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1.
Nano Lett ; 23(23): 10779-10787, 2023 Dec 13.
Artículo en Inglés | MEDLINE | ID: mdl-37987745

RESUMEN

Electrochemical reduction of CO2 using Cu catalysts enables the synthesis of C2+ products including C2H4 and C2H5OH. In this study, Cu catalysts were fabricated using plasma-enhanced atomic layer deposition (PEALD), achieving conformal deposition of catalysts throughout 3-D gas diffusion electrode (GDE) substrates while maintaining tunable control of Cu nanoparticle size and areal loading. The electrochemical CO2 reduction at the Cu surface yielded a total Faradaic efficiency (FE) > 75% for C2+ products. Parasitic hydrogen evolution was minimized to a FE of ∼10%, and a selectivity of 42.2% FE for C2H4 was demonstrated. Compared to a line-of-sight physical vapor deposition method, PEALD Cu catalysts show significant suppression of C1 products compared to C2+, which is associated with improved control of catalyst morphology and conformality within the porous GDE substrate. Finally, PEALD Cu catalysts demonstrated a stable performance for 15 h with minimal reduction in the C2H4 production rate.

2.
Chem Commun (Camb) ; 51(86): 15657-60, 2015 Nov 07.
Artículo en Inglés | MEDLINE | ID: mdl-26360296

RESUMEN

A deep investigation of amorphous V2O5-P2O5 powders for magnesium batteries communicates the vital properties to achieving the superior electrochemical performance at a 75 : 25 V2O5 : P2O5 molar ratio. The manipulation of the inter-layer spacing and amorphization of V2O5 can enhance Mg(2+) diffusion and afford a cathode with high-voltage reversibility.

3.
Angew Chem Int Ed Engl ; 54(27): 7900-4, 2015 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-26013580

RESUMEN

Unlocking the full potential of rechargeable magnesium batteries has been partially hindered by the reliance on chloride-based complex systems. Despite the high anodic stability of these electrolytes, they are corrosive toward metallic battery components, which reduce their practical electrochemical window. Following on our new design concept involving boron cluster anions, monocarborane CB11H12(-) produced the first halogen-free, simple-type Mg salt that is compatible with Mg metal and displays an oxidative stability surpassing that of ether solvents. Owing to its inertness and non-corrosive nature, the Mg(CB11H12)2/tetraglyme (MMC/G4) electrolyte system permits standardized methods of high-voltage cathode testing that uses a typical coin cell. This achievement is a turning point in the research and development of Mg electrolytes that has deep implications on realizing practical rechargeable Mg batteries.

4.
ACS Appl Mater Interfaces ; 6(10): 7004-8, 2014 May 28.
Artículo en Inglés | MEDLINE | ID: mdl-24807043

RESUMEN

Batteries based on magnesium are an interesting alternative to current state-of-the-art lithium-ion systems; however, high-energy-density cathodes are needed for further development. Here we utilize TEM, EDS, and EELS in addition to soft-XAS to determine electrochemical magnesiation mechanism of a high-energy density cathode, K-αMnO2. Rather than following the typical insertion mechanism similar to Li(+), we propose the gradual reduction of K-αMnO2 to form Mn2O3 then MnO at the interface of the cathode and electrolyte, finally resulting in the formation of K-αMnO2@(Mg,Mn)O core-shell product after discharge of the battery. Understanding the mechanism is a vital guide for future magnesium battery cathodes.

5.
Angew Chem Int Ed Engl ; 53(12): 3173-7, 2014 Mar 17.
Artículo en Inglés | MEDLINE | ID: mdl-24519845

RESUMEN

Boron clusters are proposed as a new concept for the design of magnesium-battery electrolytes that are magnesium-battery-compatible, highly stable, and noncorrosive. A novel carborane-based electrolyte incorporating an unprecedented magnesium-centered complex anion is reported and shown to perform well as a magnesium-battery electrolyte. This finding opens a new approach towards the design of electrolytes whose likelihood of meeting the challenging design targets for magnesium-battery electrolytes is very high.

6.
Chem Commun (Camb) ; 49(2): 149-51, 2013 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-23168386

RESUMEN

A high energy-density Sn anode capable of displaying superior operating voltages and capacity, for rechargeable Mg-ion batteries, is highlighted. The intended application and performance of the anode is confirmed by coupling it with a Mo(6)S(8) cathode in a conventional battery electrolyte.

7.
Angew Chem Int Ed Engl ; 51(39): 9780-3, 2012 Sep 24.
Artículo en Inglés | MEDLINE | ID: mdl-22907926

RESUMEN

Beyond hydrogen storage: The first example of reversible magnesium deposition/stripping onto/from an inorganic salt was seen for a magnesium borohydride electrolyte. High coulombic efficiency of up to 94 % was achieved in dimethoxyethane solvent. This Mg(BH(4))(2) electrolyte was utilized in a rechargeable magnesium battery.

8.
Nat Commun ; 2: 427, 2011 Aug 09.
Artículo en Inglés | MEDLINE | ID: mdl-21829189

RESUMEN

Magnesium metal is an ideal rechargeable battery anode material because of its high volumetric energy density, high negative reduction potential and natural abundance. Coupling Mg with high capacity, low-cost cathode materials such as electrophilic sulphur is only possible with a non-nucleophilic electrolyte. Here we show how the crystallization of the electrochemically active species formed from the reaction between hexamethyldisilazide magnesium chloride and aluminum trichloride enables the synthesis of a non-nucleophilic electrolyte. Furthermore, crystallization was essential in the identification of the electroactive species, [Mg(2)(µ-Cl)(3)·6THF](+), and vital to improvements in the voltage stability and coulombic efficiency of the electrolyte. X-ray photoelectron spectroscopy analysis of the sulphur electrode confirmed that the electrochemical conversion between sulphur and magnesium sulfide can be successfully performed using this electrolyte.

9.
J Am Chem Soc ; 133(28): 10679-81, 2011 Jul 20.
Artículo en Inglés | MEDLINE | ID: mdl-21671640

RESUMEN

Mg nanocrystals of controllable sizes were prepared in gram quantities by chemical reduction of magnesocene using a reducing solution of potassium with an aromatic hydrocarbon (either biphenyl, phenanthrene, or naphthalene). The hydrogen sorption kinetics were shown to be dramatically faster for nanocrystals with smaller diameters, although the activation energies calculated for hydrogen absorption (115-122 kJ/mol) and desorption (126-160 kJ/mol) were within previously measured values for bulk Mg. This large rate enhancement cannot be explained by the decrease in particle size alone but is likely due to an increase in the defect density present in smaller nanocrystals.

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