Fe-Ti spinel for the selective catalytic reduction of NO with NH3: Mechanism and structure-activity relationship

被引:186
作者
Yang, Shijian [1 ,2 ]
Li, Junhua [1 ]
Wang, Chizhong [1 ]
Chen, Jinghuan [1 ]
Ma, Lei [1 ]
Chang, Huazhen [1 ]
Chen, Liang [1 ]
Peng, Yue [1 ]
Yan, Naiqiang [2 ]
机构
[1] Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
关键词
(Fe3-xTix)(1-delta)O-4; DRIFTS; Structure-activity relationship; Mechanism; Kinetic analysis; NITRIC-OXIDE; IRON; PERFORMANCE; MNOX/AL2O3; AMMONIA; SITU; SO2;
D O I
10.1016/j.apcatb.2012.01.001
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A series of non-stoichiometric Fe-Ti spine! (Fe3-xTix)(1-delta)O-4 were synthesized using a co-precipitation method and then developed as environmental-friendly and low cost catalysts for the selective catalytic reduction (SCR) of NO with NH3. As Ti was incorporated into gamma-Fe2O3, the SCR reaction over (Fe3-xTix)(1-delta)O-4 through the Langmuir-Hinshelwood mechanism was restrained. Therefore, the SCR activity of (Fe3-xTix)(1-delta)O-4 (x not equal 0) was less than that of gamma-Fe2O3 at 150-250 degrees C. However, the SCR reaction over (Fe3-xTix)(1-delta)O-4 through the Eley-Rideal mechanism was promoted due to the incorporation of Ti. The SCR activity of (Fe3-xTix)(1-delta)O-4(x not equal 0) was mainly related to the oxidative ability of Fe3+ cation on the surface, the concentration of NH3 adsorbed on the surface and the concentration of reducible Fe3+ cation on the surface. Although the oxidative ability of Fe3+ cation on the surface decreased due to the incorporation of Ti into gamma-Fe2O3, the concentration of NH3 adsorbed on the surface and the concentration of reducible Fe3+ cation on the surface both increased. As a result, (Fe2Ti)(0.8)O-4 showed excellent activity, selectivity, and H2O/SO2 durability for the SCR reaction at 300-400 degrees C. (C) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:73 / 80
页数:8
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