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1.
ACS Appl Mater Interfaces ; 10(29): 24499-24507, 2018 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-29962200

RESUMO

Hydrogen production by water electrolysis has been regarded as a promising approach to wean away from sourcing energy through fossil fuels, as the produced hydrogen gas can be converted to electrical or thermal energy without any harmful byproducts. However, an efficient hydrogen production is restricted by the sluggish oxygen evolution reaction (OER) at the counter anode. Therefore, the development of new OER catalysts with high catalytic activities is crucial for high performance water splitting. Here, we report a novel sloughing method for the fabrication of an efficient OER catalyst on a stainless steel (SS) surface. A chalcogenide (Fe-S) overlayer generated by sulfurization on the SS surface is found to play a critical role as a precursor layer in the formation of an active surface during water oxidation. Interestingly, a newly exposed catalytic layer after sloughing off the Fe-S overlayer has a nanoporous structure with changed elemental composition, resulting in a significant improvement in OER performance with an overpotential value of 267 mV at a current density of 10 mA cm-2 (in 1 M KOH). Our novel method for the preparation of OER catalyst provides an important insight into designing an efficient and stable electrocatalyst for the water splitting community.

2.
ChemSusChem ; 9(16): 2097-102, 2016 08 23.
Artigo em Inglês | MEDLINE | ID: mdl-27466025

RESUMO

The formation of a nanostructure is a popular strategy for catalyst applications because it can generate new surfaces that can significantly improve the catalytic activity and durability of the catalysts. However, the increase in the surface area resulting from nanostructuring does not fully explain the substantial improvement in the catalytic properties of the CO2 electroreduction reaction, and the underlying mechanisms have not yet been fully understood. Here, based on a combination of extended X-ray absorption fine structure analysis, X-ray photoelectron spectroscopy, and Kelvin probe force microscopy, we observed a contracted Au-Au bond length and low work function with the nanostructured Au surface that had enhanced catalytic activity for electrochemical CO2 reduction. The results may improve the understanding of the enhanced stability of the nanostructured Au electrode based on the resistance of cation adhesion during the CO2 reduction reaction.


Assuntos
Dióxido de Carbono/química , Ouro/química , Nanoestruturas/química , Catálise , Eletroquímica , Eletrodos , Oxirredução , Propriedades de Superfície
3.
J Am Chem Soc ; 137(43): 13844-50, 2015 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-26447349

RESUMO

Selective electrochemical reduction of CO2 is one of the most sought-after processes because of the potential to convert a harmful greenhouse gas to a useful chemical. We have discovered that immobilized Ag nanoparticles supported on carbon exhibit enhanced Faradaic efficiency and a lower overpotential for selective reduction of CO2 to CO. These electrocatalysts were synthesized directly on the carbon support by a facile one-pot method using a cysteamine anchoring agent resulting in controlled monodispersed particle sizes. These synthesized Ag/C electrodes showed improved activities, specifically decrease of the overpotential by 300 mV at 1 mA/cm(2), and 4-fold enhanced CO Faradaic efficiency at -0.75 V vs RHE with the optimal particle size of 5 nm compared to polycrystalline Ag foil. DFT calculations enlightened that the specific interaction between Ag nanoparticle and the anchoring agents modified the catalyst surface to have a selectively higher affinity to the intermediate COOH over CO, which effectively lowers the overpotential.

4.
ACS Appl Mater Interfaces ; 7(44): 24550-5, 2015 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-26489005

RESUMO

Oxygen evolution reaction (OER) is the key reaction in electrochemical processes, such as water splitting, metal-air batteries, and solar fuel production. Herein, we developed a facile chemical solution deposition method to prepare a highly active Co3O4 thin film electrode for OER, showing a low overpotential of 377 mV at 10 mA/cm(2) with good stability. An optimal loading of ethyl cellulose additive in a precursor solution was found to be essential for the morphology control and thus its electrocatalytic activity. Our results also show that the distribution of Co3O4 nanoparticle catalysts on the substrate is crucial in enhancing the inherent OER catalytic performance.

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