CuOx/Al₂O₃催化剂上苯酚的湿式空气氧化特性：铜负载量的影响
The characteristics of wet air oxidation of phenol over CuOx/Al2O3 catalysts: effect of copper loading.
作者信息
Kim Sang-Kyung, Kim Kyoung-Hun, Ihm Son-Ki
机构信息
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, 373-1 Guseong-dong, Yuseong-gu, Daejeon 305-701, Republic of Korea.
出版信息
Chemosphere. 2007 Jun;68(2):287-92. doi: 10.1016/j.chemosphere.2006.12.080. Epub 2007 Feb 9.
The nature of active copper species is well-known to vary with copper loading, i.e., isolated Cu(2+) to bulk CuO. In this work, however, the effect of copper loading on the activity and the selectivity was investigated for the wet oxidation of phenol over CuO(x)/Al(2)O(3) catalysts. The activity and the mineralization selectivity of the catalysts increased with copper loading up to 7wt% and remained almost the same at a higher loading. The optimum copper loading was about 7wt% for the wet oxidation of phenol over CuO(x)/Al(2)O(3) catalysts in this work. The nature of copper species with different loading was characterized with TPR, XRD, and XANES. The chemical states of copper in the CuO(x)/Al(2)O(3) catalysts were confirmed as varying with copper loading: isolated Cu(2+) ions for 1wt%; highly dispersed Cu(2+) cluster for 5wt% and 7wt%, and bulk CuO for 10-25wt%. The stability of the CuO(x)/Al(2)O(3) catalysts with different copper loading was also studied with respect to carbonaceous deposits and copper leaching.
众所周知，活性铜物种的性质会随铜负载量而变化，即从孤立的Cu(2+)到块状CuO。然而，在本工作中，研究了铜负载量对CuO(x)/Al₂O₃催化剂上苯酚湿式氧化活性和选择性的影响。催化剂的活性和矿化选择性随铜负载量增加至7wt%而提高，在更高负载量时几乎保持不变。在本工作中，对于CuO(x)/Al₂O₃催化剂上苯酚的湿式氧化，最佳铜负载量约为7wt%。用TPR、XRD和XANES对不同负载量的铜物种性质进行了表征。证实CuO(x)/Al₂O₃催化剂中铜的化学状态随铜负载量而变化：1wt%为孤立的Cu(2+)离子；5wt%和7wt%为高度分散的Cu(2+)簇；10 - 25wt%为块状CuO。还针对碳质沉积物和铜浸出研究了不同铜负载量的CuO(x)/Al₂O₃催化剂的稳定性。
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