A computer model study of multiphase chemistry in the Arctic boundary layer during polar sunrise

被引:98
作者
Michalowski, BA
Francisco, JS
Li, SM
Barrie, LA
Bottenheim, JW
Shepson, PB [1 ]
机构
[1] Purdue Univ, Dept Earth & Atmospher Sci, W Lafayette, IN 47907 USA
[2] Atmospher Environm Serv, Downsview, ON M3H 5T4, Canada
[3] Purdue Univ, Dept Chem, W Lafayette, IN 47907 USA
关键词
D O I
10.1029/2000JD900004
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
A multiphase chemical box model of Arctic halogen chemistry has been developed using a PC-based modeling program developed by Environment Canada called the Chemical Reactions Modeling System(CREAMS). The multiphase model contains 125 gas phase reactions, 19 photolysis reactions, and 16 aqueous reactions occurring in suspended aerosol particles and the quasi-liquid component of snow. The model simulates mass transfer of species between the gas phase and particles, and between the gas phase and the snowpack. Model simulations were conducted for the Arctic for the period April 16 to April 24 at 245 K within a 400 m boundary layer. The complete model simulates halogen-catalyzed ozone depletion within 5 days from the start of the model run, via known gas and heterogeneous phase activation mechanisms. A critically important model reaction is BrO + HCHO --> HOBr + CHO, which has a substantial impact on gas phase HOBr, and subsequent condensed phase chemistry. When coupled with a necessary snowpack efflux of aldehydes, required to maintain the aldehyde concentrations at observed levels, the new BrO chemistry has a significant impact on the concentrations of gas phase bromine species, particle bromide, and chlorine atoms, through chemistry occurring in the snowpack. We also find that O-3 depletion cannot be simulated without the presence of heterogeneous halogen chemistry occurring in the snowpack and that the rate of O-3 depletion is limited by the mass transfer rate of HOBr to the snowpack.
引用
收藏
页码:15131 / 15145
页数:15
相关论文
共 67 条
[1]   The BrO+Ch3O2 reaction: Kinetics and role in the atmospheric ozone budget [J].
Aranda, A ;
LeBras, G ;
LaVerdet, G ;
Poulet, G .
GEOPHYSICAL RESEARCH LETTERS, 1997, 24 (22) :2745-2748
[2]   Measurements of C2-C7 hydrocarbons during the Polar Sunrise Experiment 1994:: Further evidence for halogen chemistry in the troposphere [J].
Ariya, PA ;
Jobson, BT ;
Sander, R ;
Niki, H ;
Harris, GW ;
Hopper, JF ;
Anlauf, KG .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1998, 103 (D11) :13169-13180
[3]   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
[4]   RATE CONSTANTS FOR THE REACTIONS OF BR ATOMS WITH A SERIES OF ALKANES, ALKENES, AND ALKYNES IN THE PRESENCE OF O-2 [J].
BARNES, I ;
BASTIAN, V ;
BECKER, KH ;
OVERATH, R ;
ZHU, T .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1989, 21 (07) :499-517
[5]   OZONE DESTRUCTION AND PHOTOCHEMICAL-REACTIONS AT POLAR SUNRISE IN THE LOWER ARCTIC ATMOSPHERE [J].
BARRIE, LA ;
BOTTENHEIM, JW ;
SCHNELL, RC ;
CRUTZEN, PJ ;
RASMUSSEN, RA .
NATURE, 1988, 334 (6178) :138-141
[6]   LOWER TROPOSPHERIC MEASUREMENTS OF HALOGENS, NITRATES, AND SULFUR-OXIDES DURING POLAR SUNRISE EXPERIMENT 1992 [J].
BARRIE, LA ;
LI, SM ;
TOOM, DL ;
LANDSBERGER, S ;
STURGES, W .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D12) :25453-25467
[7]   Temperature dependencies of the Henry's Law constant and the aqueous phase dissociation constant of bromine chloride [J].
Bartlett, WP ;
Margerum, DW .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (19) :3410-3414
[8]   Equilibrium and kinetics of bromine hydrolysis [J].
Beckwith, RC ;
Wang, TX ;
Margerum, DW .
INORGANIC CHEMISTRY, 1996, 35 (04) :995-1000
[9]   DEPLETION OF LOWER TROPOSPHERIC OZONE DURING ARCTIC SPRING - THE POLAR SUNRISE EXPERIMENT 1988 [J].
BOTTENHEIM, JW ;
BARRIE, LA ;
ATLAS, E ;
HEIDT, LE ;
NIKI, H ;
RASMUSSEN, RA ;
SHEPSON, PB .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1990, 95 (D11) :18555-18568
[10]   MEASUREMENTS OF NOY SPECIES AND O-3 AT 82-DEGREES-N LATITUDE [J].
BOTTENHEIM, JW ;
GALLANT, AG ;
BRICE, KA .
GEOPHYSICAL RESEARCH LETTERS, 1986, 13 (02) :113-116