Understanding oxidative dehydrogenation of ethane on Co3O4 nanorods from density functional theory

Fung, Victor; Tao, Franklin (Feng); Jiang, De-en

doi:10.1039/c6cy00749j

Title: Understanding oxidative dehydrogenation of ethane on Co₃O₄ nanorods from density functional theory

Journal Article · Fri May 20 00:00:00 EDT 2016 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/c6cy00749j· OSTI ID:1437014

Fung, Victor ^[1]; Tao, Franklin (Feng) ^[2]; Jiang, De-en ^[1]

Univ. of California, Riverside, CA (United States). Dept. of Chemistry
Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering and Dept. of Chemistry

Co₃O₄ is a metal oxide catalyst with weak, tunable M–O bonds promising for catalysis. Here, density functional theory (DFT) is used to study the oxidative dehydrogenation (ODH) of ethane on Co₃O₄ nanorods based on the preferred surface orientation (111) from the experimental electron-microscopy image. The pathway and energetics of the full catalytic cycle including the first and second C–H bond cleavages, hydroxyl clustering, water formation, and oxygen-site regeneration are determined. We find that both lattice O and Co may participate as active sites in the dehydrogenation, with the lattice-O pathway being favored. Here, we identify the best ethane ODH pathway based on the overall energy profiles of several routes. We identify that water formation from the lattice oxygen has the highest energy barrier and is likely a rate-determining step. This work of the complete catalytic cycle of ethane ODH will allow further study into tuning the surface chemistry of Co₃O₄ nanorods for high selectivity of alkane ODH reactions.

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Research Organization:: Univ. of California, Riverside, CA (United States). Dept. of Chemistry

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014561

OSTI ID:: 1437014

Journal Information:: Catalysis Science and Technology, Vol. 6, Issue 18; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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Title: Understanding oxidative dehydrogenation of ethane on Co₃O₄ nanorods from density functional theory