The Origin of the Special Surface and Catalytic Chemistry of Ga-Rich Ni3Ga in the Direct Dehydrogenation of Ethane

Yang He, Yuanjun Song, Siris Laursen

Research output: Contribution to journalArticlepeer-review

39 Scopus citations

Abstract

Synthesis of kinetically trapped, alumina-supported Ni3Ga nanoparticles with particle surface composition partially controlled by off-stoichiometric Ni:Ga loading ratios enabled active, highly selective, and stable catalysts to be developed for the direct dehydrogenation of ethane to ethylene. Experimental studies indicated a direct correlation between superstoichiometric Ga loading and ethylene selectivity yet an inverse correlation with ethane conversion. A catalyst with a 1:1 Ni:Ga loading ratio exhibited a good balance between activity (TOF 5.0 × 10-2 s-1), selectivity (94%), and stability (94 to 90% over the 32-h test). The catalyst could also be easily regenerated using an oxidation and reduction cycle. DFT calculations and in situ DRIFTS CO adsorption confirm that surface reactivity is attenuated as Ga concentration at the particle surface increased.

Original languageEnglish
Pages (from-to)10464-10468
Number of pages5
JournalACS Catalysis
Volume9
Issue number11
DOIs
StatePublished - Nov 2019
Externally publishedYes

Funding

This work was supported by the National Science Foundation (NSF) CAREER award (Grant CBET-1752063). Some TEM work and all in situ DRIFTS and pXRD analyses were conducted at the Center for Nanophase Materials Sciences (CNMS project number CNMS2017-151 and CNMS2017-156) at Oak Ridge National Lab (ORNL).

FundersFunder number
National Science Foundation1752063, CBET-1752063

    Keywords

    • C-C activation
    • C-H activation
    • non-noble metal catalysts
    • rational design
    • transition metal solid compounds

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