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1.
Chemistry ; 24(9): 2157-2163, 2018 Feb 09.
Artículo en Inglés | MEDLINE | ID: mdl-29205557

RESUMEN

The route of converting CO2 to CO by reverse water-gas shift (RWGS) reaction is of particular interest due to the direct use of CO as feedstock in many significant industrial processes. Here, an engineered cobalt-cobalt oxide core-shell catalyst (Co@CoO) with nanochains structure has been made for the efficient reduction of CO2 to useful CO. Owing to the excellent performance for H2 activation of metal nanoparticles and the enhanced absorption and activation for CO2 molecule of defective metal oxides, the unique synergistic effect of metallic Co and encapsulating coordinatively unsaturated CoO species shows high performance for clean generation of CO under moderate and practical conditions. Furthermore, with N-dopant into the defective CoO shell, the Co@CoO-N achieves the highest conversion of 19.2 % and an exceptional CO evolution rate of 96 mL min-1 gcat-1 at 523 K with a gas hourly space velocity (GHSV) of 42,000 mL gcat-1 h-1 , which is comparable with the previously reported materials under identical conditions.

2.
Dalton Trans ; 46(4): 1047-1051, 2017 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-28009899

RESUMEN

Black titania prepared by metal-reduction methods is systematically studied and found the best controllable Mg-reduction method. Colored titania products from white, light blue, dark blue, to black were obtained with a crystalline/amorphous core-shell structure. The black titania shows a five times higher H2 production rate in photoelectrochemical (PEC) water splitting.

3.
ChemSusChem ; 10(15): 3044-3048, 2017 08 10.
Artículo en Inglés | MEDLINE | ID: mdl-28691286

RESUMEN

The chemical transformation of CO2 is an efficient approach in low-carbon energy system. The development of nonprecious metal catalysts with sufficient activity, selectivity, and stability for the generation of CO by CO2 reduction under mild conditions remains a major challenge. A hierarchical architecture catalyst composed of ultrathin graphene shells (2-4 layers) encapsulating homogeneous FeNi alloy nanoparticles shows enhance catalytic performance. Electron transfer from the encapsulated alloy can extend from the inner to the outer shell, resulting in an increased charge density on graphene. Nitrogen atom dopants can synergistically increase the electron density on the catalyst surface and modulate the adsorption capability for acidic CO2 molecules. The optimized FeNi3 @NG (NG=N-doped graphene) catalyst, with significant electron penetration through the graphene layer, effects exceptional CO2 conversion of 20.2 % with a CO selectivity of nearly 100 %, as well as excellent thermal stability at 523 K.


Asunto(s)
Dióxido de Carbono/química , Monóxido de Carbono/química , Grafito/química , Hierro/química , Níquel/química , Transporte de Electrón , Modelos Moleculares , Conformación Molecular
4.
ACS Appl Mater Interfaces ; 8(41): 27654-27660, 2016 Oct 19.
Artículo en Inglés | MEDLINE | ID: mdl-27668946

RESUMEN

One-dimensional nanocrystals favoring efficient charge transfer have attracted enormous attentions, and conductive nanobelts of black titania with a unique band structure and high electrical conductivity would be interestingly used in electrocatalysis. Here, Pd nanodots supported by two kinds of black titania, the oxygen-deficient titania (TiO2-x) and nitrogen-doped titania (TiO2-x:N), were synthesized as efficient composite catalysts for oxygen-reduction reaction (ORR). These composite catalysts show improved catalytic activity with lower overpotential and higher limited current, compared to the Pd nanodots supported on the white titania (Pd/TiO2). The improved activity is attributed to the relatively high conductivity of black titania nanobelts for efficient charge transfer (CT) between Ti3+ species and Pd nanodots. The CT process enhances the strong metal-support interaction (SMSI) between Pd and TiO2, which lowers the absorption energy of O2 on Pd and makes it more suitable for oxygen reduction. Because of the stronger interaction between Pd and support, the Pd/TiO2-x:N also shows excellent durability and immunity to methanol poisoning.

5.
Chem Commun (Camb) ; 52(99): 14226-14229, 2016 Dec 06.
Artículo en Inglés | MEDLINE | ID: mdl-27872913

RESUMEN

An efficient titania supported Au nanocluster (NC) has been prepared for the direct synthesis of useful EtOH from CO2 and H2. The unique creation of an excellent synergistic effect between Au NCs and the underlying TiO2 support, especially the anatase crystal phase with abundant oxygen vacancies, can achieve the high performance for EtOH synthesis under moderate and practical conditions.

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