Computational Approaches to the Chemical Conversion of Carbon Dioxide

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.