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Title: Global distribution and surface activity of macromolecules in offline simulations of marine organic chemistry

Abstract

Organic macromolecules constitute a high percentage of remote sea spray. They enter the atmosphere through adsorption onto bubbles followed by bursting at the ocean surface, and go on to influence the chemistry of the fine mode aerosol. We present a global estimate of mixed-layer macromolecular distributions, driven by offline marine systems model output. The approach permits estimation of oceanic concentrations and bubble film surface coverages for several classes of organic compound. Mixed layer levels are computed from the output of a global ocean ecodynamics model by relating the macromolecules to standard biogeochemical tracers. Steady state is assumed for labile forms, and for longer-lived components we rely on ratios to existing transported variables. Adsorption is then represented through conventional Langmuir isotherms, with equilibria deduced from laboratory analogs. Open water concentrations locally exceed one micromolar carbon for the total of proteins, polysaccharides and refractory heteropolycondensates. The shorter-lived lipids remain confined to regions of strong biological activity. Results are evaluated against available measurements for all compound types, and agreement is generally well within an order of magnitude. Global distributions are further estimated for both fractional coverage of bubble films at the air-water interface and the two-dimensional concentration excess. Altogether, we show that macromolecularmore » mapping provides a novel tool for the comprehension of oceanic surfactant patterns. These results may prove useful in planning field experiments and assessing the potential response of surface chemical behaviors to global change.« less

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1503048
Alternate Identifier(s):
OSTI ID: 1229982; OSTI ID: 1327640
Report Number(s):
PNNL-SA-106391
Journal ID: ISSN 0168-2563; PII: 136
Grant/Contract Number:  
ACES4BGC; AC05-76RL01830; AC05-00OR22725
Resource Type:
Published Article
Journal Name:
Biogeochemistry
Additional Journal Information:
Journal Name: Biogeochemistry Journal Volume: 126 Journal Issue: 1-2; Journal ID: ISSN 0168-2563
Publisher:
Springer Science + Business Media
Country of Publication:
Netherlands
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; organic macromolecules; mixed layer distributions; Langmuir adsorption; fractional coverage; bubble films; air-water interface; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Ogunro, Oluwaseun O., Burrows, Susannah M., Elliott, Scott, Frossard, Amanda A., Hoffman, Forrest, Letscher, Robert T., Moore, J. Keith, Russell, Lynn M., Wang, Shanlin, and Wingenter, Oliver W. Global distribution and surface activity of macromolecules in offline simulations of marine organic chemistry. Netherlands: N. p., 2015. Web. doi:10.1007/s10533-015-0136-x.
Ogunro, Oluwaseun O., Burrows, Susannah M., Elliott, Scott, Frossard, Amanda A., Hoffman, Forrest, Letscher, Robert T., Moore, J. Keith, Russell, Lynn M., Wang, Shanlin, & Wingenter, Oliver W. Global distribution and surface activity of macromolecules in offline simulations of marine organic chemistry. Netherlands. https://doi.org/10.1007/s10533-015-0136-x
Ogunro, Oluwaseun O., Burrows, Susannah M., Elliott, Scott, Frossard, Amanda A., Hoffman, Forrest, Letscher, Robert T., Moore, J. Keith, Russell, Lynn M., Wang, Shanlin, and Wingenter, Oliver W. Tue . "Global distribution and surface activity of macromolecules in offline simulations of marine organic chemistry". Netherlands. https://doi.org/10.1007/s10533-015-0136-x.
@article{osti_1503048,
title = {Global distribution and surface activity of macromolecules in offline simulations of marine organic chemistry},
author = {Ogunro, Oluwaseun O. and Burrows, Susannah M. and Elliott, Scott and Frossard, Amanda A. and Hoffman, Forrest and Letscher, Robert T. and Moore, J. Keith and Russell, Lynn M. and Wang, Shanlin and Wingenter, Oliver W.},
abstractNote = {Organic macromolecules constitute a high percentage of remote sea spray. They enter the atmosphere through adsorption onto bubbles followed by bursting at the ocean surface, and go on to influence the chemistry of the fine mode aerosol. We present a global estimate of mixed-layer macromolecular distributions, driven by offline marine systems model output. The approach permits estimation of oceanic concentrations and bubble film surface coverages for several classes of organic compound. Mixed layer levels are computed from the output of a global ocean ecodynamics model by relating the macromolecules to standard biogeochemical tracers. Steady state is assumed for labile forms, and for longer-lived components we rely on ratios to existing transported variables. Adsorption is then represented through conventional Langmuir isotherms, with equilibria deduced from laboratory analogs. Open water concentrations locally exceed one micromolar carbon for the total of proteins, polysaccharides and refractory heteropolycondensates. The shorter-lived lipids remain confined to regions of strong biological activity. Results are evaluated against available measurements for all compound types, and agreement is generally well within an order of magnitude. Global distributions are further estimated for both fractional coverage of bubble films at the air-water interface and the two-dimensional concentration excess. Altogether, we show that macromolecular mapping provides a novel tool for the comprehension of oceanic surfactant patterns. These results may prove useful in planning field experiments and assessing the potential response of surface chemical behaviors to global change.},
doi = {10.1007/s10533-015-0136-x},
journal = {Biogeochemistry},
number = 1-2,
volume = 126,
place = {Netherlands},
year = {Tue Oct 13 00:00:00 EDT 2015},
month = {Tue Oct 13 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1007/s10533-015-0136-x

Citation Metrics:
Cited by: 13 works
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