Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrogen- and energy-intensive operations of the Haber–Bosch process. However, it is severely challenged by nitrogen activation and requires efficient catalysts for the nitrogen reduction reaction. Here we report that a boron carbide nanosheet acts as a metal-free catalyst for high-performance electrochemical nitrogen-to-ammonia fixation at ambient conditions. The catalyst can achieve a high ammonia yield of 26.57 μg h–1 mg–1cat. and a fairly high Faradaic efficiency of 15.95% at –0.75 V versus reversible hydrogen electrode, placing it among the most active aqueous-based nitrogen reduction reaction electrocatalysts. Notably, it also shows high electrochemical stability and excellent selectivity. The catalytic mechanism is assessed using density functional theory calculations.
Platinum nanoparticles (Pt NPs) with uniform size and high dispersion have been successfully assembled on poly(diallyldimethylammonium chloride) functionalized graphene oxide via a sodium borohydride reduction process. The loading concentration of Pt NPs on graphene can be adjusted in the range of 18À78 wt %. The obtained Pt/graphene nanocomposites are characterized by transmission electron microscopy, high resolution transmission electron microscopy, energy dispersive spectrometry, X-ray diffraction, and thermogravimetric analysis. The results show that the Pt NPs with sizes of approximate 4.6 nm uniformly disperse on graphene surface for all Pt loading densities. Electrochemical studies reveal that the Pt/graphene nanocomposites with electrochemically active surface area of 141.6 m 2 /g show excellent electrocatalytic activity toward methanol oxidation and oxygen reduction. The present method is promising for the synthesis of high performance catalysts for fuel cells, gas phase catalysis, and sensors.
Uranium is a key element in the nuclear industry, but its unintended leakage has caused health and environmental concerns. Here we report a sp 2 carbon-conjugated fluorescent covalent organic framework (COF) named TFPT-BTAN-AO with excellent chemical, thermal and radiation stability is synthesized by integrating triazine-based building blocks with amidoxime-substituted linkers. TFPT-BTAN-AO shows an exceptional UO 2 2+ adsorption capacity of 427 mg g −1 attributable to the abundant selective uranium-binding groups on the highly accessible pore walls of open 1D channels. In addition, it has an ultra-fast response time (2 s) and an ultra-low detection limit of 6.7 nM UO 2 2+ suitable for on-site and real-time monitoring of UO 2 2+ , allowing not only extraction but also monitoring the quality of the extracted water. This study demonstrates great potential of fluorescent COFs for radionuclide detection and extraction. By rational designing target ligands, this strategy can be extended to the detection and extraction of other contaminants.
A hydrothermal approach for the cutting of boron-doped graphene (BG) into boron-doped graphene quantum dots (BGQDs) has been proposed. Various characterizations reveal that the boron atoms have been successfully doped into graphene structures with the atomic percentage of 3.45%. The generation of boronic acid groups on the BGQDs surfaces facilitates their application as a new photoluminescence (PL) probe for label free glucose sensing. It is postulated that the reaction of the two cis-diol units in glucose with the two boronic acid groups on the BGQDs surfaces creates structurally rigid BGQDs-glucose aggregates, restricting the intramolecular rotations and thus resulting in a great boost in the PL intensity. The present unusual "aggregation-induced PL increasing" sensing process excludes any saccharide with only one cis-diol unit, as manifested by the high specificity of BGQDs for glucose over its close isomeric cousins fructose, galactose, and mannose. It is believed that the doping of boron can introduce the GQDs to a new kind of surface state and offer great scientific insights to the PL enhancement mechanism with treatment of glucose.
Au nanoparticles modified with electroactive Prussian blue (PB) were for the first time synthesized by a simple chemical method. Transmission electronic microscopy showed that the average size of the Prussian blue shell/Au core hybrid composite (PB@Au) was about 50 nm, and Fourier transform IR, UV-vis spectra, and cyclic voltammetry confirmed the existence of PB on the surface of Au nanoparticles. Using the LbL technique, multilayer thin films of PB@Au nanoparticles were prepared by the alternate adsorption of oppositely charged linear polyelectrolyte poly(allylamine hydrochloride) (PAH) onto ITO glass for the construction of a hydrogen peroxide sensor. The novel multilayer films were characterized by SEM, cyclic voltammetry, and UV-visible absorption spectroscopy. The {PAH/PB@Au}n multilayer-modified electrode showed a well-defined pair of redox peaks and dramatic catalytic activity toward the reduction of hydrogen peroxide.
Because of its high activity and selectivity toward the reduction of hydrogen peroxide and oxygen, Prussian blue (PB) is usually considered as an “artificial enzyme peroxidase” and has been extensively used in the construction of electrochemical biosensors. In this study, we report on the construction of amperometric biosensors via grafting PB nanoparticles on the polymeric matrix of multiwalled carbon nanotubes (MWCNTs) and poly(4‐vinylpyridine) (PVP). The MWCNT/PVP/PB composite films were synthesized by casting films of MWCNTs wrapped with PVP on gold electrodes followed by electrochemical deposition of PB on the MWCNT/PVP matrix. The electrode modified with the MWCNT/PVP/PB composite film shows prominent electrocatalytic activity toward the reduction of hydrogen peroxide, which can be explained by the remarkable synergistic effect of the MWCNTs and PB. Therefore, fast amperometric response of this sensor to hydrogen peroxide was observed with a detection sensitivity of 1.3 μA μM–1 of H2O2 per square centimeter area and a detection limit of 25 nM. These results are much better than those reported for PB‐based amperometric sensors. In addition, a glucose biosensor fabricated by casting an additional glucose oxidase (GOD) containing Nafion film above the MWCNT/PVP/PB composite film shows promise for the sensitive and fast detection of glucose. The observed high stability, high sensitivity, and high reproducibility of the MWCNT/PVP/PB composite films make them promising for the reliable and durable detection of hydrogen peroxide and glucose.
The sense of it: A new type of rapid, sensitive, and specific photoluminescence (PL)-based assay has been proposed for the detection of phosphate (Pi) based on the competition of oxygen-donor atoms from Pi with those from the carboxylate groups on a graphene-quantum-dot (GQD) surface for Eu(3+) ions. The graphene-like structures combined with QD-like optical properties suggest the promising nature of the GQDs as versatile tools in the fields of analytical science and biotechnology.
We reported here a method to enhance detection sensitivity in surface plasmon resonance (SPR) spectroscopy integrated with a surface molecular imprinting recognition system and employing magnetic molecular imprinting polymer nanoparticles for amplifying SPR response. The proposed magnetic molecular imprinting polymer was designed by self-polymerization of dopamine on the Fe3O4 NPs surface in weak base aqueous solution in the presence of template chlorpyrifos (CPF). The imprinted Fe3O4@polydopamine nanoparticles (Fe3O4@PDA NPs) were characterized by Fourier transform infrared spectroscopy, UV-vis absorption spectroscopy, and transmission electron microscopy. The biosensor showed a good linear relationship between the SPR angle shift and the chlorpyrifos concentration over a range from 0.001 to 10 μM with a detection limit of 0.76 nM. A significant increase in sensitivity was therefore afforded through the use of imprinted Fe3O4@PDA NPs as an amplifier, and meanwhile, the imprinted Fe3O4@PDA NPs had an excellent recognition capacity to chlorpyrifos over other pesticides. The excellent sensitivity and selectivity and high stability of the designed biosensor make this magnetic imprinted Fe3O4@PDA NP an attractive recognition element for various SPR sensors for detecting pesticide residuals and other environmentally deleterious chemicals.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
334 Leonard St
Brooklyn, NY 11211
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.