Synergistic effect of the framework boron and Al-rich region to enhance the metal-support interaction for boosting Pd-based catalyst activity of dimethyl carbonate synthesis
Efficient production of dimethyl carbonate (DMC) from methyl nitrite (MN) carbonylation based on PdCu/NaY zeolite catalysts is highly desired for industrial applications. The introduction of boron species into the initial gels of NaY synthesis is a cost-effective modification strategy for boosting the catalytic performance. It not only introduces trace amounts of framework boron but also regulates the distribution of framework aluminum (Al F ) species. Most importantly, the synergistic effect of framework boron and Al-rich region significantly enhanced the metal − support interaction, thus promoting more electrons to be transferred from metal to support. This strategy allows the palladium active species to remain in an electron-deficient state more easily. The carbon monoxide (CO) adsorption and the critical intermediate species *CH 3 COO are more easily formatted on PdCu/NaBY catalyst, which leads to superior weight-time yields (WTY DMC up to 1507·g·kg cat − 1 ·h − 1 ), and CO conversion to DMC (C CO up to 83 %). Our design is of great importance for developing metal-zeolites catalysts, which motivates the industrial application of Pd-based catalysts in the MN carbonation of DMC field.
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