Advisor

Linda A. George

Date of Award

6-5-2017

Document Type

Dissertation

Degree Name

Doctor of Philosophy (Ph.D.) in Environmental Sciences and Resources

Department

Environmental Sciences and Resources

Physical Description

1 online resource (ix, 101 pages)

DOI

10.15760/etd.3408

Abstract

Anthropogenic reactive nitrogen is emitted into the atmosphere from fossil fuel combustion (nitrogen oxides) and agricultural activities (nitrogen oxides and ammonia). Nitrogen oxide emissions have long been controlled for their role in ambient air pollution and human health effects. However, reactive nitrogen deposition is less understood even though it can play a significant role in altering biodiversity, impairing ecosystem and biogeochemical function and degrading cultural artifacts. Although nitrogen deposition is a natural part of biogeochemical cycling, many ecosystems across the United States are at risk of exceeding the critical nitrogen deposition load. While nitrogen oxides are routinely measured in urban areas, far less is known in non-urban landscapes where ecosystems may be especially sensitive. Regional chemical transport models have been used to predict the impacts of ambient reactive nitrogen deposition in non-urban areas, but models have difficulty simulating reactive nitrogen due to poorly quantified emissions, especially from the agricultural sector.

My research explores the speciated deposition of reactive nitrogen through monitoring and modeling in the unique field setting of the 150 mile Columbia River Gorge (CRG) located along the border of Oregon and Washington. This site is ideally suited for this investigation due to the large sources of reactive nitrogen at either end of the CRG and unique seasonally driven channel wind flow. Seasonally driven wind allowed us to look at the reactive nitrogen emissions flowing through the CRG to assess ambient the reactive nitrogen partitioning and deposition gradient. Using data collected by the United States Forest Service to control ambient haze in the CRG and our co-located nitrogen oxides (NOx) gas analyzer, we first characterized the influence of seasonal, bimodal wind distributions on the spatial distribution of reactive nitrogen. We found that during winter months with predominantly easterly winds, particulate nitrate and ammonium and gas-phase nitrogen dioxide levels create a gradient from the eastern end to the western end. Particulate nitrate and sulfate mass concentrations influence the CRG gradient during summer months with predominantly western winds. We also found that the magnitude of the impact from east is greater than the magnitude of impact from the west. When we compared our observations to regional chemistry transport models, we found that models are significantly under-predicting levels of reactive nitrogen in the CRG. This bias is not isolated to a single station within the Gorge, but throughout the whole Columbia Basin. Our results indicate that there are under-represented emissions in the region leading to this bias.

Partly due to the bias in reactive N gas-phase species in the CRG, regional models have been underestimating the impact of gas-phase reactive N on dry N deposition. We conducted field studies at two sites within the CRG monitoring reactive nitrogen species (nitric oxide, nitrogen dioxide, ammonia, nitric acid, particulate nitrate, particulate ammonium, and particulate sulfate) as well as ozone and meteorological parameters. These measurements allowed us to conduct the first comprehensive analysis of reactive nitrogen partitioning and deposition in the CRG.

Through our measurements, we found reactive nitrogen was higher in the spring than the summer. We found concentrations ranging from 0-15 ppbv ammonia, 0-7 ppbv nitric acid, 0-2 μg/m3 ammonium nitrate and 0-1 μg/m3 ammonium sulfate at the sites. Through the measurements of all these species, we evaluated the limiting gas-phase precursor to inorganic nitrogen particle formation. In the springtime, ammonia limits the formation of particulate reactive nitrogen; while in the summer, nitric acid and oxidized sulfur limit the formation of inorganic nitrogen particles. This suggests that there may be more sources of ammonia in the spring with fertilizer application or perhaps reactive nitrogen reservoirs are renoxified through thermal dissociation during warmer summer months.

Our estimated deposition from gas and particle phase reactive nitrogen ranged from 0 – 0.14 kg N/ha per day. We also found that gas-phase reactive nitrogen plays the largest role in dry N deposition in the CRG with particle-phase contributing less than 15% of total dry N deposition. These results are important for land managers to understand the total impact of reactive nitrogen to non-urban areas. This research can inform mitigation strategies for haze formation, identify the major species and sources involved in dry N deposition and assess the potential impacts to ecosystems and cultural artifacts.

Persistent Identifier

http://archives.pdx.edu/ds/psu/20612

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