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The development of new electrically conductive polymer composites is one of the most important research areas of composite materials science community nowadays. This work is devoted to the preparation and study of electrically conductive polymer composites with a segregated network structure with mixtures of reduced graphene oxide/multi-walled carbon nanotubes (rGO/MWCNTs) in various ratios. At a fixed value of the total mass fraction of rGO/MWCNTs (1 wt.%), the set of samples with different rGO/MWCNTs ratio was obtained and examined via scanning electron microscopy, wide range dielectric spectroscopy and tested under compression. We have shown that the use of graphene oxide in a mixture with MWCNTs makes it possible to significantly improve the uniformity of MWCNTs distribution during the formation of a filler layer on polymer particles, which leads to an increase in the electrical conductivity of the composites in comparison with samples containing only rGO or MWCNTs. It was also shown adding 1 wt.% of rGO to the polymer increases the elastic modulus by 18% compared to the pure polymer. In turn, adding of MWCNTs, there is a drop in the elastic modulus by a quarter. It was found that fillers do not affect the plastic flow initiation stress of the material, which is 21 ± 1 MPa.

Derivatization of 2D materials for bioapplications is at the forefront of nanomaterials research nowadays. Facile synthesis of the biografted 2D derivatives and insight into the conformation of the conjugated biomolecules are two pillars, promoting advances in the field of biosensing, drug delivery and regeneration techniques. This work is devoted to the synthesis and conjugation of carboxylated graphene by aptamers followed by theoretical analysis of their conformation in the immobilized state. Employing the developed method, the hole-matrixed graphene with up to 11.1 at.% reactive carboxyl groups was synthesized and thoroughly examined via core-level spectroscopy and time-resolved methods. The mechanism of the performed carboxylation with conversion of graphene oxide into carboxylated graphene is proposed, unveiling commonly disregarded impact of ether-like components to the fingerprints of the carboxyl groups. We show successful covalent immobilization of the AO-01 aptamer against Hepatitis B protein on the synthesized C-xy graphene and for the first time reveal its conformation both in free and immobilized forms via a combination of density functional theory (DFT) calculations and molecular dynamic (MD) modeling. Taken together, these results advance the application of graphene derivatives grafted with the biomolecules in the field of biosensing.

A structural study of graphene oxide complexes with detonation nanodiamonds (particle size 4–5 nm, positive surface potential) in aqueous suspensions by small-angle neutron scattering is reported. While the pure graphene oxide suspension exhibits a completely planar structure, the grafting of detonation nanodiamond particles results in a slightly curved surface of the graphene oxide flakes. The complexes “graphene oxide–detonation nanodiamonds” washed out from free detonation nanodiamonds show that the effective curvature of the graphene oxide plane is the result of binding of detonation nanodiamonds in the form of planar aggregates.

Here, the synthesis of holey carbonylated (C-ny) graphene derivative and its application for gas sensing is demonstrated. The carbonylation of graphene oxide leads to the 3-fold increase in the concentration of carbonyl groups’ up to 9 at.% with a substantial elimination of other oxygen functionalities. Such a chemical modification is accompanied by the perforation of the graphene layer with the appearance of matrices of nanoscale holes, leading to corrugation of the layer and its sectioning into localized domains of the π-conjugated network. Combined with the predominant presence of carbonyls, granting the specificity in gas molecules adsorption, these features result in the enhanced gas sensing properties of C-ny graphene at room temperature with a selective response to NH3. Opposite chemiresistive response towards ammonia when compared to other analytes, such as ethanol, acetone, CO2, is demonstrated for the C-ny graphene layer both in humid and dry air background. Moreover, a selective discrimination of all of the studied analytes is further approached by employing a vector signal generated by C-ny multielectrode chip. Comparing the experimental results with the calculations performed in framework of density functional theory, we clarify the effect of partial charge transfer caused by water and ammonia adsorption on the chemiresistive response.

In this paper, we propose a facile approach to the management of graphene oxide (GO) chemistry via its synthesis using KMnO4/K2Cr2O7 oxidizing agents at different ratios. Using Fourier Transformed Infrared Spectroscopy, X-ray Photoelectron Spectroscopy, and X-ray Absorption Spectroscopy, we show that the number of basal-plane and edge-located oxygenic groups can be controllably tuned by altering the KMnO4/K2Cr2O7 ratio. The linear two-fold reduction in the number of the hydroxyls and epoxides with the simultaneous three-fold rise in the content of carbonyls and carboxyls is indicated upon the transition from KMnO4 to K2Cr2O7 as a predominant oxidizing agent. The effect of the oxidation mixture’s composition on the structure of the synthesized GOs is also comprehensively studied by means of X-ray diffraction, Raman spectroscopy, transmission electron microscopy, atomic-force microscopy, optical microscopy, and the laser diffraction method. The nanoscale corrugation of the GO platelets with the increase of the K2Cr2O7 content is signified, whereas the 10–100 μm lateral size, lamellar, and defect-free structure is demonstrated for all of the synthesized GOs regardless of the KMnO4/K2Cr2O7 ratio. The proposed method for the synthesis of GO with the desired chemistry opens up new horizons for the development of graphene-based materials with tunable functional properties.

Scientific reports 10(1), 6902 (2020). doi:10.1038/s41598-020-63935-3, In this paper we present a facile method for the synthesis of aminated graphene derivative through simultaneous reduction and amination of graphene oxide via two-step liquid phase treatment with hydrobromic acid and ammonia solution in mild conditions. The amination degree of the obtained aminated reduced graphene oxide is of about 4 at.%, whereas C/O ratio is up to 8.8 as determined by means of X-ray photoelectron spectroscopy. The chemical reactivity of the introduced amine groups is further verified by successful test covalent bonding of the obtained aminated graphene with 3-Chlorobenzoyl chloride. The morphological features and electronic properties, namely conductivity, valence band structure and work function are studied as well, illustrating the influence of amine groups on graphene structure and physical properties. Particularly, the increase of the electrical conductivity, reduction of the work function value and tendency to form wrinkled and corrugated graphene layers are observed in the aminated graphene derivative compared to the pristine reduced graphene oxide. As obtained aminated graphene could be used for photovoltaic, biosensing and catalysis application as well as a starting material for further chemical modifications., Published by Macmillan Publishers Limited, part of Springer Nature, [London]

In this paper, we for the first time demonstrate efficient nitrogen doping of graphene oxide (GO) with nitrogen concentration of up to 5 at.% via modified Hummers' method. Using X-ray photoelectron spectroscopy (XPS), X-ray absorbance spectroscopy (XAS) and Fourier transform infrared spectroscopy (FTIR) techniques, we have found out graphitic nitrogen to be the dominant type of the implemented nitrogen species. At the same time, the subsequent GO thermal reduction to graphene appears to result in a transformation of the graphitic nitrogen into pyridines and pyrroles. The mechanisms of the observed GO nitrogen doping and conversion of the nitrogen species are proposed, providing an opportunity to control the type and concentration of the implemented nitrogen within the approach. A two-time increase of the graphenes' conductivity is observed due to the performed nitrogen doping. Further comprehensive electrical studies combined with the transmission electron microscopy (TEM) and density functional theory (DFT) modeling have allowed us to estimate the conductivity mechanism and the impact of the implemented nitrogen. As a net result, a simple method to synthesize N-doped graphene with the desired type of the nitrogen species is developed, which leads to new perspective applications for graphene, i.e. supercapacitors, catalysis, and sensors.