Catalytic reduction of NH4NO3 by NO:: Effects of solid acids and implications for low temperature DeNOx processes

被引:84
作者
Savara, Aditya
Li, Mei-Jun
Sachtler, Wolfgang M. H.
Weitz, Eric [1 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
关键词
ammonium nitrate; ammonium nitrite; NO; NO2; DeNO(x);
D O I
10.1016/j.apcatb.2007.12.008
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
Ammonium nitrate is thermally stable below 250 degrees C and could potentially deactivate low temperature NOx reduction catalysts by blocking active sites. It is shown that NO reduces neat NH4NO3 above its 170 degrees C melting point, while acidic solids catalyze this reaction even at temperatures below 100 degrees C. NO2, a product of the reduction, can dimerize and then dissociate in molten NH4NO3 to NO+ NO3-, and may be stabilized within the melt as either an adduct or as HNO2 formed from the hydrolysis of NO+ or N2O4. The other product of reduction, NH4NO2, readily decomposes at <= 100 degrees C to N-2 and H2O, the desired end products of DeNO(x) catalysis. A mechanism for the acid catalyzed reduction of NH4NO3 by NO is proposed, with HNO3 as an intermediate. These findings indicate that the use of acidic catalysts or promoters in DeNO(x) systems could help mitigate catalyst deactivation at low operating temperatures (<150 degrees C). (C) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:251 / 257
页数:7
相关论文
共 58 条
[1]   DINITROGEN TETROXIDE, NITRIC-ACID, AND THEIR MIXTURES AS MEDIA FOR INORGANIC REACTIONS [J].
ADDISON, CC .
CHEMICAL REVIEWS, 1980, 80 (01) :21-39
[2]  
ADHYA SK, 1980, J INDIAN CHEM SOC, V57, P321
[3]  
Austin L.G., 1984, PROCESS ENG SIZE RED
[4]   A structural study of haematite samples prepared from sulfated goethite precursors: the generation of axial mesoporous voids [J].
Baker, ASJ ;
Brown, ASC ;
Edwards, MA ;
Hargreaves, JSJ ;
Kiely, CJ ;
Meagher, A ;
Pankhurst, QA .
JOURNAL OF MATERIALS CHEMISTRY, 2000, 10 (03) :761-766
[5]   EVIDENCE FOR HOMOLYTIC DECOMPOSITION OF AMMONIUM-NITRATE AT HIGH-TEMPERATURE [J].
BROWER, KR ;
OXLEY, JC ;
TEWARI, M .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (10) :4029-4033
[6]   ON MECHANISM OF THERMAL TRANSFORMATIONS IN SOLID AMMONIUM NITRATE [J].
BROWN, RN ;
MCLAREN, AC .
PROCEEDINGS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL AND PHYSICAL SCIENCES, 1962, 266 (1326) :329-&
[7]   Nitrate occlusion studies in Y zeolite and in a clay pillared with aluminium oxide [J].
Carvalho, A ;
Pires, J ;
Veloso, P ;
Machado, M ;
de Carvalho, MB ;
Rocha, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 2003, 58 (02) :163-173
[8]   A "Nitrate Route'' for the low temperature "Fast SCR'' reaction over a V2O5-WO3/TiO2 commercial catalyst [J].
Ciardelli, C ;
Nova, I ;
Tronconi, E ;
Chatterjee, D ;
Bandl-Konrad, B .
CHEMICAL COMMUNICATIONS, 2004, (23) :2718-2719
[9]  
COTTON FA, 1988, ADV INORG CHEM, P322
[10]   Evidence of the existence of three types of species at the quartz-aqueous solution interface at pH 0-10: XPS surface group quantification and surface complexation modeling [J].
Duval, Y ;
Mielczarski, JA ;
Pokrovsky, OS ;
Mielczarski, E ;
Ehrhardt, JJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (11) :2937-2945