THE REACTION OF AMMONIA WITH NITROGEN-DIOXIDE IN A FLOW REACTOR - IMPLICATIONS FOR THE NH2+NO2 REACTION

被引:102
作者
GLARBORG, P [1 ]
DAMJOHANSEN, K [1 ]
MILLER, JA [1 ]
机构
[1] SANDIA NATL LABS,COMBUST RES FACIL,LIVERMORE,CA 94551
关键词
D O I
10.1002/kin.550271207
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 NH3/NO2 system has been investigated experimentally in an isothermal flow reactor in the temperature range 850-1350 X. The experimental data were interpreted in terms of a detailed reaction mechanism. The flow reactor results, supported by a theoretical analysis of the NH2-NO2 complex, suggest that the NH2 + NO2 reaction has two major product channels, both proceeding without activation barriers: (R20) NH2 reversible arrow N2O + H2O (R20) NH2 reversible arrow H2NO + NO Our findings indicate that the N2O + H2O channel is dominant at low temperatures while H2NO + NO dominates at high temperatures. The rate constant for reaction (R21) is estimated to be 3.5 . 10(12) cm(3)/mol-s in the temperature range studied with an uncertainty of a factor of 3. (C) 1995 John Wiley & Sons, Inc.
引用
收藏
页码:1207 / 1220
页数:14
相关论文
共 31 条
[1]   EVALUATED KINETIC AND PHOTOCHEMICAL DATA FOR ATMOSPHERIC CHEMISTRY .3. IUPAC SUBCOMMITTEE ON GAS KINETIC DATA EVALUATION FOR ATMOSPHERIC CHEMISTRY [J].
ATKINSON, R ;
BAULCH, DL ;
COX, RA ;
HAMPSON, RF ;
KERR, JA ;
TROE, J .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1989, 18 (02) :881-1097
[2]   EVALUATED KINETIC AND PHOTOCHEMICAL DATA FOR ATMOSPHERIC CHEMISTRY SUPPLEMENT-IV - IUPAC SUBCOMMITTEE ON GAS KINETIC DATA EVALUATION FOR ATMOSPHERIC CHEMISTRY [J].
ATKINSON, R ;
BAULCH, DL ;
COX, RA ;
HAMPSON, RF ;
KERR, JA ;
TROE, J .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1992, 21 (06) :1125-1568
[3]   EVALUATED KINETIC DATA FOR COMBUSTION MODELING [J].
BAULCH, DL ;
COBOS, CJ ;
COX, RA ;
ESSER, C ;
FRANK, P ;
JUST, T ;
KERR, JA ;
PILLING, MJ ;
TROE, J ;
WALKER, RW ;
WARNATZ, J .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1992, 21 (03) :411-734
[4]   REACTION BETWEEN AMMONIA AND NITROGEN-DIOXIDE [J].
BEDFORD, G ;
THOMAS, JH .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1972, 68 (11) :2163-&
[5]   ON THE REACTION OF THE NH2 RADICAL WITH NO2 AT 295-620-K [J].
BULATOV, VP ;
IOFFE, AA ;
LOZOVSKY, VA ;
SARKISOV, OM .
CHEMICAL PHYSICS LETTERS, 1989, 159 (2-3) :171-174
[6]   KINETICS OF THE GAS-PHASE REACTION BETWEEN NITRIC-OXIDE, AMMONIA AND OXYGEN [J].
DUO, W ;
DAMJOHANSEN, K ;
OSTERGAARD, K .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1992, 70 (05) :1014-1020
[7]  
DUO W, 1990, 23RD S INT COMB PITT, P297
[8]   MODELING THE THERMAL DENOX PROCESS IN FLOW REACTORS - SURFACE EFFECTS AND NITROUS-OXIDE FORMATION [J].
GLARBORG, P ;
DAMJOHANSEN, K ;
MILLER, JA ;
KEE, RJ ;
COLTRIN, ME .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1994, 26 (04) :421-436
[9]   KINETICS OF HOMOGENEOUS NITROUS-OXIDE DECOMPOSITION [J].
GLARBORG, P ;
JOHNSSON, JE ;
DAMJOHANSEN, K .
COMBUSTION AND FLAME, 1994, 99 (3-4) :523-532
[10]  
HACK W, 1979, 17TH S INT COMB PITT, P505