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Title: Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates

Abstract

Reacting CO2 and ethane to synthesize value-added oxygenate molecules represents opportunities to simultaneously reduce CO2 emissions and upgrade underutilized ethane in shale gas. Herein, we propose a strategy to produce C3 oxygenates using a tandem reactor. This strategy is achieved with a Fe3Ni1/CeO2 catalyst (first reactor at 600–800 °C) for CO2- assisted dehydrogenation and reforming of ethane to produce ethylene, CO, and H2, and a RhCox/MCM-41 catalyst (second reactor at 200 °C) enabling CO insertion for the production of C3 oxygenates (propanal and 1-propanol) via the heterogeneous hydroformylation reaction at ambient pressure. In-situ characterization using synchrotron spectroscopies and density functional theory (DFT) calculations reveal the effect of Rh–Co bimetallic formation in facilitating the production of C3 oxygenates. The proposed strategy provides an opportunity for upgrading light alkanes in shale gas by reacting with CO2 to produce aldehydes and alcohols.

Authors:
; ; ; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1619676
Alternate Identifier(s):
OSTI ID: 1631024
Report Number(s):
BNL-215945-2020-JAAM
Journal ID: ISSN 2041-1723; 1887; PII: 15849
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Xie, Zhenhua, Xu, Yuanguo, Xie, Meng, Chen, Xiaobo, Lee, Ji Hoon, Stavitski, Eli, Kattel, Shyam, and Chen, Jingguang G. Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates. United Kingdom: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-15849-x.
Xie, Zhenhua, Xu, Yuanguo, Xie, Meng, Chen, Xiaobo, Lee, Ji Hoon, Stavitski, Eli, Kattel, Shyam, & Chen, Jingguang G. Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates. United Kingdom. https://doi.org/10.1038/s41467-020-15849-x
Xie, Zhenhua, Xu, Yuanguo, Xie, Meng, Chen, Xiaobo, Lee, Ji Hoon, Stavitski, Eli, Kattel, Shyam, and Chen, Jingguang G. Mon . "Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates". United Kingdom. https://doi.org/10.1038/s41467-020-15849-x.
@article{osti_1619676,
title = {Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates},
author = {Xie, Zhenhua and Xu, Yuanguo and Xie, Meng and Chen, Xiaobo and Lee, Ji Hoon and Stavitski, Eli and Kattel, Shyam and Chen, Jingguang G.},
abstractNote = {Reacting CO2 and ethane to synthesize value-added oxygenate molecules represents opportunities to simultaneously reduce CO2 emissions and upgrade underutilized ethane in shale gas. Herein, we propose a strategy to produce C3 oxygenates using a tandem reactor. This strategy is achieved with a Fe3Ni1/CeO2 catalyst (first reactor at 600–800 °C) for CO2- assisted dehydrogenation and reforming of ethane to produce ethylene, CO, and H2, and a RhCox/MCM-41 catalyst (second reactor at 200 °C) enabling CO insertion for the production of C3 oxygenates (propanal and 1-propanol) via the heterogeneous hydroformylation reaction at ambient pressure. In-situ characterization using synchrotron spectroscopies and density functional theory (DFT) calculations reveal the effect of Rh–Co bimetallic formation in facilitating the production of C3 oxygenates. The proposed strategy provides an opportunity for upgrading light alkanes in shale gas by reacting with CO2 to produce aldehydes and alcohols.},
doi = {10.1038/s41467-020-15849-x},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {4}
}

Journal Article:
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https://doi.org/10.1038/s41467-020-15849-x

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