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

Dragos Stoian, Toshiyuki Sugiyama, Atul Bansode, Francisco Medina, Wouter van Beek, Jun-ya Hasegawa, Akira Nakayama*, A. Urakawa*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

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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.
Original languageEnglish
Article numberd3sc04466a
Pages (from-to)13908-13914
JournalChemical Science
Volume14
Issue number47
DOIs
Publication statusPublished - 2023

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