Temporal and spatial trends of fine particulate matter composition in Fairbanks, Alaska

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Author
Nattinger, Kristian C.
Chair
Simpson, William R.
Committee
Guerard, Jennifer J.
Cahill, Catherine F.
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URI
http://hdl.handle.net/11122/6830
Abstract
Fairbanks, AK experiences extreme winter pollution episodes that result in violations of the Fine Particulate (PM₂.₅) National Ambient Air Quality Standards and pose significant health risks for inhabitants. We analyzed the 2006-2014 wintertime (November 1 to the end of February) PM₂.₅ composition from four sampling sites in the Fairbanks North Star Borough (FNSB) to provide insight into sources and trends. We developed conversions for particulate carbon measurements that were sampled/analyzed with different methods to allow quantitative comparisons. Using these conversions, we found excellent mass closure between PM₂.₅ mass concentration reconstructed from particulate composition and directly measured PM₂.₅ mass concentration. The North Pole Fire Station #3 site (NPFS3) PM₂.₅ mass concentration is nearly double the concentration at other sites in the FNSB and significantly different (t-test on log normalized data, 95% conf.). We observe significant differences (t-test, 95% conf.) in the PM₂.₅ composition between the NPFS3 site and all other sites for most components. Comparison to source profiles indicates that the difference in SO₄²⁻/PM₂.₅ and organic carbon (OC)/PM₂.₅ ratios is attributable to greater use of wood heat in the areas surrounding the NPFS3 site than in Fairbanks. This interpretation is supported by the results of the Home Heating Survey, which found a greater reported use of wood for heat in North Pole than in Fairbanks. Interannual variability is observed in the PM₂.₅ composition. The increase in fuel oil price in 2009 is correlated with an increase in OC/PM₂.₅ ratio and a decrease in the SO₄²⁻/PM₂.₅. The interannual variability of the SO₄²⁻/PM₂.₅ and NH₄⁺/PM₂.₅ ratios are correlated. The particles appear to be neutralized until 2010 when a drop in NH₄⁺ is not accompanied by as large of a drop in anions leaving the particles acidic. The mean sulfur oxidation ratio is 5%, attributable to primary and possible secondary oxidation of SO₂. The results of our analysis supports modeling results that wood smoke contributes a large fraction to the Fairbanks area PM₂.₅. Our work also identified changes in the concentration, composition and spatial distribution of PM₂.₅ that may help air quality managers in identifying effective PM₂.₅ control strategies.
Description
Thesis (M.S.) University of Alaska Fairbanks, 2016
Table of Contents
Chapter 1: Introduction -- 1.1 Motivation -- 1.2 Review of Health Effects of Fine Particulates -- 1.3 Background -- 1.3.1 Fairbanks Emission Sources -- 1.3.2 Current Mitigation -- 1.4 Particle Formation -- 1.4.1 Primary Particles -- 1.4.2 Secondary Particle Formation -- 1.4.3 Sulfur Oxidation -- 1.5 Transport -- 1.6 Source Profiles -- 1.7 Prior Modeling Results -- 1.7.1 SANDWICH Mass Balance Modeling -- 1.7.2 Organic Carbon Mass Estimations -- 1.7.3 Source Apportionment Modeling -- 1.8 Hypotheses -- 1.8.1 Hypothesis 1: Significant differences in PM₂.₅ composition and mass concentration will exist between Norh Pole and Fairbanks sampling sites -- 1.8.2 Hypothesis 2: A reduction in the OC/PM2.5 ratio will be observed after 2010 -- 1.8.3 Hypothesis 3: Secondary sulfur oxidation is taking place during Fairbanks Winter -- Chapter 2: Methods, Sampling Sites and Data Sources -- 2.1 Sampling and Analysis Methods -- 2.1.1 Sampling Methods -- 2.1.1.1 Sampling Methods Overview -- 2.1.1.2 Carbon Sampling Method Discrepancies -- 2.1.2 Analysis Methods -- 2.1.2.1 Inorganic Analysis -- 2.1.2.2 Carbon Analysis -- 2.1.2.3 Carbon Analysis Method Discrepancies -- 2.2 Associated Error -- 2.2.1 Sampling Error -- 2.2.2 Analytical Error -- 2.3 Data Acquisition and Processing Overview -- 2.4 Initial Data Processing -- 2.4.1 Data Processing- Blank Correction -- 2.4.2 Calculation of the Reconstructed Mass Concentration -- 2.4.3 Data Processing: OC/EC Correction Methods -- 2.4.3.1 Motivation -- 2.4.3.2 Fresno OC/EC Correction -- 2.4.3.3 Fairbanks OC/EC Correction -- 2.4.3.4 OC/EC Correction Checks -- 2.5 Data Processing– Sample Variability -- 2.6 Data Processing- Quality Control (QC) -- 2.7 Data Processing- Statistical Methods -- 2.8 Data Processing– Sulfur Oxidation -- 2.8.1 Sulfur Oxidation Ratio (SOR) Calculation -- 2.8.2 Determination of Secondary Oxidation -- 2.8.3 Metal Catalyst Investigation -- 2.9 Data Processing - Non-Sulfate Sulfur (NSS) -- 2.10 Data Processing– Spatial Analysis -- 2.11 Data Processing – Temporal Analysis -- 2.12 Source Profile Selection Methods -- 2.13 Source Profile Processing Methods -- Chapter 3: Results of PM2.5 Analysis -- 3.1 OC/EC Correction -- 3.1.1 Method Performance -- 3.1.2 Comparison to Fresno Based Method -- 3.2 Temporal Trends -- 3.2.1 Meteorological Impacts on PM₂.₅ -- 3.2.2 Component Mass Concentrations in Air -- 3.2.3 Interannual and Daily Variability in Component/PM₂.₅ Ratios -- 3.2.4 Trends in Component/PM₂.₅ Ratios -- 3.2.5 Correlation of Component/PM₂.₅ Ratios with Temperature -- 3.3 Spatial Trends -- 3.3.1 Gravimetric PM₂.₅ -- 3.3.2 Component/PM₂.₅ Ratio Trends -- 3.4 Sulfur Oxidation -- 3.4.1 Sulfur Oxidation Ratio (SOR) -- 3.4.2 Non-Sulfate Sulfur -- 3.5 Source Profile Averages -- Chapter 4: Discussion -- 4.1 OC/EC Correction -- 4.2 Temporal Trends -- 4.2.1 Meteorological Impacts on PM₂.₅ -- 4.2.2 Component Mass Concentrations -- 4.2.3 Interannual and Daily Variability in Component/PM₂.₅ Ratios -- 4.2.4 Trends in Component/PM₂.₅ Ratios -- 4.3 Spatial Trends -- 4.3.1 Gravimetric PM₂.₅ -- 4.3.2 Composition Differences -- 4.4 Sulfur Oxidation -- 4.5 Non-Sulfate Sulfur (NSS) -- 4.6 Applications and Limitations of Source Profiles -- Chapter 5: Conclusions and Future Work -- 5.1 Conclusions with Regard to the Three Hypotheses -- 5.1.1 Hypothesis 1: Significant differences in PM2.5 composition and mass concentration will exist between North Pole and Fairbanks sampling sites -- 5.1.2 Hypothesis 2: A reduction in the OC/PM2.5 ratio will be observed after 2010 -- 5.1.3 Hypothesis 3: Secondary sulfur oxidation is taking place during the Fairbanks winter -- 5.3 Future Work: Investigating Recent Changes in Emissions -- 5.4 Future Work: Improved Statistics and Trend Analyses -- 5.5 Future Work: Improved Source Apportionment -- 5.6 Accessing Data for Future Research -- Literature Cited.
Date
2016-08
Type
Thesis
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