilized as a nanocarrier platform for small-interfering RNA (siRNA) delivery with interest also for future theranostic applications.…”

Section: Lateral Sizementioning

confidence: 99%

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Graphene Oxide as an Optical Biosensing Platform: A Progress Report

2018

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IntroductionAs a 2D material, graphene oxide (GO) is a lattice-like nanostructure of hexagonal carbon rings disrupted by oxygen-containing moieties. In 2012, we discussed the outstanding physicochemical properties offered by GO and how these features can be exploited in unprecedented optical biosensing systems. [1] In fact, GO can be processed in suspension, easily complexed with biomolecules, and offers a universal highly efficient long-range photoluminescence quenching agent-among other functional properties. Furthermore, we highlighted that GO photoluminescences with energy transfer donor/acceptor molecules exposed A few years ago, crucial graphene oxide (GO) features such as the carbon/oxygen ratio, number of layers, and lateral size were scarcely investigated and, thus, their impact on the overall optical biosensing performance was almost unknown. Nowadays valuable insights about these features are well documented in the literature, whereas others remain controversial. Moreover, most of the biosensing systems based on GO were amenable to operating as colloidal suspensions. Currently, the literature reports conceptually new approaches obviating the need of GO colloidal suspensions, enabling the integration of GO onto a solid phase and leading to their application in new biosensing devices. Furthermore, most GO-based biosensing devices exploit photoluminescent signals. However, further progress is also achieved in powerful label-free optical techniques exploiting GO in biosensing, particularly using optical fibers, surface plasmon resonance, and surface enhanced Raman scattering. Herein, a critical overview on these topics is offered, highlighting the key role of the physicochemical properties of GO. New challenges and opportunities in this exciting field are also highlighted.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201805043.in a planar surface. [1] However, GO properties can be tailored according to its oxidation degree, lateral size, and number of layers, which was something little explored 6 years ago, and thus their impact on the overall biosensing performance was almost unknown. In addition, most of the biosensing systems based on GO were amenable to working as colloidal suspensions. Though, recent literature reports conceptually new approaches obviating the need of colloidal suspensions, which facilitates integration of GO-based biosensors into the solid phase and allows for their applications in new devices. Furthermore, the majority of the GO-based optical biosensing techniques rely on photoluminescent signals. However, further progress has also been achieved in powerful label-free optical techniques exploiting GO in biosensing. Here, we introduce a progress report on this exciting topic, underscoring challenges and opportunities in (bio)sensing accordingly. Number of LayersGO aqueous suspensions are highly stable in the form of mono layers. However, GO multilayer films can be built via

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Section: Lateral Sizementioning

confidence: 99%

Section: Lateral Sizementioning

confidence: 99%

Graphene Oxide as an Optical Biosensing Platform: A Progress Report

2018

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“…However, their size,f unctionality,a nd dispersability in aqueous solutions are factors that have to be optimized before proceeding for any biomedical study.O ur previous work showed that hyperbranched polyglycerol (hPG) coverage could effectively improve the biocompatibility of graphene sheets,w hich provide anew idea for the biological application of functional graphene sheets. [6] Recently,t he Haag research group has developed am ethod [7] to produce high quality nanographene sheets (nG) with narrow size distribution, in as uitable regime (50 nm-100 nm) for in vivo administration. According to Raman spectra and other characterizations,t he composition and structure of the produced nG is close to CVD samples, [7] leading to outstanding optoelectronic properties.H owever, poor water dispersability and functionality of the nG is ac hallenge and hampers in vivo studies.…”

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confidence: 99%

“…[7] Recently,w ea nd others implemented an ew method for the controlled nondestructive functionalization of carbon based nanomaterials through nitrene [2+ +1] cycloaddition reaction at ambient conditions. [6,8] Controlled post-modification of the triazinefunctionalized graphene sheets by different (macro)molecules resulted in graphene sheets with desired functionalities. [8c,d] In this work, nG was produced and functionalized by triazine,and consequently post-modified with hyperbranched polyglycerolamine (hPG NH 2 )according to previously reported methods.…”

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confidence: 99%

“…[8c,d] In this work, nG was produced and functionalized by triazine,and consequently post-modified with hyperbranched polyglycerolamine (hPG NH 2 )according to previously reported methods. [6] Afterwards,t riphenylphosphonium (TPP; Scheme 1), amitochondrial targeting ligand, [9] was conjugated to the surface of the nanosystem. Polyglycerol-functionalized nG (GP) and their analogues with TPP ligands (GPT) were further functionalized by 2,3-dimethylmaleic anhydride (DA) to obtain graphene derivatives with pH-triggered surface charge conversion (GPD and GPTD,r espectively).…”

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confidence: 99%

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Directed Graphene‐Based Nanoplatforms for Hyperthermia: Overcoming Multiple Drug Resistance

Qiao

Yan

et al. 2018

Angew Chem Int Ed

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Multidrug resistance (MDR), which leads tumors resistance to traditional anticancer drugs, can cause the failure of chemotherapy treatments. Herein, we present a new way to overcome this problem using smart multifunctional graphene-based drug delivery systems which can target subcellular organelles and show synergistic hyperthermia and chemotherapy. Mitochondria-targeting ligands are conjugated onto the doxorubicin-loaded, polyglycerol-covered nanographene sheets to actively accumulate them inside the mitochondria after charge-mediated cellular internalization. Upon near-infrared (NIR) irradiation, adenosine triphosphate (ATP) synthesis and mitochondrial function were inhibited and doxorubicin released into the cellular interior. The hyperthermia-accelerated drug release led to a highly selective anticancer efficiency, confirmed by in vitro and in vivo experiments.

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Surface Functionalization of Graphene‐Based Materials: Biological Behavior, Toxicology, and Safe‐By‐Design Aspects

et al. 2021

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drug delivery, bioimaging probes, antibacterial agents, and tissue engineering. [2] The advantage of GBMs over other nanomaterials (NMs) in biomedical application is their high specific surface area which allows high density functionalization and drug loading on both sides of the planar structure. [3] The π-conjugated system offers high capacity for GBMs to interact with various organic compounds with aromatic structures through π-π stacking during fabrication of graphene composites or for immobilization of biomolecules such as nucleic acids, peptides, antibodies, or other therapeutic substances. [4] The same properties may also raise concerns regarding the potential risk that GBMs may cause to human health through binding of key signaling molecules for example. GBMs may interact with biomolecules, changing the structure of protein or DNA or induce oxidative damage, and so on. [5] Therefore, prior to the widespread use of GBMs, it is imperative to evaluate their potential risk to environmental and human health and to establish a proactive approach for the safe design of these materials.In a recent review article, Fadeel et al. comprehensively examined the literature on the effects of GBMs on human health and the environment and gave an overview of the state-of-the-art of safety assessment of GBMs, highlighting the importance of The increasing exploitation of graphene-based materials (GBMs) is driven by their unique properties and structures, which ignite the imagination of scientists and engineers. At the same time, the very properties that make them so useful for applications lead to growing concerns regarding their potential impacts on human health and the environment. Since GBMs are inert to reaction, various attempts of surface functionalization are made to make them reactive. Herein, surface functionalization of GBMs, including those intentionally designed for specific applications, as well as those unintentionally acquired (e.g., protein corona formation) from the environment and biota, are reviewed through the lenses of nanotoxicity and design of safe materials (safe-by-design). Uptake and toxicity of functionalized GBMs and the underlying mechanisms are discussed and linked with the surface functionalization. Computational tools that can predict the interaction of GBMs behavior with their toxicity are discussed. A concise framing of current knowledge and key features of GBMs to be controlled for safe and sustainable applications are provided for the community.

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Combination of Surface Charge and Size Controls the Cellular Uptake of Functionalized Graphene Sheets

Cited by 105 publications

References 59 publications

Graphene Oxide as an Optical Biosensing Platform: A Progress Report

Graphene Oxide as an Optical Biosensing Platform: A Progress Report

Directed Graphene‐Based Nanoplatforms for Hyperthermia: Overcoming Multiple Drug Resistance

Surface Functionalization of Graphene‐Based Materials: Biological Behavior, Toxicology, and Safe‐By‐Design Aspects

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