Carbon formation in catalytic partial oxidation of methane on platinum: Model studies on a polycrystalline Pt foil
Carbon formation in catalytic partial oxidation of methane on platinum: Model studies on a polycrystalline Pt foil
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铂上甲烷催化部分氧化过程中碳的形成：多晶铂箔的模型研究
DOI：
10.1016/j.cattod.2011.04.051
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发表时间：
2012
期刊：
影响因子：
5.3
通讯作者：
Horn R.
中科院分区：
文献类型：
--
作者：
Korup O;Schlögl R;Horn R.
研究了多晶铂箔作为甲烷催化部分氧化制合成气的模型催化剂。结果表明，在反应发光时，铂箔上形成了大量的碳质沉积物，阻挡了大部分铂表面原子。利用原位拉曼光谱和定量光谱分析表征了这些碳质化合物随反应温度和反应时间的演化和空间分布。在800℃的反应温度下，经过数小时的反应，碳材料的化学成分由反应点燃后的高活性和强无序转变为高度有序、抗氧化和抗蒸汽重整。值得注意的是，铂表面的碳分布是不均匀的，并且与微晶的性质有关，以一种未知的方式形成多晶箔。
A polycrystalline Pt foil has been investigated as model catalyst in methane catalytic partial oxidation to synthesis gas. It is demonstrated that a substantial amount of carbonaceous deposits forms on the Pt foil upon reaction light-off blocking a large fraction of Pt surface atoms. By using in situ Raman spectroscopy and quantitative spectral analysis the evolution and spatial distribution of these carbonaceous compounds with reaction temperature and reaction time have been characterized. The chemical composition of the carbon material changes from highly reactive and strongly disordered directly after reaction light-off to highly ordered, oxidation and steam reforming resistant after several hours time on stream at 800°C reaction temperature. Remarkably the carbon distribution at the Pt surface was found to be inhomogeneous and related to the nature of the microcrystals forming the polycrystalline foil in a yet unknown manner.