Abstract
With increasing applications of metal-organic frameworks (MOFs) in the field of gas separation and catalysis, the preparation and performance research of encapsulating metal nanoparticles (NPs) into MOFs (M@MOF) have attracted extensive attention recently. Herein, an Ru@UiO-66 catalyst is prepared by a one-step method. Ru NPs are encapsulated in situ in the UiO-66 skeleton structure during the synthesis of UiO-66 metal-organic framework via a solvothermal method, and its catalytic activity for CO2 methanation with the synergy of cold plasma is studied. The crystallinity and structural integrity of UiO-66 is maintained after encapsulating Ru NPs according to the X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). As illustrated by X-ray photoelectron spectroscopy (XPS), high resolution transmission electron microscopy (HRTEM), and mapping analysis, the Ru species of the hydration ruthenium trichloride precursor are reduced to metallic Ru NPs without additional reducing processes during the synthesis of Ru@UiO-66, and the Ru NPs are uniformly distributed inside the Ru@UiO-66. Thermogravimetric analysis (TGA) and N2 sorption analysis show that the specific surface area and thermal stability of Ru@UiO-66 decrease slightly compared with that of UiO-66 and was ascribed to the encapsulation of Ru NPs in the UiO-66 skeleton. The results of plasma-assisted catalytic CO2 methanation indicate that Ru@UiO-66 exhibits excellent catalytic activity. CO2 conversion and CH4 selectivity over Ru@UiO-66 reached 72.2% and 95.4% under 13.0 W of discharge power and a 30 mL·min−1 gas flow rate (), respectively. Both values are significantly higher than pure UiO-66 with plasma and Ru/Al2O3 with plasma. The enhanced performance of Ru@UiO-66 is attributed to its unique framework structure and excellent dispersion of Ru NPs.
Highlights
Metal-organic frameworks (MOFs) are a series of porous crystal materials self-assembled by metal ions and organic ligands through coordination bonds [1,2,3]
We report a simple and efficient method for synthesizing Ru@UiO-66 via in situ encapsulation of Ru NPs by the reduction of the RuCl3 precursor during the growth of UiO-66 framework structure
The crystallinity and structural integrity of UiO-66 were maintained well after encapsulating Ru NPs, and the Ru NPs were uniformly distributed inside the framework of UiO-66
Summary
Metal-organic frameworks (MOFs) are a series of porous crystal materials self-assembled by metal ions and organic ligands through coordination bonds [1,2,3]. To synthesize the above MOFs-supported metal catalysts, there are two or more steps required, the synthesis of the MOF support and the impregnation, and the reduction of the supported/encapsulated metal precursors in the presence of reducing agents [18]. This process is generally sophisticated and time-consuming. We report a simple and efficient method for synthesizing Ru@UiO-66 via in situ encapsulation of Ru NPs by the reduction of the RuCl3 precursor during the growth of UiO-66 framework structure. The synthesized Ru@UiO-66 exhibits high performance for plasma-assisted catalytic CO2 methanation
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