Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation
Abstract
Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Bronsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C-H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. Furthermore, these results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield.
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Purdue Univ., West Lafayette, IN (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office
- OSTI Identifier:
- 1357736
- Report Number(s):
- NREL/JA-5100-67284
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 5; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; copper; C-H activation; dehydrogenation; heterogeneous catalysis; zeolites
Citation Formats
Farberow, Carrie A., Cheah, Singfoong, Kim, Seonah, Miller, Jeffrey T., Gallagher, James R., Hensley, Jesse E., Schaidle, Joshua A., and Ruddy, Daniel A. Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation. United States: N. p., 2017.
Web. doi:10.1021/acscatal.6b03582.
Farberow, Carrie A., Cheah, Singfoong, Kim, Seonah, Miller, Jeffrey T., Gallagher, James R., Hensley, Jesse E., Schaidle, Joshua A., & Ruddy, Daniel A. Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation. United States. https://doi.org/10.1021/acscatal.6b03582
Farberow, Carrie A., Cheah, Singfoong, Kim, Seonah, Miller, Jeffrey T., Gallagher, James R., Hensley, Jesse E., Schaidle, Joshua A., and Ruddy, Daniel A. Mon .
"Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation". United States. https://doi.org/10.1021/acscatal.6b03582. https://www.osti.gov/servlets/purl/1357736.
@article{osti_1357736,
title = {Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation},
author = {Farberow, Carrie A. and Cheah, Singfoong and Kim, Seonah and Miller, Jeffrey T. and Gallagher, James R. and Hensley, Jesse E. and Schaidle, Joshua A. and Ruddy, Daniel A.},
abstractNote = {Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Bronsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C-H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. Furthermore, these results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield.},
doi = {10.1021/acscatal.6b03582},
journal = {ACS Catalysis},
number = 5,
volume = 7,
place = {United States},
year = {Mon Apr 24 00:00:00 EDT 2017},
month = {Mon Apr 24 00:00:00 EDT 2017}
}
Web of Science
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