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1.
J Colloid Interface Sci ; 625: 640-650, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35764044

RESUMO

Chemoselective hydrogenation of unsaturated organic compounds is a significant research topic in the catalysis field. Herein, a sulfur-doped ordered mesoporous carbon (SMC) material was prepared to anchor ultrafine platinum (Pt) clusters for the chemoselective hydrogenation of halogenated nitroarenes. The confinement effect of the ordered pores and the strong metal-support interaction caused by Pt clusters and sulfur atoms, efficiently suppress the aggregation and regulate the electronic states of the ultrafine Pt clusters. Thus, the hydrogenation of parachloronitrobenzene (p-CNB) shows high selectivity catalyzed by the ultrafine Pt clusters with electron-rich states. Meanwhile, the catalytic performance of the hydrogenation reaction catalyzed by Pt/SMC is capable of being maintained after at least 5 cycles, and the catalytic universality can also be applied to different halogenated nitroarenes hydrogenation. Therefore, this study may promote the research into the construction of noble metal-based catalysts for chemoselective hydrogenation reactions in green and sustainable chemical processes.

2.
J Colloid Interface Sci ; 623: 905-914, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35636298

RESUMO

The catalytic transformation of the biomass platform compound levulinic acid (LA) to γ-valerolactone (GVL) is a vital reaction to produce related renewable chemicals and fuels. Developing stable catalysts with highly dispersed and accessible ultrafine metal nanoparticle (NP) active sites for the hydrogenation of LA under solvent-free conditions is still a major challenge. Herein, a versatile nano-emulsion self-assembly method was employed to fabricate N-doped carbon nanospheres with a high specific surface area and hierarchically porous structure. Ultrafine Ru NPs were successfully anchored on the hierarchal porous N-doped carbon nanospheres (HPNC) with high dispersion. The obtained Ru/HPNC catalyst exhibited excellent catalytic performance for LA hydrogenation to GVL under solvent-free conditions with outstanding reusability. In contrast, Ru NPs embedded in other supports (including activated carbon and carbon nanotubes) were observed to be less effective under the same reaction conditions. The superior catalytic performance of the Ru/HPNC catalyst is due to the hierarchically porous catalyst structure, and accessible ultrafine Ru active sites which can promote the activation of CO bonds and H2 absorption during the catalytic process. The reaction pathway of LA hydrogenation to GVL is clearly researched by theoretical calculations. Thus, the current work provides a facile strategy for the synthesis of highly dispersed ultrafine metal NP-based catalysts for an important biomass transformation.


Assuntos
Nanosferas , Nanotubos de Carbono , Hidrogenação , Lactonas , Ácidos Levulínicos , Porosidade , Solventes
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