Silicon hydride, as a new efficient catalyst for CO2 conversion to CO, is receiving ever-increasing attention. Thus, a precise catalytic mechanism is needed to provide a guideline for the design of new efficient catalysts based on silicon hydride. Qian et al. recently proposed a one-step mechanism for the catalytic process. The present work, based on the recently proposed WMS and revM06 quantum mechanical model chemistries, provides a multistep mechanism that has a lower free energy of activation than the one-step model. A key point in favor of the new mechanism is that it is consistent with experimental details of the infrared spectrum that cannot be explained by the previous mechanism.
Bibliographical noteFunding Information:
This work was supported in part by the Thousand Innovative Talents Plan of the Chinese Government and by the Inorganometallic Catalyst Design Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under award DE-SC0012702. H. W. acknowledges support from the Fundamental Research Funds for the Central Universities (WUT: 2019IVA006).
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- quantum chemistry
- reaction mechanisms
- redox chemistry