Temperature-programmed reduction and x-ray photoelectron spectroscopy of copper oxide on alumina following exposure to sulfur dioxide and oxygen
Temperature-programmed reduction and x-ray photoelectron spectroscopy of copper oxide on alumina following exposure to sulfur dioxide and oxygen
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DOI：
10.1021/ie00057a008
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发表时间：
1991-09
影响因子：
4.2
通讯作者：
B. Kartheuser;B. K. Hodnett;A. Riva;G. Centi;H. Matralis;M. Ruwet;P. Grange;N. Passarini
中科院分区：
文献类型：
--
作者：
B. Kartheuser;B. K. Hodnett;A. Riva;G. Centi;H. Matralis;M. Ruwet;P. Grange;N. Passarini
吸附剂/催化剂的基础上氧化铝负载的氧化铜制备通过浸渍使用硫酸铜溶液，活化下H2，并暴露于SO2和O2。随后的还原这些样品（之前和之后的硫酸化）进行了研究，通过程序升温还原（TPR）使用H-2或CH 4作为还原气体。通过质谱分析反应产物。此外，还进行了铜和硫酸盐的化学分析、X射线光电子能谱和傅里叶变换红外分析。在硫酸化之前，将浸渍为硫酸铜的硫酸盐转移至氧化铝以形成硫酸铝。TPR曲线则对应于CuO或CuAl 2 O 4的还原，随后是Al 2（SO 4）3的还原。任何残余的CuSO 4被还原成硫化铜。硫酸化后，硫与铜的比例通常大于2：1。在这些情况下，铜以CuSO 4的形式存在。这种化合物被还原形成金属铜和SO2，但也形成了一些硫化铜。在较高温度下，Al 2（SO 4）3被还原，而硫化铜在较低温度下形成。甲烷是一种比氢气更弱的还原剂，但它的使用避免了硫化铜的形成。
Sorbents/catalysts based on alumina-supported CuO were prepared by impregnation using a copper sulfate solution, activated under H2, and exposed to SO2 and O2. The subsequent reduction of those samples (before and after sulfation) was studied by temperature-programmed reduction (TPR) using H-2 or CH4 as the reducing gas. The reaction products were analyzed by mass spectrometry. In addition, chemical analysis for copper and sulfate, X-ray photoelectron spectroscopy, and Fourier transform infrared analyses were carried out. Prior to sulfation, sulfate impregnated as copper sulfate is transferred to the alumina to form aluminum sulfate. The TPR profile then corresponds to the reduction of CuO or CuAl2O4, followed by the reduction of Al2(SO4)3. Any residual CuSO4 is reduced to copper sulfide. After sulfation the sulfur to copper ratio achieved was usually greater than 2:1. In these circumstances the copper was present as CuSO4. This compound was reduced to form metallic copper and SO2, but some copper sulfide also formed. At higher temperatures Al2(SO4)3 was reduced as well as the copper sulfide formed at the lower temperatures. Methane is a less powerful reducing agent than hydrogen, but its utilization avoided the formation of copper sulfide.