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Template‐free Scalable Synthesis of Flower‐like Co3‐xMnxO4 Spinel Catalysts for Toluene Oxidation
ChemCatChem ( IF 3.8 ) Pub Date : 2018-07-11 , DOI: 10.1002/cctc.201800598
Yuan Wang 1 , Hamidreza Arandiyan 1, 2 , Yuxi Liu 3 , Yijing Liang 3 , Yue Peng 4 , Stuart Bartlett 2 , Hongxing Dai 3 , Sadegh Rostamnia 5 , Junhua Li 4
Affiliation  

The rational design of low‐cost transition metal catalysts that exhibit high activity and selectivity may be the most significantly investigated in heterogeneous catalysis. In this study, Co3‐xMnxO4 (x=0.75, 1.0, and 1.5) mixed metal oxides were successfully synthesized by a controlled template‐free autoclave strategy and studied for toluene oxidation. It is found that the Co‐rich sample showed markedly enhanced activity and the 3D dandelion‐like Co2.25Mn0.75O4 catalyst exhibited in the highest toluene oxidation rate (8.9 μmol/(gcats)) and a 100 % toluene conversion at 239 °C. In situ DRIFTS study indicates that toluene was sequentially oxidized to benzyl radical, benzaldehyde, benzene, oxalic acid, and finally to CO2 and H2O. The interaction between Co and Mn, in conjunction with the high concentration of surface oxygen species and rich surface oxygen vacancies, reasonably explains the elevated catalytic activity and thermal stability for toluene oxidation over 3D flower‐like Co3‐xMnxO4 spinel catalysts.

中文翻译:

花状Co3-xMnxO4尖晶石催化剂的无模板可扩展合成,用于甲苯氧化

表现出高活性和选择性的低成本过渡金属催化剂的合理设计可能是非均相催化研究中最受关注的问题。在这项研究中,通过无模板的高压釜策略成功合成了Co 3 x Mn x O 4x = 0.75、1.0和1.5)混合金属氧化物,并研究了甲苯的氧化作用。发现富钴样品显示出显着增强的活性,而3D蒲公英样Co 2.25 Mn 0.75 O 4催化剂表现出最高的甲苯氧化速率(8.9μmol/(g cats))和在239°C下100%的甲苯转化率。原位DRIFTS研究表明,甲苯依次氧化为苄基,苯甲醛,苯,草酸,最后到CO 2和H 2 O.与表面氧物种和丰富的高浓度结合Co和Mn,之间的相互作用表面氧空位,可以合理地解释在3D花状Co 3 x Mn x O 4尖晶石催化剂上甲苯氧化的催化活性和热稳定性提高。
更新日期:2018-07-11
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