Comparative investigation of Ga- and In-CHA in the non-oxidative ethane dehydrogenation reaction

Pan, Jian; Lee, Jason; Li, Muyuan; Trump, Benjamin A.; Lobo, Raul F.

doi:10.1016/j.jcat.2022.07.018

Title: Comparative investigation of Ga- and In-CHA in the non-oxidative ethane dehydrogenation reaction

Journal Article · Mon Aug 01 00:00:00 EDT 2022 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2022.07.018· OSTI ID:1977258

^[1];

^[1]; Trump, Benjamin A. ^[2];

^[1]

Univ. of Delaware, Newark, DE (United States). Center for Catalytic Science and Technology
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)

Ga- and In-exchanged chabazite (CHA) zeolites with same Si/Al and metal/Al ratios were prepared via the incipient wetness impregnation method, were characterized using N₂ adsorption, electron microscopy, temperature-programed reactions and were evaluated for the ethane dehydrogenation reaction using flow microreactors. Ga-CHA has higher reaction rates and a lower activation energy of 107 kJ/mol than In-CHA (E_a = 175 kJ/mol). Rietveld refinement of the X-ray powder diffraction pattern shows that the In⁺ cation is predominantly located above the 6-ring of the CHA cage. It is proposed that the reaction proceeds through the alkyl mechanism based on stability of alkyl hydride intermediates as determined using DFT calculations. The oxidative addition of ethane to the metal shows much lower Gibbs free energy for Ga-CHA (+27.95 kJ/mol) vs In-CHA (+124.85 kJ/mol). Finally, these results indicate that oxidative addition may be the rate-limiting step of ethane dehydrogenation in these materials.

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Research Organization:: American Institute of Chemical Engineers (AIChE), New York, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0007888; EE0007888-6.5

OSTI ID:: 1977258

Alternate ID(s):: OSTI ID: 1880171

Journal Information:: Journal of Catalysis, Vol. 413, Issue C; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Comparative investigation of Ga- and In-CHA in the non-oxidative ethane dehydrogenation reaction

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