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1.
Chem Soc Rev ; 50(9): 5590-5630, 2021 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-33690780

RESUMO

Catalytic non-oxidative direct dehydrogenation of light alkanes serves as an effective reinforcement to selectively produce the corresponding olefins, and the heterogeneous metals and metal oxides, not limited to the commercially used Pt- and Cr-based catalysts, are widely investigated to enhance the efficiency. In this review, we outline the progress of these dehydrogenation catalysts that have been mainly developed in the past five years. For different classes of the most-promising catalysts in the selective dehydrogenation of ethane-to-ethylene and propane-to-propylene, their syntheses, structural information, catalytic properties and mechanisms are comparatively summarized.

2.
J Cell Physiol ; 235(11): 7681-7695, 2020 11.
Artigo em Inglês | MEDLINE | ID: mdl-32324301

RESUMO

Despite the administration of new effective drugs in recent years, relapse and drug resistance are still the main obstacles in multiple myeloma (MM) treatment, making MM an incurable disease. To overcome drug resistance in MM, it is critical to understand the underlying mechanisms of malfunctioning gene expression and develop novel targeted therapies. During the past few decades, with the discovery and characterization of noncoding RNAs (ncRNAs), the landscape of dysregulated ncRNAs of cancers as well as their biological and pathobiological functions in tumorigenesis and drug resistance have been recognized. Studies about ncRNAs improved the understanding of variations of drug response among individuals at a level distinguished from genetic polymorphism, and provided with new orientations for targeted therapies. In this review, we will summarize the emerging impact and underlying molecular mechanisms of the most relevant classes of ncRNAs in drug resistance of MM, and discuss the potential as well as strategies of treating ncRNAs as therapeutic targets.


Assuntos
Resistencia a Medicamentos Antineoplásicos/genética , Mieloma Múltiplo/genética , RNA não Traduzido/genética , Animais , Regulação Neoplásica da Expressão Gênica/genética , Humanos , Mieloma Múltiplo/tratamento farmacológico
3.
Angew Chem Int Ed Engl ; 58(44): 15863-15868, 2019 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-31411807

RESUMO

A molecular design strategy is used to construct ordered mesoporous Ti3+ -doped Li4 Ti5 O12 nanocrystal frameworks (OM-Ti3+ -Li4 Ti5 O12 ) by the stoichiometric cationic coordination assembly process. Ti4+ /Li+ -citrate chelate is designed as a new molecular precursor, in which the citrate can not only stoichiometrically coordinate Ti4+ with Li+ homogeneously at the atomic scale, but also interact strongly with the PEO segments in the Pluronic F127. These features make the co-assembly and crystallization process more controllable, thus benefiting for the formation of the ordered mesostructures. The resultant OM-Ti3+ -Li4 Ti5 O12 shows excellent rate (143 mAh g-1 at 30 C) and cycling performances (<0.005 % fading per cycle). This work could open a facile avenue to constructing stoichiometric ordered mesoporous oxides or minerals with highly crystalline frameworks.

4.
ACS Nano ; 16(10): 15681-15704, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36121680

RESUMO

The electrochemical carbon dioxide reduction reaction (CO2RR) is a promising method to realize carbon recycling and sustainable development because of its mild reaction conditions and capability to utilize the electric power generated by renewable energy such as solar, wind, or tidal energy to produce high-value-added liquid fuels and chemicals. However, it is still a great challenge to deeply understand the reaction mechanism of CO2RRs involving multiple chemical processes and multiple products due to the complexity of the traditional catalyst's surface. Organic ligand-protected metal nanoclusters (NCs) with accurate compositions and definite atom packing structures show advantages for revealing the reaction mechanism of CO2RRs. This Review focuses on the recent progress in CO2RRs catalyzed by atomically precise metal NCs, including gold, copper, and silver NCs. Particularly, the influences of charge, ligand, surface structure, doping of Au NCs, and binders on the CO2RR are discussed in detail. Meanwhile the reaction mechanisms of CO2RRs including the active sites and the key reaction intermediates are also discussed. It is expected that progress in this research area could promote the development of metal NCs and CO2RRs.

5.
Front Oncol ; 10: 577890, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-33194698

RESUMO

In recent years, emerging evidence has suggested that noncoding RNAs (ncRNAs) participate in nearly every aspect of biological processes and play a crucial role in the genesis and progression of numerous tumors, including B-cell lymphoma. The exploration of ncRNA dysregulations and their functions in B-cell lymphoma provides new insights into lymphoma pathogenesis and is essential for indicating future clinical trials and optimizing the diagnostic and therapeutic strategies. In this review, we summarize the role of ncRNAs in B-cell lymphoma and discuss their potential in clinical applications.

6.
ACS Appl Mater Interfaces ; 12(2): 2516-2524, 2020 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-31854963

RESUMO

The heterogeneous hydrogenation of α,ß-unsaturated compounds requires understanding of the structure-activity relationship of metallic catalysts in consideration of solvent-mediated processes. In this work, a CoAl hydrotalcites (CoAl-HTs)-supported Pt nanoparticle catalyst is employed to study the effect of solvent water and HTs interlayer water on the aqueous-phase selective hydrogenation of cinnamaldehyde (CALD). Pt/Co2Al1-HTs catalyst displays 5075 h-1 of specific reaction rate and 89% of C═O hydrogenation selectivity at 80 °C under 20 bar of H2. Combined results of isotope-labeling experiments and theoretical DFT calculations demonstrate that the water-mediated hydrogen-exchange pathway exists in the reaction with a relatively lower-energy barrier in comparison to the direct H2-dissociated hydrogenation pathway. The results also reveal that the interlayer water species of HTs support participate in the hydrogen-exchange reaction. Based on the H2-D2 exchange results, these HTs interlayer water species can promote H2 activation and dissociation processes and thus accelerate the CALD hydrogenation reaction even under solvent-free conditions.

8.
ChemSusChem ; 7(6): 1557-67, 2014 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-24798653

RESUMO

The transformation of cellulose or cellulose-derived carbohydrates into platform chemicals is the key to establish biomass-based sustainable chemical processes. The systems able to catalyze the conversion of cellulose into key chemicals in water without the consumption of hydrogen are limited. We report that simple vanadyl (VO(2+)) cations catalyze the conversions of cellulose and its monomer, glucose, into lactic acid and formic acid in water. We have discovered an interesting shift of the major product from formic acid to lactic acid on switching the reaction atmosphere from oxygen to nitrogen. Our studies suggest that VO(2+) catalyzes the isomerization of glucose to fructose, the retro-aldol fragmentation of fructose to two trioses, and the isomerization of trioses, which leads to the formation of lactic acid under anaerobic conditions. The oxidative cleavage of C-C bonds in the intermediates caused by the redox conversion of VO2(+)/VO(2+) under aerobic conditions results in formic acid and CO2. We demonstrate that the addition of an alcohol suppresses the formation of CO2 and enhances the formic acid yield significantly to 70-75 %.


Assuntos
Celulose/química , Formiatos/química , Ácido Láctico/química , Compostos de Vanádio/química , Catálise , Glucose/química , Oxigênio/química
9.
Nat Commun ; 4: 2141, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23846730

RESUMO

The direct transformation of cellulose, which is the main component of lignocellulosic biomass, into building-block chemicals is the key to establishing biomass-based sustainable chemical processes. Only limited successes have been achieved for such transformations under mild conditions. Here we report the simple and efficient chemocatalytic conversion of cellulose in water in the presence of dilute lead(II) ions, into lactic acid, which is a high-value chemical used for the production of fine chemicals and biodegradable plastics. The lactic acid yield from microcrystalline cellulose and several lignocellulose-based raw biomasses is >60% at 463 K. Both theoretical and experimental studies suggest that lead(II) in combination with water catalyses a series of cascading steps for lactic acid formation, including the isomerization of glucose formed via the hydrolysis of cellulose into fructose, the selective cleavage of the C3-C4 bond of fructose to trioses and the selective conversion of trioses into lactic acid.


Assuntos
Celulose/química , Ácido Láctico/síntese química , Chumbo/química , Água/química , Biomassa , Catálise , Glucose/química , Temperatura Alta , Hidrólise , Cinética , Espectrometria de Massas em Tandem , Termodinâmica
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