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1.
J Environ Manage ; 238: 243-250, 2019 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-30852400

RESUMEN

We report the synthesis of mesoporous TiO2 and mesoporous Fe2O3-TiO2 catalysts by using a structure-directing-surfactant method, their characterization and their employment as photocatalysts for norfloxacin degradation in aqueous solution. The main findings show that in the presence of both O2 and H2O2, Fe-containing mesoporous titania (Fe2O3-TiO2), with iron percentages between 1 and 3 wt%, exhibited norfloxacin degradation rates more than 60% greater than otherwise identical mesoporous titania without iron. Furthermore, the activity of the mesoporous composite catalysts also exceeds that of titania when illuminated with 405 nm light-emitting diodes. Iron loading improved the photocatalytic activity for norfloxacin degradation with values of apparent reaction rate constants of 0.037 min-1 and 0.076 min-1 with 1 and 3 surface wt.% of iron, respectively. An optimum of activity was found with the 3 wt% Fe2O3-TiO2 catalyst. Under these conditions, 10 mg/L of norfloxacin is reacted essentially to completion and 90% of total organic carbon conversion was obtained within 120 min of reaction. This higher organic carbon conversion degree was reached due to the photo-oxidation of short-chain organic acids. The high activity of the as-synthesized mesoporous composites is attributed to the additional iron phase which led to the different reactions for H2O2 decomposition, but also due to the improvement in light absorbance. Finally, the activity of the most active catalyst was found to be stable over multiple sequential runs, which was related to a negligible amount of iron leaching (<0.1%) from these materials.


Asunto(s)
Norfloxacino , Agua , Catálisis , Compuestos Férricos , Peróxido de Hidrógeno
2.
ACS Appl Mater Interfaces ; 10(30): 25337-25349, 2018 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-30036030

RESUMEN

The synthesis, characterization, and electrocatalytic properties of mesoporous carbon materials doped with nitrogen atoms and iron are reported and compared for the catalyzed reduction of oxygen gas at fuel cell cathodes. Mixtures of common and inexpensive organic precursors, melamine, and formaldehyde were pyrolyzed in the presence of transition-metal salts (e.g., nitrates) within a mesoporous silica template to yield mesoporous carbon materials with greater extents of graphitization than those of others prepared from small-molecule precursors. In particular, Fe,N-doped carbon materials possessed high surface areas (∼800 m2/g) and high electrical conductivities (∼19 S/cm), which make them attractive for electrocatalyst applications. The surface compositions of the mesoporous Fe,N-doped carbon materials were postsynthetically modified by acid washing and followed by high-temperature thermal treatments, which were shown by X-ray photoelectron spectroscopy to favor the formation of graphitic and pyridinic nitrogen moieties. Such surface-modified materials exhibited high electrocatalytic oxygen reduction activities under alkaline conditions, as established by their high onset and half-wave potentials (1.04 and 0.87 V, respectively vs reversible hydrogen electrode) and low Tafel slope (53 mV/decade). These values are superior to many similar transition-metal- and N-doped carbon materials and compare favorably with commercially available precious-metal catalysts, e.g., 20 wt % Pt supported on activated carbon. The analyses indicate that inexpensive mesoporous Fe,N-doped carbon materials are promising alternatives to precious metal-containing catalysts for electrochemical reduction of oxygen in polymer electrolyte fuel cells.

3.
Nat Nanotechnol ; 11(2): 198-203, 2016 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-26551015

RESUMEN

Risk research for nanomaterials is currently prioritized by means of expert workshops and other deliberative processes. However, analytical techniques that quantify and compare alternative research investments are increasingly recommended. Here, we apply value of information and portfolio decision analysis-methods commonly applied in financial and operations management-to prioritize risk research for multiwalled carbon nanotubes and nanoparticulate silver and titanium dioxide. We modify the widely accepted CB Nanotool hazard evaluation framework, which combines nano- and bulk-material properties into a hazard score, to operate probabilistically with uncertain inputs. Literature is reviewed to develop uncertain estimates for each input parameter, and a Monte Carlo simulation is applied to assess how different research strategies can improve hazard classification. The relative cost of each research experiment is elicited from experts, which enables identification of efficient research portfolios-combinations of experiments that lead to the greatest improvement in hazard classification at the lowest cost. Nanoparticle shape, diameter, solubility and surface reactivity were most frequently identified within efficient portfolios in our results.

4.
Adv Mater ; 28(6): 1287-94, 2016 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-26178584

RESUMEN

Mixtures of phenols/ketones and urea show eutectic behavior upon gentle heating. These mixtures possess liquid-crystalline-like phases that can be processed. The architecture of phenol/ketone acts as structure-donating motif, while urea serves as melting-point reduction agent. Condensation at elevated temperatures results in nitrogen-containing carbons with remarkably high nitrogen content of mainly pyrazinic nature.

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