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The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon.

ABSTRACT: The Earth's atmosphere contains a multitude of emitted (primary) and chemically formed (secondary) gases and particles that degrade air quality and modulate the climate. Reactive organic carbon (ROC) species are the fuel of the chemistry of the atmosphere, dominating short-lived emissions, reactivity, and the secondary production of key species such as ozone, particulate matter, and carbon dioxide. Despite the central importance of ROC, the diversity and complexity of this class of species has been a longstanding obstacle to developing a comprehensive understanding of how the composition of our atmosphere, and the associated environmental implications, will evolve. Here, we characterize the role of ROC in atmospheric chemistry and the challenges inherent in measuring and modeling ROC, and highlight recent progress toward achieving mass closure for the complete description of atmospheric ROC.

SUBMITTER: Heald CL

PROVIDER: S-EPMC7002119 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon.

Heald C L CL Kroll J H JH

Science advances 20200205 6

The Earth's atmosphere contains a multitude of emitted (primary) and chemically formed (secondary) gases and particles that degrade air quality and modulate the climate. Reactive organic carbon (ROC) species are the fuel of the chemistry of the atmosphere, dominating short-lived emissions, reactivity, and the secondary production of key species such as ozone, particulate matter, and carbon dioxide. Despite the central importance of ROC, the diversity and complexity of this class of species has b ...[more]

PMID: 32076652

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Project description:Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon (ROC) emissions. Among these sources are everyday items, such as personal care products, general cleaners, architectural coatings, pesticides, adhesives, and printing inks. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States, including spatial allocation to regional and local scales. Evaporation of a species from a VCP mixture in the VCPy framework is a function of the compound-specific physiochemical properties that govern volatilization and the timescale relevant for product evaporation. We introduce two terms to describe these processes: evaporation timescale and use timescale. Using this framework, predicted national per capita organic emissions from VCPs are 9.5 kg per person per year (6.4 kg C per person per year) for 2016, which translates to 3.05 Tg (2.06 Tg C), making VCPs a dominant source of anthropogenic organic emissions in the United States. Uncertainty associated with this framework and sensitivity to select parameters were characterized through Monte Carlo analysis, resulting in a 95 % confidence interval of national VCP emissions for 2016 of 2.61-3.53 Tg (1.76-2.38 Tg C). This nationwide total is broadly consistent with the U.S. EPA's 2017 National Emission Inventory (NEI); however, county-level and categorical estimates can differ substantially from NEI values. VCPy predicts higher VCP emissions than the NEI for approximately half of all counties, with 5 % of all counties having greater than 55 % higher emissions. Categorically, application of the VCPy framework yields higher emissions for personal care products (150 %) and paints and coatings (25 %) when compared to the NEI, whereas pesticides (-54 %) and printing inks (-13 %) feature lower emissions. An observational evaluation indicates emissions of key species from VCPs are reproduced with high fidelity using the VCPy framework (normalized mean bias of -13 % with r =0.95). Sector-wide, the effective secondary organic aerosol yield and maximum incremental reactivity of VCPs are 5.3 % by mass and 1.58 gO3 g-1, respectively, indicating VCPs are an important, and likely to date underrepresented, source of secondary pollution in urban environments.

Dataset Information

The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon.

Publications

The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon.

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