Coupling of Methane and Carbon Dioxide Mediated by Diatomic Copper Boride Cations

The use of CH4 and CO2 to produce value‐added chemicals via direct C−C coupling is a challenging chemistry problem because of the inertness of these two molecules. Herein, mass spectrometric experiments and high‐level quantum‐chemical calculations have identified the first diatomic species (CuB+) th...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2018-10, Vol.57 (43), p.14134-14138
Main Authors: Chen, Qiang, Zhao, Yan‐Xia, Jiang, Li‐Xue, Chen, Jiao‐Jiao, He, Sheng‐Gui
Format: Article
Language:English
Subjects:
Carbon dioxide
Cations
Coupling (molecular)
C−C coupling
mass spectrometry
Methane
Organic chemistry
quantum-chemical calculations
Spectrometry
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Summary:The use of CH4 and CO2 to produce value‐added chemicals via direct C−C coupling is a challenging chemistry problem because of the inertness of these two molecules. Herein, mass spectrometric experiments and high‐level quantum‐chemical calculations have identified the first diatomic species (CuB+) that can couple CH4 with CO2 under thermal collision conditions to produce ketene (H2C=C=O), an important intermediate in synthetic chemistry. The order to feed the reactants (CH4 and CO2) is important and CH4 should be firstly fed to produce the C2 product. Molecular‐level mechanisms including control of product selectivity have been revealed for coupling of CH4 with CO2 under mild conditions. Reactive clusters: Direct coupling of CH4 and CO2 mediated by diatomic CuB+ to the C2 product H2C=C=O under thermal collision conditions has been identified by mass spectrometric experiments. The experimental findings are supported by and consistent with high‐level quantum‐chemical calculations.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201808780