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 ZrO2-Ru interface could be engineered by loading the ZrO2 promoter onto silica-supported Ru nanoparticles (ZrRu/SiO2), achieving 7.6 times higher intrinsic activity and ~45% reduction in the apparent activation energy compared with the unpromoted Ru/SiO2 catalyst. Various characterizations and theoretical calculations reveal that the highly dispersed ZrO2 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.
| Original language | English |
|---|---|
| Article number | 5143 |
| Journal | Nature Communications |
| Volume | 15 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2024 |
Funding
This work was financially supported by the Natural Science Foundation of China (U22B20136 and 22293023 received by L.Z., 22072177 received by T.L., 22172188 received by S.L., 22202230 received by Y.A.), the National Key R&D Program of China (2023YFB4103104 received by T.L.), the Natural Science Foundation of Shanghai (22JC1404200 received by L.Z., 21ZR1471700 received by T.L.), Program of Shanghai Academic/Technology Research Leader (20XD1404000 received by L.Z.), and the Youth Innovation Promotion Association of CAS. Specifically, we acknowledge the XAFS station (BL14W1) of the Shanghai Synchrotron Radiation Facility for the XAS test and Shanghai Key Laboratory of High-resolution Electron Microscopy of ShanghaiTech University for the (AC)-HAADF-STEM and STEM-EDS characterization support.