Preparation of molybdenum carbides using butane and their catalytic performance

作者：Xiao TC; York APE; Williams VC; Al Megren H; Hanif A; Zhou XY; Green MLH^*

来源：Chemistry of Materials, 2000, 12(12): 3896-3905.

DOI：10.1021/cm001157t

The synthesis of high surface area molybdenum carbides from molybdenum oxide and butane has been studied via temperature-programmed reaction (TPRe), X-ray diffraction (XRD), scanning electron microscopy (SEM), C-13 solid-state NMR, infrared (IR), and Raman spectroscopy (LR). The molybdenum oxygen/carbon system passes through four phase transitions before transforming into the pure Mo2C carbide. Carbon exists in two forms within high surface area molybdenum carbide. The initially produced molybdenum carbide has a face-centered-cubic (fcc) structure but is gradually converted into the hexagonal-close-packed (hcp) structure with increasing carburization temperature, and eventually at high temperature coke is deposited. During the early stages, MoO3 is reduced by H-2, but at higher temperatures, butane also takes part in the reduction and, besides being consumed in the formation of carbide, is catalytically converted into methane, ethane, propane, and benzene. The high surface area of the molybdenum carbide materials is a consequence of preliminary cracking of oxide crystallites during reduction with hydrogen and later from the deposition of amorphous carbon. Catalytic activity tests indicate that molybdenum carbide material, prepared at 823 K, is a good catalyst for the dehydrogenation of butane. The carbide obtained between 923 and 973 K has excellent performance for pyridine HDN with good selectivity.

• 出版日期2000-12