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Published in: Topics in Catalysis 1-8/2013

01-05-2013 | OriginalPaper

Diesel Soot Catalyzes the Selective Catalytic Reduction of NOx with NH3

Authors: Max Mehring, Martin Elsener, Oliver Kröcher

Published in: Topics in Catalysis | Issue 1-8/2013

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Abstract

The catalytic activity of soot samples for the selective catalytic reduction (SCR) of NOx with NH3 was investigated in dependence of the NO2, NO and NH3 concentration in the temperature range between 200 and 350 °C. The highest NOx reduction of up to 25 % was measured in the presence of both NO2 and NO at a GHSV of 35,000 h−1. Decreasing space velocities resulted in an increase of the SCR activity. In the absence of NO2, NOx reduction was not observed. Carbon oxidation and SCR reaction occurred in parallel due to the presence of NO2 and O2, but hardly influenced each other, which suggested that in the NOx reduction on soot most probably physisorbed species were involved. The observed stoichiometries indicated the action of the fast SCR reaction in the presence of NO and the NO 2 SCR reaction in the absence of NO, while the observed gas phase and surface species pointed at reaction steps similar to those on classical SCR catalysts.

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Literature
1.
go back to reference Busca G, Lietti L, Ramis G, Berti F (1998) Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: a review. Appl Catal B 18(1–2):1–36 Busca G, Lietti L, Ramis G, Berti F (1998) Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: a review. Appl Catal B 18(1–2):1–36
2.
go back to reference Kröcher O (2007) Aspects of catalyst development for mobile urea-SCR systems—from vanadia-titania catalysts to metal-exchanged zeolites. Stud Surf Sci Catal 171:261–289CrossRef Kröcher O (2007) Aspects of catalyst development for mobile urea-SCR systems—from vanadia-titania catalysts to metal-exchanged zeolites. Stud Surf Sci Catal 171:261–289CrossRef
3.
go back to reference Andersen H, Green W, Steele D (1961) The catalytic treatment of nitric acid plant tail gas. Ind Eng Chem 53(3):199–204CrossRef Andersen H, Green W, Steele D (1961) The catalytic treatment of nitric acid plant tail gas. Ind Eng Chem 53(3):199–204CrossRef
4.
go back to reference Heck RM (1999) Catalytic abatement of nitrogen oxides-stationary applications. Catal Today 53(4):519–523CrossRef Heck RM (1999) Catalytic abatement of nitrogen oxides-stationary applications. Catal Today 53(4):519–523CrossRef
5.
go back to reference Jüntgen H (1986) Activated carbon as catalyst. Erd Koh Erdg Petr V 39(12):546–551 Jüntgen H (1986) Activated carbon as catalyst. Erd Koh Erdg Petr V 39(12):546–551
6.
go back to reference Jüntgen H, Richter E, Knoblauch K, Hoang-Phu T (1988) Catalytic NOx reduction by ammonia on carbon catalysts. Chem Eng Sci 43(3):419–428CrossRef Jüntgen H, Richter E, Knoblauch K, Hoang-Phu T (1988) Catalytic NOx reduction by ammonia on carbon catalysts. Chem Eng Sci 43(3):419–428CrossRef
7.
go back to reference Jüntgen H, Richter E, Kuhl H (1988) Catalytic activity of carbon catalysts for the reaction of NOx with NH3. Fuel 67(6):775–780CrossRef Jüntgen H, Richter E, Kuhl H (1988) Catalytic activity of carbon catalysts for the reaction of NOx with NH3. Fuel 67(6):775–780CrossRef
8.
go back to reference Knoblauch K, Richter E, Jüntgen H (1981) Application of active coke in processes of SO2- and NOx-removal from flue gases. Fuel 60(9):832–838CrossRef Knoblauch K, Richter E, Jüntgen H (1981) Application of active coke in processes of SO2- and NOx-removal from flue gases. Fuel 60(9):832–838CrossRef
9.
go back to reference Komatsubara Y, Ida S, Fujitsu H, Mochida I (1984) Catalytic activity of PAN-based active carbon fibre (PAN-ACF) activated with sulphuric acid for reduction of nitric oxide with ammonia. Fuel 63(12):1738–1742CrossRef Komatsubara Y, Ida S, Fujitsu H, Mochida I (1984) Catalytic activity of PAN-based active carbon fibre (PAN-ACF) activated with sulphuric acid for reduction of nitric oxide with ammonia. Fuel 63(12):1738–1742CrossRef
10.
go back to reference Kusakabe K, Kashima M, Morooka S, Kato Y (1988) Rate of reduction of nitric oxide with ammonia on coke catalysts activated with sulphuric acid. Fuel 67(5):714–718CrossRef Kusakabe K, Kashima M, Morooka S, Kato Y (1988) Rate of reduction of nitric oxide with ammonia on coke catalysts activated with sulphuric acid. Fuel 67(5):714–718CrossRef
11.
go back to reference Mochida I, Ogaki M, Fujitsu H, Komatsubara Y, Ida S (1983) Catalytic activity of coke activated with sulphuric acid for the reduction of nitric oxide. Fuel 62(7):867–868CrossRef Mochida I, Ogaki M, Fujitsu H, Komatsubara Y, Ida S (1983) Catalytic activity of coke activated with sulphuric acid for the reduction of nitric oxide. Fuel 62(7):867–868CrossRef
12.
go back to reference Mochida I, Ogaki M, Fujitsu H, Komatsubara Y, Ida S (1985) Reduction of nitric oxide with activated PAN fibres. Fuel 64(8):1054–1057CrossRef Mochida I, Ogaki M, Fujitsu H, Komatsubara Y, Ida S (1985) Reduction of nitric oxide with activated PAN fibres. Fuel 64(8):1054–1057CrossRef
13.
go back to reference Richter E, Kleinschmidt R, Pilarczyk E, Knoblauch K, Jüntgen H (1985) Thermal desorption of nitrogen oxides from activated carbon. Thermochim Acta 85:315–318CrossRef Richter E, Kleinschmidt R, Pilarczyk E, Knoblauch K, Jüntgen H (1985) Thermal desorption of nitrogen oxides from activated carbon. Thermochim Acta 85:315–318CrossRef
14.
go back to reference Richter E, Knoblauch K, Jüntgen H (1987) Mechanisms and kinetics of SO2 adsorption and NOx reduction on active coke. Gas Sep Purif 1(1):35–43CrossRef Richter E, Knoblauch K, Jüntgen H (1987) Mechanisms and kinetics of SO2 adsorption and NOx reduction on active coke. Gas Sep Purif 1(1):35–43CrossRef
15.
go back to reference Ahmed SN, Baldwin R, Derbyshire F, McEnaney B, Stencel J (1993) Catalytic reduction of nitric oxide over activated carbons. Fuel 72(3):287–292CrossRef Ahmed SN, Baldwin R, Derbyshire F, McEnaney B, Stencel J (1993) Catalytic reduction of nitric oxide over activated carbons. Fuel 72(3):287–292CrossRef
16.
go back to reference Ku BJ, Lee JK, Park D, Rhee H-K (1994) Treatment of activated carbon to enhance catalytic activity for reduction of nitric oxide with ammonia. Ind Eng Chem Res 33(11):2868–2874CrossRef Ku BJ, Lee JK, Park D, Rhee H-K (1994) Treatment of activated carbon to enhance catalytic activity for reduction of nitric oxide with ammonia. Ind Eng Chem Res 33(11):2868–2874CrossRef
17.
go back to reference Martin-Martinez JM, Singoredjo L, Mittelmeijer-Hazeleger M, Kapteijn F, Moulijn JA (1994) Selective catalytic reduction of NO with NH3 over activated carbons. I: Effect of origin and activation procedure on activity. Carbon 32(5):897–904CrossRef Martin-Martinez JM, Singoredjo L, Mittelmeijer-Hazeleger M, Kapteijn F, Moulijn JA (1994) Selective catalytic reduction of NO with NH3 over activated carbons. I: Effect of origin and activation procedure on activity. Carbon 32(5):897–904CrossRef
18.
go back to reference Szymanski GS, Grzybek T, Papp H (2004) Influence of nitrogen surface functionalities on the catalytic activity of activated carbon in low temperature SCR of NOx with NH3. Catal Today 90(1–2):51–59CrossRef Szymanski GS, Grzybek T, Papp H (2004) Influence of nitrogen surface functionalities on the catalytic activity of activated carbon in low temperature SCR of NOx with NH3. Catal Today 90(1–2):51–59CrossRef
19.
go back to reference Grzybek T, Klinik J, Samojeden B, Suprun V, Papp H (2008) Nitrogen-promoted active carbons as DeNOx catalysts: 1. The influence of modification parameters on the structure and catalytic properties. Catal Today 137(2–4):228–234CrossRef Grzybek T, Klinik J, Samojeden B, Suprun V, Papp H (2008) Nitrogen-promoted active carbons as DeNOx catalysts: 1. The influence of modification parameters on the structure and catalytic properties. Catal Today 137(2–4):228–234CrossRef
20.
go back to reference Muniz J, Marban G, Fuertes AB (1999) Low temperature selective catalytic reduction of NO over polyarylamide-based carbon fibres. Appl Catal B 23(1):25–35CrossRef Muniz J, Marban G, Fuertes AB (1999) Low temperature selective catalytic reduction of NO over polyarylamide-based carbon fibres. Appl Catal B 23(1):25–35CrossRef
21.
go back to reference Shirahama N, Mochida I, Korai Y, Choi KH, Enjoji T, Shimohara T, Yasutake A (2005) Reaction of NO with urea supported on activated carbons. Appl Catal B 57(4):237–245CrossRef Shirahama N, Mochida I, Korai Y, Choi KH, Enjoji T, Shimohara T, Yasutake A (2005) Reaction of NO with urea supported on activated carbons. Appl Catal B 57(4):237–245CrossRef
22.
go back to reference Mehring M (2011) Composition and reactivity analysis of diesel soot with advanced FTIR spectroscopy and a new TG-FTIR system, at the example of the oxidation with O2, NO2 and H2SO4 and the SCR reaction with NOx and NH3. Ph.D thesis No. 19993, Zürich Mehring M (2011) Composition and reactivity analysis of diesel soot with advanced FTIR spectroscopy and a new TG-FTIR system, at the example of the oxidation with O2, NO2 and H2SO4 and the SCR reaction with NOx and NH3. Ph.D thesis No. 19993, Zürich
23.
go back to reference Mehring M, Elsener M, Kröcher O (2012) Selective catalytic reduction of NOx with ammonia over soot. ACS Catal 2(7):1507–1518 Mehring M, Elsener M, Kröcher O (2012) Selective catalytic reduction of NOx with ammonia over soot. ACS Catal 2(7):1507–1518
24.
go back to reference Kuhl H, Baumann H, Juntgen H, Ehrburger P, Dentzer J, Lahaye J (1989) The importance of active surface area on the NO-reduction with ammonia on carbon catalysts. Fuel 68(1):129–130CrossRef Kuhl H, Baumann H, Juntgen H, Ehrburger P, Dentzer J, Lahaye J (1989) The importance of active surface area on the NO-reduction with ammonia on carbon catalysts. Fuel 68(1):129–130CrossRef
25.
go back to reference Zawadzki J, Wisniewski M (2003) In situ characterization of interaction of ammonia with carbon surface in oxygen atmosphere. Carbon 41(12):2257–2267CrossRef Zawadzki J, Wisniewski M (2003) In situ characterization of interaction of ammonia with carbon surface in oxygen atmosphere. Carbon 41(12):2257–2267CrossRef
26.
go back to reference Azambre B, Collura S, Trichard JM, Weber JV (2006) Nature and thermal stability of adsorbed intermediates formed during the reaction of diesel soot with nitrogen dioxide. Appl Surf Sci 253(4):2296–2303CrossRef Azambre B, Collura S, Trichard JM, Weber JV (2006) Nature and thermal stability of adsorbed intermediates formed during the reaction of diesel soot with nitrogen dioxide. Appl Surf Sci 253(4):2296–2303CrossRef
27.
go back to reference Gao X, Liu S, Zhang Y, Luo Z, Ni M, Cen K (2011) Adsorption and reduction of NO2 over activated carbon at low temperature. Fuel Process Technol 92(1):139–146CrossRef Gao X, Liu S, Zhang Y, Luo Z, Ni M, Cen K (2011) Adsorption and reduction of NO2 over activated carbon at low temperature. Fuel Process Technol 92(1):139–146CrossRef
28.
go back to reference Kirchner U, Scheer V, Vogt R (2000) FTIR spectroscopic investigation of the mechanism and kinetics of the heterogeneous reactions of NO2 and HNO3 with soot. J Phys Chem A 104(39):8908–8915CrossRef Kirchner U, Scheer V, Vogt R (2000) FTIR spectroscopic investigation of the mechanism and kinetics of the heterogeneous reactions of NO2 and HNO3 with soot. J Phys Chem A 104(39):8908–8915CrossRef
29.
go back to reference Shirahama N, Moon SH, Choi KH, Enjoji T, Kawano S, Korai Y, Tanoura M, Mochida I (2002) Mechanistic study on adsorption and reduction of NO2 over activated carbon fibers. Carbon 40(14):2605–2611CrossRef Shirahama N, Moon SH, Choi KH, Enjoji T, Kawano S, Korai Y, Tanoura M, Mochida I (2002) Mechanistic study on adsorption and reduction of NO2 over activated carbon fibers. Carbon 40(14):2605–2611CrossRef
30.
go back to reference Akimoto H, Bandow H, Sakamaki F, Inoue G, Hoshino M, Okuda M (1980) Photooxidation of the propylene-NOx-air system studied by long-path Fourier transform infrared spectrometry. Environ Sci Technol 14(2):172–179CrossRef Akimoto H, Bandow H, Sakamaki F, Inoue G, Hoshino M, Okuda M (1980) Photooxidation of the propylene-NOx-air system studied by long-path Fourier transform infrared spectrometry. Environ Sci Technol 14(2):172–179CrossRef
31.
go back to reference Kleffmann J, Becker KH, Wiesen P (1998) Heterogeneous NO2 conversion processes on acid surfaces: possible atmospheric implications. Atmos Environ 32(16):2721–2729CrossRef Kleffmann J, Becker KH, Wiesen P (1998) Heterogeneous NO2 conversion processes on acid surfaces: possible atmospheric implications. Atmos Environ 32(16):2721–2729CrossRef
32.
go back to reference Sakamaki F, Shiro H, Akimoto H (1980) Formation of nitrous acid and nitric oxide in the heterogeneous dark reaction of nitrogen dioxide and water vapor in a smog chamber. Int J Chem Kinet 15:1013–1029CrossRef Sakamaki F, Shiro H, Akimoto H (1980) Formation of nitrous acid and nitric oxide in the heterogeneous dark reaction of nitrogen dioxide and water vapor in a smog chamber. Int J Chem Kinet 15:1013–1029CrossRef
33.
go back to reference Stadler D, Rossi MJ (2000) The reactivity of NO2 and HONO on flame soot at ambient temperature: the influence of combustion conditions. Phys Chem Chem Phys 2(23):5420–5429CrossRef Stadler D, Rossi MJ (2000) The reactivity of NO2 and HONO on flame soot at ambient temperature: the influence of combustion conditions. Phys Chem Chem Phys 2(23):5420–5429CrossRef
34.
go back to reference Otsuka K, Takahashi R, Amakawa K, Yamanaka I (1998) Partial oxidation of light alkanes by NOx in the gas phase. Catal Today 45(1–4):23–28CrossRef Otsuka K, Takahashi R, Amakawa K, Yamanaka I (1998) Partial oxidation of light alkanes by NOx in the gas phase. Catal Today 45(1–4):23–28CrossRef
35.
go back to reference Izquierdo MT, Rubio B, Mayoral C, Andrés JM (2001) Modifications to the surface chemistry of low-rank coal-based carbon catalysts to improve flue gas nitric oxide removal. Appl Catal B 33(4):315–324CrossRef Izquierdo MT, Rubio B, Mayoral C, Andrés JM (2001) Modifications to the surface chemistry of low-rank coal-based carbon catalysts to improve flue gas nitric oxide removal. Appl Catal B 33(4):315–324CrossRef
36.
go back to reference Mochida I, Kawano S (1991) Capture of ammonia by active carbon fibers further activated with sulfuric acid. Ind Eng Chem Res 30(10):2322–2327CrossRef Mochida I, Kawano S (1991) Capture of ammonia by active carbon fibers further activated with sulfuric acid. Ind Eng Chem Res 30(10):2322–2327CrossRef
37.
go back to reference Muckenhuber H, Grothe H (2007) A DRIFTS study of the heterogeneous reaction of NO2 with carbonaceous materials at elevated temperature. Carbon 45(2):321–329CrossRef Muckenhuber H, Grothe H (2007) A DRIFTS study of the heterogeneous reaction of NO2 with carbonaceous materials at elevated temperature. Carbon 45(2):321–329CrossRef
38.
go back to reference Lee JK, Park TJ, Park D, Park S (1993) Catalytic activity of chars prepared by fluidized bed pyrolysis for the reduction of nitric oxide with ammonia. Ind Eng Chem Res 32(9):1882–1887CrossRef Lee JK, Park TJ, Park D, Park S (1993) Catalytic activity of chars prepared by fluidized bed pyrolysis for the reduction of nitric oxide with ammonia. Ind Eng Chem Res 32(9):1882–1887CrossRef
39.
go back to reference Singoredjo L, Kapteijn F, Moulijn JA, Martin-Martinez J-M, Boehm H-P (1993) Modified activated carbons for the selective catalytic reduction of NO with NH3. Carbon 31(1):213–222CrossRef Singoredjo L, Kapteijn F, Moulijn JA, Martin-Martinez J-M, Boehm H-P (1993) Modified activated carbons for the selective catalytic reduction of NO with NH3. Carbon 31(1):213–222CrossRef
40.
go back to reference Ahmed SN, Stencel JM, Derbyshire FJ, Baldwin RM (1993) Activated carbons for the removal of nitric oxide. Fuel Process Technol 34(2):123–136CrossRef Ahmed SN, Stencel JM, Derbyshire FJ, Baldwin RM (1993) Activated carbons for the removal of nitric oxide. Fuel Process Technol 34(2):123–136CrossRef
Metadata
Title
Diesel Soot Catalyzes the Selective Catalytic Reduction of NOx with NH3
Authors
Max Mehring
Martin Elsener
Oliver Kröcher
Publication date
01-05-2013
Publisher
Springer US
Published in
Topics in Catalysis / Issue 1-8/2013
Print ISSN: 1022-5528
Electronic ISSN: 1572-9028
DOI
https://doi.org/10.1007/s11244-013-9993-5

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