Cu改性MIL-100(Fe)催化剂的SCR-C_(3)H_(6)脱硝特性  

SCR-C_(3)H_(6) denitrification performance of Cu-modified MIL-100(Fe)catalysts

作　　者：付维 宁淑英 蔡晨 陈佳音 周皞[2] 苏亚欣[1] FU Wei;NING Shuying;CAI Chen;CHEN Jiayin;ZHOU Hao;SU Yaxin(School of Environmental Science and Engineering,Donghua University,Shanghai 201620,China;Changzhou Engineering Vocational and Technical College,Changzhou 213164,Jiangsu,China)

机构地区：[1]东华大学环境科学与工程学院,上海201620 [2]常州工程职业技术学院,江苏常州213164

出　　处：《化工进展》2024年第9期4951-4960,共10页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(52276103)。

摘　　要：烃类化合物选择性催化还原氮氧化物(SCR-HC)是一种很有发展前景的脱硝技术。催化剂有效的氧化-还原能力是影响其活性的关键因素。利用水热法制备了新型有机金属骨架MIL-100(Fe),通过超声浸渍法合成不同Cu含量的m Cu-MIL-100(Fe)催化剂,在固定床微反应器中对其催化C_(3)H_(6)选择性还原NO的特性进行了实验研究。结果表明Cu的引入使MIL-100(Fe)催化活性得到改善。2.3Cu-MIL-100(Fe)的NO转化率在275℃下可达到100%,275~400℃范围内可维持85%以上NO转化率及90%以上N_(2)选择性,且具有较好抗SO_(2)的能力。通过各种技术手段对催化剂的微观结构及物化性质进行了表征,并对反应机理作了进一步讨论。N_(2)吸附-脱附结果表明,加入适量Cu可以增大催化剂的比表面积,并增强催化剂表面对反应气体的吸附能力;XPS研究结果表明,Cu可以提高催化剂表面的氧空位数目。Cu与Fe之间具有协同作用,二者之间存在电子转移现象。H_(2)-TPR曲线表明Cu使催化剂的还原特征峰向低温方向移动,增强了其还原性能。Selective catalytic reduction of nitrogen oxides by hydrocarbons(SCR-HC)is a promising denitrification method.The efficient redox ability of the catalyst is a key factor to influence its activity.A novel metallic organic framework,MIL-100(Fe),was prepared by hydrothermal method,and mCu-MIL-100(Fe)catalysts with different copper contents were synthesized by ultrasonic impregnation,and the performance of the SCR of NO with C_(3)H_(6)was experimentally investigated in a fixed-bed microreactor.The results showed that the catalytic activity of MIL-100(Fe)was improved by the introduction of Cu.The NO conversion rate of 2.3Cu-MIL-100(Fe)was 100%at 275℃and maintained above 85%with the N_(2)selectivity higher than 90%in the range of 275—400℃.It also has good ability to resist SO_(2).The microstructure and physicochemical properties of the catalysts were characterized by various techniques,and the reaction mechanism was further discussed.The N_(2)adsorption-desorption results showed that the addition of an appropriate amount of Cu increased the specific surface area of the catalyst and enhanced the adsorption of the reaction gases on the catalyst surface.XPS results proved that the addition of Cu increased the number of oxygen vacancies on the catalyst surface.There was a synergistic effect and electron transfer between Cu and Fe.The H_(2)-TPR curve indicated that Cu shifted the reduction characteristic peak of the catalyst towards low temperature,enhancing the catalyst’s reduction ability.

关 键 词：氮氧化物 选择催化还原 碳氢化合物 催化剂 Cu改性 抗SO_(2)性能 

分 类 号：X511[环境科学与工程—环境工程]