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

文献情報

出版日 2023-11-21

DOI 10.1039/D3SC04466A

インパクトファクター 9.825

著者

Toshiyuki Sugiyama, Francisco Medina, Wouter van Beek, Jun-ya Hasegawa

原文を見る

要旨

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.

掲載誌

Chemical Science

CiteScore: 14.4

自己引用率: 3.9%

年間論文数: 1413

Our journal has a wide-ranging scope which covers the full breadth of the chemical sciences. The research we publish contains the sorts of novel ideas, challenging questions and progressive thinking that bring undiscovered breakthroughs within reach. Your paper could focus on a single area, or cross many. It could be beyond the accepted bounds of the chemical sciences. It might address an immediate challenge, contribute to a future breakthrough or be wholly conceptual. We’re a team from every field of the chemical sciences, and know from experience that breakthroughs that drive the solutions to global challenges can come from anywhere, at any time. You could even start an entirely new area of research. Too bold? Too progressive? No such thing