碱土金属掺杂对钴基尖晶石复合金属氧化物催化分解N_2O性能的影响  

Effect of alkaline earth metal doping on the catalytic performance of cobalt-based spinel composite metal oxides in N_2O decomposition

作　　者：李思漩 夏蕾 李靖宇 刘晓刚 孙巾茹 王虹 迟姚玲 李翠清 宋永吉 LI Si-xuan;XIA Lei;LI Jing-yu;LIU Xiao-gang;SUN Jin-ru;WANG Hong;CHI Yao-ling;LI Cui-qing;SONG Yong-ji(College of Chemical Engineering,Beijing Institute of Petrochemical Technology/Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology,Beijing 102617,China;College of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029,China;College of Environmental and Energy Engineering,Beijing University of Technology,Beijing 100124,China)

机构地区：[1]北京石油化工学院化学工程学院燃料清洁化及高效催化减排技术北京市重点实验室,北京102617 [2]北京化工大学化学工程学院,北京100029 [3]北京工业大学环境与能源工程学院,北京100124

出　　处：《燃料化学学报》2018年第11期1377-1385,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21343009;U1662103;2167329);燃料清洁化及高效催化减排技术北京市重点实验室(BZ041420180007);北京市大学生创新创业训练计划(2018J00035)资助项目~~

摘　　要：采用共沉淀法制备碱土金属掺杂的钴基尖晶石型复合金属氧化物M_xCo_(3-x)O_4(M=Mg、Ca、Sr、Ba;x=0、0.1、0.3、0.5、0.7、0.9)催化剂,使用XRD、SEM、氮吸附、H_2-TPR、O_2-TPD-M S和XPS等技术对催化剂进行表征,并在固定床微型反应器中评价了M_xCo_(3-x)O_4催化剂催化分解N_2O的活性,研究了碱土金属掺杂对其催化性能的影响。结果表明,碱土金属掺杂后,M_(x )Co_(3-x)O_4催化剂颗粒粒径减小,比表面积增大,表面吸附氧和Co^(2+)数量增加,氧化还原性能增强;在反应气组成为0.68%N_2O,3%O_2,Ar为平衡气的条件下,碱土金属锶掺杂、掺杂量x为0.7时,Sr_(0.7)Co_(2.3)O_4的N_2O分解催化活性最高,N_2O转化率为10%和95%时所需的温度分别为312和451℃。A series of cobalt-based spinel composite metal oxides doped with alkaline earth metals,viz.,M x Co 3-x O 4(M=Mg,Ca,Sr and Ba;x=0,0.1,0.3,0.5,0.7 and 0.9),were prepared by the coprecipitation method and characterized by XRD,SEM,nitrogen sorption,H 2-TPR,O 2-TPD-MS and XPS;the effect of alkaline earth metal doping on the catalytic performance of M x Co 3-x O 4 composites in N 2O decomposition was investigated in a fixed bed micro-reactor.The results showed that after doping with the alkaline earth metals,the particle size of M x Co 3-x O 4 catalysts is decreased,accompanying with an increase in the specific surface area and the amount of surface adsorbed oxygen and Co 2+species.Meanwhile,the redox performance and catalytic activity of M x Co 3-x O 4 in N 2O decomposition are also greatly enhanced.Under the conditions of 0.68%N 2O,3%O 2 and Ar as balance gas,the Sr 0.7 Co 2.3 O 4 catalyst doped with Sr(x=0.7)exhibits highest activity in N 2O decomposition;the reaction temperatures where the N 2O conversion reaches 10%and 95%are as low as 312 and 451℃,respectively.

关 键 词：催化分解 氧化亚氮 钴基尖晶石 碱土金属 掺杂 复合氧化物 

分 类 号：O643[理学—物理化学]