陈诗宇,莘玉风,王琦,张印民,张永锋,孙俊民,郝志飞.化学通报,2024,87(9):1111-1118,1124. |
介孔锰氧化物催化剂的合成及其催化氧化甲苯性能研究 |
Synthesis of mesoporous manganese oxide catalysts and their catalytic oxidation properties of toluene |
投稿时间:2024-04-24 修订日期:2024-06-09 |
DOI: |
中文关键词: 甲苯 催化氧化 介孔结构 锰氧化物 |
英文关键词:Toluene Catalytic oxidation Mesoporous structure Manganese oxides |
基金项目:国家自然科学基金项目(22206090)、内蒙古自然科学基金项目(2022QN02009)和内蒙古自治区高等学校“青年科技英才计划”项目(NJYT24025)资助 |
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中文摘要: |
本文采用SBA-15模板法制备了有序介孔氧化锰(m-MnOx)催化剂,并评价了其应用于甲苯催化氧化反应的催化活性。对比没有有序介孔结构的MnOx,m-MnOx具有优异的催化性能(T90 = 235℃ vs. T90 > 300℃),同时m-MnOx表现出更低的表观活化能(Ea =55.94 kJ/mol)、更好的催化稳定性和抗水性。通过使用XRD、TEM、XPS、H2-TPR和O2-TPD技术对催化剂进行了测试与表征,结果表明m-MnOx催化性能的增强主要归因于其内部有序介孔结构,且其孔结构具有良好的结构热稳定性。这种有序介孔结构极大的增加了催化剂的比表面积,同时降低了催化剂的结晶度,导致其表面具有更多Mn3+物种和氧空位的含量,增强了催化剂的低温还原性,从而增强了m-MnOx催化甲苯氧化的性能。 |
英文摘要: |
In this study, ordered mesoporous manganese oxide (m-MnOx) catalyst was prepared by SBA-15 template method, and its catalytic activity for catalytic oxidation of toluene was evaluated. Compared with MnOx without ordered mesoporous structure, m-MnOx exhibit excellent catalytic performance (T90 = 235℃ vs. T90 > 300℃), lower apparent activation energy (Ea =55.94 kJ/mol), better catalytic stability and water resistance. The results of XRD, TEM, XPS, H2-TPR and O2-TPD indicate that the enhancement of catalytic performance of m-MnOx is mainly due to its internal ordered mesoporous structure, and its pore structure has good structural thermal stability. The ordered mesoporous structure greatly increases the specific surface area of the catalyst, while reducing the crystallinity of the catalyst, resulting in more Mn3+ species and oxygen vacancy content on the surface, enhancing the low temperature reducibility of the catalyst, and thus enhancing the catalytic performance of m-MnOx for toluene oxidation. |
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