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铁铈复合催化剂的低温SCR脱硝性能
引用本文:杨瀚, 仲兆平, 朱林, 王春华. 铁铈复合催化剂的低温SCR脱硝性能[J]. 环境工程学报, 2017, 11(4): 2413-2418. doi: 10.12030/j.cjee.201602108
作者姓名:杨瀚  仲兆平  朱林  王春华
作者单位: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, 南京 210096; 2.南京航空航天大学能源与动力学院, 南京 210016
基金项目:江苏省政策引导类计划(产学研合作)项目(BY2015070-21) 江苏省自然科学基金项目(BK20150749)
摘    要:以柠檬酸酸法制备了不同铁铈比例的脱硝催化剂并将其用于NOx的低温NH3选择性催化还原,通过N2吸附、XRD和TPD手段对催化剂进行表征,并考察了H2O和SO2对催化剂性能的影响。结果表明:Ce的掺杂显著提高铁基催化剂的低温SCR性能,0.10CeFeOx催化剂在200~300 ℃,60 000 h-1空速下能达到85%以上的效率;Ce的掺杂能够提高催化剂比表面积和改善催化剂孔结构,有助于反应气体吸附以及提供更多的活性位点;铁铈之间有较强的相互作用,掺杂Ce后,Fe、Ce以无定型态存在,形成良好固溶体,并且大幅提高了催化剂表面酸性强度;在250 ℃,由于5%(vol)H2O竞争吸附导致0.10CeFeOx催化剂反应效率有所下降,但仍保持在90%左右;对于模拟烟气中SO2的毒化作用,250 ℃时0.10CeFeOx催化剂反应效率下降明显。

关 键 词:低温脱硝   选择性催化还原   铁铈复合氧化物   铈掺杂   氮氧化物
收稿时间:2016-04-02

Low temperature selective catalytic reduction of NO with NH3 over CeFeOx catalyst
YANG Han, ZHONG Zhaopin, ZHU Lin, WANG Chunhua. Low temperature selective catalytic reduction of NO with NH3 over CeFeOx catalyst[J]. Chinese Journal of Environmental Engineering, 2017, 11(4): 2413-2418. doi: 10.12030/j.cjee.201602108
Authors:YANG Han  ZHONG Zhaopin  ZHU Lin  WANG Chunhua
Affiliation:1.Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, China; 2.College of Energy & Power Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China
Abstract:A series of cerium-iron mixed oxide catalysts were synthesized using the citric acid method and were investigated for use in the low temperature selective catalytic reduction (SCR) of NOx. The catalysts were characterized by N2 adsorption, X-ray diffraction (XRD), and temperature programmed desorption (TPD) techniques. The H2O and SO2 durability of the catalyst was studied. The SCR of NOx at low temperatures was greatly improved by Ce-doping of the iron oxide catalyst. Indeed, mixed oxide catalysts with a Ce/(Fe+Ce) molar ratio of 0.10 yielded >85% NOx conversion between 200 and 300 ℃at a space velocity of 60 000 h-1. Greater specific areas and improved pore structures were obtained upon Ce-doping of the iron oxide catalyst, which contributed to the adsorption of reaction gases and provided additional active sites. In addition, a solid solution was formed due to the strong interactions between Fe and Ce. Furthermore, cerium doping significantly enhanced the surface acidity of the catalyst. Finally, due to competitive adsorption in the presence of 5 vol% H2O, the SCR activity of the 0.10 CeFeOx catalyst declined slightly, reaching a constant value of 90% at 250 ℃. However, due to deactivation by SO2, the SCR activity decreased significantly at 250 ℃.
Keywords:low-temperature de-NOx  selective catalytic reduction  Ce-Fe oxides  Ce-doping  nitrogen oxide
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