Boosting the propylene selectivity over embryonic borosilicate zeolite catalyst for oxidative dehydrogenation of propane

Boron-containing zeolites have been proven potential in catalyzing the oxidative dehydrogenation (ODH) process and the boron sites in open coordination are considered as the active center. By considering the diversity and adjustability in the crystal structure of zeolite, there is a great opportunity to further tune the activity and selectivity. Herein, the embryonic borosilicate zeolite with abundant defective sites and developed large porosity is prepared for catalyzing ODH of propane reaction. Anti 20 % improvement in propylene selectivity is achieved at propane conversion of 21.5 % at 540 degrees C, with propylene productivity nearly an order of magnitude higher compared with crystalline MFI-type borosilicate zeolite. Solid-state NMR reveals the formation of boron sites in open coordination derived from the defect-rich structure of embryonic borosilicate zeolite, guaranteeing ample exposure of the active center. Combined with kinetic measurements, the reaction in the gas phase initiated by the active boron sites is mainly responsible for the high catalytic performance in ODH of propane reaction. The designed experiment indicates the strengthened gas-phase reaction facilitates the activation of propane, consequently resulting in the increase of reaction order of propane from 1.06 to 2.30. This work reveals the significant role of gas -phase reactions during the ODH of propane reaction and provides a new insight for boosting the propy-lene selectivity of zeolite-based catalysts.(c) 2022 Elsevier Inc. All rights reserved.

Automated summary

Embryonic borosilicate zeolite with abundant defective sites and large porosity is used to catalyze the oxidative dehydrogenation of propane, achieving high propylene selectivity and activity. Solid-state NMR reveals the formation of active boron sites derived from the defect-rich structure of the zeolite. Gas-phase reactions play a significant role in the activation of propane and increase the reaction order.