Different Reaction Mechanisms of Ammonia Oxidation Reaction on Pt/Al2O3 and Pt/CeZrO2 with Various Pt States

催化作用 氨 金属 材料科学 氧化还原 铂金 选择性 透射电子显微镜 氧气 无机化学 反应机理 纳米技术 化学 冶金 有机化学
作者
Mengmeng Sun,Jingying Liu,Chang Weon Song,Yoshito Ogata,Hanbing Rao,Xiao‐Qing Zhao,Haidi Xu,Yaoqiang Chen
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:11 (26): 23102-23111 被引量:142
标识
DOI:10.1021/acsami.9b02128
摘要

NH 3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al 2 O 3 and Pt/CeZrO 2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal–support interactions. The homogeneously dispersed Pt species over Pt/Al 2 O 3 exposed Pt(111) because of weak metal–support interactions; there even existed an obvious interface between Pt and Al 2 O 3 . While obscure even an overlapped interface was observed over Pt/CeZrO 2, resulting in the formation of PtO because of the oxygen migration from CeZrO 2 to Pt species (confirmed by CO-FTIR, the cycled H 2 -TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al 2 O 3, but two kinds of intermediates, N 2 H 4 and HNO, were observed for Pt/CeZrO 2 . It consequently resulted in the obvious distinction of the NH 3 -SCO catalytic performance; the light-off temperatures of NH 3 over Pt/Al 2 O 3 and Pt/CeZrO 2 were 231 and 275 °C, respectively, while the maximum N 2 selectivity (65%) was obtained over Pt/CeZrO 2, it was obviously better than that over Pt/Al 2 O 3 .
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