Fully Exposed Ru Clusters for the Efficient Multi-Step Toluene Hydrogenation Reaction.

Angew Chem Int Ed Engl

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, P. R. China.

Published: September 2024

Liquid organic hydrogen carriers (LOHCs) are attractive platform molecules that play an important role in hydrogen energy storage and utilization. The multi-step hydrogenation of toluene (TOL) to methylcyclohexane (MCH) has been widely studied in the LOCHs systems, due to their relatively low toxicity and reasonable hydrogen storage capacity. Noble metal catalysts such as Ru has exhibited good performance in multi-step hydrogenation reactions, while the application is still hindered by their high cost and low specific activity. Therefore, the primary challenge lies in the development of noble metal catalysts with both robust activity and efficient atomic utilization. In this study, a series of Ru species ranging from single atoms, fully exposed clusters to nanoparticles were fabricated to investigate their structural evolution in the TOL multi-step hydrogenation reaction. The fully exposed and atomically dispersed Ru clusters, composed of an average of 3 Ru atoms, exhibit superior catalytic performance and recycle ability in TOL multi-step hydrogenation. Moreover, it delivers a high turnover frequency of 9850.3 h under the relatively mild reaction (100 °C, 1.5 MPa), compared with those of single atoms and nanoparticles, and shows a notable advantage over catalysts reported in previous studies. From density functional theory (DFT) calculations, the overall barrier of the TOL multi-step hydrogenation reaction over the fully exposed Ru clusters is significantly lower than that of single atoms and nanoparticles, resulting in its higher activity. The present work provides an efficient strategy to regulate the reaction pathway of multi-step complicated catalytic reactions by designing fully exposed metal cluster catalysts.

Download full-text PDF

Source
http://dx.doi.org/10.1002/anie.202415542DOI Listing

Publication Analysis

Top Keywords

fully exposed
20
multi-step hydrogenation
20
exposed clusters
12
hydrogenation reaction
12
single atoms
12
tol multi-step
12
noble metal
8
metal catalysts
8
reaction fully
8
atoms nanoparticles
8

Similar Publications

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!