The synthesis of acrylic acid from CO2-ethylene coupling represents an alternate approach to produce an industrially important chemical. However, implement of this reaction is currently hindered by the low activity and stability of molecular catalysts. Therefore, the development of heterogeneous catalysts is desirable. Zeolite-based catalysis offers advantages such as porosity (providing confinement effects), tunability of active sites, and stability. In this study, we investigated CO2-ethylene coupling on single metal atom and diatomic active sites within the porous structure of MFI zeolites using density functional theory. Single metal atom-exchanged MFI zeolites mimic the reaction mechanisms of molecular catalysts and face similar limitations in reaction kinetics such as the β-H transfer step. To overcome this, we designed diatomic sites (M-O-M active sites) in MFI zeolites, which can steer the reaction mechanism to bypass the β-H transfer step. We will discuss the mechanistic details of CO2-ethylene coupling on both active sites, along with descriptors for activation barriers for this reaction.
