Abstract A mechanochemical redox reaction between KMnO4 and CoCl2 was developed to obtain a CoxMn1–xOy catalyst with a specific surface area of 479 m2 g−1, which was higher than that obtained using a co-precipitation (CP) method (34 m2 g−1), sol-gel (SG) method (72 m2 g−1), or solution redox process (131 m2 g−1). During catalytic combustion, this CoxMn1–xOy catalyst exhibited better activity (T100 for propylene = ~200 °C) than the control catalysts obtained using the SG (325 °C) or CP (450 °C) methods. The mechanical action, mainly in the form of kinetic energy and frictional heating, may generate a high degree of interstitial porosity, while the redox reaction could contribute to good dispersion of cobalt and manganese species. Moreover, the as-prepared CoxMn1–xOy catalyst worked well in the presence of water vapor (H2O 4.2%, >60 h) or SO2 (100 ppm) and at high temperature (400 °C, > 60 h). The structure MnO2·(CoOOH)2.93 was suggested for the current CoxMn1–xOy catalyst. This catalyst could be extended to the total oxidation of other typical hydrocarbons (T90 = 150 °C for ethanol, T90 = 225 °C for acetone, T90 = 250 °C for toluene, T90 = 120 °C for CO, and T90 = 540 °C for CH4). Scale-up of the synthesis of CoxMn1–xOy catalyst (1 kg) can be achieved via ball milling, which may provide a potential strategy for real world catalysis.

中文翻译：

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基于机械化学氧化还原的高多孔 Co Mn1-O 催化剂合成用于全氧化

摘要 通过 KMnO4 和 CoCl2 之间的机械化学氧化还原反应，获得了比表面积为 479 m2 g-1 的 CoxMn1-xOy 催化剂，比使用共沉淀 (CP) 方法获得的比表面积 (34 m2 g- 1)、溶胶-凝胶 (SG) 方法（72 m2 g-1）或溶液氧化还原工艺（131 m2 g-1）。在催化燃烧过程中，这种 CoxMn1-xOy 催化剂表现出比使用 SG (325 °C) 或 CP (450 °C) 方法获得的对照催化剂更好的活性（丙烯的 T100 = ~200 °C）。主要以动能和摩擦加热形式的机械作用可能会产生高度的间隙孔隙，而氧化还原反应可能有助于钴和锰物种的良好分散。此外，所制备的 CoxMn1-xOy 催化剂在水蒸气（H2O 4.2%，> 60 小时）或 SO2 (100 ppm) 和高温（400 °C，> 60 小时）。目前的 CoxMn1-xOy 催化剂结构为 MnO2·(CoOOH)2.93。这种催化剂可以扩展到其他典型碳氢化合物的总氧化（乙醇的 T90 = 150 °C，丙酮的 T90 = 225 °C，甲苯的 T90 = 250 °C，CO 的 T90 = 120 °C，T90 = 540 ℃，CH4）。CoxMn1-xOy 催化剂（1 kg）合成的放大可以通过球磨实现，这可能为现实世界的催化提供一种潜在的策略。