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富铈Ce1-xLaxO2催化甲烷氧氯化性能
引用本文:徐术,费兆阳,陈献,汤吉海,崔咪芬,乔旭.富铈Ce1-xLaxO2催化甲烷氧氯化性能[J].化工进展,2015,34(12):4248-4253.
作者姓名:徐术  费兆阳  陈献  汤吉海  崔咪芬  乔旭
作者单位:1.南京工业大学材料化学工程国家重点实验室, 江苏 南京 210009;2.南京工业大学化学化工学院, 江苏 南京 210009
基金项目:国家科技支撑计划(2011BAE18B01)及国家自然科学基金青年基金(21306089)项目。
摘    要:以硝酸铈、硝酸镧为前体,用氨水共沉淀法制备了一系列Ce1-xLaxO2(x≤0.5)催化剂,利用XRD、N2吸附-脱附、SEM、Raman、H2-TPR和OSC对催化剂的物理化学性质进行了表征,并考察其在甲烷氧氯化反应中的催化性能。结果表明:Ce1-xLaxO2催化剂的氧化还原性质随着镧含量的变化发生显著改变,并且这一性质的变化与反应的转化率及产物分布具有较强的联系。Ce1-xLaxO2表面氧物种的活泼性对催化剂活性影响显著,而体相氧物种容易将生成的甲烷氯化物深度氧化。在Ce1-xLaxO2(x<0.3)催化剂上表面氧物种起主导作用,氯甲烷为主要反应产物,Ce0.8La0.2O2催化剂上氯甲烷选择性最高为52%。在体相氧物种更活泼的Ce0.7La0.3O2和Ce0.5La0.5O2上产物中CO的选择性显著上升,Ce0.5La0.5O2催化剂上CO选择性高达48%。稳定性测试表明Ce0.8La0.2O2催化剂具有良好的稳定性。

关 键 词:甲烷  活化  氧化  Ce1-xLaxO2  氧氯化  氯甲烷  
收稿时间:2015-03-06

Catalytic performance of Ce-rich Ce1-xLaxO2 oxides in CH4 oxy-chlorination
XU Shu,FEI Zhaoyang,CHEN Xian,TANG Jihai,CUI Mifen,QIAO Xu.Catalytic performance of Ce-rich Ce1-xLaxO2 oxides in CH4 oxy-chlorination[J].Chemical Industry and Engineering Progress,2015,34(12):4248-4253.
Authors:XU Shu  FEI Zhaoyang  CHEN Xian  TANG Jihai  CUI Mifen  QIAO Xu
Affiliation:1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech. University, Nanjing 210009, Jiangsu, China;2 College of Chemistry and Chemical Engineering, Nanjing Tech. University, Nanjing 210009, Jiangsu, China
Abstract:A series of Ce1-xLaxO2(x≤0.5) catalysts were prepared by ammonia co-precipitation method and characterized by XRD,N2 adsorption-desorption,SEM,Raman,H2-TPR and OSC. Then their catalytic performances in CH4 oxy-chlorination to chloromethane were investigated. The results showed that the redox properties of Ce1-xLaxO2 changed significantly with the change of the lanthanum content,and there should be a strong link between this change and the conversion and product distribution. More specificly,the surface oxygen species had a remarkable influence on the activities of the catalysts,while advanced oxidation of the generated methane chloride was easily induced by bulk oxygen species. Chloromethane was the main product over Ce1-xLaxO2(x<0.3) and the highest selectivity of chloromethane (52%) could be obtained over Ce0.8La0.2O2. A significant increase of CO selectivity was found over Ce0.7La0.3O2 and Ce0.5La0.5O2 as they had more active bulk oxygen species,and Ce0.5La0.5O2 showed the highest selectivity of CO (48%). The long-term stability test showed that Ce0.8La0.2O2 catalyst had a good stability.
Keywords:methane  activation  oxidation  Ce1-xLaxO2  oxy-chlorination  methyl chloride  
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