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USGS2014

Anthropogenic organic compounds in source water of select community water systems in the United States, 2002-10

Drinking water delivered by community water systems (CWSs) comes from one or both of two sources: surface water and groundwater. Source water is raw, untreated water used by CWSs and is usually treated before distribution to consumers. Beginning in 2002, the U.S. Geological Survey’s (USGS) National Water-Quality Assessment Program initiated Source Water-Quality Assessments (SWQAs) at select CWSs across the United States, primarily to characterize the occurrence of a large number of anthropogenic organic compounds that are predominantly unregulated by the U.S. Environmental Protection Agency. Source-water samples from CWSs were collected during 2002–10 from 20 surface-water sites (river intakes) and during 2002–09 from 448 groundwater sites (supply wells). River intakes were sampled approximately 16 times during a 1-year sampling period, and supply wells were sampled once. Samples were monitored for 265 anthropogenic organic compounds. An additional 3 herbicides and 16 herbicide degradates were monitored in samples collected from 8 river intakes and 118 supply wells in areas where these compounds likely have been used. Thirty-seven compounds have an established U.S. Environmental Protection Agency (EPA) Maximum Contaminant Level (MCL) for drinking water, 123 have USGS Health-Based Screening Levels (HBSLs), and 29 are included on the EPA Contaminant Candidate List 3. All compounds detected in source water were evaluated both with and without an assessment level and were grouped into 13 categories (hereafter termed as “use groups”) based on their primary use or source. The CWS sites were characterized in a national context using an extract of the EPA Safe Drinking Water Information System to develop spatially derived and system-specific ancillary data. Community water system information is contained in the EPA Public Supply Database, which includes 2,016 active river intakes and 112,099 active supply wells. Ancillary variables including population served, watershed size, land use, population density, and recharge were characterized for each of the watersheds for river intakes and contributing areas for supply wells. A total of 313 samples were collected from 20 river intakes. Between the years of 2002 through 2010, samples were collected approximately 16 times over the course of a year. Seventy-one compounds from 12 of the 13 use groups commonly occurred (detected in greater than or equal to 1 percent of samples using an assessment level of 0.05 microgram per liter or when a compound was detected in greater than or equal to 10 percent of samples without an assessment level) indicating a wide variety of sources and pathways to these rivers and highlighting the importance of source-water protection strategies. A total of 448 supply wells were sampled once during 2002–10 as part of 30 independent groundwater studies. About 15 CWS supply wells were sampled for each independent groundwater study. Twenty-eight compounds from 7 of the 13 use groups commonly occurred indicating a wide variety of sources and pathways exist for these compounds to reach these wells and highlighting the importance of wellhead protection strategies. About one-half the 265 compounds monitored (122) were detected in both surface water and groundwater samples. A more diverse suite of compounds were detected in surface water in comparison to groundwater. However, herbicides and herbicide degradates were the most frequent group of compounds detected in both surface water and groundwater. Sixty-five of the most commonly occurring compounds were detected in one or more samples from both surface water and groundwater. Human-health benchmarks (MCLs for regulated compounds and HBSLs for unregulated compounds) were available for more than one-half the compounds (160 of the 265) monitored in this study. Fifty-eight percent (41 of 71) of the commonly occurring compounds in surface water have a human-health benchmark to which concentrations can be compared; 19 have MCLs and 22 have HBSLs. Eighty-three percent (24 of 28) of the most commonly occurring compounds in groundwater have a human-health benchmark for which concentrations can be compared; 14 have MCLs and 10 have HBSLs. To put results from this study into context with the national distribution of river intakes and supply wells used by CWSs, sites were grouped into the respective national population of land-use quartiles. The increase in compound occurrence with increasing urban and agricultural land use in the watershed or contributing area was more evident for rivers than for supply wells. The increase in detection frequency of herbicides and herbicide degradates with increasing agricultural land use was more evident for rivers than for supply wells. The occurrence of solvents did not change substantially with increasing urban land use for rivers or supply wells. Basic co-occurrence analyses were completed with and without an assessment level. Considering all detections in surface water without an assessment level, approximately 86 percent of source-water samples contained 2 or more compounds, and 50 percent of samples contained at least 14 compounds. Considering all detections in groundwater without an assessment level, 50 percent of samples contained at least three compounds. For the most part, the compounds detected most frequently as individual compounds in the environment often composed the most frequent unique mixtures. Five of the 10 most frequently co-occurring unique mixtures in both surface water and groundwater were the same: atrazine and deethylatrazine; atrazine and chloroform; deethylatrazine and simazine; atrazine and simazine; and deethylatrazine, atrazine, and simazine. Because similar mixtures were identified in both surface water and groundwater without an assessment level, future studies could be directed toward better understanding the toxicological importance of these unique mixtures. Summed concentrations of herbicide degradates were compared to concentrations of the parent herbicides in surface-water and groundwater samples collected from 8 river intakes and 118 CWS wells, from which samples were analyzed for an additional 3 herbicides and 16 degradates. The toxicity to humans for many of these degradate products is largely unknown and thus points to the importance of monitoring these compounds (both the parent and degradate) in the environment. This study highlights the importance of anthropogenic organic compounds in source water of select CWSs in the United States by characterizing their occurrence in surface-water and groundwater samples. Compound concentrations and occurrence are summarized and evaluated in a human-health context, when possible. Additionally, compounds found to co-occur as mixtures for both surface water and groundwater highlight the significance of low-level compound co-occurrence.

Scientific Investigations Report↗

USGS2013

Mobile Bay

Mobile Bay is the largest bay found in Alabama’s coastal area (Handley et al., 2007). It was named an Estuary of National Significance in 1995 under the U.S. Environmental Protection Agency’s (EPA) National Estuary Program (NEP), and its Comprehensive Conservation Management Plan was completed in 2002. Mobile Bay is 1,070 km 2 (413 miles 2 ) in area and 51 km (32 miles) long, making it the sixth largest estuary in the continental United States (Mobile Bay NEP, 2008). Its ecosystem provides habitat for more than 300 species of birds, 310 species of fish, 68 species of reptiles, 57 species of mammals, 40 species of amphibians, and 15 species of shrimp (Mobile Bay NEP, 1997). Mobile Bay lies between the Mississippi and Atlantic Flyways (Mobile Bay NEP, 2003). Commercial and residential development and industrial use is heavy in the Mobile Bay area. Although local growth and industrial markets support the Mobile Bay area economy, the resulting environmental damage to the very ecosystem upon which they depend remains a threat to the environment, economy, and population. The Mobile Bay ecosystem boasts high biological diversity and productivity and supports many freshwater and saltwater species of recreational and commercial importance. The great diversity of Mobile Bay reflects the diversity of Alabama, which is home to the largest number of different plant and animal species of all states east of the Mississippi River (Stein, 2002), and is bolstered by the unique climate and geographic conditions surrounding the bay. Freshwater inflow from the Mobile-Tensaw River Delta, ranging from 60,000 to 3,700,000 gallons per second (Wallace, 1996), mixes with saltwater from the Gulf of Mexico, which enters Mobile Bay via wind and tides (Burgan and Engle, 2006). Because of the unique conditions surrounding Mobile Bay, including shallow waters, a dynamic climate, and artificial hydrologic modifications—such as the construction of the Mobile Bay Causeway in the 1920s, which serves as an unintentional barrier between Delta waters north of the Causeway and saline waters south of the Causeway, the salinity of Mobile Bay is highly variable. Mobile Bay receives an average of 165 cm (65 inches) of rain per year from tropical storms, summer thunderstorms, and winter cold fronts (Stout et al., 1998). The climate and geography that have made Mobile Bay so rich in resources have also contributed to the threats surrounding its ecosystem. The extensive amount of rain in Mobile Bay creates large amounts of runoff, polluting the waters with fertilizers, chemicals, sediment, oil, trash, and sewage (Mobile Bay NEP, 1997). Tourism, ecotourism, recreational and commercial fishing, recreational boating, shipping, and chemical, pulp, and paper production are significant industries in Mobile Bay and the surrounding areas. Despite the approximate \$3 billion and 55,000 jobs these industries bring into the community (Alabama Tourism Department, 2010), the growth, development, and environmental stress they create are major threats to the Mobile Bay ecosystem. Among the nation’s states, Alabama ranks fifth in number of different species (144 endemic species), second in number of extinctions that have already occurred (90 extinct species) and fourth in number of species at risk for extinction (14.8% at risk out of 4,533 total species; Stein, 2002). Twenty-one of these threatened and endangered species are found in Mobile Bay, whose brackish waters provide a nursery area for many species of vertebrates and invertebrates. Some of these species include the Alabama sturgeon, Gulf sturgeon, heavy pigtoe mussel, inflated heel-splitter mussel, West Indian manatee, Alabama beach mouse, Perdido beach mouse, Alabama red-bellied turtle, gopher tortoise, Kemp’s ridley sea turtle, green sea turtle, loggerhead sea turtle, eastern indigo snake, flatwoods salamander, piping plover, red-cockaded woodpecker, and wood stork. Habitat loss underlies the decline of some bird species in Mobile Bay, and large mammals such as the red wolf, Florida panther, and Florida black bear are no longer found in the area. However, some rare species, such as the swallow-tailed kite, sandhill crane, and gopher tortoise can still be found (Duke and Kruczynski, 1992). The value of wetlands in Mobile Bay and the rest of the Gulf of Mexico is still being investigated. Although various monetary valuations of wetlands exist, critics remark that undervaluation of wetlands is inevitable (Mobile Bay NEP, 2008) and that estimates often do not place appropriate value on ecological services (Mitsch and Gosselink, 2000). Additionally, many estimates account only for anthropogenic values. One estimate concludes that one acre of wetlands performs \$3,000 worth of water purification each year (Mobile Bay NEP, 1997). With more than 76,890 hectares (190,000 acres) of wetlands in the Mobile Bay area, that equates to a value exceeding one-half billion dollars every year. Tourism, fishing, boating, production, and shipping are significant industries in the Mobile Bay area. More than 90% of fish landed in recreational and commercial fishing in the bay depend on bay habitat, including wetlands, for life requirements (Mobile Bay NEP, 1997). The Port of Mobile is Alabama’s only ocean-ship port (Mobile Bay NEP, 2008). Baldwin County, on the eastern side of the bay, experienced a population increase of 75% from 1990 to 2007, with an 89% increase in housing units (Mobile Bay NEP, 2008). Development and industry support the Mobile Bay economy, but they depend on the continued health, sustainability, and production of the water and living resources of the Mobile Bay ecosystem. Wetland loss, along with other forms of environmental degradation, remains a threat to the Mobile Bay ecosystem and Mobile Bay’s socioeconomic foundation.

Alabama↗

USGS2014

Assessment of ethylene dibromide, dibromochloropropane, other volatile organic compounds, radium isotopes, radon, and inorganic compounds in groundwater and spring water from the Crouch Branch and McQueen Branch aquifers near McBee, South Carolina, 2010-2012

Public-supply wells near the rural town of McBee, in southwestern Chesterfield County, South Carolina, have provided potable water to more than 35,000 residents throughout Chesterfield County since the early 1990s. Groundwater samples collected between 2002 and 2008 in the McBee area by South Carolina Department of Health and Environmental Control (DHEC) officials indicated that groundwater from two public-supply wells was characterized by the anthropogenic compounds ethylene dibromide (EDB) and dibromochloropropane (DBCP) at concentrations that exceeded their respective maximum contaminant levels (MCLs) established by the U.S. Environmental Protection Agency’s (EPA) National Primary Drinking Water Regulations (NPDWR). Groundwater samples from all public-supply wells in the McBee area were characterized by the naturally occurring isotopes of radium-226 and radium-228 at concentrations that approached, and in one well exceeded, the MCL for the combined isotopes. The local water utility installed granulated activated carbon filtration units at the two EDB- and DBCP-contaminated wells and has, since 2011, shut down these two wells. Groundwater pumped by the remaining public-supply wells is currently (2014) centrally treated at a water-filtration plant. To assess the occurrence, distribution, and potential sources of the anthropogenic and naturally occurring compounds detected in groundwater in the McBee area, samples of groundwater and spring water were collected from public-supply, domestic-supply, agricultural-supply, and monitoring wells and springs, respectively, between 2010 and 2012 by the U.S. Geological Survey. The water samples were analyzed for concentrations of EDB, DBCP, other volatile organic compounds (VOCs), radium-226 and radium-228, radon, and inorganic compounds. All wells sampled were screened in the shallow Crouch Branch aquifer, the deeper McQueen Branch aquifer, or, for most public-supply wells, both aquifers. In areas where no wells existed or wells could not be installed, passive samplers that adsorb EDB, DBCP, and various VOCs, were installed in the shallow subsurface. A representative groundwater flow pathway to each public supply well and selected other wells was determined by using a calibrated three-dimensional groundwater-flow model of the Atlantic Coastal Plain in Chesterfield County and particle-tracking analysis. The aerial extent of the groundwater flow pathway to public-supply wells was mapped by using chlorofluorocarbon-concentration based, apparent-age dates of the groundwater. The water-quality data collected between 2010 and 2012, in conjunction with groundwater flow pathways and historical aerial photographs of land uses near McBee, indicate an area where EDB-, DBCP-, 1,2-dichloropropane-, 1,3-dichloropropane-, and carbon disulfide-contaminated groundwater exists in the Crouch Branch aquifer in the Cedar Creek Basin and north of McBee and is most likely related to the past use of these compounds between the early 1900s and the 1980s as soil fumigants in predominately agricultural areas north of McBee. The highest EDB concentration detected (18.6 micrograms per liter) during the 3-year study was in a groundwater sample from an agricultural-supply well located north of McBee. Other VOCs, such as dichloromethane and 1,1,2-trichloroethane, also were detected in groundwater samples from this EDB-contaminated agricultural-supply well but are from unknown source(s). The fact that the agricultural area north of McBee is located in a recharge area for the Crouch Branch aquifer most likely facilitated the groundwater contamination in this area. DBCP-contaminated groundwater detected in three public-supply wells south of McBee in the deeper McQueen Branch aquifer appears to be related to past soil fumigation practices that used DBCP in agricultural areas located south of McBee. One of the three DBCP-contaminated public-supply wells also contained EDB, most likely present in groundwater due to the release of leaded gasolines that contained EDB as a fuel additive between the 1940s and 1970s. A gasoline-source of EDB, rather than a soil-fumigation source, is supported by the co-detection in groundwater from the well of 1,2-dichloroethane, a lead scavenger compound also added to leaded gasoline. Groundwater pumped from two public-supply wells located within and to the east of the McBee town limits and one domestic-supply well east of McBee was characterized by the detection of 1,1-dichloroethane, trichloroethylene, 1,1-dichloroethylene, and perchloroethylene. Groundwater flow pathways determined for these wells indicate that the potential source(s) of these compounds detected in one public-supply well and the domestic-supply well may be located within the McBee town limits, and that the potential source(s) of these compounds detected in the public-supply well to the east of McBee may be located in an area north of McBee formerly used for agriculture, but used for industry since at least the 1970s. Radium isotopes (defined in this study as the sum of radium-226 and radium-228 concentrations) and radon were detected in all wells sampled in the McBee area between 2010 and 2012. Wells characterized by radium isotope concentrations in groundwater that exceeded the MCL of 5.0 picocuries per liter were also characterized by specific conductance values greater than 30 microsiemens per centimeter and clustered north of McBee in a predominately agricultural area, and in agricultural and urban areas located within and east of McBee. The elevated specific conductance values measured in groundwater from these wells most likely are due to recharge by water mineralized by fertilizer application in agricultural areas, or due to the recharge by water mineralized by septic-tank drain-field effluent near urban areas. Radon was detected in groundwater from all wells sampled, and radon concentrations in groundwater from three monitoring wells exceeded the proposed MCL of 300 picocuries per liter. Concentrations of uranium in groundwater in the McBee area increased with increased groundwater-sample depth, most likely due to the proximity of the sample-collection location to basement rock that contains uranium-bearing minerals.

South Carolina↗

USGS2015

In-situ arsenic removal during groundwater recharge through unsaturated alluvium

OBJECTIVES The purpose of this study was to determine the feasibility and sustainability of in-situ removal of arsenic from water infiltrated through unsaturated alluvium. BACKGROUND Arsenic is naturally present in aquifers throughout the southwestern United States and elsewhere. In January 2006, the U.S. Environmental Protection Agency (EPA) lowered the Maximum Contaminant Level (MCL) for arsenic from 50 to 10 micrograms per liter (g/L). This raised concerns about naturally-occurring arsenic in groundwater. Although commercially available systems using sorbent iron or aluminum oxide resins are available to treat high-arsenic water, these systems are expensive to build and operate, and may generate hazardous waste. Iron and aluminum oxides occur naturally on the surfaces of mineral grains that compose alluvial aquifers. In areas where alluvial deposits are unsaturated, these oxides may sorb arsenic in the same manner as commercial resins, potentially providing an effective low-cost alternative to commercially engineered treatment systems. APPROACH The Antelope Valley within the Mojave Desert of southern California contains a shallow water-table aquifer with arsenic concentrations of 5 g/L, and a deeper aquifer with arsenic concentrations of 30 g/L. Water was pumped from the deep aquifer into a pond and infiltrated through an 80 m-thick unsaturated zone as part of field-scale and laboratory experiments to treat high-arsenic groundwater and recharge the shallow water table aquifer at the site. The field-scale recharge experiment included the following steps: 1) construction of a recharge pond 2) test drilling for sample collection and instrument installation adjacent to the pond 3) monitoring downward migration of water infiltrated from the pond 4) monitoring changes in selected trace-element concentrations as water infiltrated through the unsaturated zone Data from instruments within the borehole adjacent to the pond were supplemented with borehole and surface geophysical data to evaluate the lateral spreading of water as it moved downward through the unsaturated zone. Three laboratory studies were undertaken. Sequential extraction was used to evaluate the abundance of iron, aluminum, and manganese oxides and selected trace elements on operationally defined sites on the surfaces of mineral grains collected before and after infiltration from the pond. Secondly, radio-labeled arsenic-73 microcosm experiments evaluated the potential for incorporation of arsenic sorbed to exchange sites on mineral grains into less reactive crystalline mineral structures with time. Finally, column studies evaluated arsenic sorption and the pH dependence of sorption for selected unsaturated zone materials. RESULTS/CONCLUSIONS Between December 2010 and July 2012, more than 120,000 cubic meters (m3 ) (about 97 acre-feet) of high-arsenic groundwater was pumped from the deep aquifer into a 0.11 hectare (about 0.27 acres) pond and infiltrated though an 80-meter (about 260 feet) thick unsaturated zone to recharge a water-table aquifer. Arsenic concentrations were lowered from 30 to 2 g/L as water infiltrated though the unsaturated zone at the site. Some uranium, possibly associated with past agricultural land use at the site, was mobilized to concentrations as high as 66 g/L within the unsaturated zone during the experiment. Uranium was resorbed and the high uranium concentrations did not reach the water table at the site. Concentrations of other trace elements, including antimony, chromium, vanadium, and selenium were low throughout the study. Infiltration rates from the pond were as high as 0.4 meters per day (1.1 feet per day, ft/d), and the wetting front moved downward about 25 centimeters per day (cm/d) (0.8 ft/d) to a depth of about 50 m (about 165 feet). Clay layers at that depth slowed the downward movement of the wetting front to about 5 cm/d (0.16 ft/d). Lateral movement of the wetting front was monitored using sequential direct-current (DC) surface and sequential electromagnetic (EM) and DC borehole resistivity. Most lateral movement occurred on a clay layer about 50 m (about 165 feet) below land surface. Infiltrated water reached the water table in January 2013. At the water table, the “wetted footprint” of water infiltrated from the pond, indicated by surface resistivity data, was about 13 hectares (about 32 acres). On the basis of data collected at the site, there is enough sorbent material to operate this pond and treat groundwater having an arsenic concentration of 30 g/L to 2 g/L for about 500 years. Toxicity Characteristic Leaching Procedure (TCLP) data showed arsenic concentrations to be below hazardous levels beneath the pond after the experiment. Pond maintenance may be required to keep infiltration rates high, and prevent accumulation of organic material on the pond bottom, although organic material on the pond bottom may increase removal of other trace elements in infiltrated water including chromium, selenium, and vanadium. Laboratory results are consistent with the field data and show sorption of arsenic in 10 cm (0.3 feet) columns to about 2 g/L over a pH range of 6 to 8, and at influent arsenic concentrations as high as 300 g/L, without breakthrough in 50 pore volumes. Column results suggest that the insitu treatment may remove arsenic in a range of hydrogeologic settings, and would not necessarily be restricted to alkaline alluvial aquifers common throughout the southwestern United States. Radiolabeled arsenic-73 experiments show that although arsenic is initially weakly sorbed (and potentially mobile), with time arsenic is incorporated into amorphous materials. One year after sorption onto surface exchange sites, most sorbed arsenic is incorporated into crystalline oxide minerals on the surfaces of primary mineral grains and is less mobile. Results of the study suggest that long-term land use restrictions on sites used for in-situ treatment of arsenic may not be needed to control water applied to surface materials. This minimizes some regulatory concerns about future land use at sites used for in-situ arsenic treatment. However, future land uses that may alter reduction-oxidation conditions in the subsurface should be avoided, such as infiltration of stormwater recharge or recharge with other water having high organic carbon concentrations (including unsewered residential land use, dairy or other confined animal operations).

Report↗

USGS2022

Sources and characteristics of dissolved organic carbon in the McKenzie River, Oregon, related to the formation of disinfection by-products in treated drinking water

Executive Summary This study characterized the concentration and quality of dissolved organic carbon (DOC) in the McKenzie River, a relatively undeveloped watershed in western Oregon, and its link to forming disinfection by-products (DBPs) in treated drinking water. The study aimed to identify the primary source(s) of DOC in source water for the Eugene Water & Electric Board’s (EWEB) conventional treatment plant on the McKenzie River near river mile 11, upstream of Hayden Bridge. The two classes of regulated compounds examined—trihalomethanes (THMs) and haloacetic acids (HAAs)—form when organic carbon in raw source water reacts with chlorine and (or) bromine during water treatment. The objectives of the study were to: characterize the amount and quality of DOC in the McKenzie River and select tributaries during storms; identify the most common types of carbon using UV-vis spectroscopy and other methods; evaluate optical properties for predicting DBP precursors in surface water; and identify land cover classes or vegetation types that may be important sources of organic carbon and DBP precursors in EWEB’s source water. Eleven storms were sampled synoptically in upstream-to-downstream fashion to provide a “snapshot” of water quality conditions at four sites on the McKenzie River from Frissell Bridge (6 miles downstream from Trail Bridge Reservoir) to the EWEB water treatment plant at Hayden Bridge and nine contributing tributaries. Storms included late summer and early autumn “first flush” events and late autumn, winter, and spring storms spanning a range in streamflows from 3,000 to 26,000 cubic feet per second as measured in the main stem McKenzie River at the EWEB water intake. Water samples were analyzed for DOC concentrations and optical properties (fluorescence and ultraviolet absorbance [UVA]) across a range of wavelengths to characterize the quantity and quality of dissolved organic matter (DOM) in the McKenzie River at the drinking water intake and upstream locations. Paired sets of source and finished water samples were collected at the EWEB treatment plant to identify DOC quality parameters in raw source water that might predict DBP concentrations in finished drinking water. DOC concentrations were relatively low in the McKenzie River (0.4–3 milligrams per liter [mg/L]; average 1.5 mg/L) but much higher in the tributaries. The highest DOC concentrations occurred during “first flush” storms in October 2012 and September 2013; the highest value (16 mg/L) was measured at the 52nd Street stormwater outfall. The average DOC concentration in the lower basin-tributaries was 3.8 mg/L; three middle basin tributaries—Quartz, Gate, and Haagen Creeks, which drain private forestland with less coniferous forest compared with other higher elevation tributaries— had slightly lower average DOC concentrations (2.8 mg/L). These middle-basin watersheds may be important sources of DOC and DBP precursors to the McKenzie River, even more so than the lower basin tributaries, depending on their flows (and loads). This is particularly true after the September 2020 Holiday Farm fire, which burned much of this area. DOC concentrations increased 68 percent in the McKenzie River between the uppermost reference site at Frissell Bridge and Vida; this includes drainage from Quartz Creek, Blue River Lake and Cougar Reservoir, which all contributed DOC to the main stem. In contrast, the lowermost tributaries draining most of the agricultural and urban land did not have a large effect on DOC in the McKenzie River despite their higher DOC concentrations because of their presumed relatively low streamflows and, consequently, DOC loads. Apart from the continuous flow monitors in the McKenzie River and some tributaries (Blue River and South Fork McKenzie River, and streamflow at Hayden Bridge and Vida, Camp Creek and some other locations), streamflow was not assessed during sample collection for this study. This lack of streamflow data precludes a detailed analysis of loads, which is discussed in the future studies section. All DBP concentrations in finished drinking water were less than EPA maximum contaminant levels (MCLs) of 0.080 mg/L for the four trihalomethanes (THM4) and 0.060 mg/L for five haloacetic acids (HAA5). During the 11 storm sampling events the maximum summed concentrations were about 0.040 mg/L for both THM4 and HAA5. Compliance monitoring samples, collected separately by EWEB, yielded some higher concentrations—0.046 mg/L THM4 and 0.047 HAA5—during the December 2012 storm. The corresponding benchmark quotient (BQ) values, which indicate how close a measured DBP concentration is to the MCL, were 0.58 and 0.78, respectively, for THM4 and HAA5. Compared with a similar 2007–08 McKenzie River study that did not target storm events, concentrations of THM4 and HAA5 in finished water were 68 percent and 33 percent higher, respectively, during the current study. Due to the high dilution rates in the McKenzie River main stem, many of the individual fluorescence excitation-emission measurements were low (<0.1 Raman units) and approached analytical detection limits. Parallel factor analysis (PARAFAC) resulted in a five-component model (C1–C5) that represents five unique organic fluorophores. Components C1, C2, and C3 represent DOM associated with soil-derived, humic-like, more degraded organic matter. In contrast, components C4 and C5 represent “fresher” DOM, derived from terrestrial and aquatic plants, including algae and cyanobacteria that are common in the McKenzie River and its tributaries and reservoirs. The fluorescence data and PARAFAC modeling suggest that most of the DOC in the McKenzie River originated from terrestrial sources (primarily components C1 and C2). The largest increases in DOC in the main stem occurred in the reach upstream of Vida, from inflows by Quartz Creek, Blue River, South Fork McKenzie River, and other tributaries. Concentrations of DBPs in EWEB’s finished drinking water were positively correlated with DOC concentrations in raw source water (THM4, p <0.05; HAA5, p <0.01) for paired samples collected 12−24 hours apart. DOC concentrations were significantly positively correlated ( p <0.001) with laboratory-based fluorescent dissolved organic matter (fDOM) measurements, suggesting fDOM as a useful parameter for monitoring and predicting DOC concentration in surface water and DBP concentrations in finished water. Of all the PARAFAC components in surface water, C5 had the highest correlations with DBPs in finished water (rho = 0.77–0.84, p <0.01), followed by components C1 and C2 (rho = 0.75 and 0.71, respectively, p <0.01). This C5 carbon is associated with recently produced DOM, possibly from decomposed terrestrial and aquatic vegetation. Model loadings of these three components were considerably higher in the sampled tributaries relative to the main stem McKenzie River, with most of the observed increases in the main stem apparent at Vida. This points to Quartz Creek or other tributaries in the reach between Frissell Bridge and the sampling site near Vida (South Fork McKenzie and Blue Rivers) as potentially key contributors of DOM source material that leads to the production of DBPs in treated drinking water. A limited load analysis showed that the reservoirs contributed 8–37 percent of the instantaneous DOC loads observed at Vida at the time of sampling, which suggests other sources such as Quartz Creek and other streams in the reach between Frissell Bridge and Vida are more important. Random forest analyses identified PARAFAC components C1 and C5 and fluorescence peaks A, C, M, T and N as the best predictors for HAA5 concentrations in finished drinking water, explaining 62.5 percent of the variation. The best predictors for THM4 were C1, C4 + C5, and peaks T, A, and N, which explained 33 percent of the variation. Several land cover and vegetation classes were correlated with DOC concentration and other optical measurements. The percentage of evergreen forest in each of the subwatersheds sampled was negatively correlated ( p <0.001) with DOC concentration and many optical indicators of DOM quantity: UVA 254 , fDOM, and all of the fluorescence peaks. In contrast, mixed (deciduous) forest was positively correlated ( p <0.001) with DOC, fDOM, UVA 254 , and several fluorescence peaks, demonstrating the importance of deciduous leaf fall in generating DOC and DBP precursors. The high level of human activities in the middle and lower portion of the basin—including timber harvesting and road construction on private forestland, agricultural, rural, industrial, and urban development—have resulted in the greatest loss in native coniferous and mixed deciduous forests in the basin. DOC loading from these tributaries and reservoir releases, which contain DOC from terrestrial and aquatic productivity, both enrich the McKenzie River. Concentrations of DOC increased an average of 71 percent (range 30–120 percent) in the McKenzie River between Frissell Bridge, the upstream reference site, and Vida. PARAFAC components C1, C2, and C5—which were correlated with DBPs in finished water—increased, on average, 109–136 percent (range 20–250 percent) in this same Frissell-to-Vida reach. These increases occur from input of tributaries in the middle basin such as Quartz Creek and others, as noted above. Future monitoring, field, and lab studies can improve our understanding of seasonal and spatial sources of organic carbon contributing DBP precursors to the McKenzie River and allow detection of long-term trends resulting from the recent Holiday Farm Fire, which burned 173,393 acres of forestland, including riparian areas along the main stem, and numerous structures, homes, and outbuildings in September 2020. Future studies could examine DOC fluxes and flushing of carbon from the watershed, investigate the role of precipitation amount and intensity in mobilizing carbon and sediment, and evaluate impacts to aquatic communities and human health as part of a post-fire assessment. Other areas ripe for study include evaluating the impacts of potential temperature increases on carbon sequestration and decomposition in the burned and unburned forests and identifying practices that foster sequestration of carbon in forest soils. The use of fluorescence sensors such as fDOM to monitor the concentration and composition of raw water supplies may be improved for detection of specific DBP precursors, to provide continuous and real-time information to treatment plant operators. Future studies that monitor DOM amount and quality, and DBP Formation Potential (FP), particularly during storm events, paired with streamflow measurements, as suggested above, could help identify areas that contribute high DOC loads and thus help managers identify the key areas to focus restoration activities. Other studies could examine treatment options for currently regulated DBPs and potentially unregulated compounds, including advanced biological treatments for their removal. This study was a collaboration between the U.S. Geological Survey (USGS) and EWEB in Eugene, Oregon, with additional funding provided from USGS Cooperative Matching Funds Program.

Oregon↗

USGS2017

Geology and mining history of the Southeast Missouri Barite District and the Valles Mines, Washington, Jefferson, and St. Francois Counties, Missouri

The Southeast Missouri Barite District and the Valles Mines are located in Washington, Jefferson, and St. Francois Counties, Missouri, where barite and lead ore are present together in surficial and near-surface deposits. Lead mining in the area began in the early 1700’s and extended into the early 1900’s. Hand mining of lead in the residuum resulted in widespread pits (also called shafts or diggings), and there was some underground mining of lead in bedrock. By the 1860’s barite was recovered from the residuum by hand mining, also resulting in widespread diggings, but generally not underground mines in bedrock. Mechanized open-pit mining of the residuum for barite began in the 1920’s. Barite production slowed by the 1980’s, and there has not been any barite mining since 1998. Mechanized barite mining resulted in large mined areas and tailings ponds containing waste from barite mills. The U.S. Environmental Protection Agency (EPA) has determined that lead is present in surface soils in Washington and Jefferson Counties at concentrations exceeding health-based screening levels. Also, elevated concentrations of barium, arsenic, and cadmium have been identified in surface soils, and lead concentrations exceeding the Federal drinking-water standard of 15 micrograms per liter have been identified in private drinking-water wells. Potential sources of these contaminants are wastes associated with barite mining, wastes associated with lead mining, or unmined natural deposits of barium, lead, and other metals. As a first step in helping EPA determine the source of soil and groundwater contamination, the U.S. Geological Survey (USGS), in cooperation with the EPA, investigated the geology and mining history of the Southeast Missouri Barite District and the Valles Mines. Ore minerals are barite (barium sulfate), galena (lead sulfide), cerussite (lead carbonate), anglesite (lead sulfate), sphalerite (zinc sulfide), smithsonite (zinc carbonate), and chalcopyrite (copper-iron sulfide). The Cambrian Potosi Dolomite is the most important formation for the ore deposits, followed by the Eminence Dolomite. Because galena, sphalerite, and barite are less soluble than dolomite, chemical weathering of the ore-bearing dolomite bedrock resulted in the concentration of ore minerals in the residuum. Most of the barite and lead mining was in the residuum, which averages 10 to 15 feet thick. Lead mining by French explorers may have begun in 1719 along Old Mines Creek at Cabanage de Renaudiere, which was followed shortly by the discovery of lead and the development of lead mines at Mine Renault (also called Forche a Renault Mine), Old Mines, and at other places along the Big River, Mineral Fork, and Forche a Renault Creek. Lead mining began sometime between 1775 and 1780 at Mine a Breton, the name of which was later changed to Potosi. Other mining areas were developed in the early part of the 19th century, including Fourche a Courtois (Palmer Mines), the French Diggings, and the Richwoods Mines. Zinc became a valuable resource after the Civil War, and the Valles Mines was an important supplier of zinc as well as lead, with at least some production up until the 1920’s. Lead mining declined in the early part of the 20th century as mining in the Old Lead Belt, Mine La Motte, and the Tri-State District expanded. The earliest lead mines were diggings in the residuum and were round holes (shafts) about 4 feet in diameter dug with pick and shovel about 15–20 feet deep, with drifts dug a short distance laterally from the bottom of the shafts. This mining process was repeated a short distance away until a large area was covered with pits. Some mining in bedrock began by about 1800, with shafts as deep as 170 feet and as much as several hundred feet of lateral drifts. Smelting of the lead ore to elemental lead was first done using a log furnace, which was inefficient; estimates have been made that only about 50 percent of the lead was recovered, and the remainder was lost to the ashes (slags) and to volatilization. Starting in 1798, ash furnaces were used to smelt the ashes from the log furnaces. These two furnaces were worked in tandem for many years but were gradually replaced by other furnaces, including the Scotch hearth. Estimates of lead recovery as high as 80–90 percent have been made for the Scotch hearth. By the mid-1870’s the air furnace was being used, also with estimated lead recovery as high as 80–90 percent. Zinc furnaces were built when zinc became a valuable commodity, but much of the zinc ore was shipped out of the area, either to a smelter in St. Louis, Missouri, or to other smelters. The total lead and zinc production from the Southeast Missouri Barite District and the Valles Mines is estimated at 180,000 tons of lead and 60,000 tons of zinc. An estimated 97,000 tons of lead and an estimated 120,000 tons of zinc were lost during smelting. The estimated losses do not include losses at the mine site during mining and preparation for smelting, such as the loss of fine-grained galena during hand cleaning or the discarding of zinc ore before its value was known, for which no estimates are available. Hand mining for barite in the residuum was active by at least the 1860’s and peaked from 1905 to the 1930’s when several thousand people were engaged in barite mining. Hand mining (diggings) and cleaning of the ore was done in much the same way as earlier lead mining, with the additional use of a rattle box to further clean the barite. Mechanized open-pit mining of old barite diggings began in 1924 to recover barite left behind by hand mining, and washing plants were used to clean the clay from the barite. Hand mining, however, continued to thrive, and washer plants began to close temporarily in 1931; nearly all of the barite produced before 1937 was by hand mining. By the 1940’s, however, all barite mining was mechanized. Mechanized mining used shovels powered by steam, gasoline, or electricity (and by the 1950’s draglines and front-end loaders) to mine the residuum. The ore was loaded onto rail cars (and by the 1940’s, trucks) for shipment to washer plants. Clay was removed from the barite using a log washer, and a jig was used to concentrate the barite. Overflow from the log washers was waste and went to a mud (tailings) pond. The coarse jig tailings went to tailings piles or were used as railroad ballast and, later, to create roads within the mine pit. Some barite was ground, depending on its final use, and some ground barite was bleached using a hot solution of sulfuric acid to remove impurities such as iron minerals and lead sulfide (galena). An earlier bleaching process used lead-lined tanks. Large quantities of water were required for milling the barite; some was recirculated water and the remainder came from dammed streams or was pumped from wells. Tailings and wastewater were impounded behind dikes that were built across small valleys and were increased in height as necessary using washer waste and any overburden that had been stripped. In some cases, dikes were built across valleys that had already been mined for barite. The total production of barite from the Southeast Missouri Barite District and the Valles Mines is estimated to have been about 13.1 million tons. Most of the barite production was from Washington County. Hand mining and processing of barite was inefficient. Estimates of barite recovery range from less than one-fourth to about one-half because pillars between the shafts in the residuum needed to be left unmined for stability. With mechanized mining, large amounts of barite were lost during the milling process. It has been estimated that about 30 percent of the barite was lost and that about two-thirds of the lost barite was fine-grained and was discharged to the tailings ponds. Some galena was lost to the tailings ponds. A 1972 inventory of tailings ponds by the Missouri Geological Survey identified 67 ponds in the Southeast Missouri Barite District (there are more than this currently documented). Results from samples from four ponds that were drilled were used to estimate that the 67 ponds contained almost 39 million tons (or cubic yards) of tailings averaging about 5 percent barite, for a potential reserve of 1.935 million tons of barite. It is not known how much lead was removed during barite mining, either by hand or mechanized mining and processing, how much lead was recovered, or how much lead went as fines to the tailing ponds or as coarse material to mine roads or was otherwise lost.

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