Engineering ZrO2–Ru interface to boost Fischer-Tropsch synthesis to olefins
Hailing Yu,
Caiqi Wang,
Xin Xin,
Yao Wei,
Shenggang Li (),
Yunlei An,
Fanfei Sun,
Tiejun Lin () and
Liangshu Zhong ()
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Hailing Yu: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Caiqi Wang: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Xin Xin: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Yao Wei: University of Chinese Academy of Sciences
Shenggang Li: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Yunlei An: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Fanfei Sun: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Tiejun Lin: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Liangshu Zhong: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Nature Communications, 2024, vol. 15, issue 1, 1-11
Abstract:
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.
Date: 2024
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DOI: 10.1038/s41467-024-49392-w
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