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1.
Nat Commun ; 15(1): 3868, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38719793

RESUMO

This study introduces a distributed electrified heating approach that is able to innovate chemical engineering involving endothermic reactions. It enables rapid and uniform heating of gaseous reactants, facilitating efficient conversion and high product selectivity at specific equilibrium. Demonstrated in catalyst-free CH4 pyrolysis, this approach achieves stable production of H2 (530 g h-1 L reactor -1) and carbon nanotube/fibers through 100% conversion of high-throughput CH4 at 1150 °C, surpassing the results obtained from many complex metal catalysts and high-temperature technologies. Additionally, in catalytic CH4 dry reforming, the distributed electrified heating using metallic monolith with unmodified Ni/MgO catalyst washcoat showcased excellent CH4 and CO2 conversion rates, and syngas production capacity. This innovative heating approach eliminates the need for elongated reactor tubes and external furnaces, promising an energy-concentrated and ultra-compact reactor design significantly smaller than traditional industrial systems, marking a significant advance towards more sustainable and efficient chemical engineering society.

2.
Sci Rep ; 14(1): 3966, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38368434

RESUMO

Producing sustainable anode materials for lithium-ion batteries (LIBs) through catalytic graphitization of renewable biomass has gained significant attention. However, the technology is in its early stages due to the bio-graphite's comparatively low electrochemical performance in LIBs. This study aims to develop a process for producing LIB anode materials using a hybrid catalyst to enhance battery performance, along with readily available market biochar as the raw material. Results indicate that a trimetallic hybrid catalyst (Ni, Fe, and Mn in a 1:1:1 ratio) is superior to single or bimetallic catalysts in converting biochar to bio-graphite. The bio-graphite produced under this catalyst exhibits an 89.28% degree of graphitization and a 73.95% conversion rate. High-resolution transmission electron microscopy (HRTEM) reveals the dissolution-precipitation mechanism involved in catalytic graphitization. Electrochemical performance evaluation showed that the trimetallic hybrid catalyst yielded bio-graphite with better electrochemical performances than those obtained through single or bimetallic hybrid catalysts, including a good reversible capacity of about 293 mAh g-1 at a current density of 20 mA/g and a stable cycle performance with a capacity retention of over 98% after 100 cycles. This study proves the synergistic efficacy of different metals in catalytic graphitization, impacting both graphite crystalline structure and electrochemical performance.

3.
ChemSusChem ; 15(15): e202200753, 2022 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-35504842

RESUMO

N-heteroarenes represents one of the most important chemicals in pharmaceuticals and other bio-active molecules, which can be easily accessed from the oxidation of N-heterocycles over metal catalysts. Herein, the metal-free oxidative dehydrogenation of N-heterocycles into N-heteroarenes was developed using molecular oxygen as the terminal oxidant. The nitrogen-doped carbon materials were facilely prepared via the simple pyrolysis process using biomass (carboxymethyl cellulose sodium) and dicyandiamide as the carbon and nitrogen source, respectively, and they were discovered to be robust for the oxidative dehydrogenation of N-heterocycles into N-heteroarenes under mild conditions (80 °C under 1 bar O2 ) with water as the green solvent. Diverse N-heterocycles including 1,2,3,4-tetrahydroisoquinolines, indolines and 1,2,3,4-tetrahydroquinoxalines were smoothly converted into N-heteroarenes with high to excellent yields (76->99 %). Superoxide radical (⋅O2 - ) and hydroxyl radical (⋅OH) were probed as the reactive oxygen species for the oxidation of N-heterocycles into N-heteroarenes. More importantly, the nitrogen-doped carbon catalyst can be reused with a high stability. The method provides an environmentally friendly and economical route to access important N-hetero-aromatic commodities.


Assuntos
Carbono , Nitrogênio , Carbono/química , Catálise , Metais , Nitrogênio/química , Oxirredução , Estresse Oxidativo
4.
Chem Commun (Camb) ; 58(25): 4067-4070, 2022 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-35262544

RESUMO

The Meerwein-Ponndorf-Verley (MPV) reaction is an important chemoselective route for carbonyl group hydrogenation, and thus designing new and effective catalysts for this transformation remains important and challenging. In this work, a new sulfonate coordinated Zr(IV) catalyst was prepared by the coordination of Zr(IV) onto the sulfonate groups of Amberlyst-15, which can effectively catalyze the MPV reaction and quantitatively convert carbonyl compounds to the corresponding alcohols with high reactivity and stability. Detailed mechanistic investigations reveal that the catalytic performance of Zr-AIER can be attributed to the synergetic effect between Zr4+ and the sulfonate group, and the porous structure with high surface area.

5.
ChemSusChem ; 12(6): 1246-1255, 2019 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-30600939

RESUMO

An efficient method was developed for the synthesis of primary amines either from the hydrogenation of nitriles or reductive amination of carbonyl compounds. The reactions were catalyzed by nitrogen-doped mesoporous carbon (MC)-supported nickel nanoparticles (abbreviated as MC/Ni). The MC/Ni catalyst demonstrated high catalytic activity for the hydrogenation of nitriles into primary amines in high yields (81.9-99 %) under mild reaction conditions (80 °C and 2.5 bar H2 ). The MC/Ni catalyst also promoted the reductive amination of carbonyl compounds for the synthesis of primary amines at 80 °C and 1 bar H2 . The hydrogenation of nitriles and the reductive amination proceeded through the same intermediates for the generation of the primary amines. To the best of our knowledge, no other heterogeneous non-noble metal catalysts have been reported for the synthesis of primary amines under mild conditions, both from the hydrogenation of nitriles and reductive amination.

6.
J Colloid Interface Sci ; 415: 117-26, 2014 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-24267338

RESUMO

Ionic liquid (1-butyl-2,3-dimethylimidazolium acetate, [BMMIm]OAc)-Pluronic P123 mixed micelle stabilized water-soluble Ni nanoparticles were characterized by UV-vis, XRD, XPS and TEM and then employed for catalytic hydrogenation. It was demonstrated that the mixed-micelle stabilized Ni NPs showed excellent catalytic performance for the selective hydrogenation of CC and nitro compounds in the aqueous phase under very mild reaction conditions, and also the Ni NPs catalysts can be recycled at least for eight times without significant decrease in catalytic activity. The results of characterization revealed that the mixed micelle-stabilized Ni NPs catalysts were highly dispersed in aqueous phases even after five catalytic recycles. In addition, adding ionic liquid ([BMMIm]OAc) can affect the micelle structure of P123 solutions and thus afford an additional steric protection from aggregation of Ni NPs, resulting in enhancing stability and catalytic activity of Ni NPs.


Assuntos
Imidazóis/química , Líquidos Iônicos/química , Nanopartículas Metálicas/química , Níquel/química , Poloxaleno/química , Alcenos/química , Catálise , Reutilização de Equipamento , Hidrogenação , Nanopartículas Metálicas/ultraestrutura , Micelas , Microscopia Eletrônica de Transmissão , Nitrocompostos/química , Espectroscopia Fotoeletrônica , Água/química
7.
Chemistry ; 19(6): 2059-66, 2013 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-23255466

RESUMO

The use of transition-metal nanoparticles/ionic liquid (IL) as a thermoregulated and recyclable catalytic system for hydrogenation has been investigated under mild conditions. The functionalized ionic liquid was composed of poly(ethylene glycol)-functionalized alkylimidazolium as the cation and tris(meta-sulfonatophenyl)phosphine ([P(C(6)H(4)-m-SO(3))(3)](3-)) as the anion. Ethyl acetate was chosen as the thermomorphic solvent to avoid the use of toxic organic solvents. Due to a cooperative effect regulated by both the cation and anion of the ionic liquid, the nanocatalysts displayed distinguished temperature-dependent phase behavior and excellent catalytic activity and selectivity, coupled with high stability. In the hydrogenation of α,ß-unsaturated aldehydes, the ionic-liquid-stabilized palladium and rhodium nanoparticles exhibited higher selectivity for the hydrogenation of the C=C bonds than commercially available catalysts (Pd/C and Rh/C). We believe that the anion of the ionic liquid, [P(C(6)H(4)-m-SO(3))(3)](3-), plays a role in changing the surrounding electronic characteristics of the nanoparticles through its coordination capacity, whereas the poly(ethylene glycol)-functionalized alkylimidazolium cation is responsible for the thermomorphic properties of the nanocatalyst in ethyl acetate. The present catalytic systems can be employed for the hydrogenation of a wide range of substrates bearing different functional groups. The catalysts could be easily separated from the products by thermoregulated phase separation and efficiently recycled ten times without significant changes in their catalytic activity.

8.
Langmuir ; 26(4): 2505-13, 2010 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-20039597

RESUMO

The preparation, characterization, and catalytic properties of water-soluble palladium nanoparticles stabilized by the functionalized-poly(ethylene glycol) as a protective ligand were demonstrated for aerobic oxidation of alcohols in aqueous phase. UV/vis spectra and X-ray photoelectron spectroscopy (XPS) proved that there was an electronic interaction between the bidentate nitrogen ligand and palladium atoms. Transmission electron microscopy and XPS analysis showed that the particle size and surface properties of the generated palladium nanoparticles can be controlled by varying the amount of protective ligand and the kinds of reducing agents. It was found that both the size and surface properties of palladium nanoparticles played very important roles in affecting catalytic performance. The stabilized metallic palladium nanoparticles were proven to be the active centers for benzyl alcohol oxidation in the present system, and the water-soluble Pd nanocatalysts can also be extended to the selective oxidation of various alcohols.


Assuntos
Álcoois/química , Nanopartículas Metálicas/química , Paládio/química , Polietilenoglicóis/química , Água/química , Oxirredução , Tamanho da Partícula , Solubilidade , Propriedades de Superfície
9.
Ying Yong Sheng Tai Xue Bao ; 14(8): 1391-4, 2003 Aug.
Artigo em Chinês | MEDLINE | ID: mdl-14655382

RESUMO

Epiblema strenuana is the most important natural enemy against Ambrosia artemisiifolia, A. trifida and Parthenium hysterophorus. In this paper, its ecological adaptability and application risk as a biological agent against ragweed was analyzed and reviewed. Epiblema strenuana had a restrict host specificity, with all the field hosts belonging to Ambrosinae, and its selective risk on sunflower and chrysanthemum was less than 0.01 or/and zero (no risk). 15-35 degrees C was the suitable temperature regimes for E. strenuana to develop, and lower constraint temperature could reach -8(-)-12 degrees C. The population size of this insect could increase 23 and 4 times on A. artemisiifolia, A. trifida and Xanthium sibiricum after each generation, respectively. In the field, the infected plants had an average of 20-30 galls per plant, and died with 5.2 and 26 galls before and after rosette stage. The spread distance of this moth within 12 months after release was more than 100 km. It indicated that E. strenuana was an effective and safe agent for cereal and economic crops, ornamental plants, and indigenous natural enemy in the introduced region.


Assuntos
Ambrosia , Ecologia , Mariposas/fisiologia , Controle Biológico de Vetores/métodos , Adaptação Fisiológica , Animais , Segurança
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