| 谢兴星,费兆阳,戴勇,徐希化,陈献,汤吉海,崔咪芬,乔旭.铈基复合氧化物的结构及其对HCl催化氧化性能的影响[J].分子催化,2014,(6):507-514 |
| 铈基复合氧化物的结构及其对HCl催化氧化性能的影响 |
| Structure of Ceria-based Mixed Oxides and Its Influence on HCl Catalytic Oxidation Performance |
| 投稿时间：2014-09-09 修订日期：2014-11-10 |
| DOI： |
| 中文关键词: 铈基复合氧化物 氯化氢 催化氧化 循环利用 氯气 |
| 英文关键词:Ceria-based mixed oxide HCl Catalytic oxidation Recycle Chlorine |
| 基金项目:国家科技支撑计划(2011BAE18B01)；国家自然科学青年基金(21306089)；江苏省科技支撑计划(BE2011830)；江苏省高校自然科学基金面上项目（13KJB530006）；中国博士后基金（2013M531340）。;中国博士后科学基金 |
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| 中文摘要: |
| 采用氨水共沉淀法制备了一系列铈基复合氧化物(Ce0.9M0.1O2，M= Cu、Cr、Zr、Ti、La)，借助XRD、Raman、N2吸附-脱附、ESEM和H2-TPR等手段对复合氧化物的结构进行了表征并考察了其在HCl催化氧化制Cl2过程中的性能。结果显示：Cu、Cr和Zr掺杂能显著减小复合氧化物晶粒尺寸，提高复合氧化物的比表面积和孔容，并提供更多的低温可还原氧物种。而La和Ti的掺杂可以获得较大的表面氧空位浓度以及增加高温可还原氧物种数目。复合氧化物结构和表面性质的变化显著影响了其HCl催化氧化活性，在430 癈下铈基复合氧化物催化剂活性顺序为：Ce0.9Cu0.1O2 > Ce0.9Cr0.1O2 > Ce0.9Zr0.1O2 > Ce0.9Ti0.1O2 > CeO2 > Ce0.9La0.1O2。反应动力学测试显示催化剂低温可还原氧物种有利于HCl在催化剂表面的吸附和活化，而催化剂表面的氧空位可以促进氧分子的吸附和活化。 |
| 英文摘要: |
| The physiochemical properties of ceria-based mixed oxides (Ce0.9M0.1O2，M= Cu, Cr, Zr, Ti and La) prepared by ammonia co-precipitation method were characterized by XRD, Raman, N2 adsorption-desorption, ESEM and H2-TPR. The performances of catalysts for gas-phase HCl catalytic oxidation to Cl2 were also investigated. The results showed that the incorporation of Cu, Cr and Zr could greatly reduce the grain size of ceria-based mixed oxides, leading to a higher surface area and pore volume, and enhance the reduction of oxygen species at low temperature. While more surface oxygen vacancies and improved reduction of oxygen species at high temperature could be obtained in Ce0.9Ti0.1O2 and Ce0.9La0.1O2. The changed structure and surface property of mixed oxides showed a significant influence on its HCl catalytic oxidation performance, the order of the activities of various ceria-based mixed oxide catalysts at 430 癈 was as follows: Ce0.9Cu0.1O2 > Ce0.9Cr0.1O2 > Ce0.9Zr0.1O2 > Ce0.9Ti0.1O2 > CeO2 > Ce0.9La0.1O2. Kinetic studies showed that the catalysts with more reduction of oxygen species at low temperature provided more active sites for HCl adsorption and activation, while the oxygen vacancies were conducive to the adsorption and activation of gas-phase oxygen. |
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