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Nitrogen-doped graphene-activated metallic nanoparticle-incorporated ordered mesoporous carbon nanocomposites for the hydrogenation of nitroarenes.

ABSTRACT: Herein, nanoscale metallic nanoparticle-incorporated ordered mesoporous carbon catalysts activated by nitrogen-doped graphene (NGr) were fabricated via an efficient multi-component co-assembly of a phenolic resin, nitrate, acetylacetone, the nitrogen-containing compound 1,10-phenanthroline, and Pluronic F127, followed by carbonization. The obtained well-dispersed nitrogen-doped graphene-activated transition metal nanocatalysts possess a 2-D hexagonally arranged pore structure with a high surface area (∼500 m² g^-1) and uniform pore size (∼4.0 nm) and show excellent activity for the selective hydrogenation-reduction of substituted nitroarenes to anilines in an environmentally friendly aqueous solution. The high catalytic performance and durability is attributed to the synergistic effects among the components, the unique structure of the nitrogen-doped graphene layer-coated metallic nanoparticles, and electronic activation of the doped nitrogen.

SUBMITTER: Huang H

PROVIDER: S-EPMC9078627 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Nitrogen-doped graphene-activated metallic nanoparticle-incorporated ordered mesoporous carbon nanocomposites for the hydrogenation of nitroarenes.

Huang Haigen H Wang Xueguang X Sheng Yao Y Chen Chenju C Zou Xiujing X Shang Xingfu X Lu Xionggang X

RSC advances 20180226 16

Herein, nanoscale metallic nanoparticle-incorporated ordered mesoporous carbon catalysts activated by nitrogen-doped graphene (NGr) were fabricated <i>via</i> an efficient multi-component co-assembly of a phenolic resin, nitrate, acetylacetone, the nitrogen-containing compound 1,10-phenanthroline, and Pluronic F127, followed by carbonization. The obtained well-dispersed nitrogen-doped graphene-activated transition metal nanocatalysts possess a 2-D hexagonally arranged pore structure with a high ...[more]

PMID: 35539833

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Project description:One of the most promising solutions to the current energy crisis is an efficient catalytic transformation of abundant low-cost renewable raw biomass into high-quality biofuel. Herein, a highly effective catalyst was constructed systematically for the selective synthesis of 2,5-dimethylfuran (DMF) biofuel from biomass-derived 5-hydroxymethylfurfural (HMF) via green catalytic transfer hydrogenolysis (CTH) using a nitrogen-doped ordered mesoporous carbon (N-CMK-1) decorated ruthenium (Ru)-based catalyst in i-propanol as hydrogen source. The structures and properties of different catalysts were characterized by different characterization techniques such as FTIR, XRD, N2-sorption, CO2-sorption, TGA, TEM, ICP-AES, CHNO analysis, and acid-base back titration. A complete HMF conversion with a high DMF yield of 88% was achieved under optimized reaction conditions. Regarding substrate conversion and product yield, the influence of reaction temperature, time, and hydrogen donors was thoroughly investigated. The nitrogen-promoted carbon support enhanced the dispersion of Ru due to the formation of appropriate basic site density which could efficiently promote the activation of alcohol hydroxyl in i-propanol and subsequent release of active hydrogen species. In the meantime, highly dispersed surface Ru nanoparticles (NPs) were beneficial for hydrogen transfer and activation of both carbonyl and hydroxyl groups in HMF. Moreover, Arrhenius kinetic analysis was studied by identifying 5-methyl furfural (5-MF) and 2,5-bishydroxymethylfuran (BHMF) as two key intermediates that dominate a distinct reaction pathway during hydrogenolysis of HMF to DMF via CTH. Furthermore, high stability without obvious loss of activity after three consecutive cycles was observed in a fabricated N-CMK-1 decorated Ru-based catalyst as a result of superior metal-support interaction and the mesoporous framework nature of the catalyst. These findings would not only offer a robust catalyst synthetic approach but also open a new avenue for the exploitation of biomass to specialty chemicals and advanced biofuels.

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Nitrogen-doped graphene-activated metallic nanoparticle-incorporated ordered mesoporous carbon nanocomposites for the hydrogenation of nitroarenes.

Publications

Nitrogen-doped graphene-activated metallic nanoparticle-incorporated ordered mesoporous carbon nanocomposites for the hydrogenation of nitroarenes.

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