Print Email Facebook Twitter Dimethyl carbonate synthesis from CO2 and methanol over CeO2: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism Title Dimethyl carbonate synthesis from CO2 and methanol over CeO2: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism Author Stoian, Dragos (European Synchrotron Radiation Facility; Barcelona Institute of Science and Technology (BIST); University Rovira i Virgili) Sugiyama, Toshiyuki (Hokkaido University) Bansode, Atul (TU Delft ChemE/Catalysis Engineering; Barcelona Institute of Science and Technology (BIST)) Medina, Francisco (University Rovira i Virgili) van Beek, Wouter (European Synchrotron Radiation Facility) Hasegawa, Jun-ya (Hokkaido University) Nakayama, Akira (Hokkaido University; University of Tokyo) Urakawa, A. (TU Delft ChemE/Catalysis Engineering; Barcelona Institute of Science and Technology (BIST)) Date 2023 Abstract Surface intermediate species and oxygen vacancy-assisted mechanism over CeO2 catalyst in the direct dimethyl carbonate (DMC) synthesis from carbon dioxide and methanol are suggested by means of transient spectroscopic methodologies in conjunction with multivariate spectral analysis. How the two reactants, i.e. CO2 and methanol, interact with the CeO2 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. To reference this document use: http://resolver.tudelft.nl/uuid:257c4ab1-123c-495a-941f-b79f84295dd9 DOI https://doi.org/10.1039/D3SC04466A ISSN 2041-6520 Source Chemical Science, 14 (47), 13908-13914 Part of collection Institutional Repository Document type journal article Rights © 2023 Dragos Stoian, Toshiyuki Sugiyama, Atul Bansode, Francisco Medina, Wouter van Beek, Jun-ya Hasegawa, Akira Nakayama, A. Urakawa Files PDF d3sc04466a.pdf 1.01 MB Close viewer /islandora/object/uuid:257c4ab1-123c-495a-941f-b79f84295dd9/datastream/OBJ/view