The Effects of Platinum Dispersion and Pt State on Catalytic Properties of Pt/Al2O3 in NH3 Oxidation

催化作用 铂金 色散(光学) 选择性 粒径 氧化态 化学 离子键合 部分氧化 无机化学 材料科学 物理化学 离子 有机化学 光学 物理
作者
Elena M. Slavinskaya,Lidiya S. Kibis,Olga A. Stonkus,Dmitry A. Svintsitskiy,Andrey I. Stadnichenko,Elizaveta A. Fedorova,А. С. Романенко,Vasyl Marchuk,Dmitry E. Doronkin,А. И. Боронин
出处
期刊:Chemcatchem [Wiley]
卷期号:13 (1): 313-327 被引量:25
标识
DOI:10.1002/cctc.202001320
摘要

Abstract Dependence of NH 3 oxidation on the state and dispersion of Pt species in Pt/γ‐Al 2 O 3 catalysts was investigated. Prereduced Pt/γ‐Al 2 O 3 catalysts containing Pt 0 nanoparticles exhibited significantly higher activity than preoxidized ones with the same Pt dispersion. The most significant improvement of the catalytic activity (TOF increased by 30 times) was observed when the size of Pt 0 particles increased from ∼1 to ∼8 nm. N 2 selectivity was found to be mainly determined by the reaction temperature, with a minor influence of Pt particle size. Preoxidized catalysts containing ionic Pt were activated by the reaction medium, while partial deactivation was observed for the prereduced ones. The activity improvement was associated with the presence of Pt 4+ /Pt 2+ species on the surface of preoxidized catalysts. The activity decrease of the prereduced catalysts was due to the partial oxidation and subsequent redispersion of Pt particles. Introduction of H 2 O and CO 2 to the reaction mixture only moderately influenced NH 3 oxidation activity shifting NH 3 conversion curves by about +15 °C.
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