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Unraveling the active sites of Cs-promoted Ru/γ-Al2O3 catalysts for ammonia synthesis
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Unraveling the active sites of Cs-promoted Ru/γ-Al2O3 catalysts for ammonia synthesis

Shih-Yuan Chen, Chih-Li Chang, Masayasu Nishi, Wei-Chih Hsiao, Yves Ira A. Reyes, Hiroyuki Tateno, Ho-Hsiu Chou, Chia-Min Yang, Hsin-Yi Tiffany Chen, Takehisa Mochizuki, …
Applied Catalysis B: Environmental, 卷.310, 121269
08/2022

摘要

Active sites Ammonia synthesis Dynamic Cs species Intermittent operation Ru catalyst Catalysis Environmental Science (all) Process Chemistry and Technology
The development of efficient and stable Ru catalysts is crucial for synthesis of decarbonized NH 3 . Herein, a series of γ-Al 2 O 3 -supported Cs-promoted Ru catalysts were prepared, among which a 1.5Cs-Ru/γ-Al 2 O 3 catalyst with a Cs/Ru molar ratio of 1.5 and a Ru size of ~2 nm exhibited high NH 3 synthesis rates (6.9–30 mmol g cat –1 h –1 ) at ~400 °C and 1 MPa. We unraveled that the surface acidity/basicity could be changed, and new active sites could be generated at the interfaces between the Ru particles and the CsOH-Cs 0 species by tuning the Cs/Ru molar ratio. Among the active sites, Cs 0 (minor), which transferred electrons to Ru, was present at the boundaries of the Ru particles and CsOH (major), which attracted the dissociative hydrogen atoms from the metallic Ru surfaces via a spillover effect and changed the surface acidity/basicity. This facilitated the adsorption/desorption of reactant species, thus promoting NH 3 synthesis.

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