基于钛锡载体的SCR低温脱硝催化剂的表面性质研究

郭婉秋; 张亚平; 王文选; 赵明; 王俊杰; 沈凯; 王龙飞; 杨林军

基于钛锡载体的SCR低温脱硝催化剂的表面性质研究

1.
东南大学能源与环境学院能源热转换及其过程测控教育部重点实验室, 江苏南京 210096;
2.
江苏万德环保科技有限公司, 江苏扬州 225131;
3.
云南电网有限责任公司电力科学研究院, 云南昆明 650217

基金项目: 国家自然科学基金(51306034),国家重点基础研究发展规划(973计划,2013CB228505)和江苏省自然科学基金(BK2012347)资助项目

详细信息

通讯作者:
张亚平,Tel:025-83790667,E-mail:amflora@seu.edu.Cn

中图分类号: O643.36
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出版历程
- 收稿日期: 2015-05-22
- 修回日期: 2015-07-28
- 刊出日期: 2015-11-30

Study on the surface properties of TiO₂-SnO₂ supported catalysts for low temperature selective catalytic reduction of NO_x

1.
Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, China;
2.
Jiangsu Wande Environmental Protection Technology CO. , LTD, Yangzhou 225131, China;
3.
Electric Power Research Institute, Yunnan Electric Power Test and Research Institute, Kunming 650217, China

Funds: The project was supported by the National Natural Science Foundation of China (51306034), the Major State Basic Research Development Program of China (973 Program, 2013CB228505), the Natural Science Foundation of Jiangsu Province (BK2012347).

摘要

摘要: 采用共沉淀法制备TiO₂-SnO₂固溶体,浸渍法负载CeO₂得到一系列xCeO₂/TiO₂-SnO₂负载型催化剂,在模拟NH₃选择性催化还原NO_x(NH₃-SCR)反应条件下考察催化剂低温脱硝活性。通过X射线衍射(XRD)、比表面积测定(BET)、程序升温还原(H₂-TPR)、程序升温脱附(NH₃-TPD)、高分辨率透射电子显微镜(HRTEM)、原位漫反射傅里叶变换红外光谱(in situ DRIFTS)等表征技术,研究了氧化铈负载后催化剂的微观结构、表面物种的存在状态、表面酸位等表面性质及NH₃吸附特性。结果表明,Ce:Ti物质的量比为0.1时,催化剂催化脱硝反应活性最高,同时具有较宽的温度窗口(250~300℃)和热稳定性;铈的过量负载会导致催化剂比表面积减小、活性窗口变窄,同时其氧化还原能力和NH₃吸附能力也减弱。NH₃-TPD结果显示,CeO₂的负载导致催化剂NH₃在弱酸及中等酸位的吸附显著增强,与催化剂NH₃-SCR最佳反应物温度降低有关。in situ DRIFTS表明,xCeO₂/TiO₂-SnO₂催化剂的Lewis酸位和Brønsted酸位强度均明显增强,同时,在1657~1666cm^-1处出现新的Brønsted酸位,参与SCR反应的主要物质是NH₄⁺分子。
- CeO₂ /
- TiO₂-SnO₂固溶体 /
- SCR低温脱硝 /
- 表面性质 /
- NH₃吸附
Abstract: TiO₂-SnO₂ mixed oxide was prepared by a co-precipitation method and xCeO₂/TiO₂-SnO₂ catalysts were prepared using the impregnation method. The physicochemical properties were investigated by X-ray diffraction (XRD), BET specific surface area measurement, H₂ temperature-programmed reduction (H₂-TPR), NH₃ temperature-programmed desorption (NH₃-TPD), high-resolution transmission electron microscopy (HRTEM), and in situ diffuse reflectance infrared spectroscopy (DRIFTS). Meanwhile, their catalytic performance for the selective catalytic reduction of NO_x with NH₃(NH₃-SCR)was tested. It was found that 0.1Ce/TiO₂-SnO₂ had higher NO_x conversion and wider temperature range of 250~350℃. Excess loading of CeO₂ could lead to the decrease of specific surface area, redox ability and adsorption capacity of ammonia as well as the shrink of effective catalytic temperature range. NH₃-TPD result showed that the adsorption of NH₃ in weak acid and medium acid sites were significantly enhanced by CeO₂, which was related to the decrease of NH₃-SCR reaction temperature. In situ DRIFTS indicated that the strength of Lewis acid sites and Brønsted acid Sites were markedly enhanced for xCeO₂/TiO₂-SnO₂ catalyst. Besides, new Brønsted acid Sites appeared at 1657~1666cm^-1 and NH₄⁺ played the dominant role in the SCR reaction.
- cerium dioxide /
- TiO₂-SnO₂solid solution /
- SCR denitrification at low temperature /
- surface property /
- ammonia adsorption

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