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Title: Catalytic dehydration of biomass derived 1-propanol to propene over M-ZSM-5 (M = H, V, Cu, or Zn)

Here, the impetus to explore biomass derived chemicals arises from a desire to enable renewable and sustainable commodity chemicals. To this end, we report catalytic production of propene, a building-block molecule, from 1-propanol. We found that zeolite catalysts are quite versatile and can produce propene at or below 230 C with high selectivity. Increasing the reaction temperature above 230 C shifted product selectivity towards C4+ hydrocarbons. Cu-ZSM-5 was found to exhibit a broader temperature window for high propene selectivity and could function at higher 1-propanol space velocities than H-ZSM-5. A series of experiments with 1-propan(ol-D) showed deuterium incorporation in the hydrocarbon product stream including propene suggesting that hydrocarbon pool type pathway might be operational concurrent with dehydration to produce C4+ hydrocarbons. Diffuse reflectance infra-red spectroscopy of 1-propanol and 1-propan(ol-D) over Cu-ZSM-5 in combination with deuterium labeling experiments suggest that deuterium incorporation occurs in two steps. Incorporation of deuterium occurs post dehydration via exchange with the partially deuterated catalyst surface.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 56; Journal Issue: 1; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Carbon Fiber Technology Facility (CFTF)
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
OSTI Identifier:
1350920

Lepore, Andrew W., Li, Zhenglong, Davison, Brian H., Foo, Guo -Shiou, Wu, Zili, and Narula, Chaitanya Kumar. Catalytic dehydration of biomass derived 1-propanol to propene over M-ZSM-5 (M = H, V, Cu, or Zn). United States: N. p., Web. doi:10.1021/acs.iecr.7b00592.
Lepore, Andrew W., Li, Zhenglong, Davison, Brian H., Foo, Guo -Shiou, Wu, Zili, & Narula, Chaitanya Kumar. Catalytic dehydration of biomass derived 1-propanol to propene over M-ZSM-5 (M = H, V, Cu, or Zn). United States. doi:10.1021/acs.iecr.7b00592.
Lepore, Andrew W., Li, Zhenglong, Davison, Brian H., Foo, Guo -Shiou, Wu, Zili, and Narula, Chaitanya Kumar. 2017. "Catalytic dehydration of biomass derived 1-propanol to propene over M-ZSM-5 (M = H, V, Cu, or Zn)". United States. doi:10.1021/acs.iecr.7b00592. https://www.osti.gov/servlets/purl/1350920.
@article{osti_1350920,
title = {Catalytic dehydration of biomass derived 1-propanol to propene over M-ZSM-5 (M = H, V, Cu, or Zn)},
author = {Lepore, Andrew W. and Li, Zhenglong and Davison, Brian H. and Foo, Guo -Shiou and Wu, Zili and Narula, Chaitanya Kumar},
abstractNote = {Here, the impetus to explore biomass derived chemicals arises from a desire to enable renewable and sustainable commodity chemicals. To this end, we report catalytic production of propene, a building-block molecule, from 1-propanol. We found that zeolite catalysts are quite versatile and can produce propene at or below 230 C with high selectivity. Increasing the reaction temperature above 230 C shifted product selectivity towards C4+ hydrocarbons. Cu-ZSM-5 was found to exhibit a broader temperature window for high propene selectivity and could function at higher 1-propanol space velocities than H-ZSM-5. A series of experiments with 1-propan(ol-D) showed deuterium incorporation in the hydrocarbon product stream including propene suggesting that hydrocarbon pool type pathway might be operational concurrent with dehydration to produce C4+ hydrocarbons. Diffuse reflectance infra-red spectroscopy of 1-propanol and 1-propan(ol-D) over Cu-ZSM-5 in combination with deuterium labeling experiments suggest that deuterium incorporation occurs in two steps. Incorporation of deuterium occurs post dehydration via exchange with the partially deuterated catalyst surface.},
doi = {10.1021/acs.iecr.7b00592},
journal = {Industrial and Engineering Chemistry Research},
number = 1,
volume = 56,
place = {United States},
year = {2017},
month = {4}
}