Active chlorine in the remote marine boundary layer:: Modeling anomalous measurements of δ13C in methane

被引:31
作者
Allan, W [1 ]
Lowe, DC [1 ]
Cainey, JM [1 ]
机构
[1] Natl Inst Water & Atmospher Res, Wellington 6003, New Zealand
关键词
D O I
10.1029/2001GL013064
中图分类号
P [天文学、地球科学];
学科分类号
07 ;
摘要
Measurements of delta C-13 in methane in the marine boundary layer (MBL) of the extratropical Southern Hemisphere imply a kinetic isotope fractionation much larger than would be expected if the hydroxyl radical were the only tropospheric methane sink. We use a simple chemical box model to show that the assumption of a MBL active chlorine (Cl-.) sink can explain these anomalous observations provided there is a seasonal cycle in the Cl-. sink with a summer-winter concentration difference similar to 6 . 10(3) cm(-3). The required summer maximum and yearly mean Cl-. concentrations are plausible, and imply a global Cl-. sink strength for methane of < 5 Tg yr(-1). Choice of a Cl-. sink seasonal cycle linked to the nonsinusoidal dimethyl sulfide seasonal cycle gives the observed fractionation with a smaller yearly mean Cl-. concentration than equivalent sinusoidal Cl-. cycles.
引用
收藏
页码:3239 / 3242
页数:4
相关论文
共 23 条
[1]   Modeling the variation of δ13C in atmospheric methane:: Phase ellipses and the kinetic isotope effect [J].
Allan, W ;
Manning, MR ;
Lassey, KR ;
Lowe, DC ;
Gomez, AJ .
GLOBAL BIOGEOCHEMICAL CYCLES, 2001, 15 (02) :467-481
[2]   Chloride and bromide loss from sea-salt particles in southern ocean air [J].
Ayers, GP ;
Gillett, RW ;
Cainey, JM ;
Dick, AL .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 1999, 33 (03) :299-319
[3]   CARBON KINETIC ISOTOPE EFFECT IN THE OXIDATION OF METHANE BY THE HYDROXYL RADICAL [J].
CANTRELL, CA ;
SHETTER, RE ;
MCDANIEL, AH ;
CALVERT, JG ;
DAVIDSON, JA ;
LOWE, DC ;
TYLER, SC ;
CICERONE, RJ ;
GREENBERG, JP .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1990, 95 (D13) :22455-22462
[5]  
CURTIS PJ, 1988, AERER128085 HARW LAB
[6]  
DEMORE WB, 1997, PUBL JET PROPULSION
[7]   CHLORINE ATOMS AS A POTENTIAL TROPOSPHERIC OXIDANT IN THE MARINE BOUNDARY-LAYER [J].
FINLAYSONPITTS, BJ .
RESEARCH ON CHEMICAL INTERMEDIATES, 1993, 19 (03) :235-249
[8]  
GILLETT RW, 1993, DIMETHYLSULFIDE: OCEANS, ATMOSPHERE AND CLIMATE, P117
[9]   Modeling atmospheric delta(CH4)-C-13 and the causes of recent changes in atmospheric CH4 amounts [J].
Gupta, M ;
Tyler, S ;
Cicerone, R .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1996, 101 (D17) :22923-22932
[10]   Climatic context of the First Aerosol Characterization Experiment (ACE 1): A meteorological and chemical overview [J].
Hainsworth, AHW ;
Dick, AL ;
Gras, JL .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1998, 103 (D13) :16319-16340