English (United Kingdom)

https://curated-unify.zendy.io/wp-json/zendy-region/v1/featured_content/oa?rat=en

https://curated-unify.zendy.io/wp-json/zendy-region/v1/highlighted_journal/

Zendy Open

Presents the pdf analysis as premium feature

PDF Analysis

Insights

Presents the summarisation as premium feature

Summarisation

Presents the keyphrase highlighting as premium feature

Keyphrase Highlighting

Presents the zaia usage as premium feature

ZAIA

Zendy Tools

Zendy Plus

Presents the access of premium content as premium feature

Premium Content

Heterogenous hydrogenation reactions are essential in a wide range of chemical industries. In this work, we find that the hydrogenation of acetaldehyde on birnessite cannot occur through the traditional mechanisms due to the strong adsorption of the aldehyde and hydrogen on the surface, using first-principles calculations. We discover that this reaction can occur feasibly via a solvent-cocatalyzed mechanism with molecular hydrogen in the liquid phase: a methanol solvent or a similar solvent is required for the reaction. Free energy calculations shows that the methanol solvent preferentially fills the oxygen vacancies of the catalyst surface and spontaneously dissociates on the surface, in which the resulting hydroxyl group then acts as the coordination site for the carbonyl bond and allows the reaction to proceed without adsorption of the reactants on the surface. The reasons this new mechanism is more favorable over the traditional mechanisms in the literature are scrutinized and discussed. The new mechanism may be followed in many other systems.

jacs au

Discovery of a New Solvent Co-Catalyzed Mechanism in Heterogeneous Catalysis: A First-Principles Study with Molecular Dynamics on Acetaldehyde Hydrogenation on Birnessite