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Title: Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins

Abstract

Here, the catalytic CO hydrogenation is one of the most versatile large-scale chemical syntheses leading to variable chemical feedstock. While traditionally mainly methanol and long-chain hydrocarbons are produced by CO hydrogenation, here we show that the same reaction can be tuned to produce long-chain n-aldehydes, 1-alcohols and olefins, as well as n-paraffins over potassium-promoted CoMn catalysts. The sum selectivity of aldehydes and alcohols is usually >50 wt% whereof up to ~97% can be n-aldehydes. While the product slate contains ~60% n-aldehydes at /p CO=0.5, a 65/35% slate of paraffins/alcohols is obtained at a ratio of 9. A linear Anderson–Schulz–Flory behaviour, independent of the /p CO ratio, is found for the sum of C 4+ products. We advocate a synergistic interaction between a Mn 5O 8 oxide and a bulk Co 2C phase, promoted by the presence of potassium, to be responsible for the unique product spectra in our studies.

Authors:
 [1];  [2]
  1. Washington State Univ., Pullman, WA (United States)
  2. Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1373015
Report Number(s):
PNNL-SA-122449
Journal ID: ISSN 2041-1723; 49398
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Fischer-Tropsch synthesis; carbon-monoxide; higher alcohols; iron catalysts; oxygenate selectivity; cobalt carbide; nanoparticles; stability; promoter; olefins; Environmental Molecular Sciences Laboratory

Citation Formats

Xiang, Yizhi, and Kruse, Norbert. Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins. United States: N. p., 2016. Web. doi:10.1038/ncomms13058.
Xiang, Yizhi, & Kruse, Norbert. Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins. United States. doi:10.1038/ncomms13058.
Xiang, Yizhi, and Kruse, Norbert. Thu . "Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins". United States. doi:10.1038/ncomms13058. https://www.osti.gov/servlets/purl/1373015.
@article{osti_1373015,
title = {Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins},
author = {Xiang, Yizhi and Kruse, Norbert},
abstractNote = {Here, the catalytic CO hydrogenation is one of the most versatile large-scale chemical syntheses leading to variable chemical feedstock. While traditionally mainly methanol and long-chain hydrocarbons are produced by CO hydrogenation, here we show that the same reaction can be tuned to produce long-chain n-aldehydes, 1-alcohols and olefins, as well as n-paraffins over potassium-promoted CoMn catalysts. The sum selectivity of aldehydes and alcohols is usually >50 wt% whereof up to ~97% can be n-aldehydes. While the product slate contains ~60% n-aldehydes at /pCO=0.5, a 65/35% slate of paraffins/alcohols is obtained at a ratio of 9. A linear Anderson–Schulz–Flory behaviour, independent of the /pCO ratio, is found for the sum of C4+ products. We advocate a synergistic interaction between a Mn5O8 oxide and a bulk Co2C phase, promoted by the presence of potassium, to be responsible for the unique product spectra in our studies.},
doi = {10.1038/ncomms13058},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Thu Oct 06 00:00:00 EDT 2016},
month = {Thu Oct 06 00:00:00 EDT 2016}
}

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Works referenced in this record:

Supported Iron Nanoparticles as Catalysts for Sustainable Production of Lower Olefins
journal, February 2012

  • Torres Galvis, H. M.; Bitter, J. H.; Khare, C. B.
  • Science, Vol. 335, Issue 6070, p. 835-838
  • DOI: 10.1126/science.1215614