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

作　　者：陈诗宇 莘玉风 王琦 张印民[1] 张永锋[1] 孙俊民[1] 郝志飞 Chen Shiyu;Xin Yufeng;Wang Qi;Zhang Yinmin;Zhang Yongfeng;Sun Junmin;Hao Zhifei(College of Chemical Engineering,Inner Mongolia University of Technology,National Local Joint Engineering Research Center for High Value Utilization of Coal-based Solid Waste,Hohhot,010051)

机构地区：[1]内蒙古工业大学化工学院、资源循环高等学校重点实验室、煤基固废高值化利用国家地方联合工程研究中心,呼和浩特010051

出　　处：《化学通报》2024年第9期1111-1118,1124,共9页Chemistry

基　　金：国家自然科学基金项目(22206090);内蒙古自然科学基金项目(2022QN02009);内蒙古自治区高等学校“青年科技英才计划”项目(NJYT24025)资助。

摘　　要：本文采用SBA-15模板法制备了有序介孔氧化锰(m-MnO_(x))催化剂,并评价了其应用于甲苯催化氧化反应的活性。对比没有有序介孔结构的MnO_(x),m-MnO_(x)具有优异的催化性能(T_(90)=235℃vs.T_(90)>300℃),同时表现出更低的表观活化能(E_(a)=55.94kJ/mol)、更好的催化稳定性和抗水性。通过XRD、TEM、XPS、H_(2)-TPR和O_(2)-TPD等对催化剂进行了测试与表征,结果表明,m-MnO_(x)催化性能增强主要归因于其内部具有良好结构热稳定性的有序介孔结构。这种有序介孔结构极大增加了催化剂的比表面积,同时降低了催化剂的结晶度,使其表面具有更多Mn^(3+)物种和氧空位,增强了催化剂的低温还原性能,从而增强了m-MnO_(x)催化甲苯氧化的性能。In this study,ordered mesoporous manganese oxide(m-MnO_(x))catalyst was prepared by SBA-15 template method,and its catalytic activity for oxidation of toluene was evaluated.Compared with MnO_(x)without ordered mesoporous structure,m-MnO_(x)exhibit excellent catalytic performance(T_(90)=235℃vs.T_(90)>300℃),lower apparent activation energy(E_(a)=55.94 kJ/mol),better catalytic stability and water resistance.The characterization results of XRD,TEM,XPS,H_(2)-TPR and O_(2)-TPD indicate that the enhancement of catalytic performance of m-MnO_(x)is mainly due to its internal ordered mesoporous structure with good 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 Mn^(3+)species and oxygen vacancy content on the surface,enhancing the low temperature reducibility of the catalyst,and thus enhancing the catalytic performance of m-MnO_(x)for toluene oxidation.

关 键 词：甲苯 催化氧化 介孔结构 锰氧化物 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学]