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Crystal Phase-Dependent Ga-H Chemistry and H2 Roles in Ga2O3-Catalyzed Propane Dehydrogenation Reaction
Hantao Peng1, Jialin Li1, Zeyue Wei1
1State Key Laboratory of Precision and Intelligent Chemistry, iChEM, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, P. R. China.
Abstract:
Roles of H2 in the oxide-catalyzed propane dehydrogenation reaction (PDH) are interesting. Here we report phase-dependent H2 roles in the Ga2O3-catalyzed PDH reaction, in which H2 co-feeding suppresses the PDH reaction catalyzed by α-Ga2O3 with an unchanged apparent activation energy and a negative reaction order against H2 but promotes the PDH reaction catalyzed by β-Ga2O3 with a decreased apparent activation energy and a positive reaction order against H2. The Ga-H hydride species formed by H2 activation on α-Ga2O3 is much more stable than that on β-Ga2O3. During the PDH reaction with co-fed H2 at 500 °C, the irreversibly adsorbed Gaα-Ga2O3-H species is inert toward C3H8 activation and blocks the active site to decrease the C3H8 conversion but meanwhile promotes the C3H6 desorption to increase the TOF, whereas the reversibly adsorbed Gaβ-Ga2O3-H species reactively activates C3H8 at a decreased barrier to promote the PDH reaction via the formation of the more active dynamically cycled Gaβ-Ga2O3-H active site.
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