Simultaneous Noncovalent Modification and Exfoliation of 2D Carbon Nitride for Enhanced Electrochemiluminescent Biosensing
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As an emerging nitrogen-rich 2D carbon material, graphitic carbon nitride (CN) has drawn much attention for applications ranging from photo-/electrocatalysts to biosensors. Interfacial modification of CN is fundamentally vital but is still in its infancy and remains challenging due to the low reactivity of CN. Here we report that, in conjunction with a π-π stacking interaction, bulk CN could be simultaneously exfoliated via facile mechanical grinding. The obtained CN nanosheets (m-CNNS) not only retained the pristine optoelectronic properties of bulk CN but also enriched a friendly interface for further coupling biomolecules with advanced properties, overcoming the deficiencies of CN in surface science. The m-CNNS were further covalently linked to a DNA probe, and the resultant electrochemiluminescent biosensor for the target DNA exhibited much enhanced sensitivity with respect to that obtained by direct physical absorption of the DNA probe on unmodified CNNS. This noncovalent exfoliation and interfacial modification should greatly expand the scope of potential applications of CN in areas such as biosensing and should also be applicable to other 2D materials in interface modulation.Keywords:
Biomolecule
Exfoliation joint
Carbon nitride
Graphitic carbon nitride
Surface Modification
Carbon fibers
Nanosheets of a crystalline 2D carbon nitride were obtained by ionothermal synthesis of the layered bulk material poly(triazine imide), PTI, followed by one-step liquid exfoliation in water. Triazine-based nanosheets are 1-2 nm in height and afford chemically and colloidally stable suspensions under both basic and acidic conditions. We use solid-state NMR spectroscopy of isotopically enriched, restacked nanosheets as a tool to indirectly monitor the exfoliation process and carve out the chemical changes occurring upon exfoliation, as well as to determine the nanosheet thickness. PTI nanosheets show significantly enhanced visible-light driven photocatalytic activity toward hydrogen evolution compared to their bulk counterpart, which highlights the crucial role of morphology and surface area on the photocatalytic performance of carbon nitride materials.
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Nanomaterials
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Graphitic carbon nitride materials show some promising properties for applications such as photocatalytic water splitting. However, the conversion efficiency is still low due to factors such as a low surface area and limited light absorption. In this paper, we describe a “triple templating” approach to generating porous graphitic carbon nitride. The introduction of pores on several length-scales results in enhanced photocatalytic properties.
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The MoS2/S-doped graphitic carbon nitride (MoS2/S-g-C3N4) was synthesized by a simple method and applied for methylene blue (MB) removal as an organic pollutant. The structure of MoS2/S-doped graphitic carbon nitride was characterized using FTIR, XRD, SEM, TGA and BET techniques. The accomplishment of MoS2/S-doped graphitic carbon nitride as an adsorbent was investigated to removal of MB from aqueous solution. The various parameters were studied such as: pH, initial MB concentration, adsorbent dose, temperature and time. The best findings were obtained at pH=8, 8 ppm MB concentration, 0.05 g MoS2/S-g-C3N4, 30 min and 22 ˚C. The Langmuir isotherm model was adopted with the obtained data. The kinetic studies were showed that the adsorption of methylene blue can be well described by the second-order equation. Maximum adsorption was calculated as 166 mg/g. The degradation of MB was studied by MoS2/S-doped graphitic carbon nitride under Light Emmition Diode (LED). Results showed that the MoS2/S-doped graphitic carbon nitride can enhance photocatalytic activity compared to pure g-C3N4 and MoS2/g-C3N4. The findings confirmed that the MoS2/S-doped graphitic carbon nitride can be applied as an efficient, low-cost adsorbent, and photocatalyst to remove of cationic dyes such as methylene blue.
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In this article we report on the one-step, rapid, high-yield synthesis of graphitic carbon nitride (g-C3N4) nanosheets for the first time. The nanosheets were obtained by pyrolyzing a melamine–KBH4 mixture under Ar. As a fluorosensor for Cu2+, the g-C3N4 nanosheets exhibit a detection limit as low as 0.5 nM and high selectivity in buffer solutions, and this sensor was applied to the analysis of lake water samples. The electrogenerated chemiluminescence (ECL) behavior of the g-C3N4 nanosheets using Na2S2O8 as the coreactant was also studied. Results suggest that the ECL intensity of the g-C3N4 nanosheets was linear over concentrations of 0–45 nM, with a detection limit of 1.2 nM for Cu2+.
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We demonstrate that graphitic carbon nitride can photoreduce CO2 to CO in the presence of water vapor and exhibit interesting porous structure dependent reactivity on photoreduction and photooxidation under visible light (λ > 420 nm). Graphitic carbon nitride was synthesized by directly heating the inexpensive melamine and the replacement of melamine with melamine hydrochloride could result in porousification in the final graphitic carbon nitride with much higher surface area (39 times) and more abundant pores, accompanied by a band gap increase of 0.13 eV. The porousification could significantly enhance the photoreactivity of graphitic carbon nitride in rhodamine B photooxidation by 9.4 times, but lower its activity in CO2 photoreduction by 4.6 times. The reasons for the porous structure dependent photoreactivity were investigated in detail. These new findings could shed light on the design of efficient photocatalysts and the tuning of their photoreactivity for environmental and energy applications.
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Abstract Free‐standing graphitic C 3 N 4 nanosheets are prepared by liquid phase exfoliation from graphitic C 3 N 4 powders dispersed in various solvents such as isopropanol, N‐methylpyrrolidone, water, ethanol, or acetone (sonication for 10 h).
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