Sulfur poisoning and regeneration of the Ag/γ-Al2O3 catalyst for H2-assisted SCR of NOx by ammonia

被引:33
作者
Doronkin, Dmitry E. [1 ]
Khan, Tuhin Suvra [2 ]
Bligaard, Thomas [3 ]
Fogel, Sebastian [1 ,4 ]
Gabrielsson, Par [4 ]
Dahl, Soren [1 ]
机构
[1] Tech Univ Denmark, Dept Phys, CINF, DK-2800 Lyngby, Denmark
[2] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design CAMD, DK-2800 Lyngby, Denmark
[3] SLAC Natl Accelerator Lab, SUNCAT Ctr Interface Sci & Catalysis, Menlo Pk, CA 94025 USA
[4] Haldor Topsoe Res Labs, DK-2800 Lyngby, Denmark
关键词
Ag/Al2O3; SO2; NOx SCR; Poisoning; Regeneration; LEAN-BURN CONDITIONS; SELECTIVE REDUCTION; SILVER-ALUMINA; AG/AL2O3; SO2; HYDROCARBONS; ADSORPTION; OXIDE; TOLERANCE; SUPPORT;
D O I
10.1016/j.apcatb.2012.01.002
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
Sulfur poisoning and regeneration mechanisms for a 2% Ag/gamma-Al2O3 catalyst for the H-2-assisted selective catalytic reduction of NOx by NH3 are investigated. The catalyst has medium sulfur tolerance at low temperatures, however a good capability of regeneration at 670 degrees C under lean conditions when H-2 is present. These heating conditions can easily be established during soot filter regeneration. Furthermore, two types of active sites could be identified with different regeneration capabilities, namely finely dispersed Ag and larger Ag nanoparticles. The most active sites are associated with the finely dispersed Ag. These sites are irreversibly poisoned and cannot be regenerated under driving conditions. On the other hand the larger Ag nanoparticles are reversibly poisoned by direct SOx adsorption. The interpretation of the data is supported by DFT calculations. (C) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:49 / 58
页数:10
相关论文
共 33 条
[1]   Effect of SO2 on NOx reduction by ethanol over Ag/Al2O3 catalyst [J].
Abe, A ;
Aoyama, N ;
Sumiya, S ;
Kakuta, N ;
Yoshida, K .
CATALYSIS LETTERS, 1998, 51 (1-2) :5-9
[2]  
[Anonymous], 2007, Official Journal of the European Union, L, V324/121
[3]  
[Anonymous], 1998, J. Phys. Chem. Ref. Data
[4]  
[Anonymous], 2009, Official Journal of the European Union, L, V286/36
[5]   An investigation of the thermal stability and sulphur tolerance of Ag/γ-Al2O3 catalysts for the SCR of NOx with hydrocarbons and hydrogen [J].
Breen, J. P. ;
Burch, R. ;
Hardacre, C. ;
Hill, C. J. ;
Krutzsch, B. ;
Bandl-Konrad, B. ;
Jobson, E. ;
Cider, L. ;
Blakeman, P. G. ;
Peace, L. J. ;
Twigg, M. V. ;
Preis, M. ;
Gottschling, M. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 70 (1-4) :36-44
[6]   Microkinetic modeling of the fast selective catalytic reduction of nitrogen oxide with ammonia on H-ZSM5 based on first principles [J].
Brueggemann, Till C. ;
Vlachos, Dionisios G. ;
Keil, French J. .
JOURNAL OF CATALYSIS, 2011, 283 (02) :178-191
[7]   A review of the selective reduction of NOx, with hydrocarbons under lean-burn conditions with non-zeolitic oxide and platinum group metal catalysts [J].
Burch, R ;
Breen, JP ;
Meunier, FC .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2002, 39 (04) :283-303
[8]   Use of DFT to achieve a rational understanding of acid-basic properties of γ-alumina surfaces [J].
Digne, M ;
Sautet, P ;
Raybaud, P ;
Euzen, P ;
Toulhoat, H .
JOURNAL OF CATALYSIS, 2004, 226 (01) :54-68
[9]   Study of the "Fast SCR"-like mechanism of H2-assisted SCR of NOx with ammonia over Ag/Al2O3 [J].
Doronkin, Dmitry E. ;
Fogel, Sebastian ;
Tamm, Stefanie ;
Olsson, Louise ;
Khan, Tuhin Suvra ;
Bligaard, Thomas ;
Gabrielsson, Par ;
Dahl, Soren .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 113 :228-236
[10]  
Fogel S., UNPUB