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Effective low-temperature catalytic methane oxidation over MnCeOx catalytic compositions
Catalysis Today ( IF 5.3 ) Pub Date : 2020-11-24 , DOI: 10.1016/j.cattod.2020.11.010
Alessandra Palella , Lorenzo Spadaro , Roberto Di Chio , Francesco Arena

Methane is classified as one of the most dangerous air pollutant with a warming potential over 20 times higher than that of CO2. Then, methane abatement trough catalytic oxidation processes, especially using low-cost, noble-metal-free catalysts, falls in line with the most important challenges of environmental catalysis. Therefore, a series of MnCeOx composite materials, with different compositions (0.10 < χCe<0.75), have been prepared via, a facile, eco-friendly redox-precipitation route and their catalytic performance on methane total oxidation reaction were evaluated from 200 °C to 700 °C, at a space velocity of 30,000 h−1. A significant improvement of activity was observed by increasing the fraction of CeO2 in the catalytic compositions. An almost complete methane conversion (already at 600 °C) and characteristic T50 value of 475 °C were recorded with the most active catalyst (i.e. Mn-to-Ce ratio of 1:3). Bulk and surface characterization techniques provide evidence of strong synergism between the different oxide phases, favouring Mn ions dispersion at quasi-molecular level, through the incorporation of Mn2+ ions into ceria lattice, enhancing surface area and redox functionality too. The superior catalytic performance of the MnCeOx composite catalysts, especially at high χCe, is therefore associated with enhanced textural properties, along with the presence of highly dispersed manganese species and structural defects on the surface, leading to an improved “oxygen mobility” and low-temperature reducibility.



中文翻译:

MnCeOx 催化组合物上有效的低温催化甲烷氧化

甲烷被归类为最危险的空气污染物之一,其变暖潜力比 CO 2高 20 多倍。然后,通过催化氧化过程减少甲烷,特别是使用低成本、不含贵金属的催化剂,符合环境催化最重要的挑战。因此,一系列MnCeO的X复合材料,具有不同组成(0.10 <χ<0.75),已经制备通过一个轻便,生态友好的氧化还原-沉淀路线以及它们对甲烷总氧化反应催化性能,从200评价°C 至 700 °C,空速为 30,000 h -1. 通过增加催化组合物中CeO 2的比例,观察到活性的显着提高。几乎完全的甲烷转化(已经在 600 °C 下)和475 °C 的特征 T 50值被记录到使用最活跃的催化剂(即 Mn 与 Ce 的比例为 1:3)。本体和表面表征技术提供了不同氧化物相之间强协同作用的证据,通过将 Mn 2+离子结合到氧化铈晶格中,也增加了表面积和氧化还原功能,从而有利于 Mn 离子在准分子水平上的分散。MnCeO x复合催化剂的优异催化性能,尤其是在高 χ Ce,因此与增强的质地特性有关,以及表面上存在高度分散的锰物种和结构缺陷,从而导致“氧迁移率”和低温还原性的改善。

更新日期:2020-11-24
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