Dimethyl carbonate synthesis from CO₂ and methanol over CeO₂: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism

Abstract

surface and how they form decisive surface intermediates leading to DMC are unraveled by DFT-based molecular dynamics simulation by precise statistical sampling of various configurations of surface states and intermediates. The atomistic simulations and uncovered stability of different intermediate states perfectly explain the unique DMC formation profile experimentally observed upon transient operations, strongly supporting the proposed oxygen vacancy-assisted reaction mechanism.