Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide
Artikel i vetenskaplig tidskrift, 2013

Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (https://halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1 degrees x 1 degrees grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr(-1) for CHBr3, 0.78/0.98 Gmol Br yr(-1) for CH2Br2 and 1.24/1.45 Gmol Br yr(-1) for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

HALOGENATED ORGANIC-COMPOUNDS

MARINE BOUNDARY-LAYER

WIND-SPEED

ATLANTIC-OCEAN

TROPICAL TROPOPAUSE LAYER

PHYTOPLANKTON CULTURES

GAS-EXCHANGE

OZONE DEPLETION

STRATOSPHERIC BROMINE

PHOTOCHEMICAL PRODUCTION

Författare

F. Ziska

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

B. Quack

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

Katarina Abrahamsson

Chalmers, Kemi- och bioteknik, Analytisk kemi

S. D. Archer

Bigelow Laboratory of Ocean Sciences

Plymouth Marine Laboratory

E. Atlas

Rosenstiel School of Marine and Atmospheric Science

T. A. Bell

UC Irvine

J. H. Butler

National Oceanic and Atmospheric Administration

L. J. Carpenter

University of York

C. E. Jones

Kyoto University

University of York

N. R. P. Harris

University of Cambridge

H. Hepach

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

K. G. Heumann

Johannes Gutenberg-Universität Mainz

C. Hughes

Centre for Ocean and Atmospheric Sciences

J. Kuss

Institut fur Ostseeforschung Warnemunde

K. Krüger

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

P. Liss

Centre for Ocean and Atmospheric Sciences

R. M. Moore

Dalhousie University

A. Orlikowska

Institut fur Ostseeforschung Warnemunde

S Raimund

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

Adaptation et Diversite en Milieu Marin

C.E. Reeves

Centre for Ocean and Atmospheric Sciences

W. Reifenhäuser

Bayerisches Landesamt F̈ur Umwelt

A. D. Robinson

University of Cambridge

C. Schall

Fresenius Medical Care AG & Co. KGaA

T. Tanhua

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

S. Tegtmeier

GEOMAR - Helmholtz Zentrum für Ozeanforschung Kiel

S. Turner

Centre for Ocean and Atmospheric Sciences

L. Wang

Rutgers, The State University of New Jersey

D. Wallace

Dalhousie University

J. Williams

Max Planck-institutet

H. Yamamoto

National Institute for Environmental Studies of Japan

Marine Works Japan Ltd.

S. Yvon-Lewis

Texas A&M University

Y. Yokouchi

National Institute for Environmental Studies of Japan

Atmospheric Chemistry and Physics

1680-7316 (ISSN) 1680-7324 (eISSN)

Vol. 13 17 8915-8934

Ämneskategorier

Meteorologi och atmosfärforskning

DOI

10.5194/acp-13-8915-2013