In:
Inorganic Chemistry Frontiers, Royal Society of Chemistry (RSC), Vol. 9, No. 10 ( 2022), p. 2379-2388
Abstract:
Metal–organic frameworks (MOFs) have recently been applied as versatile platforms for constructing efficient catalysts with improved performance in many fields. Herein, for the first time, we prepare a MOF UiO-66 based catalyst showing the synergistic effect of Lewis acid and Pd( ii ) active sites, and it shows highly efficient methyl nitrite (MN) carbonylation to dimethyl carbonate (DMC). Lewis acid sites were first introduced to UiO-66 by adding different amounts of trifluoroacetic acid (TFA) and activating at different temperatures. Pd( ii ) sites were then supported on UiO-66 x - X to obtain the resulting Pd-UiO-66 x - X ( x , the molar percentage of TFA; X , activation temperature). The Lewis acid sites not only act as the center of CO adsorption, but affect the electron density of Pd( ii ) for the generation of more COOCH 3 * intermediates, resulting in a higher catalytic performance. As a result, the best catalytic performance based on the DMC selectivity based on CO ( S DMC/CO ) near 100%, S DMC/MN up to 67.4%, CO conversion to DMC ( C CO ) as high as 68.4%, and the weight time yield (WTY) of DMC up to 2056 g kg cat −1 h −1 was achieved by the composite material Pd-UiO-66 TFA-0.25 -290. This work provides efficient catalysts for carbonylation of MN to DMC and presents a significant synergistic methodology for improving the catalytic performance of MOF materials.
Type of Medium:
Online Resource
ISSN:
2052-1553
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
detail.hit.zdb_id:
2757213-4
