Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation
Abstract
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 compositionalmore »
- Authors:
-
[2];
[4];
[5];
[1];
[7];
[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)
- Publication Date:
- Research Org.:
- 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 Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1657156
- Alternate Identifier(s):
- OSTI ID: 1638111; OSTI ID: 1755821; OSTI ID: 1843581
- Report Number(s):
- BNL-216328-2020-JAAM; LLNL-JRNL-776816
Journal ID: ISSN 2044-4753
- Grant/Contract Number:
- SC0012704; SC0012573; AC52-07NA27344; 1541959
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Catalysis Science and Technology
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 15; Journal ID: ISSN 2044-4753
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE
Citation Formats
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, and Friend, Cynthia M. Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation. United States: N. p., 2020.
Web. doi:10.1039/D0CY00683A.
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. Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation. United States. https://doi.org/10.1039/D0CY00683A
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, and Friend, Cynthia M. Tue .
"Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation". United States. https://doi.org/10.1039/D0CY00683A. https://www.osti.gov/servlets/purl/1657156.
@article{osti_1657156,
title = {Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation},
author = {Janvelyan, Nare and van Spronsen, Matthijs A. and Wu, Cheng Hao and Qi, Zhen and Montemore, Matthew M. and Shan, Junjun and Zakharov, Dmitri N. and Xu, Fang and Boscoboinik, J. Anibal and Salmeron, Miquel B. and Stach, Eric A. and Flyztani-Stephanopoulos, Maria and Biener, Juergen and Friend, Cynthia M.},
abstractNote = {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.},
doi = {10.1039/D0CY00683A},
journal = {Catalysis Science and Technology},
number = 15,
volume = 10,
place = {United States},
year = {Tue Jul 07 00:00:00 EDT 2020},
month = {Tue Jul 07 00:00:00 EDT 2020}
}
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