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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
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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.
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)
出处 《燃料化学学报》 EI CAS CSCD 北大核心 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~~
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 catalytic decomposition nitrous oxide cobalt-based spinel alkaline earth metal doping composite metal oxides
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