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Abstract Mercury (Hg) is a naturally occurring element that bonds with organic matter and, when converted to methylmercury, is a potent neurotoxicant. Here we estimate potential future releases of Hg from thawing permafrost for low and high greenhouse gas emissions scenarios using a mechanistic model. By 2200, the high emissions scenario shows annual permafrost Hg emissions to the atmosphere comparable to current global anthropogenic emissions. By 2100, simulated Hg concentrations in the Yukon River increase by 14% for the low emissions scenario, but double for the high emissions scenario. Fish Hg concentrations do not exceed United States Environmental Protection Agency guidelines for the low emissions scenario by 2300, but for the high emissions scenario, fish in the Yukon River exceed EPA guidelines by 2050. Our results indicate minimal impacts to Hg concentrations in water and fish for the low emissions scenario and high impacts for the high emissions scenario. 

Abstract. Here we present measurement results of temporal distributions of nitrous acid (HONO) along with several chemical and meteorologicalparameters during the spring and the late summer of 2019 at Tudor Hill Marine Atmospheric Observatory in Bermuda. Large temporal variations inHONO concentration were controlled by several factors including local pollutant emissions, air mass interaction with the island, andlong-range atmospheric transport of HONO precursors. In polluted plumes emitted from local traffic, power plant, and cruise ship emissions,HONO and nitrogen oxides (NOx) existed at substantial levels (up to 278 pptv and 48 ppbv, respectively),and NOx-related reactions played dominant roles in daytime formation of HONO. The lowest concentration of HONO wasobserved in marine air, with median concentrations at ∼ 3 pptv around solar noon and < 1 pptv during thenighttime. Considerably higher levels of HONO were observed during the day in the low-NOx island-influenced air([NO2] < 1 ppbv), with a median HONO concentration of ∼ 17 pptv. HONO mixing ratios exhibiteddistinct diurnal cycles that peaked around solar noon and were lowest before sunrise, indicating the importance of photochemical processes forHONO formation. In clean marine air, NOx-related reactions contribute to ∼ 21 % of the daytime HONOsource, and the photolysis of particulate nitrate (pNO3) can account for the missing source assuming a moderate enhancement factorof 29 relative to gaseous nitric acid photolysis. In low-NOx island-influenced air, the contribution from bothNOx-related reactions and pNO3 photolysis accounts for only ∼ 48 % of the daytime HONOproduction, and the photochemical processes on surfaces of the island, such as the photolysis of nitric acid on the forest canopy, might contributesignificantly to the daytime HONO production. The concentrations of HONO, NOx, and pNO3 were lowerwhen the site was dominated by the aged marine air in the summer and were higher when the site was dominated by North American air in the spring,reflecting the effects of long-range transport on the reactive nitrogen chemistry in background marine environments. 

The recent COVID-19 pandemic has prompted global governments to take several measures to limit and contain the spread of the novel virus. In the United States (US), most states have imposed a partial to complete lockdown that has led to decreased traffic volumes and reduced vehicle emissions. In this study, we investigate the impacts of the pandemic-related lockdown on air quality in the US using remote sensing products for nitrogen dioxide tropospheric column (NO2), carbon monoxide atmospheric column (CO), tropospheric ozone column (O3), and aerosol optical depth (AOD). We focus on states with distinctive anomalies and high traffic volume, New York (NY), Illinois (IL), Florida (FL), Texas (TX), and California (CA). We evaluate the effectiveness of reduced traffic volume to improve air quality by comparing the significant reductions during the pandemic to the interannual variability (IAV) of a respective reference period for each pollutant. We also investigate and address the potential factors that might have contributed to changes in air quality during the pandemic. As a result of the lockdown and the significant reduction in traffic volume, there have been reductions in CO and NO2. These reductions were, in many instances, compensated by local emissions and, or affected by meteorological conditions. Ozone was reduced by varying magnitude in all cases related to the decrease or increase of NO2 concentrations, depending on ozone photochemical sensitivity. Regarding the policy impacts of this large-scale experiment, our results indicate that reduction of traffic volume during the pandemic was effective in improving air quality in regions where traffic is the main pollution source, such as in New York City and FL, while was not effective in reducing pollution events where other pollution sources dominate, such as in IL, TX and CA. Therefore, policies to reduce other emissions sources (e.g., industrial emissions) should also be considered, especially in places where the reduction in traffic volume was not effective in improving air quality (AQ). 

Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050–2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation.