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1.
Angew Chem Int Ed Engl ; 59(15): 6187-6191, 2020 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-31972063

RESUMO

Induction heating of magnetic nanoparticles (NPs) is a method to activate heterogeneous catalytic reactions. It requires nano-objects displaying high heating power and excellent catalytic activity. Here, using a surface engineering approach, bimetallic NPs are used for magnetically induced CO2 methanation, acting both as heating agent and catalyst. The organometallic synthesis of Fe30 Ni70 NPs displaying high heating powers at low magnetic field amplitudes is described. The NPs are active but only slightly selective for CH4 after deposition on SiRAlOx owing to an iron-rich shell (25 mL min-1 , 25 mT, 300 kHz, conversion 71 %, methane selectivity 65 %). Proper surface engineering consisting of depositing a thin Ni layer leads to Fe30 Ni70 @Ni NPs displaying a very high activity for CO2 hydrogenation and a full selectivity. A quantitative yield in methane is obtained at low magnetic field and mild conditions (25 mL min-1 , 19 mT, 300 kHz, conversion 100 %, methane selectivity 100 %).

2.
Chemistry ; 24(69): 18436-18443, 2018 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-30125410

RESUMO

Au and Ru nanoparticles (NPs) have been deposited on Siralox® substrate by impregnation and chemical reduction, respectively (Au-Ru-S). The as-prepared material is very active in the selective CO2 methanation to CH4 at temperatures below 250 °C. In addition, Au-Ru-S shows enhanced CH4 production upon irradiation with UV/Vis light starting at temperatures higher than 200 °C, although the contribution of the photoassisted pathway of CH4 production decreases as the temperature increases. Thus, a maximum CH4 production of 204 mmol gRu -1 at 250 °C upon 100 mW cm-2 irradiation was achieved. Control experiments, in which Ru-S and Au-S materials were used, revealed that Ru NPs are the CO2 methanation active sites, while Au NPs contribute by harvesting light, mainly visible as a consequence of the strong Au plasmon band centered at 529 nm. The visible light absorbed by the plasmonic band of Au NPs could make them act ass local heaters of the neighboring Ru NPs, increasing their temperature and enhancing CH4 production.

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