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Isolated boron in zeolite for oxidative dehydrogenation of propane

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Science  02 Apr 2021:
Vol. 372, Issue 6537, pp. 76-80
DOI: 10.1126/science.abe7935

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Isolating and stabilizing boron

Oxidative dehydrogenation of propane can produce propene from shale gas and help to replace petroleum as a propene feedstock. Boron-based catalysts can have high selectivity to propene, but the water by-product can deactivate the catalyst by hydrolyzing boron. Zhou et al. synthesized boron-doped silicate zeolites containing isolated boron sites that were stable against hydrolysis. The catalyst could achieve one-pass propane conversions up to ∼44% with selectivities for propene and >80% for ethene. They observed no deactivation after a 210-hour continuous test.

Science, this issue p. 76

Abstract

Oxidative dehydrogenation of propane (ODHP) is a key technology for producing propene from shale gas, but conventional metal oxide catalysts are prone to overoxidation to form valueless COx. Boron-based catalysts were recently found to be selective for this reaction, and B–O–B oligomers are generally regarded as active centers. We show here that the isolated boron in a zeolite framework without such oligomers exhibits high activity and selectivity for ODHP, which also hinders full hydrolysis for boron leaching in a humid atmosphere because of the B–O–SiOx linkage, achieving superior durability in a long-period test. Furthermore, we demonstrate an isolated boron with a –B[OH…O(H)–Si]2 structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon–hydrogen bond to catalyze the ODHP.

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