类水滑石衍生复合氧化物MgM_(2)AlO材料上苯-甲苯协同催化氧化过程  

The synergistically catalytic oxidation process of benzene and toluene on hydrotalcite-like derived composite oxides MgM_(2)AlO

作　　者：邢欣 王一昕 李哲[1] 刘炳言 孙永刚[2] XING Xin;WANG Yixin;LI Zhe;LIU Bingyan;SUN Yonggang(Taiyuan University of Science and Technology,College of Environment and Resources,Taiyuan 030024,China;State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering,School of chemistry and chemical engineering,Ningxia University,Yinchuan 750021,China)

机构地区：[1]太原科技大学环境与资源学院,太原030024 [2]宁夏大学化学化工学院,省部共建煤炭高效利用与绿色化工国家重点实验室,银川750021

出　　处：《环境工程学报》2024年第12期3557-3569,共13页Chinese Journal of Environmental Engineering

基　　金：国家自然科学青年基金资助项目(22206146);国家自然科学地区基金项目(22368040);山西省基础研究计划青年项目(202103021223280);山西省大学生创新创业训练计划项目(20240823);太原科技大学研究生教育创新项目(SY2023025)。

摘　　要：挥发性有机化合物(volatile organic compounds,VOCs)作为大气复合污染的重要前体物广泛存在于工业废气中,因此,研究工业废气中多组分VOCs协同催化氧化过程与技术是推进大气污染防治攻坚战,打赢蓝天保卫战的关键举措。本研究采用共沉淀法成功制备了系列类水滑石衍生复合氧化物MgM_(2)AlO(M=Co,Mn,Ni,Mg)催化剂,以苯、甲苯为探针物分子研究了系列催化材料协同催化降解苯-甲苯的催化性能。MgMn_(2)AlO材料的催化性能最优,在300°C时苯-甲苯混合体系下,苯和甲苯转化率均为100%,CO_(2)选择性为100%。通过单一反应物(苯或甲苯)与苯-甲苯协同催化氧化反应活性对比,发现苯-甲苯协同催化氧化过程中存在相互抑制作用。此外,采用XRD、N_(2)吸脱附、SEM、TEM-EDS、NH_(3)-TPD、H_(2)-TPR和XPS表征技术研究了催化材料的构效关系。结果表明,催化剂的氧化还原性特性对苯-甲苯协同催化氧化活性影响至关重要,弱酸性位点有利于苯、甲苯的化学吸附和活化,且表面吸附氧的存在有利于苯-甲苯协同催化氧化生成CO_(2)和H_(2)O。Volatile organic compounds(VOCs),as important precursors of atmospheric composite pollution,are widely present in industrial waste gas.Therefore,the study of the synergistically catalytic oxidation process and technology of multi-component VOCs in industrial waste gas is a key measure to advance the battle against air pollution and win the battle for blue sky defense.In this study,a series of catalysts of hydrotalcite derived composite oxides MgM_(2)AlO(M=Co,Mn,Ni,Mg)were successfully prepared using the co-precipitation method.The catalytic performance of the series of catalytic materials for synergistic degradation of benzene and toluene was studied using benzene and toluene as probe molecules.MgMn_(2)AlO had the optimal catalytic performance with the conversion rates of 100%for both benzene and toluene,as well as CO_(2)selectivity of 100%,in the benzene-toluene mixed system at 300°C.By comparing the activity of a single reactant(benzene or toluene)with that of the synergistically catalytic oxidation of benzene and toluene,the mutual inhibition occurred in the latter process.In addition,XRD,N_(2)adsorption-desorption,NH_(3)-TPD,H_(2)-TPR,and XPS characterization techniques were used to study the structure-activity relationship of the catalytic materials.The characterization results indicated that the redox performance of the catalyst is key factor affecting the activity of synergistically catalytic oxidation of benzene and toluene.Weak acidic sites were conducive to the chemical adsorption and activation of benzene and toluene,and the presence of oxygen vacancies was beneficial for the synergistically catalytic oxidation of benzene and toluene to generate CO_(2)and H_(2)O.

关 键 词：苯 甲苯 协同催化氧化 类水滑石衍生复合氧化物 相互影响 

分 类 号：X703[环境科学与工程—环境工程]