On-road emissions of ammonia: An underappreciated source of atmospheric nitrogen deposition

We provide updated spatial distribution and inventory data for on-road NH3 emissions for the continental United States (U.S.) On-road NH3 emissions were determined from on-road CO2 emissions data and empirical NH3:CO2 vehicle emissions ratios. Emissions of NH3 from on-road sources in urbanized regions are typically 0.1-1.3 t km(-2) yr(-1) while NH3 emissions in agricultural regions generally range from 0.4-5.5 t km(-2) yr(-1), with a few hotspots as high as 5.5-11.2 t km(-2) yr(-1). Counties with higher vehicle NH3 emissions than from agriculture include 40% of the U.S. population. The amount of wet inorganic N deposition as NH4+ from the National Atmospheric Deposition Program(NADP) network ranged from 37 to 83% with a mean of 58.7%. Only 4% of the NADP sites across the U.S. had <45% of the N deposition as NH4+ based on data from 2014 to 2016, illustrating the near-universal elevated proportions of NH4+ in deposition across the U.S. Case studies of on-road NH3 emissions in relation to N deposition include four urban sites in Oregon and Washington where the average NH4-N:NO3-N ratio in bulk deposition was 2.3. At urban sites in the greater Los Angeles Basin, bulk deposition of NH4-N and NO3-N were equivalent, while NH4-N:NO3-N in throughfall under shrubs ranged from 0.6 to 1.7. The NH4-N:NO3-N ratio at 7-10 sites in the Lake Tahoe Basin averaged 1.4 and 1.6 in bulk deposition and throughfall, and deposition of NH4-N was strongly correlated with summertime NH3 concentrations. On-road emissions of NH3 should not be ignored as an important source of atmospheric NH3, as a major contributor to particulate air pollution, and as a driver of N deposition in urban and urban-affected regions. Published by Elsevier B.V.