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On the interaction of NO{sub 3} radicals with aqueous solutions: Estimation of the Henry coefficient and the mass accomodation coefficient; Zur Wechselwirkung von NO{sub 3}-Radikalen mit waessrigen Loesungen: Bestimmung des Henry- und des Massenakkommodationskoeffizienten

Abstract

The Henry coefficient of NO{sub 3} radicals, K{sub h}(NO{sub 3}), was studied in coiled denuder tubes of 2 mm diameter and variable length, e.g. 4-350 cm. The radicals were produced in a flow system by oxidation of NO with excess O{sub 3} at a temperature of 393 K. A small flow of pure H{sub 2}O was metered to the gas-flow and allowed to form a thin film on the denuder wall. Behind the denuder, gas and liquid were separated and the concentration of the dissolved NO{sub 3} was determined indirectly, after conversion to nitrate by reaction with Cl{sup -}-ions, which were added to the effluent of the denuder. The partial pressure of NO{sub 3} in the gas-phase behind the denuder was determined by quantitative conversion to nitrate in another denuder. The same experimental set-up was used to determine the mass accommodation coefficient of NO{sub 3} to an aqueous surface. There, a high Cl{sup -}-concentration (0.1 M) was used in the stripping solution to efficiently convert the dissolved NO{sub 3} to NO{sub 3-} and thus prevent phase-equilibrium to be reached. The mass accommodation coefficient was derived from the transmittance of the denuder as a function of length. The method requires the  More>>
Publication Date:
Apr 01, 1993
Product Type:
Thesis/Dissertation
Report Number:
Juel-2755
Reference Number:
SCA: 540120; PA: DE-94:0G1540; EDB-94:032340; NTS-94:010123; ERA-19:010307; SN: 94001143082
Resource Relation:
Other Information: DN: Dissertation submitted by K. Thomas; TH: Diss.; PBD: Apr 1993
Subject:
54 ENVIRONMENTAL SCIENCES; NITROGEN OXIDES; CHEMICAL REACTIONS; ATMOSPHERIC CHEMISTRY; BOUNDARY LAYERS; EARTH ATMOSPHERE; RADICALS; OXIDATION; AQUEOUS SOLUTIONS; DIFFUSION; 540120; CHEMICALS MONITORING AND TRANSPORT
OSTI ID:
10122259
Research Organizations:
Forschungszentrum Juelich GmbH (Germany). Inst. fuer Chemie 2 - Chemie der Belasteten Atmosphaere; Wuppertal Univ. (Gesamthochschule) (Germany)
Country of Origin:
Germany
Language:
German
Other Identifying Numbers:
Journal ID: ISSN 0366-0885; Other: ON: DE94739080; TRN: DE94G1540
Availability:
OSTI; NTIS (US Sales Only)
Submitting Site:
DE
Size:
149 p.
Announcement Date:
Jun 30, 2005

Citation Formats

Thomas, K, Volz-Thomas, A, and Kley, D. On the interaction of NO{sub 3} radicals with aqueous solutions: Estimation of the Henry coefficient and the mass accomodation coefficient; Zur Wechselwirkung von NO{sub 3}-Radikalen mit waessrigen Loesungen: Bestimmung des Henry- und des Massenakkommodationskoeffizienten. Germany: N. p., 1993. Web.
Thomas, K, Volz-Thomas, A, & Kley, D. On the interaction of NO{sub 3} radicals with aqueous solutions: Estimation of the Henry coefficient and the mass accomodation coefficient; Zur Wechselwirkung von NO{sub 3}-Radikalen mit waessrigen Loesungen: Bestimmung des Henry- und des Massenakkommodationskoeffizienten. Germany.
Thomas, K, Volz-Thomas, A, and Kley, D. 1993. "On the interaction of NO{sub 3} radicals with aqueous solutions: Estimation of the Henry coefficient and the mass accomodation coefficient; Zur Wechselwirkung von NO{sub 3}-Radikalen mit waessrigen Loesungen: Bestimmung des Henry- und des Massenakkommodationskoeffizienten." Germany.
@misc{etde_10122259,
title = {On the interaction of NO{sub 3} radicals with aqueous solutions: Estimation of the Henry coefficient and the mass accomodation coefficient; Zur Wechselwirkung von NO{sub 3}-Radikalen mit waessrigen Loesungen: Bestimmung des Henry- und des Massenakkommodationskoeffizienten}
author = {Thomas, K, Volz-Thomas, A, and Kley, D}
abstractNote = {The Henry coefficient of NO{sub 3} radicals, K{sub h}(NO{sub 3}), was studied in coiled denuder tubes of 2 mm diameter and variable length, e.g. 4-350 cm. The radicals were produced in a flow system by oxidation of NO with excess O{sub 3} at a temperature of 393 K. A small flow of pure H{sub 2}O was metered to the gas-flow and allowed to form a thin film on the denuder wall. Behind the denuder, gas and liquid were separated and the concentration of the dissolved NO{sub 3} was determined indirectly, after conversion to nitrate by reaction with Cl{sup -}-ions, which were added to the effluent of the denuder. The partial pressure of NO{sub 3} in the gas-phase behind the denuder was determined by quantitative conversion to nitrate in another denuder. The same experimental set-up was used to determine the mass accommodation coefficient of NO{sub 3} to an aqueous surface. There, a high Cl{sup -}-concentration (0.1 M) was used in the stripping solution to efficiently convert the dissolved NO{sub 3} to NO{sub 3-} and thus prevent phase-equilibrium to be reached. The mass accommodation coefficient was derived from the transmittance of the denuder as a function of length. The method requires the knowledge of the diffusion coefficient, which was determined in separate experiments conducted under the same conditions with HNO{sub 3}. The mass accommodation coefficient of NO{sub 3} was found to be {>=}2.5.10{sup -3}. Theoretical considerations and time-dependent box-model calculations show that even under favourable conditions, heterogeneous losses of NO{sub 3} are important for the budget of NO{sub x} only, if NO{sub x}-concentrations are below 0.5 ppb. At higher NO{sub x}-concentrations, the night-time losses proceed predominantly via N{sub 2}O{sub 5}. In the maritime boundary layer, night-time losses of NO{sub 3} radicals can compete with NO{sub x} caused by OH radicals during day-time. (orig./KW)}
place = {Germany}
year = {1993}
month = {Apr}
}