Reactive organic carbon emissions from volatile chemical products

Abstract

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 kgC per person per year) for 2016, which translates to 3.05 Tg (2.06 TgC), 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 TgC). This nationwide total is broadly consistent with the U.S. EPA's 2017 National Emission Inventory (NEI); however, countylevel 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 D0.95). Sector-wide, the effective secondary organic aerosol yield and maximum incremental reactivity of VCPs are 5.3% by mass and 1.58 gO3g..1, respectively, indicating VCPs are an important, and likely to date underrepresented, source of secondary pollution in urban environments.