Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation

Janvelyan, Nare; van Spronsen, Matthijs A.; Wu, Cheng Hao; Qi, Zhen; Montemore, Matthew M.; Shan, Junjun; Zakharov, Dmitri N.; Xu, Fang; Boscoboinik, J. Anibal; Salmeron, Miquel B.; Stach, Eric A.; Flyztani-Stephanopoulos, Maria; Biener, Juergen; Friend, Cynthia M.

doi:10.1039/D0CY00683A

Title: Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation

Journal Article · Tue Jul 07 00:00:00 EDT 2020 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/D0CY00683A· OSTI ID:1657156

Janvelyan, Nare ^[1];

^[2]; Wu, Cheng Hao ^[3];

^[4];

^[5]; Shan, Junjun ^[6]; Zakharov, Dmitri N. ^[7];

^[1];

^[7]; Salmeron, Miquel B. ^[8]; Stach, Eric A. ^[7]; Flyztani-Stephanopoulos, Maria ^[9];

^[4];

^[1]

Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nanoscale Synthesis and Characterization Lab.
Harvard Univ., Cambridge, MA (United States); NICE America Research Inc., Mountain View, CA (United States)
Tufts Univ., Medford, MA (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Tufts Univ., Medford, MA (United States)

Producing acetaldehyde, an important industrial chemical, by direct catalytic non-oxidative dehydrogenation of ethanol presents many advantages over current production methods, including generating hydrogen. However, a stable, active, and selective catalyst is currently unavailable. This work demonstrates that the high activity and selectivity of nanoporous (np) NiCu for this reaction can be stabilized by keeping the catalyst in a metastable (“kinetically trapped”) state. Using a combination of in situ ambient-pressure and ex situ X-ray photoelectron spectroscopy, environmental transmission electron microscopy, and density functional theory calculations enabled correlating changes in surface composition with the changes in activity and stability upon treatment of np NiCu with H₂ and O₂. Furthermore, reduction of Ni-doped nanoporous Cu by H₂ exposure enhanced the initial activity but led to complete catalyst deactivation within ~40 hours. In contrast, O₂ pretreatment of the same catalyst increased both activity and long-term stability, with only 15% activity loss over 40 hours. The stability of np NiCu as a catalyst inversely correlates with the amount of metallic Ni at the surface, which is enriched by the H₂ pretreatment, while the O₂ pretreatment leads to a kinetically trapped Ni²⁺ subsurface state. This work emphasizes that detailed understanding of pretreatment-induced nanoscale structural and compositional changes is necessary to optimize catalyst performance.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN) and National Synchrotron Light Source II (NSLS-II); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Harvard Univ., Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: SC0012704; SC0012573; AC52-07NA27344; 1541959

OSTI ID:: 1657156

Alternate ID(s):: OSTI ID: 1638111; OSTI ID: 1755821; OSTI ID: 1843581

Report Number(s):: BNL-216328-2020-JAAM; LLNL-JRNL-776816

Journal Information:: Catalysis Science and Technology, Vol. 10, Issue 15; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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