Investigations of emissions and heterogeneous formation of HONO in a road traffic tunnel
Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO 2) using a differential optical absorption spectroscopy system, nitrogen oxide (NO) by an in situ chemiluminescence analyser and carbon dioxide (CO 2) by a gas chromatographic technique were carried out in the Wuppertal Kiesbe...
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Published in | Atmospheric environment (1994) Vol. 35; no. 20; pp. 3385 - 3394 |
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Main Authors | , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Oxford
Elsevier Ltd
01.07.2001
Elsevier Science |
Subjects | |
Online Access | Get full text |
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Abstract | Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO
2) using a differential optical absorption spectroscopy system, nitrogen oxide (NO) by an in situ chemiluminescence analyser and carbon dioxide (CO
2) by a gas chromatographic technique were carried out in the Wuppertal Kiesbergtunnel. At high traffic density HONO concentrations of up to 45
ppbV were observed. However, at low traffic density unexpectedly high HONO concentrations of up to 10
ppbV were measured caused by heterogeneous HONO formation on the tunnel walls. In addition to the tunnel campaigns, emission measurements of HONO, NO
2, NO and CO
2 from different single vehicles (a truck, a diesel and a gasoline passenger car) were also performed. For the correction of the HONO emission data, the heterogeneous HONO formation on the tunnel walls was quantified by two different approaches (a) in different NO
2 emission experiments in the tunnel without traffic and (b) on tunnel wall residue in the laboratory. The HONO concentration corrected for heterogeneous formation on the tunnel walls, in relation to the CO
2 concentration can be used to estimate the amount of HONO, which is directly emitted from the vehicle fleet. From the measured data, emission ratios (e.g. HONO/NO
x
) and emission indices (e.g. mg HONO
kg
−1 fuel) were calculated. The calculated emission index of 88±18
mg HONO
kg
−1 fuel allows an estimation of the HONO emission rates from traffic into the atmosphere. Furthermore, the heterogeneous formation of HONO from NO
2 on freshly emitted exhaust particles is discussed. |
---|---|
AbstractList | Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO sub(2)) using a differential optical absorption spectroscopy system, nitrogen oxide (NO) by an in situ chemiluminescence analyser and carbon dioxide (CO sub(2)) by a gas chromatographic technique were carried out in the Wuppertal Kiesbergtunnel. At high traffic density HONO concentrations of up to 45ppbV were observed. However, at low traffic density unexpectedly high HONO concentrations of up to 10ppbV were measured caused by heterogeneous HONO formation on the tunnel walls. In addition to the tunnel campaigns, emission measurements of HONO, NO sub(2), NO and CO sub(2) from different single vehicles (a truck, a diesel and a gasoline passenger car) were also performed. For the correction of the HONO emission data, the heterogeneous HONO formation on the tunnel walls was quantified by two different approaches (a) in different NO sub(2) emission experiments in the tunnel without traffic and (b) on tunnel wall residue in the laboratory. The HONO concentration corrected for heterogeneous formation on the tunnel walls, in relation to the CO sub(2) concentration can be used to estimate the amount of HONO, which is directly emitted from the vehicle fleet. From the measured data, emission ratios (e.g. HONO/NO sub(x)) and emission indices (e.g. mg HONO kg super(-1) fuel) were calculated. The calculated emission index of 88 plus or minus 18 mg HONO kg super(-1) fuel allows an estimation of the HONO emission rates from traffic into the atmosphere. Furthermore, the heterogeneous formation of HONO from NO sub(2) on freshly emitted exhaust particles is discussed. In a road tunnel in Wuppertal, Germany, nitrous acid (HONO) emissions from the traffic fleet and from single vehicles were measured. In addition, HONO formation was studied in the laboratory using sampled tunnel-wall residue. During the day, a good correlation was found between HONO, nitric oxide, nitrogen dioxide, and traffic density, but at low traffic density, high HONO mixing ratios were recorded. In the single-vehicle experiments, the difference in the lifetimes of HONO and NO sub(2) increased with increasing maximum NO sub(2) concentration, which was attributed to the heterogeneous formation of HONO from NO sub(2) and water on the tunnel walls. This phenomenon was confirmed in the laboratory. The HONO/nitrogen oxides ratio of 8 10 super(-3) and the HONO emission index of 88 mg/kg fuel, which were calculated from the traffic-fleet data, were in good agreement with values from the single-vehicle experiments. Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO 2) using a differential optical absorption spectroscopy system, nitrogen oxide (NO) by an in situ chemiluminescence analyser and carbon dioxide (CO 2) by a gas chromatographic technique were carried out in the Wuppertal Kiesbergtunnel. At high traffic density HONO concentrations of up to 45 ppbV were observed. However, at low traffic density unexpectedly high HONO concentrations of up to 10 ppbV were measured caused by heterogeneous HONO formation on the tunnel walls. In addition to the tunnel campaigns, emission measurements of HONO, NO 2, NO and CO 2 from different single vehicles (a truck, a diesel and a gasoline passenger car) were also performed. For the correction of the HONO emission data, the heterogeneous HONO formation on the tunnel walls was quantified by two different approaches (a) in different NO 2 emission experiments in the tunnel without traffic and (b) on tunnel wall residue in the laboratory. The HONO concentration corrected for heterogeneous formation on the tunnel walls, in relation to the CO 2 concentration can be used to estimate the amount of HONO, which is directly emitted from the vehicle fleet. From the measured data, emission ratios (e.g. HONO/NO x ) and emission indices (e.g. mg HONO kg −1 fuel) were calculated. The calculated emission index of 88±18 mg HONO kg −1 fuel allows an estimation of the HONO emission rates from traffic into the atmosphere. Furthermore, the heterogeneous formation of HONO from NO 2 on freshly emitted exhaust particles is discussed. |
Author | Gomes, J.A.G. Spittler, M. Becker, K.H. Platt, U. Kleffmann, J. Lörzer, J.C. Wiesen, P. Kurtenbach, R. Geyer, A. Ackermann, R. |
Author_xml | – sequence: 1 givenname: R. surname: Kurtenbach fullname: Kurtenbach, R. email: kurtenbach@physchem.uni-wuppertal.de organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 2 givenname: K.H. surname: Becker fullname: Becker, K.H. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 3 givenname: J.A.G. surname: Gomes fullname: Gomes, J.A.G. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 4 givenname: J. surname: Kleffmann fullname: Kleffmann, J. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 5 givenname: J.C. surname: Lörzer fullname: Lörzer, J.C. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 6 givenname: M. surname: Spittler fullname: Spittler, M. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 7 givenname: P. surname: Wiesen fullname: Wiesen, P. organization: Bergische Universität-GH Wuppertal, Physikalische Chemie/FB 9, Gaußstr. 20, D-42097 Wuppertal, Germany – sequence: 8 givenname: R. surname: Ackermann fullname: Ackermann, R. organization: Universität Heidelberg, Institut für Umweltphysik, INF 229, D-69120 Heidelberg, Germany – sequence: 9 givenname: A. surname: Geyer fullname: Geyer, A. organization: Universität Heidelberg, Institut für Umweltphysik, INF 229, D-69120 Heidelberg, Germany – sequence: 10 givenname: U. surname: Platt fullname: Platt, U. organization: Universität Heidelberg, Institut für Umweltphysik, INF 229, D-69120 Heidelberg, Germany |
BackLink | http://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=14100348$$DView record in Pascal Francis |
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Keywords | Heterogeneous reactions Emission indices Emission ratios Road traffic tunnel Nitrous acid Road traffic emissions Pollutant formation Emission content Motor vehicle Diurnal variation Pollutant emission Time variation Road tunnel Air pollution Road traffic Mixing ratio Formation mechanism Heterogeneous reaction |
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Sources and formation pathways contributor: fullname: Kessler – volume: 20 start-page: 463 issue: 3–5 year: 1994 ident: 10.1016/S1352-2310(01)00138-8_BIB4 article-title: An evaluation of the mechanism of nitrous acid formation in the urban atmosphere publication-title: Research on Chemical Intermediates doi: 10.1163/156856794X00423 contributor: fullname: Calvert – volume: 1 start-page: 5443 year: 1999 ident: 10.1016/S1352-2310(01)00138-8_BIB12 article-title: Heterogeneous conversion of NO2 on carbonaceous surfaces publication-title: Physical Chemistry Chemical Physics doi: 10.1039/a905545b contributor: fullname: Kleffmann – ident: 10.1016/S1352-2310(01)00138-8_BIB1 – volume: 32 start-page: 2721 year: 1998 ident: 10.1016/S1352-2310(01)00138-8_BIB13 article-title: Heterogeneous NO2 conversion processes on acid surfaces publication-title: Atmospheric Environment doi: 10.1016/S1352-2310(98)00065-X contributor: fullname: Kleffmann – volume: 395 start-page: 157 year: 1998 ident: 10.1016/S1352-2310(01)00138-8_BIB2 article-title: Heterogeneous production of nitrous acid on soot in polluted air masses publication-title: Nature doi: 10.1038/25965 contributor: fullname: Ammann – volume: 101 start-page: 14429 year: 1996 ident: 10.1016/S1352-2310(01)00138-8_BIB6 article-title: Tropospheric cycle of nitrous acid publication-title: Journal of Geophysical Research doi: 10.1029/96JD00341 contributor: fullname: Harrison – volume: 30 start-page: 3017 year: 1996 ident: 10.1016/S1352-2310(01)00138-8_BIB18 article-title: Measurements of concentration gradients of HNO2 and HNO3 over a semi-natural ecosystem publication-title: Atmospheric Environment doi: 10.1016/1352-2310(96)00011-8 contributor: fullname: Neftel – ident: 10.1016/S1352-2310(01)00138-8_BIB7 – volume: 30 start-page: 2843 year: 1996 ident: 10.1016/S1352-2310(01)00138-8_BIB11 article-title: Measurement of nitrous acid in motor vehicle exhaust publication-title: Environmental Science and Technology doi: 10.1021/es960135y contributor: fullname: Kirchstetter – ident: 10.1016/S1352-2310(01)00138-8_BIB15 doi: 10.1007/978-94-009-0567-2_70 – volume: 99 start-page: 25469 year: 1994 ident: 10.1016/S1352-2310(01)00138-8_BIB16 article-title: Equilibrium of particle nitrite with gas phase HONO publication-title: Journal of Geophysical Research doi: 10.1029/94JD00620 contributor: fullname: Li – volume: 18 start-page: 847 year: 1984 ident: 10.1016/S1352-2310(01)00138-8_BIB20 article-title: Spectroscopic identification and measurement of gaseous nitrous acid in dilute auto exhaust publication-title: Atmospheric Environment doi: 10.1016/0004-6981(84)90270-1 contributor: fullname: Pitts – volume: 6 start-page: 917 year: 1979 ident: 10.1016/S1352-2310(01)00138-8_BIB19 article-title: Detection of nitrous acid in the atmosphere by differential optical absorption publication-title: Geophysical Research Letters doi: 10.1029/GL006i012p00917 contributor: fullname: Perner – ident: 10.1016/S1352-2310(01)00138-8_BIB9 – ident: 10.1016/S1352-2310(01)00138-8_BIB21 – volume: 104 start-page: 13833 year: 1999 ident: 10.1016/S1352-2310(01)00138-8_BIB17 article-title: Reactive uptake on hydrocarbon soot publication-title: Journal of Geophysical Research doi: 10.1029/1999JD900145 contributor: fullname: Longfellow – volume: 21 start-page: 1529 year: 1987 ident: 10.1016/S1352-2310(01)00138-8_BIB24 article-title: Kinetics of the reaction between nitrogen dioxide and water vapour publication-title: Atmospheric Environment doi: 10.1016/0004-6981(87)90315-5 contributor: fullname: Svensson – volume: 33 start-page: 4134 year: 1999 ident: 10.1016/S1352-2310(01)00138-8_BIB3 article-title: Nitrous oxide (N2O) emissions from vehicles publication-title: Environmental Science and Technology doi: 10.1021/es9903330 contributor: fullname: Becker – volume: 104 start-page: 13825 year: 1999 ident: 10.1016/S1352-2310(01)00138-8_BIB8 article-title: Heterogeneous formation of nitrous acid (HONO) on soot aerosol particles publication-title: Journal of Geophysical Research doi: 10.1029/1999JD900141 contributor: fullname: Kalberer – volume: 25 start-page: 2453 year: 1998 ident: 10.1016/S1352-2310(01)00138-8_BIB5 article-title: The chemical kinetics of HONO formation resulting from heterogeneous interaction of NO2 with flame soot publication-title: Geophysical Research Letters doi: 10.1029/98GL01796 contributor: fullname: Gerecke – volume: 105 start-page: 14585 year: 2000 ident: 10.1016/S1352-2310(01)00138-8_BIB23 article-title: UV-visible absorption cross section of nitrous acid publication-title: Journal of Geophysical Research doi: 10.1029/2000JD900003 contributor: fullname: Stutz – volume: 20 start-page: 409 year: 1986 ident: 10.1016/S1352-2310(01)00138-8_BIB22 article-title: Measurements of nitrous acid in an urban area (Authors’reply) publication-title: Atmospheric Environment doi: 10.1016/0004-6981(86)90048-X contributor: fullname: Sjödin |
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Snippet | Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO
2) using a differential optical absorption spectroscopy system, nitrogen oxide (NO)... In a road tunnel in Wuppertal, Germany, nitrous acid (HONO) emissions from the traffic fleet and from single vehicles were measured. In addition, HONO... Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO sub(2)) using a differential optical absorption spectroscopy system, nitrogen oxide... |
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SubjectTerms | Applied sciences Atmospheric pollution Emission indices Emission ratios Exact sciences and technology Germany, Wuppertal Heterogeneous reactions Nitrous acid Pollution Pollution sources. Measurement results Road traffic emissions Road traffic tunnel Transports |
Title | Investigations of emissions and heterogeneous formation of HONO in a road traffic tunnel |
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