Computational Modeling of CO 2 Reduction and Conversion via Heterogeneous and Homogeneous Catalysis

CO 2 capture and utilization has been attracting intensive attention owing to its vital importance in long-standing carbon emission reduction. Numerous novel catalysts and strategies for the integrated conversion of CO 2 have been developed in past decades. Here, we review our recent electronic structure calculations and molecular dynamics (MD) simulations on CO 2 activation and catalytic transformation. The focus is mainly on the computational design of several types of low-dimensional, nanomaterial-supported, atomically dispersed metal and nonmetal catalysts for electrocatalytic and thermocatalytic reduction of CO 2 as well as metal macrocycles for the coupling of CO 2 with epoxides. Based on extensive calculations and simulations, detailed reaction mechanisms, performances of catalysts, and structure-activity relationships for homogeneous and heterogeneous catalytic transformation of CO 2 have been discussed.