Computational Approaches to the Chemical Conversion of Carbon Dioxide

Authors

  • Prof. Dr. Daojian Cheng,

    Corresponding author
    1. Division of Molecular and Materials Simulation, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029 (P.R. China)
    • Division of Molecular and Materials Simulation, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029 (P.R. China)
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  • Dr. Fabio R. Negreiros,

    1. CNR-IPCF, Istituto per i Processi Chimico-Fisici (IPCF) del Consiglio Nazionale delle Ricerche (CNR) via G. Moruzzi 1, I-56124, Pisa (Italy)
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  • Dr. Edoardo Aprà,

    1. William R. Wiley Environmental Molecular Sciences Laboratory, Battelle, Pacific Northwest National Laboratory, K8-91, P.O.Box 999, Richland, WA 99352 (USA)
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  • Dr. Alessandro Fortunelli

    Corresponding author
    1. CNR-IPCF, Istituto per i Processi Chimico-Fisici (IPCF) del Consiglio Nazionale delle Ricerche (CNR) via G. Moruzzi 1, I-56124, Pisa (Italy)
    • CNR-IPCF, Istituto per i Processi Chimico-Fisici (IPCF) del Consiglio Nazionale delle Ricerche (CNR) via G. Moruzzi 1, I-56124, Pisa (Italy)
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Abstract

The conversion of CO2 into fuels and chemicals is viewed as an attractive route for controlling the atmospheric concentration and recycling of this greenhouse gas, but its industrial application is limited by the low selectivity and activity of the current catalysts. Theoretical modeling, in particular density functional theory (DFT) simulations, provides a powerful and effective tool to discover chemical reaction mechanisms and design new catalysts for the chemical conversion of CO2, overcoming the repetitious and time/labor consuming trial-and-error experimental processes. In this article we give a comprehensive survey of recent advances on mechanism determination by DFT calculations for the catalytic hydrogenation of CO2 into CO, CH4, CH3OH, and HCOOH, and CO2 methanation, as well as the photo- and electrochemical reduction of CO2. DFT-guided design procedures of new catalytic systems are also reviewed, and challenges and perspectives in this field are outlined.

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