NiAu Single Atom Alloys for the Non-oxidative Dehydrogenation of Ethanol to Acetaldehyde and Hydrogen

Giannakakis, Georgios; Trimpalis, Antonios; Shan, Junjun; Qi, Zhen; Cao, Sufeng; Liu, Jilei; Ye, Jianchao; Biener, Juergen; Flytzani-Stephanopoulos, Maria

doi:10.1007/s11244-017-0883-0

NiAu Single Atom Alloys for the Non-oxidative Dehydrogenation of Ethanol to Acetaldehyde and Hydrogen

Journal Article · Mon Mar 19 00:00:00 EDT 2018 · Topics in Catalysis

DOI:https://doi.org/10.1007/s11244-017-0883-0· OSTI ID:1502035

Giannakakis, Georgios ^[1]; Trimpalis, Antonios ^[1]; Shan, Junjun ^[2]; Qi, Zhen ^[3]; Cao, Sufeng ^[1]; Liu, Jilei ^[1]; Ye, Jianchao ^[3]; Biener, Juergen ^[3]; Flytzani-Stephanopoulos, Maria ^[1]

Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering
Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering; NICE America Research, Inc., Mountain View, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Gold is examined here as an alternative to copper for the selective dehydrogenation of ethanol to acetaldehyde and hydrogen. Despite its high selectivity, gold is only active at temperatures higher than 250 °C for this reaction. We demonstrate that addition of a small amount of Ni on either supported or unsupported Au surfaces induces resistance to sintering, along with a beneficial effect on the catalytic activity. NiAu alloys prepared here with Ni as the minority component to the limit of atomic dispersion in the gold surfaces, catalyze the reaction beginning below 150 °C. A significant decrease of the apparent activation energy from 96 ± 3 kJ/mol for the monometallic Au to 59 ± 5 kJ/mol for the alloy was found. The Ni dispersion and concentration as a function of gas environment was followed by in situ DRIFTS and by XPS. The stability of the catalyst morphology was investigated through post-reaction microscopy imaging and long-term stability tests under reaction conditions. As shown via dynamic reaction experiments, acetaldehyde and H₂ were selectively produced up to 280 °C. A small drop of selectivity at higher temperatures is attributed to the formation of Ni clusters, as proven by CO-DRIFTS on the used sample. Comparison with samples of higher Ni loading, where Ni clusters are formed, clearly shows that they catalyze the undesired full decomposition of ethanol to CO, CH₄, and H₂.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1502035

Alternate ID(s):: OSTI ID: 1470259

Report Number(s):: LLNL-JRNL--740707; 894694

Journal Information:: Topics in Catalysis, Journal Name: Topics in Catalysis Journal Issue: 5-6 Vol. 61; ISSN 1022-5528

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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Acetaldehyde
Ethanol dehydrogenation
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Hydrogen
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Single atom alloys

NiAu Single Atom Alloys for the Non-oxidative Dehydrogenation of Ethanol to Acetaldehyde and Hydrogen

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