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

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms13058· OSTI ID:1373015
 [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)

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.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1373015
Report Number(s):
PNNL-SA-122449; 49398
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 103 works
Citation information provided by
Web of Science

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An Amorphous Nickel–Iron‐Based Electrocatalyst with Unusual Local Structures for Ultrafast Oxygen Evolution Reaction journal May 2019
Direct Production of Higher Oxygenates by Syngas Conversion over a Multifunctional Catalyst journal February 2019
Direct Production of Higher Oxygenates by Syngas Conversion over a Multifunctional Catalyst journal February 2019
Manipulation of Fischer-Tropsch Synthesis for Production of Higher Alcohols Using Manganese Promoters journal October 2018
Discovery of a Fischer-Tropsch Hybrid Reaction: Hydrogenation of Methylformate to Long-Chain Hydrocarbons with Anderson-Schulz-Flory Chain Length Distribution journal January 2019
Beyond Cars: Fischer‐Tropsch Synthesis for Non‐Automotive Applications journal February 2019
Elucidating the K‐Edge X‐Ray Absorption Near‐Edge Structure of Cobalt Carbide journal June 2019
Advances in direct production of value-added chemicals via syngas conversion journal April 2017
Direct conversion of CO2 into liquid fuels with high selectivity over a bifunctional catalyst journal June 2017
Promoted cobalt metal catalysts suitable for the production of lower olefins from natural gas journal January 2019
Rate and selectivity hysteresis during the carbon monoxide hydrogenation over promoted Co/MnOx catalysts journal September 2019
Interfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols journal January 2020
Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis journal February 2020
CO oxidative coupling to dimethyl oxalate over Pd–Me (Me = Cu, Al) catalysts: a combined DFT and kinetic study journal January 2018
Bimetallic Ni–Co catalysts supported on Mn–Al oxide for selective catalytic CO hydrogenation to higher alcohols journal January 2018
The challenge of catalyst prediction journal January 2018
Facile efficient earth abundant NiO/C composite electrocatalyst for the oxygen evolution reaction journal January 2019
Chemical imaging of Fischer-Tropsch catalysts under operating conditions journal March 2017
Atom Probe Tomography for Catalysis Applications: A Review journal July 2019
Editorial: Cobalt and Iron Catalysis journal December 2019
One-pass selective conversion of syngas to para -xylene journal January 2017
Promoted Iron Nanocrystals Obtained via Ligand Exchange as Active and Selective Catalysts for Synthesis Gas Conversion journal July 2017