Tailor-made the ultrathin nanosheet and acid site accessibility of mordenite zeolite for carbonylation of dimethyl ether

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Precisely tailored nano-morphology and crystal growth endures mordenite (MOR) zeolites with reduced internal diffusion resistance, enabling greater accessibility of existing acid sites to further stimulate catalysis. Controllable synthesis nanosheet MOR zeolite thinner than 20 nm along at least one dimension is highly attractive but remains great challenge. Herein, c axis along the [001] direction shortened MOR nanosheets with a thickness of 10–20 nm was synthesized. As expected, the mass transfer performance over the nanosheet sample is significantly improved by 2.5 times compared with the conventional nano-morphology. Furthermore, more Brønsted acid sites (BAS) can be induced into 8-membered ring (8-MR) pores in the nanosheet MOR zeolite. The conversion of dimethyl ether (DME) to methyl acetate over the ultrathin MOR zeolite is increased from 17.4 % to 71.7 % compared to that of the conventional nanoparticle. The DME conversion was stable at 70.0 % after reaction 80 h, when the acid sites located in 12-membered ring pores was poisoned by the pyridine molecule. Unexpectedly, we discovered that the desorption behavior of pyridine is also influenced by the accessibility of acid site, not only by the amount of BAS in 8-MR. The unique nanosheet structure with short c axis reduces the spatial stability of pyridine adsorbed on BAS in the 8-MR side pocket and the BAS in the 8-MR side pocket can be recovered at lower temperatures. Herein, a new insight into of DME carbonylation catalyzed by ultrathin nanosheet of MOR zeolite is revealed.