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1.
ACS Appl Mater Interfaces ; 16(9): 11575-11584, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38400846

RESUMO

Hydrogen production from organic waste by gasification and reforming technologies offers major benefits to both the environment and climate. The long-term stability and regeneration of the reforming catalyst are still the biggest challenges because of carbon deposition. Here we report a recyclable salt-supported nickel oxide NiO/NaX (X: F, Cl, Br) catalyst for effective autothermal reforming of the oxygenated volatile organic compound (OVOC) ethyl acetate to hydrogen. The optimal hydrogen selectivity achieved 82.0% at 650 °C and the durability reached 43 h. Interestingly, with the decreasing of halogen electronegativity (F > Cl > Br) in NaX, the corresponding hydrogen selectivity of the catalysts decreased. Although NiO/NaX catalysts possess a very small specific surface area and a dense microstructure, their catalytic performance is better than that of normal Ni-based catalysts loaded on high-specific-surface-area supports. Detailed investigations revealed the critical roles played by halogen during the reforming reaction. First, the strong electronegative halogen in NaX induced the formation of hydrogen bonds with the reactants and reaction intermediates, which may prolong the surface residence time of such species, thus ensuring efficient hydrogen production over small-specific-surface-area catalysts under high-temperature conditions. Second, the halogen of the support NaX weakening the Ni-O bonds of the exposed Ni atoms in NiO/NaX made it easier for NiO to be reduced to Ni0, thus reducing the reaction activation energy and prompting the rapid catalytic reaction. The strength of such metal-support interaction can be easily modulated by varying the halogen electronegativity. This study provides a new prospect for the design of innovative recyclable heterogeneous catalysts with low specific surface area but high activity.

2.
Molecules ; 27(19)2022 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-36234926

RESUMO

A cascade 6-endo-dig cyclization reaction was developed for the switchable synthesis of halogen and non-halogen-functionalized pyrazolo[3,4-b]pyridines from 5-aminopyrazoles and alkynyl aldehydes via C≡C bond activation with silver, iodine, or NBS. In addition to its wide substrate scope, the reaction showed good functional group tolerance as well as excellent regional selectivity. This new protocol manipulated three natural products, and the arylation, alkynylation, alkenylation, and selenization of iodine-functionalized products. These reactions demonstrated the potential applications of this new method.


Assuntos
Produtos Biológicos , Iodo , Aldeídos/química , Iodo/química , Estrutura Molecular , Pirazóis , Piridinas/química , Prata
3.
Chin J Traumatol ; 3(2): 124-125, 2000 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-11874656

RESUMO

From 1981 to 1997, 26 cases of myositis ossificans circumscripta (MOC) were diagnosed and treated in our hospital, 22 of whom, occupying 84.6%, were confirmed by pathological examination. All the clinic data are reported as follows.

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