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Improved activity and stability for chlorobenzene oxidation over ternary Cu-Mn-O-Ce solid solution supported on
Mingyang Gu1, Qiong Huang2, Lirui Xu1
1Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technologies, Jiangsu Key Laboratory of Atmospheric Environmental Monitoring & Pollution Control, School of Environmental Science & Engineering, Nanjing University of Information Science & Technology, No. 219 Ningliu Road, Nanjing, 210044, China.
Abstract:
A series of CuMnOx/CeO2/cordierite and CuMnCeOx/cordierite catalysts prepared by a complex method with citric acid were investigated for the performance of chlorobenzene (CB) oxidation. The effects of the molar ratio of Mn/Cu, transition metal oxide loading, calcination temperature and time were investigated as the main investigation factor for the performance. Meanwhile, XRD, SEM, BET, H2-TPR, O2-TPD and XPS were conducted to characterize the physicochemical properties of these catalysts. The results demonstrated that CuMnOx/CeO2/cordierite catalysts prepared by step-by-step synthesis with the Cu/Mn molar ratio of 5:2 exhibited a high activity (T90 = 350 °C), owing to the incorporation of CuO and MnOx for forming CuMn2O4 spinel oxide supported on CeO2 surface. More importantly, CuMnCeOx/cordierite catalysts prepared by one-step exhibited the highest oxidation activity (T90 < 300 °C) attributed to the low H2 reduction temperature and desorption energy of surface oxygen, and the formed Cu-Mn-O-Ce solid solution and CeO2 promoted the high dispersion of CuMnOx in the supported catalysts. In addition, the possible oxidation mechanism was described to demonstrate the by-products generation and oxygen transfer of CuMnCeOx catalysts.
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