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| 非晶Ce-Ti氧化物用于NH3选择性催化还原NO的原位红外研究 | |
| 引用本文： | 李倩,谷华春,李萍,周钰浩,刘莹,齐中囡,辛颖,张昭良. 非晶Ce-Ti氧化物用于NH3选择性催化还原NO的原位红外研究[J]. 催化学报, 2014, 35(8): 1289-1298. DOI: 10.1016/S1872-2067(14)60154-6 |
| 作者姓名： | 李倩 谷华春 李萍 周钰浩 刘莹 齐中囡 辛颖 张昭良 |
| 作者单位： | a. 济南大学化学化工学院, 山东济南 250022; b. 南京信息工程大学环境科学与工程学院, 江苏省大气环境监测与污染控制高技术研究重点实验室, 江苏南京 210044 |
| 基金项目： | 国家自然科学基金（21277060和21107030）；山东省科技发展计划项目（2011GSF11702）；山东省优秀中青年科学家科研奖励基金（BS2011HZ002）；山东省自然科学基金（ZR2013BQ003）；江苏省大气环境监测与污染控制高技术研究重点实验室开放基金（KHK1116），江苏省环境科学与工程优势学科平台. |
| 摘 要： | 采用原位红外光谱研究了在具有短程有序Ce-O-Ti结构的非晶Ce-Ti氧化物上NH3选择性催化还原（SCR） NOx反应. 在反应条件下，催化剂表面主要被NH3吸附物种覆盖，而检测不到NOx吸附物种. 经测定，NO的反应级数为0.5-0.6，表明Langmuir-Hinshelwood机理和Eley-Rideal机理同时存在. 可能的机理是NH3吸附物种和弱吸附的NOx反应，生成NHyNO3 （y = 0-4）活性中间物种，并通过GAUSSIAN计算和原位红外结果证实了它们的存在. Ce-O-Ti结构中Ce与Ti之间表现出原子尺度的相互作用，所以在SCR反应的活性温度窗口下，催化剂的氧化还原活性提高. |
| 关 键 词： | 选择性催化还原 一氧化氮 氨气 非晶Ce-Ti氧化物 原位红外 机理 |
| 收稿时间： | 2014-03-31 |
In situ IR studies of selective catalytic reduction of NO with NH3 on Ce-Ti amorphous oxides |
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| Qian Li,Huachun Gu,Ping Li,Yuhao Zhou,Ying Liu,Zhongnan Qi,Ying Xin,Zhaoliang Zhang. In situ IR studies of selective catalytic reduction of NO with NH3 on Ce-Ti amorphous oxides[J]. Chinese Journal of Catalysis, 2014, 35(8): 1289-1298. DOI: 10.1016/S1872-2067(14)60154-6 | |
| Authors: | Qian Li Huachun Gu Ping Li Yuhao Zhou Ying Liu Zhongnan Qi Ying Xin Zhaoliang Zhang |
| Affiliation: | a. School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, Shandong, China; b. Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Sciences and Engineering, Nanjing University of Information Sciences and Engineering, Nanjing 210044, Jiangsu, China |
| Abstract: | A series of in situ infrared (IR) studies of the selective catalytic reduction (SCR) of NOx with NH3 on the short-range ordered structure Ce-O-Ti sites in amorphous Ce-Ti mixed oxides were performed. Under the reaction conditions, the catalyst surface was mainly covered by NH3 ad-species and no NOx ad-species were detected. The reaction order of 0.5-0.6 with respect to NO confirmed a hybrid Langmuir-Hinshelwood and Eley-Rideal mechanism. A possible route may involve the reaction of NH3 ad-species and weakly adsorbed NOx to form an active intermediate, NHyNO3 (y = 0-4); this was confirmed by GAUSSIAN calculations and the in situ IR results. The Ce-O-Ti structure, with Ce-Ti interactions on the atomic scale, enhanced the redox properties in the active temperature window of the SCR reactions. |
| Keywords: | Selective catalytic reduction Nitrogen oxide Ammonia Amorphous Ce-Ti mixed oxide In situ infrared Mechanism |
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