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1.
Nat Commun ; 10(1): 1340, 2019 03 22.
Artigo em Inglês | MEDLINE | ID: mdl-30902984

RESUMO

Geometric or electronic confinement of guests inside nanoporous hosts promises to deliver unusual catalytic or opto-electronic functionality from existing materials but is challenging to obtain particularly using metastable hosts, such as metal-organic frameworks (MOFs). Reagents (e.g. precursor) may be too large for impregnation and synthesis conditions may also destroy the hosts. Here we use thermodynamic Pourbaix diagrams (favorable redox and pH conditions) to describe a general method for metal-compound guest synthesis by rationally selecting reaction agents and conditions. Specifically we demonstrate a MOF-confined RuO2 catalyst (RuO2@MOF-808-P) with exceptionally high catalytic CO oxidation below 150 °C as compared to the conventionally made SiO2-supported RuO2 (RuO2/SiO2). This can be caused by weaker interactions between CO/O and the MOF-encapsulated RuO2 surface thus avoiding adsorption-induced catalytic surface passivation. We further describe applications of the Pourbaix-enabled guest synthesis (PEGS) strategy with tutorial examples for the general synthesis of arbitrary guests (e.g. metals, oxides, hydroxides, sulfides).

2.
J Am Chem Soc ; 140(19): 6130-6136, 2018 05 16.
Artigo em Inglês | MEDLINE | ID: mdl-29685030

RESUMO

Three-dimensional carbon-based structures have proven useful for tailoring material properties in structural mechanical and energy storage applications. One approach to obtain them has been by carbonization of selected metal-organic frameworks (MOFs) with catalytic metals, but this is not applicable to most common MOF structures. Here, we present a strategy to transform common MOFs, by guest inclusions and high-temperature MOF-guest interactions, into complex carbon-based, diatom-like, hierarchical structures (named for the morphological similarities with the naturally existing diatomaceous species). As an example, we introduce metal salt guests into HKUST-1-type MOFs to generate a family of carbon-based nano-diatoms with two to four levels of structural hierarchy. We report control of the morphology by simple changes in the chemistry of the MOF and guest, with implications for the formation mechanisms. We demonstrate that one of these structures has unique advantages as a fast-charging lithium-ion battery anode. The tunability of composition should enable further studies of reaction mechanisms and result in the growth of a myriad of unprecedented carbon-based structures from the enormous variety of currently available MOF-guest candidates.

3.
J Phys Chem C Nanomater Interfaces ; 121(7): 3790-3796, 2017 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-28316756

RESUMO

Cesium lead halide nanocrystals, CsPbX3 (X = Cl, Br, I), exhibit photoluminescence quantum efficiencies approaching 100% without the core-shell structures usually used in conventional semiconductor nanocrystals. These high photoluminescence efficiencies make these crystals ideal candidates for light-emitting diodes (LEDs). However, because of the large surface area to volume ratio, halogen exchange between perovskite nanocrystals of different compositions occurs rapidly, which is one of the limiting factors for white-light applications requiring a mixture of different crystal compositions to achieve a broad emission spectrum. Here, we use mixtures of chloride and iodide CsPbX3 (X = Cl, I) perovskite nanocrystals where anion exchange is significantly reduced. We investigate samples containing mixtures of perovskite nanocrystals with different compositions and study the resulting optical and electrical interactions. We report excitation transfer from CsPbCl3 to CsPbI3 in solution and within a poly(methyl methacrylate) matrix via photon reabsorption, which also occurs in electrically excited crystals in bulk heterojunction LEDs.

4.
ACS Omega ; 2(10): 7275-7280, 2017 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-31457302

RESUMO

The measurement of ζ potential of Ga-face and N-face gallium nitride has been carried out as a function of pH. Both of the faces show negative ζ potential in the pH range 5.5-9. The Ga-face has an isoelectric point at pH 5.5. The N-face shows a more negative ζ potential due to larger concentration of adsorbed oxygen. The ζ potential data clearly showed that H-terminated diamond seed solution at pH 8 will be optimal for the self-assembly of a monolayer of diamond nanoparticles on the GaN surface. The subsequent growth of thin diamond films on GaN seeded with H-terminated diamond seeds produced fully coalesced films, confirming a seeding density in excess of 1011 cm-2. This technique removes the requirement for a low thermal conduction seeding layer like silicon nitride on GaN.

5.
Nano Lett ; 15(11): 7639-43, 2015 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-26488912

RESUMO

Nanocathodoluminescence reveals the spectral properties of individual InGaN quantum wells in high efficiency light emitting diodes. We observe a variation in the emission wavelength of each quantum well, in correlation with the Si dopant concentration in the quantum barriers. This is reproduced by band profile simulations, which reveal the reduction of the Stark shift in the quantum wells by Si doping. We demonstrate nanocathodoluminescence is a powerful technique to optimize doping in optoelectronic devices.

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