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Preferential CO oxidation in hydrogen-rich stream over Pt catalysts modified with alkali metals Part II. Catalyst characterization and role of alkali metals

机译:富氢物流中经碱金属改性的Pt催化剂的优先CO氧化II。碱金属的催化剂表征和作用

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摘要

The addition of alkali metals over Pt/Al2O3 has both promoting and negative effects on the catalytic performance in the preferential CO oxidation in H2-rich stream (PROX), therefore there is an optimum amount of alkali metal. The Pt/Al2O3 catalysts modified with Na, K, Rb and Cs were characterized by means of transmission electron microscopy (TEM), extended X-ray absorption fine structure (EXAFS), X-ray absorption near-edge structure (XANES), and Fourier transform infrared spectroscopy (FTIR). The results show that the addition of larger amount of alkali metals with stronger basicity causes the aggregation of Pt metal particles. The Pt particles on Pt/Al2O3 modified with alkali metals are more electron-deficient than those on Pt/Al2O3, and this weakens the strength of CO adsorption on Pt/Al2O3 modified with alkali metals, which is related to the enhancement of turnover frequency of the PROX. In addition, in situ FTIR observation suggests that the coadsorbed species originating from H2 and O2 (e.g., the OH species) under the PROX condition, which promote the CO oxidation, can be found on highly active catalysts.
机译:在Pt / Al2O3上添加碱金属对富H2物流(PROX)中优先发生的CO氧化中的催化性能既有促进作用,又有负面影响,因此存在最佳量的碱金属。利用透射电子显微镜(TEM),扩展的X射线吸收精细结构(EXAFS),X射线吸收近边缘结构(XANES)和Na,K,Rb和Cs改性的Pt / Al2O3催化剂的特征傅立叶变换红外光谱(FTIR)。结果表明,添加大量碱度较强的碱金属会导致Pt金属颗粒的聚集。碱金属改性的Pt / Al2O3上的Pt颗粒比Pt / Al2O3上的Pt颗粒更缺乏电子,这削弱了CO在碱金属改性的Pt / Al2O3上的吸附强度,这与提高硅的周转率有关代理。另外,原位FTIR观察表明在PROX条件下源自H 2和O 2的共吸附物种(例如,OH物种)可促进CO氧化,可在高活性催化剂上发现。

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