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1.
Inorg Chem ; 62(38): 15641-15650, 2023 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-37690055

RESUMO

When it comes to an efficient catalytic oxygen evolution reaction (OER) in the production of renewable energy and chemicals, the construction of heterogeneous structures is crucial to break the linear scalar relationship of a single catalyst. This heterogeneous structure construction helps creatively achieve high activity and stability. However, the synthesis process of heterogeneous crystalline materials is often complex and challenging to capture and reproduce, which limits their application. Here, the dynamic process of structural changes in Co-MOFs in alkali was captured by in situ powder X-ray diffraction, FT-IR spectroscopy, and Raman spectroscopy, and several self-reconfigured MOF heterogeneous materials with different structures were stably isolated. The created ß-Co(OH)2/Co-MOF heterojunction structure facilitates rapid mass-charge transfer and exposure of active sites, which significantly enhanced OER activity. Experimental results show that this heterogeneous structure achieves a low overpotential of 333 mV at 10 mA cm-2. The findings provide new insights and directions for the search for highly reactive cobalt-based MOFs for sustainable energy technologies.

2.
Dalton Trans ; 46(2): 347-354, 2017 Jan 03.
Artigo em Inglês | MEDLINE | ID: mdl-27929171

RESUMO

A novel BiOBr@TiO2/carbon hybrid framework as a continuous flow sunlight water purification system has been reported in the present work. The BiOBr@TiO2/carbon hybrid framework was fabricated via the sequential growth of TiO2 nanowires and BiOBr nanoplates on carbon fiber cloth. TiO2 nanowires interweaved with carbon fibers to form a porous network, while BiOBr nanoplates were arrayed on TiO2 nanowires. The obtained BiOBr@TiO2/carbon hybrid framework possesses numerous micro/nanochannels between their adjacent one-dimensional building blocks, which can serve as an effective water transport network driven by capillary force. Furthermore, BiOBr@TiO2/carbon hybrid frameworks exhibit impressive sunlight-driven photocatalytic activity and adsorption ability because of their enhanced sunlight absorption ability, efficient charge separation features, and mesoporous architecture. The excellent reusability and durability of the BiOBr@TiO2/carbon hybrid frameworks have also been confirmed. A novel BiOBr@TiO2/carbon hybrid framework based continuous flow sunlight water purification system with a high water purification efficiency (305.6 L h-1 m-2) has been constructed in the present work. All the features make the BiOBr@TiO2/carbon hybrid framework a promising material suitable for water purification.

3.
Inorg Chem ; 50(10): 4493-502, 2011 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-21476536

RESUMO

Treatment of [Et(4)N][Tp*WS(3)] (1) (Tp* = hydridotris(3,5-dimethylpyrazol-1-yl)borate) with 2 equiv of AgSCN in MeCN afforded a novel neutral compound [(Tp*WS(2))(2)(µ-S(2))] (2). Reactions of 2 with excess CuX (X = Cl, Br, I) in MeCN and CH(2)Cl(2) or CHCl(3) formed three neutral W/Cu/S clusters [{Tp*W(µ(3)-S)(3)Cu(3)(µ-Cl)}(2)Cu(µ-Cl)(2)(µ(7)-Cl)(MeCN)](2) (3), [{Tp*W(µ(3)-S)(3)Cu(3)}(2)Br(µ-Br)(2)(µ(4)-Br)(MeCN)] (4), and [{Tp*W(µ(3)-S)(3)Cu(3)}(2){Cu(2)(µ-I)(4)(µ(3)-I)(2)}] (5), respectively. On the other hand, treatment of 2 with CuX (X = Cl, Br) in the presence of Et(4)NX (X = Cl, Br) produced two anionic W/Cu/S clusters [Et(4)N][{Tp*W(µ(3)-S)(3)Cu(3)X}(2)(µ-X)(2)(µ(4)-X)] (6: X = Cl; 7 X = Br). Compounds 2-7 were characterized by elemental analysis, IR, UV-vis, (1)H NMR, electrospray ionization (ESI) mass spectra, and single-crystal X-ray crystallography. The dimeric structure of 2 can be viewed as two [Tp*WS(2)] fragments in which two W atoms are connected by one S(2)(2-) dianion. Compounds 3-7 all possess unique halide-bridged double cubanelike frameworks. For 3, two [Tp*W(µ(3)-S)(3)Cu(3)](2+) dications are linked via a µ(7)-Cl(-) bridge, two µ-Cl(-) bridges, and a [Cu(MeCN)(µ-Cl)(2)](+) bridge. For 4, one [Tp*W(µ(3)-S)(3)Cu(3)(MeCN)](2+) dication and one [Tp*W(µ(3)-S)(3)Cu(3)Br](+) cation are linked via a µ(4)-Br(-) and two µ-Br(-) bridges. For 5, the two [Tp*W(µ(3)-S)(3)Cu(3)](2+) dications are bridged by a linear [(µ-I)(2)Cu(µ(3)-I)(2)Cu(µ-I)(2)](4+) species. For 6 and 7, two [Tp*W(µ(3)-S)(3)Cu(3)X](+) cations are linked by a µ(4)-X(-) and two µ-X(-) bridges (X = Cl, Br). In addition, the third-order nonlinear optical (NLO) properties of 2-7 in MeCN/CH(2)Cl(2) were investigated by using femtosecond degenerate four-wave mixing (DFWM) technique.


Assuntos
Boratos/síntese química , Halogênios/química , Pró-Fármacos/síntese química , Pirazóis/síntese química , Tungstênio/química , Cobre/química , Cristalografia por Raios X , Espectroscopia de Ressonância Magnética , Modelos Moleculares , Mimetismo Molecular , Estrutura Molecular , Nitrogenase/química , Compostos de Prata/química , Espectrometria de Massas por Ionização por Electrospray , Sulfetos/química
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