Metal-free nitrogen-doped carbon materials are currently considered at the forefront of potential alternative cathode catalysts for the oxygen reduction reaction (ORR) in fuel cell technology. Despite numerous efforts in this area over the past decade, rational design and development of a new catalyst system based on nitrogen-doped carbon materials via an innovative approach still present intriguing challenges in ORR catalysis research. Herein, a new kind of nitrogen-doped carbon nanoparticle-carbon nanofiber (NCNP-CNF) composite with highly efficient and stable ORR catalytic activity has been developed via a new approach assisted by a solution plasma process. The integration of NCNPs and CNFs by the solution plasma process can lead to a unique morphological feature and modify physicochemical properties. The NCNP-CNF composite exhibits a significantly enhanced ORR activity through a dominant four-electron pathway in an alkaline solution. The enhancement in ORR activity of NCNP-CNF composite can be attributed to the synergistic effects of good electron transport from highly graphitized CNFs as well as abundance of exposed catalytic sites and meso/macroporosity from NCNPs. More importantly, NCNP-CNF composite reveals excellent long-term durability and high tolerance to methanol crossover compared with those of a commercial 20 wt % supported on Vulcan XC-72. We expect that NCNP-CNF composite prepared by this synthetic approach can be a promising metal-free cathode catalyst candidate for ORR in fuel cells and metal-air batteries.
Fluorine-doped carbon nanoparticles were successfully synthesized via a simple one-step solution plasma process at room temperature and atmospheric pressure without the addition of a metal catalyst.
Although solution-plasma processing enables room-temperature synthesis of nanocarbons, the underlying mechanisms are not well understood. We investigated the routes of solution-plasma-induced nanocarbon formation from hexane, hexadecane, cyclohexane, and benzene. The synthesis rate from benzene was the highest. However, the nanocarbons from linear molecules were more crystalline than those from ring molecules. Linear molecules decomposed into shorter olefins, whereas ring molecules were reconstructed in the plasma. In the saturated ring molecules, C–H dissociation proceeded, followed by conversion into unsaturated ring molecules. However, unsaturated ring molecules were directly polymerized through cation radicals, such as benzene radical cation, and were converted into two- and three-ring molecules at the plasma–solution interface. The nanocarbons from linear molecules were synthesized in plasma from small molecules such as C2 under heat; the obtained products were the same as those obtained via pyrolysis synthesis. Conversely, the nanocarbons obtained from ring molecules were directly synthesized through an intermediate, such as benzene radical cation, at the interface between plasma and solution, resulting in the same products as those obtained via polymerization. These two different reaction fields provide a reasonable explanation for the fastest synthesis rate observed in the case of benzene.
Nitrogen-doped carbon nanoparticles were successfully synthesized by a facile solution plasma process without the addition of metal catalysts. Organic liquid mixtures of benzene and pyrazine were used as the precursors for the synthesis.
Black titania spheres (H-TiO2-x) were synthesized via a simple green method assisted by water plasma at a low temperature and atmospheric pressure. The in situ production of highly energetic hydroxyl and hydrogen species from water plasma are the prominent factors in the oxidation and hydrogenation reactions during the formation of H-TiO2-x, respectively. The visible-light photocatalytic activity toward the dye degradation of H-TiO2-x can be attributed to the synergistic effect of large-surface area, visible-light absorption and the existence of oxygen vacancies and Ti(3+) sites.
We report a novel strategy to produce stable colloidal gold nanoparticles (AuNPs) in alginate aqueous solution which can be done in one step and without any chemicals. The AuNPs were produced by applying a voltage across a pair of gold electrodes which were immersed in alginate aqueous solution.Since the generation of AuNPs was caused by the sputtering of gold electrodes, the process was named the solution plasma sputtering (SPS) process. We utilize the alginate polymer in order to meet three important requirements: (1) to promote the generation of plasma in a liquid environment, (2) to endow biocompatibility to the AuNPs, and (3) to provide colloidal stability to the AuNPs-alginate aqueous suspensions. The alginate concentrations were varied as 0.2, 0.5, and 0.9 %w/v. The concentrationdependent effect on the particle size of AuNPs, the physical absorption property and the stability of the AuNPs-alginate suspensions were studied. Results indicate that preparation of chemical-free colloidal AuNPs-alginate aqueous suspension is successful by the SPS process. The obtained colloidal suspensions were stable and able to retain their strong plasmon absorption bands within a reasonable time period. As a consequence, this is a high-potential technique to produce AuNPs suspended in alginate aqueous solution appropriate for biomedical applications.
N-doped carbon synthesized by a room temperature plasma process demonstrated the synergic effect of amino-N and graphitic-N towards advanced ORR activity.
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