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

Abstract

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 (AlF) 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 *CH3COO are more easily formatted on PdCu/NaBY catalyst, which leads to superior weight-time yields (WTYDMC up to 1507·g·kgcat − 1·h− 1), and CO conversion to DMC (CCO 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.