Engineering ZrO<sub>2</sub>-Ru interface to boost Fischer-Tropsch synthesis to olefins.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38886352.
- Also identified by DOI 10.1038/s41467-024-49392-w and PMC identifier 11183094.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Understanding the structures and reaction mechanisms of interfacial active sites in the Fisher-Tropsch synthesis reaction is highly desirable but challenging. Herein, we show that the ZrO<sub>2</sub>-Ru interface could be engineered by loading the ZrO<sub>2</sub> promoter onto silica-supported Ru nanoparticles (ZrRu/SiO<sub>2</sub>), achieving 7.6 times higher intrinsic activity and ~45% reduction in the apparent activation energy compared with the unpromoted Ru/SiO<sub>2</sub> catalyst. Various characterizations and theoretical calculations reveal that the highly dispersed ZrO<sub>2</sub> promoter strongly binds the Ru nanoparticles to form the Zr-O-Ru interfacial structure, which strengthens the hydrogen spillover effect and serves as a reservoir for active H species by forming Zr-OH* species. In particular, the formation of the Zr-O-Ru interface and presence of the hydroxyl species alter the H-assisted CO dissociation route from the formyl (HCO*) pathway to the hydroxy-methylidyne (COH*) pathway, significantly lowering the energy barrier of rate-limiting CO dissociation step and greatly increasing the reactivity. This investigation deepens our understanding of the metal-promoter interaction, and provides an effective strategy to design efficient industrial Fisher-Tropsch synthesis catalysts.