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1.
J Am Chem Soc ; 137(3): 1362-71, 2015 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-25603470

RESUMO

It is a dream that future synthetic chemistry can mimic living systems to process multistep cascade reactions in a one-pot fashion. One of the key challenges is the mutual destruction of incompatible or opposing reagents, for example, acid and base, oxidants and reductants. A conceptually novel strategy is developed here to address this challenge. This strategy is based on a layered Pickering emulsion system, which is obtained through lamination of Pickering emulsions. In this working Pickering emulsion, the dispersed phase can separately compartmentalize the incompatible reagents to avoid their mutual destruction, while the continuous phase allows other reagent molecules to diffuse freely to access the compartmentalized reagents for chemical reactions. The compartmentalization effects and molecular transport ability of the Pickering emulsion were investigated. The deacetalization-reduction, deacetalization-Knoevenagel, deacetalization-Henry and diazotization-iodization cascade reactions demonstrate well the versatility and flexibility of our strategy in processing the one-pot cascade reactions involving mutually destructive reagents.


Assuntos
Compostos Orgânicos/química , Emulsões/química , Estrutura Molecular , Tamanho da Partícula , Água/química
2.
Chem Commun (Camb) ; 50(70): 10045-8, 2014 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-24942157

RESUMO

A series of mesoporous silica-based catalysts with finely-tuned surface wettability have been synthesized, of which the catalysis efficiency towards aqueous hydrogenations is highly dependent on their surface wettability and can be five times higher than that of the commercial Pd/C catalyst.


Assuntos
Dióxido de Silício/química , Água/química , Água/metabolismo , Molhabilidade , Catálise , Nanosferas/química , Nanosferas/metabolismo , Porosidade
3.
Chemphyschem ; 15(5): 841-8, 2014 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-24692297

RESUMO

With the recent advances in nanoscience and nanotechnology, more and more nanoparticle catalysts featuring high accessibility of active sites and high surface area have been explored for their use in various chemical transformations, and their rise in popularity among the catalysis community has been unprecedented. The industrial applications of these newly discovered catalysts, however, are hampered because the existing methods for separation and recycling, such as filtration and centrifugation, are generally unsuccessful. These limitations have prompted development of new methods that facilitate separation and recycling of nanoparticle catalysts, so as to meet the burgeoning demands of green and sustainable chemistry. Recently, we have found that Pickering-emulsion inversion is an appealing strategy with which to realize in situ separation and recycling of nanoparticle catalysts and thereby to establish sustainable catalytic processes. We feel that at such an early stage, this strategy, as an alternative to conventional methods, is conceptually new for readers but that it has potential to become a popular method for green catalysis. This Concept article aims to provide a timely link between previous efforts and both current and future research on nanoparticle catalysts, and is expected to facilitate further investigation into this strategy.


Assuntos
Emulsões/química , Nanopartículas/química , Catálise , Concentração de Íons de Hidrogênio
4.
ChemSusChem ; 7(2): 391-6, 2014 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-24376132

RESUMO

A general strategy that avoids stirring for organic/aqueous reactions involving solid catalysts is reported. The strategy involves converting a conventional biphasic system into a Pickering emulsion phase with micrometer-scale droplets ensuring good mixing. In test reactions, nitrotoluene reduction and epoxidation of allylic alcohols, the reaction efficiency is comparable to conventional stirrer-driven biphasic catalysis reaction systems. Short diffusion distances, arising from the compartmentalization of densely packed droplets, play an important role in boosting the reaction efficiency.


Assuntos
Emulsões/química , Microtecnologia/métodos , Cinética , Compostos Orgânicos/química , Água/química
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