富氧条件下Fe-Mn/Beta选择性催化丙烯还原氮氧化物
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  • 英文篇名:Selective catalytic reduction of nitric oxide with propylene in excess oxygen over Fe-Mn/Beta catalysts
  • 作者:周皞 ; 李梦雨 ; 赵辉爽 ; 伍士国 ; 叶必朝 ; 苏亚欣
  • 英文作者:ZHOU Hao;LI Meng-yu;ZHAO Hui-shuang;WU Shi-guo;YE Bi-chao;SU Ya-xin;Changzhou Institute of Engineering Technology;School of Environmental Science and Engineering,Donghua University;
  • 关键词:选择性催化还原 ; NO ; 丙烯 ; ; 水热老化
  • 英文关键词:selective catalytic reduction;;NO;;C3H6;;manganese;;hydrothermal aging
  • 中文刊名:RLHX
  • 英文刊名:Journal of Fuel Chemistry and Technology
  • 机构:常州工程职业技术学院;东华大学环境科学与工程学院;
  • 出版日期:2019-06-25 14:08
  • 出版单位:燃料化学学报
  • 年:2019
  • 期:v.47
  • 基金:国家自然科学基金(51278095);; 江苏省自然科学基金(BK20181161);; 江苏省高校“青蓝工程”项目(2017)资助~~
  • 语种:中文;
  • 页:RLHX201906013
  • 页数:11
  • CN:06
  • ISSN:14-1140/TQ
  • 分类号:121-131
摘要
以Beta分子筛为载体,采用等体积浸渍法制备Fe-Mn/Beta催化剂,并对其在富氧条件下丙烯选择性催化还原NO性能进行了研究。通过N_2吸附-脱附、X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)、程序升温还原(H_2-TPR)和原位漫反射傅里叶变换红外光谱(in-situ DRIFTS)等研究手段对催化剂进行表征,考察M n组分对催化剂的物理化学性质、C_3H_6-SCR反应活性和反应中间产物的影响。结果表明,引入M n物种可以显著提高Fe-M n/Beta催化剂的低温催化活性,1.5Fe1.0Mn/Beta催化剂NO还原效率350℃最高可达99.4%,在250-400℃反应温度下显示出很高的反应活性和N_2选择性。原位红外光谱研究表明,分子筛离子交换位上孤立的铁离子是丙烯选择性氧化的主要活性位,分散良好的Mn O_2物种不能提高催化剂对丙烯的活化能力,但有助于促进形成NO_2吸附物种,从而提升了Fe-Mn/Beta催化剂的低温C_3H_6-SCR性能。经高温水热老化处理后,Fe-Mn/Beta催化剂脱硝活性明显下降,这与孤立的Fe~(3+)离子迁移形成Fe_xO_y团聚物种有关。
        Fe-Mn/Beta catalysts were prepared by incipient wet-impregnation methods and used for selective catalytic reduction of nitric oxide with propylene in excess oxygen. The catalysts were characterized using N_2-physisorption,X-ray diffraction( XRD),X-ray photoelectron spectroscopy( XPS),transmission electron microscopy( TEM),H_2-temperature programmed reduction( H_2-TPR) and in-situ diffuse reflectance infrared Fouier transform spectroscopy( in-situ DRIFTS) techniques. The effects of Mn component on the physicochemical properties,C_3H_6-SCR activity and reaction intermediates of catalysts were also investigated. The results showed that C_3H_6-SCR activity of Fe-Mn/Beta catalysts at low temperature could be significantly improved by introducing Mn species. 1. 5 Fe1. 0 Mn/Beta catalyst achieved the highest activity with a nitrogen oxide conversion of 99.4% at 350 ℃,which possessed high catalytic performance and N_2 selectivity within the temperature window of 250-400 ℃. Based on the in-situ DRIFT studies,the isolated Fe~(3+) ions at the ionexchange sites were the main active sites for selective oxidation of propylene. Although the well-dispersed MnO_2 species could not improve the activation ability of the catalysts for propylene,they would enhance the formation of NO_2 adsorption species,then promoted C_3H_6-SCR activity at the low temperature. The significant decrease of SCR activity after hydrothermal aging of Fe-Mn/Beta catalysts might be due to the migration of isolated Fe~(3+) ions into oligomeric clusters.
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