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Title: Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation

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 (C 5+) hydrocarbon yield.
Authors:
 [1] ;  [1] ; ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [1] ; ORCiD logo [4]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5100-67284
Journal ID: ISSN 2155-5435
Grant/Contract Number:
AC36-08GO28308
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)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
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
OSTI Identifier:
1357736

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., 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. doi: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.. 2017. "Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation". United States. doi: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 = {2017},
month = {4}
}