Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 48, Issue 1, Pages 429-437Publisher
AMER CHEMICAL SOC
DOI: 10.1021/es403098w
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Funding
- NSF Atmospheric Chemistry [1053658]
- Arctic Natural Sciences [1203526]
- Dynamics of Coupled Natural and Human Systems Programs [1313755]
- MIT's Leading Technology and Policy Initiative
- Directorate For Geosciences
- Office of Polar Programs (OPP) [1203526] Funding Source: National Science Foundation
- Div Atmospheric & Geospace Sciences
- Directorate For Geosciences [1053648] Funding Source: National Science Foundation
- ICER
- Directorate For Geosciences [1313755] Funding Source: National Science Foundation
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We investigate effects of 2000-2050 emissions and climate changes on the atmospheric transport of three polycyclic aromatic hydrocarbons (PAHs): phenanthrene (PHE), pyrene (PYR), and benzo[a]pyrene (BaP). We use the GEOS-Chem model coupled to meteorology from a general circulation model and focus on impacts to northern hemisphere midlatitudes and the Arctic. We project declines -in anthropogenic emissions (up to 20%) and concentrations (up to 37%), with particle-bound PAHs declining more, and greater, declines in midlatitudes versus the Arctic. Climate change causes relatively minor increases in midlatitude concentrations for the more volatile PHE and PYR (up to 4%) and decreases (3%) for particle-bound BaP. In the Arctic, all PAHs decline slightly under future climate (up to 2%). Overall, we observe a small 2050 climate penalty for volatile PAHs and climate benefit for particle-bound PAHs. The degree of penalty or benefit depends on competition between deposition and surface-to-air fluxes of previously deposited PAHs. Particles and temperature have greater impacts on future transport than oxidants, with particle changes alone accounting for 15% of BaP decline under 2050 emissions. Higher temperatures drive increasing surface-to-air fluxes that cause PHE and PYR climate penalties. Simulations suggest ratios of more-to-less volatile species can be used to diagnose signals of climate versus emissions and that these signals are best observed in the Arctic.
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