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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:碱金属改性的Pt催化剂上富氢物流中的优选CO氧化第二部分。碱金属的催化剂表征和作用

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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CO氧化过程中的催化性能既有促进作用,也有负面影响,因此有最佳的碱金属量。用Pt / Al2O3改性的Pt / Al2O3催化剂通过透射电子显微镜(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)和傅里叶变换红外光谱(FTIR)对Na,K,Rb和Cs进行表征。结果表明,添加大量碱度更高的碱金属会导致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对碱金属修饰的Pt / Al2O3的吸附强度,与提高PROX的转换频率有关。此外,原位FTIR观察表明,共吸附的物种起源于H2和O2(例如,可以在高活性催化剂上发现在PROX条件下促进OH氧化的OH类)。

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