The family of spinel compounds is a large and important class of multifunctional materials of general formulation AB2X4 with many advanced applications in energy and optoelectronic areas such as fuel ...cells, batteries, catalysis, photonics, spintronics, and thermoelectricity. In this work, it is demonstrated that the ternary ultrawide-band-gap (∼5 eV) spinel zinc gallate (ZnGa2O4) arguably is the native p-type ternary oxide semiconductor with the largest E g value (in comparison with the recently discovered binary p-type monoclinic β-Ga2O3 oxide). For nominally undoped ZnGa2O4 the high-temperature Hall effect hole concentration was determined to be as large as p = 2 × 1015 cm–3, while hole mobilities were found to be μh = 7–10 cm2/(V s) (in the 680–850 K temperature range). An acceptor-like small Fermi level was further corroborated by X-ray spectroscopy and by density functional theory calculations. Our findings, as an important step toward p-type doping, opens up further perspectives for ultrawide-band-gap bipolar spinel electronics and further promotes ultrawide-band-gap ternary oxides such as ZnGa2O4 to the forefront of the quest of the next generation of semiconductor materials for more efficient energy optoelectronics and power electronics.
The facile and controlled fabrication of homogeneously grafted cationic polymers on carbon nanotubes (CNTs) remains poorly investigated, which further hinders the understanding of interactions ...between functionalized CNTs with different nucleic acids and the rational design of appropriate gene delivery vehicles. Herein, we describe the controlled grafting of cationic poly(2-dimethylaminoethylmethacrylate) brushes on CNTs via surface-initiated atom transfer radical polymerization integrated with mussel-inspired polydopamine chemistry. The binding of nucleic acids with different brush-CNT hybrids discloses the highly architectural-dependent behavior with dense short brush-coated CNTs displaying the highest binding among all the other hybrids, namely, dense long, sparse long, and sparse short brush-coated CNTs. Additionally, different chemistries of the brush coatings were shown to influence the biocompatibility, cellular uptake, and silencing efficiency in vitro. This platform provides great flexibility for the design of polymer brush-CNT hybrids with precise control over their structure–activity relationship for the rational design of nucleic acid delivery systems.
The unique properties of two-dimensional (2D) nanomaterials make them highly attractive for a wide range of applications. As a consequence, several top-down and bottom up approaches are being ...explored to isolate or synthesize single-layers of 2D materials in a reliable manner. Here we report on the synthesis of individual layers of several 2D van der Waals solids, namely CeI3, CeCl3, TbCl3 and ZnI2 by template-assisted growth using carbon nanotubes as directing agents, thus proving the versatility of this approach. Once confined, the metal halides can adopt different structures including single-layered metal halide nanotubes, which formation is greatly enhanced by increasing the temperature of synthesis. This opens up a new strategy for the isolation of individual layers of a wide variety of metal halides, a family of 2D materials that has been barely explored.
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The electronic and optical properties of two-dimensional layered materials allow the miniaturization of nanoelectronic and optoelectronic devices in a competitive manner. Even larger opportunities ...arise when two or more layers of different materials are combined. Here, we report on an ultrafast energy efficient strategy, using laser irradiation, which allows bulk synthesis of crystalline single-layered lead iodide in the cavities of carbon nanotubes by forming cylindrical van der Waals heterostructures. In contrast to the filling of van der Waals solids into carbon nanotubes by conventional thermal annealing, which favors the formation of inorganic nanowires, the present strategy is highly selective toward the growth of monolayers forming lead iodide nanotubes. The irradiated bulk material bearing the nanotubes reveals a decrease of the resistivity as well as a significant increase in the current flow upon illumination. Both effects are attributed to the presence of single-walled lead iodide nanotubes in the cavities of carbon nanotubes, which dominate the properties of the whole matrix. The present study brings in a simple, ultrafast and energy efficient strategy for the tailored synthesis of rolled-up single-layers of lead iodide (i.e., single-walled PbI2 nanotubes), which we believe could be expanded to other two-dimensional (2D) van der Waals solids. In fact, initial tests with ZnI2 already reveal the formation of single-walled ZnI2 nanotubes, thus proving the versatility of the approach.
Topological insulators (TIs) hold promise for manipulating the magnetization of a ferromagnet (FM) through the spin–orbit torque (SOT) mechanism. However, integrating TIs with conventional FMs often ...leads to significant device-to-device variations and a broad distribution of SOT magnitudes. In this work, we present a scalable approach to grow a full van der Waals FM/TI heterostructure by molecular beam epitaxy, combining the charge-compensated TI (Bi,Sb)2Te3 with 2D FM Fe3GeTe2 (FGT). Harmonic magnetotransport measurements reveal that the SOT efficiency exhibits a non-monotonic temperature dependence and experiences a substantial enhancement with a reduction of the FGT thickness to 2 monolayers. Our study further demonstrates that the magnetization of ultrathin FGT films can be switched with a current density of J c ∼ 1010 A/m2, with minimal device-to-device variations compared to previous investigations involving traditional FMs.
Abstract Carbon nanotubes (CNTs) are a novel nanocarriers with interesting physical and chemical properties. Here we investigate the ability of amino-functionalized multi-walled carbon nanotubes ...(MWNTs-NH3+ ) to cross the Blood-Brain Barrier (BBB) in vitro using a co-culture BBB model comprising primary porcine brain endothelial cells (PBEC) and primary rat astrocytes, and in vivo following a systemic administration of radiolabelled f -MWNTs. Transmission Electron microscopy (TEM) confirmed that MWNTs-NH3+ crossed the PBEC monolayer via energy-dependent transcytosis. MWNTs-NH3+ were observed within endocytic vesicles and multi-vesicular bodies after 4 and 24 h. A complete crossing of the in vitro BBB model was observed after 48 h, which was further confirmed by the presence of MWNTs-NH3+ within the astrocytes. MWNT-NH3+ that crossed the PBEC layer was quantitatively assessed using radioactive tracers. A maximum transport of 13.0 ± 1.1% after 72 h was achieved using the co-culture model. f -MWNT exhibited significant brain uptake (1.1 ± 0.3% injected dose/g) at 5 min after intravenous injection in mice, after whole body perfusion with heparinized saline. Capillary depletion confirmed presence of f -MWNT in both brain capillaries and parenchyma fractions. These results could pave the way for use of CNTs as nanocarriers for delivery of drugs and biologics to the brain, after systemic administration.
Carbon nanomaterials offer excellent prospects as therapeutic agents, and among them, graphene quantum dots (GQDs) have gained considerable interest thanks to their aqueous solubility and intrinsic ...fluorescence, which enable their possible use in theranostic approaches, if their biocompatibility and favorable pharmacokinetic are confirmed. We prepared ultra-small GQDs using an alternative, reproducible, top-down synthesis starting from graphene oxide with a nearly 100% conversion. The materials were tested to assess their safety, demonstrating good biocompatibility and ability in passing the ultrafiltration barrier using an
in vitro
model. This leads to renal excretion without affecting the kidneys. Moreover, we studied the GQDs
in vivo
biodistribution confirming their efficient renal clearance, and we demonstrated that the internalization mechanism into podocytes is caveolae-mediated. Therefore, considering the reported characteristics, it appears possible to vehiculate compounds to kidneys by means of GQDs, overcoming problems related to lysosomal degradation.
Filled carbon nanotubes (CNTs) find application in a variety of fields that expand from sensors to supercapacitors going through targeted therapies. Bulk filling of CNTs in general results in samples ...that contain a large amount of non-encapsulated material external to the CNTs. The presence of external material can dominate the properties of the resulting hybrids and can also induce side effects when employed in the biomedical field. Unless the encapsulated payloads have a strong interaction with the inner CNT walls, an additional step is required to block the ends of the CNTs thus allowing the selective removal of the non-encapsulated compounds while preserving the inner cargo. Herein we present a fast, easy and versatile approach that allows both filling (NaI, KI, BaI2, GdCl3 and SmCl3) and end-closing of multi-walled CNTs in a single-step, forming “carbon nanocapsules”. Remarkably the encapsulation of GdCl3 and SmCl3 leads to the formation of tubular van der Waals heterostructures. The prepared nanocapsules are efficiently internalized by cells without inducing cytotoxicity, thus presenting a safe tool for the delivery of therapeutic and dianostic agents to cells. The synergies of novel carbon and inorganic hybrid materials can be explored using the present approach.
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Ochrobactrum anthropi DE2010 is a microorganism isolated from Ebro Delta microbial mats and able to resist high doses of chromium(III) due to its capacity to tolerate, absorb and accumulate this ...metal. The effect of this pollutant on O. anthropi DE2010 has been studied assessing changes in viability and biomass, sorption yields and removal efficiencies. Furthermore, and for the first time, its capacity for immobilizing Cr(III) from culture media was tested by a combination of High Angle Annular Dark Field (HAADF) Scanning Transmission Electron Microscopy (STEM) imaging coupled to Energy Dispersive X-ray spectroscopy (EDX).
The results showed that O. anthropi DE2010 was grown optimally at 0–2 mM Cr(III). On the other hand, from 2 to 10 mM Cr(III) microbial plate counts, growth rates, cell viability, and biomass decreased while extracellular polymeric substances (EPS) production increases. Furthermore, this bacterium had a great ability to remove Cr(III) at 10 mM (q = 950.00 mg g−1) immobilizing it mostly in bright polyphosphate inclusions and secondarily on the cellular surface at the EPS level. Based on these results, O. anthropi DE2010 could be considered as a potential agent for bioremediation in Cr(III) contaminated environments.
•Ochobactrum anthropi DE2010 presents a great tolerance and a high removal efficiency value for Cr(III).•Ochrobactrum anthropi DE2010 is capable of immobilizing Cr(III) in EPS and mainly in polyphosphate inclusions.•Ochrobactrum anthropi DE2010 could be considered a useful bioremediation agent of Cr(III) polluted environments.
Functionalization of nanomaterials for precise biomedical function is an emerging trend in nanotechnology. Carbon nanotubes are attractive as multifunctional carrier systems because payload can be ...encapsulated in internal space whilst outer surfaces can be chemically modified. Yet, despite potential as drug delivery systems and radiotracers, such filled-and-functionalized carbon nanotubes have not been previously investigated in vivo. Here we report covalent functionalization of radionuclide-filled single-walled carbon nanotubes and their use as radioprobes. Metal halides, including Na125I, were sealed inside single-walled carbon nanotubes to create high-density radioemitting crystals and then surfaces of these filled-sealed nanotubes were covalently modified with biantennary carbohydrates, improving dispersibility and biocompatibility. Intravenous administration of Na125I-filled glyco-single-walled carbon nanotubes in mice was tracked in vivo using single-photon emission computed tomography. Specific tissue accumulation (here lung) coupled with high in vivo stability prevented leakage of radionuclide to high-affinity organs (thyroid/stomach) or excretion, and resulted in ultrasensitive imaging and delivery of unprecedented radiodose density. Nanoencapsulation of iodide within single-walled carbon nanotubes enabled its biodistribution to be completely redirected from tissue with innate affinity (thyroid) to lung. Surface functionalization of 125I-filled single-walled carbon nanotubes offers versatility towards modulation of biodistribution of these radioemitting crystals in a manner determined by the capsule that delivers them. We envisage that organ-specific therapeutics and diagnostics can be developed on the basis of the nanocapsule model described here.
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