The Effect of Support on Sulphur Tolerance of Rh Based Catalysts for Methane Partial Oxidation
The Effect of Support on Sulphur Tolerance of Rh Based Catalysts for Methane Partial Oxidation
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载体对Rh基甲烷部分氧化催化剂耐硫性的影响
DOI：
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发表时间：
2009
期刊：
影响因子：
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通讯作者：
G. Russo
中科院分区：
文献类型：
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作者：
R. Torbati;S. Cimino;L. Lisi;G. Russo
天然气中天然存在的或作为气味剂添加的含硫化合物的存在会对用于将甲烷部分氧化成合成气的贵金属基催化剂的性能产生不利影响。本文研究了添加 SO2 对甲烷催化部分氧化的影响，研究了通过初湿浸渍法在两种不同的市售高温 γ-氧化铝载体（用 10% SiO2 或 3% La2O3 稳定）上制备的 Rh（1 wt.%）催化剂。基于催化活性测量和原位傅立叶变换红外光谱表征以及TPR/TPD研究的结果表明，硫的存在可以通过抑制甲烷催化部分氧化过程中的重整反应来严重抑制合成气的形成。结果还表明载体在部分氧化反应中起着至关重要的作用。在存在硫酸化载体（例如 La2O3-Al2O3）的情况下，部分氧化反应比硫酸化程度较低的载体（例如 SiO2-Al2O3）受到的抑制要少得多。硫酸化载体充当硫储存库，最大限度地减少毒物吸附在发生反应的活性 Rh 位点上或附近。
The presence of sulphur containing compounds, naturally occurring in natural gas or added as odorants, can adversely affect the performance of noble metals based catalysts for the partial oxidation of methane to syngas. In this paper the effect of SO2 addition on the catalytic partial oxidation of methane was investigated on Rh (1 wt.%) catalysts prepared by incipient wetness impregnation method on two different commercially available high temperature γ-alumina supports stabilized either with 10% SiO2 or 3% La2O3. Based on the results of catalytic activity measurements and in-situ FT-IR spectroscopic characterisation, as well as TPR/TPD studies, it has been shown that the presence of sulphur can severely suppress the formation of synthesis gas by inhibiting the reforming reactions during the catalytic partial oxidation of methane. The results also demonstrated that the support plays a crucial role in the partial oxidation reaction. In the presence of a sulphating support such as La2O3–Al2O3 the partial oxidation reaction was much less inhibited than a less sulphating support such as SiO2–Al2O3. The sulphating support acts as a sulphur storage reservoir, which minimises the poison from adsorbing on or near the active Rh sites where reactions take place.