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碱土金属钙沉积对Mn-Ce/TiO2低温SCR催化剂脱硝性能的影响
引用本文:周爱奕,毛华峰,盛重义,谭月,杨柳. 碱土金属钙沉积对Mn-Ce/TiO2低温SCR催化剂脱硝性能的影响[J]. 环境科学, 2014, 35(12): 4745-4751
作者姓名:周爱奕  毛华峰  盛重义  谭月  杨柳
作者单位:1. 南京师范大学环境科学与工程系,南京 210023; 江苏省物质循环与污染控制重点实验室,南京 210023
2. 江山市环境监测站,江山,324100
基金项目:江苏省自然科学基金项目,江苏省高校自然科学研究项目,南京师范大学高级人才科研启动项目,浙江省工业锅炉炉窑烟气污染控制工程技术研究中心开放基金
摘    要:本研究采用浸渍法分别制备CaCl2、CaCO3和CaSO4这3种钙盐前驱体沉积的Mn-Ce/TiO2催化剂,通过分析催化剂活性与催化剂理化特性之间的关系,考察碱土金属钙沉积对Mn-Ce/TiO2低温SCR催化剂脱硝性能的影响.结果表明,钙的加入会导致催化剂中毒,且不同钙前驱体掺杂对催化剂中毒效应不同.CaCO3的沉积对Mn-Ce/TiO2催化剂脱硝效率的影响最小,而CaCl2沉积对催化剂活性抑制作用最为强烈.通过比表面积测试(BET)、X射线光电子能谱(XPS)、X射线晶体衍射(XRD)、程序升温脱附(TPD)等方法对不同催化剂进行表征发现,催化剂的晶型变化、孔道结构破坏、表面活性元素及酸性点位的减少是催化剂中毒的主要原因.

关 键 词:低温选择性催化还原  锰铈钛复合氧化物  碱土金属  钙盐沉积  催化剂中毒
收稿时间:2014-05-12
修稿时间:2014-06-27

Poisoning Effect of Ca Depositing Over Mn-Ce/TiO2 Catalyst for Low-temperature Selective Catalytic Reduction of NO by NH3
ZHOU Ai-yi,MAO Hua-feng,SHENG Zhong-yi,TAN Yue and YANG Liu. Poisoning Effect of Ca Depositing Over Mn-Ce/TiO2 Catalyst for Low-temperature Selective Catalytic Reduction of NO by NH3[J]. Chinese Journal of Environmental Science, 2014, 35(12): 4745-4751
Authors:ZHOU Ai-yi  MAO Hua-feng  SHENG Zhong-yi  TAN Yue  YANG Liu
Affiliation:Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023, China;Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023, China;Jiangshan Environmental Monitoring Station, Jiangshan 324100, China;Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023, China;Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023, China;Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023, China;Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023, China;Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023, China;Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023, China
Abstract:Calcium carbonate (CaCO3), calcium sulfate (CaSO4), and calcium chloride (CaCl2) were chosen as the precursors to prepare the Ca salts deposited Mn-Ce/TiO2 catalysts through an impregnation method. The influence of Ca on the performance of the Mn-Ce/TiO2 catalyst for low-temperature selective catalytic reduction of NO by NH3 was investigated. Experimental results showed that Ca salts had negative effects on the activity of Mn-Ce/TiO2 and the precursors of Ca salts also affected the catalytic activity. The precursor CaCl2 had a greater impact on the catalytic activity, while CaCO3 had minimal effect. The samples were characterized by Brunner-Emmet-Teller measurements (BET), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and NH3 temperature programmed desorption (NH3-TPD). The characterization results indicated that the significant changes in physical and chemical properties of Mn-Ce/TiO2 were observed after Ca was deposited on the catalysts. The significant decreases in surface areas and NH3 adsorption amounts were observed after Ca was deposited on the catalysts, which could be considered as the main reasons for the deactivation of Ca deposited Mn-Ce/TiO2.
Keywords:low-temperature SCR  Mn-Ce/ TiO2 catalyst  alkali earth metal  Ca deposition  catalyst poisoning
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