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CexTi1-xO2负载锰基催化剂的制备及其低温NH3选择催化还原NO
引用本文:吴大旺,张秋林,林 涛,龚茂初,陈耀强. CexTi1-xO2负载锰基催化剂的制备及其低温NH3选择催化还原NO[J]. 无机化学学报, 2011, 27(1): 53-60
作者姓名:吴大旺  张秋林  林 涛  龚茂初  陈耀强
作者单位:1. 黔南民族师范学院化学与化工系,都匀,558000;四川大学化学学院,绿色化学与技术教育部重点实验室,成都,610064
2. 四川大学化学学院,绿色化学与技术教育部重点实验室,成都,610064
基金项目:贵州省教育厅自然科学基金,国家自然科学基金
摘    要:用共沉淀法制备了CexTi1-xO2复合氧化物载体。XRD和低温N2吸附-脱附结果指出,当0.2≤x≤0.4时,CexTi1-xO2载体主要以无定形态存在,且Ce0.4Ti0.6O2的比表面积和孔容最大。Mn-Fe/CexTi1-xO2系列催化剂低温NH3选择性催化还原(SCR)NO活性结果表明,Mn-Fe/CexTi1-xO2的活性随着Ce含量的增加先增大后减小,其中Mn-Fe/Ce0.4Ti0.6O2的活性最佳,在41000 h-1空速下,催化剂在75℃起燃,NO转化率在113℃时即超过90%。而XRD和XPS分析结果指出,Mn-Fe/Ce0.4Ti0.6O2催化剂主要以无定形或微晶的形式存在,催化剂表面Mn和Fe与载体间存在强相互作用,且催化剂表面存在Ce3+/Ce4+氧化还原电对和较多的化学吸附氧,有利于NO氧化成NO2,同时催化剂表现出了较好的抗H2O和SO2性能。

关 键 词:低温  选择性催化还原(SCR)  氮氧化物    

CexTi1-xO2 Supported Manganese-Based Catalyst: Preparation and Catalytic Performance for Selective Reduction of NO with NH3 at Lower Temperature
WU Da-Wang,ZHANG Qiu-Lin,LIN Tao,GONG Mao-Chu and CHEN Yao-Qiang. CexTi1-xO2 Supported Manganese-Based Catalyst: Preparation and Catalytic Performance for Selective Reduction of NO with NH3 at Lower Temperature[J]. Chinese Journal of Inorganic Chemistry, 2011, 27(1): 53-60
Authors:WU Da-Wang  ZHANG Qiu-Lin  LIN Tao  GONG Mao-Chu  CHEN Yao-Qiang
Affiliation:Department of Chemistry and Chemical Engineering, Qiannan Normal University, Duyun, Guizhou 558000, China; Key Laboratory of Green Chemistry & Technology, Ministry of Education, Sichuan University, Chengdu 610064, China,Key Laboratory of Green Chemistry & Technology, Ministry of Education, Sichuan University, Chengdu 610064, China,Key Laboratory of Green Chemistry & Technology, Ministry of Education, Sichuan University, Chengdu 610064, China,Key Laboratory of Green Chemistry & Technology, Ministry of Education, Sichuan University, Chengdu 610064, China and Key Laboratory of Green Chemistry & Technology, Ministry of Education, Sichuan University, Chengdu 610064, China
Abstract:The CexTi1-xO2 complex oxides were prepared by co-precipitation method.The XRD and low temperatureN2 adsorption-desorption results show that the CexTi1-xO2 exists in amorphous form when x is in the range of 0.2≤x≤0.4,and the Ce0.4Ti0.6O2 has the largest surface area and pore volume.The activity results of NH3 selective catalytic reduction(SCR) of NO at lower temperature indicate that the activity of Mn-Fe/CexTi1-xO2catalysts increases at the beginning and then decreases with the increase of Ce,and the activity of Mn-Fe/Ce0.4Ti0.6O2 is the best at the spacevelocity of 41 000 h-1,the light-off temperature is at 75 ℃,and the NO conversion exceeds 90% at 113 ℃.The XRDand XPS results show that the Mn-Fe/Ce0.4Ti0.6O2 mainly exists as amorphous or microcrystalline form,and there isstrong interaction between the surface Mn and Fe of Mn-Fe/Ce0.4Ti0.6O2 and its support.The surface of Mn-Fe/Ce0.4Ti0.6O2 has Ce3+/Ce4+ redox couple and more chemisorbed oxygen compared with Mn-Fe/TiO2,which is beneficialto the oxidation of NO to NO2.The Mn-Fe/Ce0.4Ti0.6O2 also exhibits excellent resistance to H2O and SO2.
Keywords:Low temperature   selective catalytic reduction(SCR)   nitrogen oxide   ammonia   cerium
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