Sources of Fine Particulate Species in Ambient Air over Lake Champlain Basin,VT

Abstract

This study is a part of an ongoing investigation of the types and locations of emission sources that contribute fine particulate air contaminants to Underhill, VT. The air quality monitoring data used for this study are from the Interagency Monitoring of Protected Visual Environments network for the period of 2001–2003 for the Underhill site. The main source-receptor modeling techniques used are the positive matrix factorization (PMF) and potential source contribution function (PSCF). This new study is intended as a comparison to a previous study of the 1988–1995 Underhill data that successfully revealed a total of 11 types of emission sources with significant contributions to this rural site. This new study has identified a total of nine sources: nitrate-rich secondary aerosol, wood smoke, East Coast oil combustion, automobile emission, metal working, soil/dust, sulfur-rich aerosol type I, sulfur-rich aerosol type II, and sea salt/road salt. Furthermore, the mass contributions from the PMF identified sources that correspond with sampling days with either good or poor visibility were analyzed to seek possible correlations. It has been shown that sulfur-rich aerosol type I, nitrate aerosol, and automobile emission are the most important contributors to visibility degradation. Soil/dust and sea salt/road salt also have an added effect.     

Sources of fine particulate species in ambient air over lake Champlain Basin, VT

This study is a part of an ongoing investigation of the types and locations of emission sources that contribute fine particulate air contaminants to Underhill, VT. The air quality monitoring data used for this study are from the Interagency Monitoring of Protected Visual Environments network for the period of 2001-2003 for the Underhill site. The main source-receptor modeling techniques used are the positive matrix factorization (PMF) and potential source contribution function (PSCF). This new study is intended as a comparison to a previous study of the 1988-1995 Underhill data that successfully revealed a total of 11 types of emission sources with significant contributions to this rural site. This new study has identified a total of nine sources: nitrate-rich secondary aerosol, wood smoke, East Coast oil combustion, automobile emission, metal working, soil/dust, sulfur-rich aerosol type I, sulfur-rich aerosol type II, and sea salt/road salt. Furthermore, the mass contributions from the PMF identified sources that correspond with sampling days with either good or poor visibility were analyzed to seek possible correlations. It has been shown that sulfur-rich aerosol type I, nitrate aerosol, and automobile emission are the most important contributors to visibility degradation. Soil/dust and sea salt/road salt also have an added effect.     

Iodine sequestration using delafossites and layered hydroxides

The objective of this document is to report on the early success for sequestering ¹²⁹I. Sorption coefficients (K _d) for I⁻ and IO₃ ⁻ onto delafossites, spinels and layered metal hydroxides were measured and compared for their applicability to sequester ¹²⁹I. The studies were performed using a dilute fluid composition representative of groundwater indigenous to the Yucca mountain area. Delafossites generally exhibited relatively poor sorption coefficients (<35 mL/g). In contrast, the composition of the layered hydroxides significantly affects their ability to sorb I. Cu/Al and Cu/Cr layered hydroxide samples exhibit K _d’s greater than 1000 mL/g for both I⁻ and IO₃ ⁻.     

Reactive barriers for Cs retention

¹³⁷Cs was dispersed globally by cold war activities and, more recently, by the Chernobyl accident. Engineered extraction of ¹³⁷Cs from soils and groundwaters is exceedingly difficult. Because the half-life of ¹³⁷Cs is only 30.2 years, remediation might be more effective (and less costly) if ¹³⁷Cs bioavailability could be demonstrably limited for even a few decades by use of a reactive barrier. Essentially permanent isolation must be demonstrated in those few settings where high nuclear level wastes contaminated the environment with ¹³⁵Cs (half-life 2.3×10⁶ years) in addition to ¹³⁷Cs. Clays are potentially a low-cost barrier to Cs movement, though their long-term effectiveness remains untested. To identify optimal clays for Cs retention, Cs desorption was measured for five common clays: Wyoming Montmorillonite (SWy-1), Georgia Kaolinites (KGa-1 and KGa-2), Fithian Illite (F-Ill), and K-Metabentonite (K-Mbt). Exchange sites were pre-saturated with 0.16 M CsCl for 14 days and readily exchangeable Cs was removed by a series of LiNO₃ and LiCl washes. Washed clays were then placed into dialysis bags and the Cs release to the deionized water outside the bags measured. Release rates from 75 to 139 days for SWy-1, K-Mbt and F-Ill were similar; 0.017% to 0.021% sorbed Cs released per day. Both kaolinites released Cs more rapidly (0.12% to 0.05% of the sorbed Cs per day). In a second set of experiments, clays were Cs-doped for 110 days and subjected to an extreme and prolonged rinsing process. All the clays exhibited some capacity for irreversible Cs uptake. However, the residual loading was greatest on K-Mbt (0.33 wt.% Cs). Thus, this clay would be the optimal material for constructing artifical reactive barriers.     

Reactive barriers for 137Cs retention

137Cs was dispersed globally by cold war activities and, more recently, by the Chernobyl accident. Engineered extraction of 137Cs from soils and groundwaters is exceedingly difficult. Because the half-life of 137Cs is only 30.2 years, remediation might be more effective (and less costly) if 137Cs bioavailability could be demonstrably limited for even a few decades by use of a reactive barrier. Essentially permanent isolation must be demonstrated in those few settings where high nuclear level wastes contaminated the environment with 135Cs (half-life 2.3 x 10(6) years) in addition to 137Cs. Clays are potentially a low-cost barrier to Cs movement, though their long-term effectiveness remains untested. To identify optimal clays for Cs retention, Cs desorption was measured for five common clays: Wyoming Montmorillonite (SWy-1), Georgia Kaolinites (KGa-1 and KGa-2), Fithian Illite (F-Ill), and K-Metabentonite (K-Mbt). Exchange sites were pre-saturated with 0.16 M CsCl for 14 days and readily exchangeable Cs was removed by a series of LiNO3 and LiCl washes. Washed clays were then placed into dialysis bags and the Cs release to the deionized water outside the bags measured. Release rates from 75 to 139 days for SWy-1, K-Mbt and F-Ill were similar; 0.017% to 0.021% sorbed Cs released per day. Both kaolinites released Cs more rapidly (0.12% to 0.05% of the sorbed Cs per day). In a second set of experiments, clays were Cs-doped for 110 days and subjected to an extreme and prolonged rinsing process. All the clays exhibited some capacity for irreversible Cs uptake. However, the residual loading was greatest on K-Mbt (approximately 0.33 wt.% Cs). Thus, this clay would be the optimal material for constructing artifical reactive barriers.