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1.
Inorg Chem ; 61(1): 633-642, 2022 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-34915701

RESUMO

Carbon-based catalysts are found to be promising metal-free species for aerobic oxidative desulfurization of fuel oil. Thus, a proper approach to promote their catalytic performances is very much in demand. In this contribution, a heteroatom bridging strategy is proposed to enhance the catalytic activities of carbon-based catalysts. As proof of the strategy, a series of boron (B)-doped graphite catalysts were synthesized. Detailed characterizations showed that the hetero-B atoms were uniformly dispersed in graphite. More importantly, it was found that the doped B atoms functioned as a bridge for electron transfer. With the existence of the heteroatom bridge, the activation of oxygen by graphite during the catalytic oxidation process was enhanced remarkably, leading to an ultradeep oxidative desulfurization performance. Moreover, the catalyst can be readily recycled five times without a significant decrease in desulfurization performance.

2.
Angew Chem Int Ed Engl ; 59(21): 8042-8046, 2020 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-32203632

RESUMO

Although hexagonal boron nitride (h-BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas-phase methyl radicals (CH3 . ) in the ODHP reaction over boron-based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV-PIMS), which uncovers the existence of gas-phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C-H activation of propane, while C2 and C1 products can be formed via both surface-mediated and gas-phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron-based catalysts.

3.
J Hazard Mater ; 391: 122183, 2020 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-32036308

RESUMO

Metal-free catalysts have been proved to be a low-cost and environmentally friendly species in aerobic oxidative desulfurization (ODS). In this work, exfoliated metal-free boron carbide with few-layered structure, small size, and abundant defects, was first employed in an aerobic ODS system for ultra-deep desulfurization. The exfoliation process was realized by employing a planetary ball mill strategy. Detailed characterizations showed that the ball milling process not only induces thinner layers and small sizes but also introduces numerous defects into the boron carbide catalysts, which is vital in metal-free catalysis. Furthermore, the exfoliated boron carbide catalyst was applied in aerobic ODS system, and 99.5 % of sulfur removal was obtained. Moreover, the catalyst can be recycled 17 times without a significant decrease in catalytic activity. In particular, it was found that ∼90 % of the sulfur compounds in real diesel oil could be removed by the current aerobic ODS system.

4.
ACS Appl Mater Interfaces ; 11(40): 36666-36675, 2019 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-31525889

RESUMO

Surface oxygen vacancy can greatly affect the properties of transition-metal oxides. However, engineering oxygen vacancy-abundant transition-metal oxides with high specific surface area (SSA) remains challenging. At present, the generation of oxygen vacancies in metal oxides is time-consuming and less environmentally friendly by chemical leaching methods that usually require additional waste treatment. Herein, a series of oxygen vacancy-abundant transition-metal oxides with high SSA are constructed via a lattice refining strategy. This strategy is realized by urea-assisted ball milling pyrolysis and is green, efficient, and universal. The oxygen vacancies promote the mobility of oxygen, leading to a boosted catalytic oxidation performance of aromatic sulfides. Such a strategy provides an efficient approach to manufacturing oxygen vacancies on transition-metal oxides, which may be beneficial for various related applications as an effective catalytic material.

5.
Int J Biol Macromol ; 82: 607-13, 2016 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-26522247

RESUMO

A polysaccharide termed Se-GP11 was extracted and purified from Se-enriched Grifola frondosa in our previous study. This study investigated the characterization, anti-tumor and immunomodulatory activity of Se-GP11. The results showed that Se-GP11 was composed of mannose, glucose and galactose with a molar ratio of 1:4.91:2.41. The weight-average molecular weight (Mw) and weight-average mean square radius (Rw) of Se-GP11 in 0.1M sodium chloride solution were 3.3×10(4)Da and 32.8 nm. Se-GP11 existed as a globular conformation with random coil structure. Se-GP11 had no anti-tumor activity against HepG-2 cells in vitro, and it significantly inhibited the growth of Heps tumor in vivo. Se-GP11 increased the relatively thymus and spleen weights as well as serum necrosis factor-alpha (TNF-α) and interleukin-2 (IL-2) levels. In addition, Se-GP11 promoted the phagocytosis and NO production of RAW264.7 as compared with that of the normal control group. The results revealed that the Se-GP11 may exhibit the anti-tumor through improving immunologic function of the tumor bearing mice.


Assuntos
Antineoplásicos/química , Antineoplásicos/farmacologia , Polissacarídeos Fúngicos/química , Polissacarídeos Fúngicos/farmacologia , Grifola/química , Fatores Imunológicos/química , Fatores Imunológicos/farmacologia , Selênio/química , Animais , Biomarcadores , Linhagem Celular Tumoral , Modelos Animais de Doenças , Feminino , Humanos , Ativação de Macrófagos/efeitos dos fármacos , Macrófagos/efeitos dos fármacos , Macrófagos/imunologia , Macrófagos/metabolismo , Camundongos , Ensaios Antitumorais Modelo de Xenoenxerto
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