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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Noble metal ionic catalysts: correlation of increase in CO oxidation activity with increasing effective charge on Pd ion in Pd ion substituted Ce1-xMxO2-delta (M = Ti, Zr and Hf)
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Noble metal ionic catalysts: correlation of increase in CO oxidation activity with increasing effective charge on Pd ion in Pd ion substituted Ce1-xMxO2-delta (M = Ti, Zr and Hf)

机译:贵金属离子催化剂:在Pd离子取代的Ce1-xMxO2-delta(M = Ti,Zr和Hf)中,CO氧化活性增加与Pd离子上有效电荷增加的相关性

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摘要

Pd ion substituted Ce1-xMxO2-delta (M = Ti, Zr, Hf) have been prepared by a single step solution combustion method. Two atom% Pd ion substitution in the title compounds is confirmed by X-ray diffraction (XRD) and Pd ion charge state and redox properties have been determined by X-ray photoelectron spectroscopy (XPS) and H-2/TPR studies. While Pd ion in CeO2 (Ce0.98Pd0.02O2-delta) showed higher catalytic activity for CO oxidation than Pd metal impregnated over CeO2, further increase in the catalytic activity is observed with Pd ion in Ce1-xTi(Hf)(x)O-2 and a decrease in the activity with Pd ion in Ce1-xZrxO2. Effective charge on Pd ion could be varied by its substitution in these solid solutions Ce1-xMxO2 (M = Ti, Zr & Hf) and also in TiO2 compared to Pd ion in PdO. Effective positive charge on Pd ion is determined from the core level binding energy shift of Pd(3d(5/2)) peak with respect to Pd metal. Rate of CO oxidation increased and activation energy decreased with increase in effective charge on the Pd ion in the Pd ion substituted fluorites.
机译:钯离子取代的Ce1-xMxO2-δ(M = Ti,Zr,Hf)已通过单步固溶燃烧方法制备。通过X射线衍射(XRD)证实了标题化合物中两个原子%的Pd离子取代,并且通过X射线光电子能谱(XPS)和H-2 / TPR研究确定了Pd离子的电荷状态和氧化还原性质。尽管CeO2(Ce0.98Pd0.02O2-delta)中的Pd离子比浸渍在CeO2上的Pd金属显示出更高的CO氧化催化活性,但观察到Ce1-xTi(Hf)(x)O中的Pd离子进一步提高了催化活性。 -2和Ce1-xZrxO2中Pd离子的活性降低。与在PdO中的Pd离子相比,在这些固溶体Ce1-xMxO2(M = Ti,Zr和Hf)中以及在TiO2中,Pd离子的有效电荷可以通过取代而变化。 Pd离子上的有效正电荷由Pd(3d(5/2))峰相对于Pd金属的核心能级结合能位移确定。随着Pd离子取代萤石中Pd离子上有效电荷的增加,CO氧化速率增加,活化能降低。

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