New Insights into the Active Surface Species of Silver Alumina Catalysts in the Selective Catalytic Reduction of NO

被引:60
|
作者
Korhonen, Satu T. [1 ,2 ]
Beale, Andrew M. [1 ]
Newton, Mark A. [3 ]
Weckhuysen, Bert M. [1 ]
机构
[1] Univ Utrecht, Debye Inst NanoMat Sci, NL-3584 CA Utrecht, Netherlands
[2] Mat Innovat Inst M2i, NL-2628 CD Delft, Netherlands
[3] European Synchrotron Facil, F-38043 Grenoble 9, France
关键词
HIGHER HYDROCARBONS; REACTION-MECHANISM; AG/AL2O3; CATALYST; NITROGEN-OXIDES; EXHAUST-GASES; HYDROGEN; H-2; SCR; PROPENE; PROPANE;
D O I
10.1021/jp102530y
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
The performance of silver alumina catalysts and silver aluminate was studied in the selective catalytic reduction (SCR) of NO by propene. The use of boehmite during the impregnation step ensured a strong interaction between the silver species and the alumina surface in the final calcined catalyst. Thus, higher silver loadings (5-7 wt % silver) could be used without significant loss in selectivity to N-2 during SCR. The nature of the silver species and the formation of adsorbed surface species during SCR and hydrogen-assisted SCR (H-2-SCR) was studied by activity measurements and by combined in situ IR and X-absorption spectroscopic measurements. The combination of these techniques in the same reaction cell allowed simultaneous monitoring of the state of silver and the formation of surface species under realistic reaction conditions. The active silver species on alumina support were concluded to be 2-dimensional oxidic Ag-n(delta+) species. Silver aluminate was ruled out as a possibility for an active phase for the SCR reaction. The oxidic Ag-n(delta+) species were present under both SCR and H-2-SCR reaction conditions and even on a prereduced catalyst under the SCR reaction conditions. Hydrogen is proposed to enhance the formation of adsorbed surface species, especially nitrites, but not to change the nature of the active silver sites.
引用
收藏
页码:885 / 896
页数:12
相关论文
共 50 条
  • [31] Review on the selective catalytic reduction of NOx with H2 by using novel catalysts
    Guan, Yu
    Liu, Yinhe
    Lv, Qiang
    Wang, Bo
    Che, Defu
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2021, 9 (06):
  • [32] Selective Reduction of Nitrogen Oxides (NOx) with Oxygenates and Hydrocarbons over Bifunctional Silver–Alumina Catalysts: a Review
    N. O. Popovych
    S. O. Soloviev
    S. M. Orlyk
    Theoretical and Experimental Chemistry, 2016, 52 : 133 - 151
  • [33] Constructing highly active vanadyl species for efficient selective catalytic reduction of NOX
    Lin, Chunxi
    Lian, Zhihua
    Huang, Weidong
    Wang, Qiang
    Zhang, Hui
    Liu, Xiaofeng
    Deng, Feng
    Shi, Xiaoyan
    Shan, Wenpo
    He, Hong
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2024, 12 (04):
  • [34] Selective catalytic reduction of NO by propene in excess oxygen on Pt- and Rh-supported alumina catalysts
    Nikolopoulos, AA
    Stergioula, ES
    Efthimiadis, EA
    Vasalos, IA
    CATALYSIS TODAY, 1999, 54 (04) : 439 - 450
  • [35] Identification of Intrinsic Active Sites for the Selective Catalytic Reduction of Nitric Oxide on Metal-Free Carbon Catalysts via Selective Passivation
    Yuan, Jin
    Mi, JinXing
    Yin, Rongqiang
    Yan, Tao
    Liu, Hao
    Chen, Xiaoping
    Liu, Jun
    Si, Wenzhe
    Peng, Yue
    Chen, Jianjun
    Li, Junhua
    ACS CATALYSIS, 2022, 12 (02) : 1024 - 1030
  • [36] Study on the Fuel-Reforming-Assisted Hydrocarbon Selective Catalytic Reduction over Silver/Alumina Catalyst
    Lee, Jaewook
    Song, Soonho
    Chun, Kwang Min
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (08) : 3553 - 3560
  • [37] Selective catalytic reduction of nitrogen oxides with methanol over the (cobalt-molybdenum)/alumina dual catalysts under the diesel methanol dual fuel exhaust conditions
    Chen, Chao
    Yao, Anren
    Yao, Chunde
    Wang, Hui
    Liu, Mingkuan
    Li, Zhuangzhuang
    CHEMICAL ENGINEERING SCIENCE, 2020, 211 (211)
  • [38] Effect of the modification of alumina supports with chloride on the structure and catalytic performance of Ag/Al2O3 catalysts for the selective catalytic reduction of NOx with propene and H2/propene
    Wang, Jia
    You, Rui
    Qian, Kun
    Pan, Yang
    Yang, Jiuzhong
    Huang, Weixin
    CHINESE JOURNAL OF CATALYSIS, 2021, 42 (12) : 2242 - 2253
  • [39] Reactivity of surface complexes in the selective catalytic reduction of NOx on supported heteropoly compounds
    Sil'chenkova, O. N.
    Matyshak, V. A.
    Tret'yakov, V. F.
    Korchak, V. N.
    KINETICS AND CATALYSIS, 2014, 55 (01) : 103 - 110
  • [40] Role of surface structures on the selective reduction of nitrogen oxides with hydrocarbons on oxide catalysts
    Matyshak, V. A.
    Tret'yakov, V. F.
    RUSSIAN JOURNAL OF GENERAL CHEMISTRY, 2009, 79 (06) : 1400 - 1411