Optimized Pore Structures of Hierarchical HY Zeolites for Highly Selective Production of Methyl Methoxyacetate

Abstract

Several organic templates were introduced during acid or alkaline treatment to optimize pore structures of hierarchical HY zeolites. The influences of category and concentration of templates on the pore structures and acidity of hierarchical HY zeolites were systemically studied. The N2 adsorption-desorption showed that the micropore amount of the optimized HY zeolites obviously increased, while both the large mesopore size and amount remained almost unchanged. The XRD and NH3-TPD revealed that the optimized HY zeolites exhibited higher relative crystallinity and medium-strong acid sites amount than those of hierarchical HY zeolites produced without the addition of templates. The optimized HY zeolites were used for the synthesis of methyl methoxyacetate (MMAc) from dimethoxymethane (DMM) carbonylation. In comparison with parent HY, the conversion and the selectivity clearly increased from 36.43% to 96.32% and from 11.06% to 92.35%, respectively. The stability of the optimized zeolite was also conducted under the same conditions. The conversion and the selectivity remained nearly unchanged even through 24 h reaction, showing that the performance was extremely stable. The TG-DTA and GC-MS also indicated that the generation of coke was effectively inhibited. This catalyst treatment method, which is facile and highly efficient, provided a route for producing mesoporous zeolites.

Keywords

• hierarchical zeolites
• pore directing agents (pdas)
• dimethoxymethane (dmm)
• carbonylation
• methyl methoxyacetate (mmac)