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George Aiken

Publications and source records attributed to George Aiken.

9 recordsLinked to original sources
USGS2019

Sulfur contamination in the Everglades, a major control on mercury methylation

In this chapter sulfur contamination of the Everglades and its role as a major control on methylmercury (MeHg) production is examined. Sulfate concentrations over large portions of the Everglades (60% of the ecosystem) are elevated or greatly elevated compared to background conditions of <1 mg/L. Land and water management practices in south Florida are the primary reason for the high levels of sulfate loading to the Everglades. Marshes in the northern Everglades that are highly enriched in sulfate have average concentrations of 60 mg/L, but water in canals in the Everglades Agricultural Area (EAA) contain the highest concentrations of sulfate averaging 60–70 mg/L. Studies that examined the mass balance of sulfur to the Everglades have determined that the primary sources of sulfate include: sulfur currently used in agriculture, and natural and legacy agricultural sulfur released by oxidation of organic soil within the EAA. The extensive loading of sulfate to the ecosystem increases microbial sulfate reduction, the dominant microbial process driving mercury methylation and MeHg production. The biogeochemical processes linking sulfate loading and MeHg production, however, are complex. MeHg production increases as sulfate levels rise from levels <1 mg/L up to about 20 mg/L. However, production of sulfide (a byproduct of microbial sulfate reduction) starts to inhibit MeHg production above 20 mg/L. Sulfate loading to canals in the EAA has impacted the northern Everglades the most, but the Everglades canal system can transport sulfate as far as Everglades National Park (ENP), 80 km further south. Plans to deliver more water to ENP as part of restoration may increase overall sulfate loads to the southern Everglades. Reduction of sulfate loading should be a major goal of Everglades restoration because of the many negative effects of sulfate on the ecosystem. The ecosystem has been shown to respond quickly to reductions in sulfate loading, and strategies for reducing sulfate loading may produce positive outcomes for the Everglades in the near-term. Strategies for reducing sulfate loading will need to include: best management practices for agricultural use of sulfate, approaches to minimize soil oxidation in the EAA, and modifications to stormwater treatment areas to improve sulfate retention.

Florida↗
USGS2019

Biogeochemical and physical processes controlling mercury methylation and bioaccumulation in Lake Powell, Glen Canyon National Recreation Area, Utah and Arizona, 2014 and 2015

Mercury monitoring results from about 300 Morone saxatilis (striped bass) muscle tissue samples collected by the State of Utah from Lake Powell resulted in a Utah/Arizona fish consumption advisory issued in 2012 for approximately the lower 100 kilometers of the reservoir. Chemical, physical, and biological data were collected during two synoptic sampling cruises on Lake Powell during May/June 2014 and August 2015 to test three hypotheses associated with a conceptual model developed to explain the observed geographic concentration gradient of Hg in fish tissue samples. This model proposes that in the transition from a primarily riverine system to a reservoir, there is a change in the concentration and composition of water-column particulate material, increasing in the proportion of organic content moving downstream, as the larger size fractions of the inorganic particulate load are deposited in the upper reservoir. This change alleviates light limitation of phytoplankton production and leads to a higher proportion of autochthonous primary production in the downstream direction. This, in turn, drives increased microbial methylmercury (MeHg) production in the benthos and potentially the water column, in the downstream direction, and results in the observed elevated fish Hg levels in the lower part of the reservoir. The model also proposes that there are differences between the main stem of Lake Powell and side canyons, embayments, or secondary rivers entering the reservoir, in terms of Hg cycling dynamics and bioaccumulations, driven mainly by differences in hydrology. Finally, seasonal differences in Hg dynamics within the reservoir are proposed, based on seasonal dynamics associated with primary production and the physical process of seasonal stratification. A total of three statistically testable hypotheses were proposed and postulated that measurable differences in key Hg and non-Hg metrics exist between: (1) the upper and lower reservoir; (2) main stem and river arm/side canyon/embayment sites; and (3) early-season (May/June 2014, less stratified) and late-season (August 2015, stratified) conditions. Statistically modeled least square means in combination with the graphical analysis of Hg and non-Hg parameters were used to examine the data collected during the study and test these hypotheses. Data collected during the study are included in a U.S. Geological Survey data release and are available online at https://doi.org/10.5066/F74X560J . In general, water-column, plankton, and surface sediment samples collected during the synoptic sampling cruises are supportive of the three hypotheses associated with the conceptual model. In support of hypothesis 1 (comparing upper and lower reservoir sites), the least square mean for turbidity was higher in the upper reservoir. In contrast, surface water particulate organic carbon (as a percentage of total particulate mass), particulate MeHg (by mass [in nanograms per gram] and as a percentage of total mercury [THg]), and particulate-dissolved partitioning coefficients for THg and MeHg were higher in the lower reservoir. Plankton THg concentrations also were significantly (probability [ p ] less than (<) 0.05) higher in the lower reservoir. Surface sediment metrics in support of hypothesis 1 include higher MeHg production potential rates in the lower reservoir. In contrast, there were no statistically significant differences between the upper and lower reservoir for surface sediment percent of MeHg and MeHg concentration, percent MeHg, or methylation rate constants. These spatial trends associated with hypothesis 1 indicate a pathway for enhanced Hg bioavailability in the lower reservoir. Hypothesis 2, which tested for differences between main stem and river arm/side canyon/embayment sites, was supported by a number of water-column parameters, including particulate THg and MeHg concentrations by mass (in nanograms per gram) and percent particulate MeHg being significantly ( p <0.05) higher in the river arms, side canyons, and embayments relative to the main stem channel. Plankton MeHg concentrations (by mass [in nanograms per gram] and volume [in nanograms per liter] and as a percentage of THg) were elevated in river arm/side canyon/embayment sites compared to main stem sites, indicating an enhanced potential for MeHg bioaccumulation at the base of the pelagic food web in river arms, side canyons, and embayments. In contrast, few of the sediment metrics differed between main stem and river arm/side canyon/embayment sampling sites; however, the potential for MeHg degradation in surface sediment was significantly higher in the main stem. The data indicate that river arm/side canyon/embayment sites may experience enhanced Hg bioaccumulation, compared to the main stem, because of higher MeHg levels at the base of the pelagic food web. This conclusion is supported by the elevated Hg detected in striped bass muscle tissue samples collected in the San Juan Arm during this study (2014). Fish collected from the lower reservoir exhibited a distinct Hg isotopic signature that was enriched in delta (δ) 202 Hg and capital delta (Δ) 199 Hg relative to fish samples collected from either Good Hope Bay or the San Juan Arm. Hypothesis 3 tested for differences between early (May/June) high-flow and late (August) low-flow seasons. This test was supported by a range of non-Hg metrics (nitrate, phosphate, chlorophyll a , dissolved oxygen, fluorescent dissolved organic matter, temperature, and pH) that reflect the increase in chlorophyll a , decrease in nutrients, and buildup of stratified conditions in the transition from early- to late-season sampling periods. Significant seasonal differences also were noted for multiple Hg metrics, including (a) water-column filtered and particulate (by mass) MeHg and THg concentrations; (b) plankton MeHg and THg concentration (by mass); and (c) sediment percent MeHg, Hg(II)-methylation rate constant, and microbial ribosomal ribonucleic acid, small subunit 16 (16S rRNA) abundance, all of which were higher during the late-season synoptic sampling. Overall, the surface sediment metrics are consistent with a seasonal shift from the early-season synoptic results, when the availability of Hg(II) exerts a primary control on MeHg production, to the late-season synoptic sampling, when microbial activity is a dominant driver of MeHg production.

Arizona, Utah↗
USGS2019

First examination of diet items consumed by wild-caught black carp (Mylopharyngodon piceus) in the U.S.

Black carp ( Mylopharyngodon piceus ) were imported to the U.S. in the 1970s to control snails in aquaculture ponds and have since escaped from captivity. The increase in captures of wild fish has raised concerns of risk to native and imperiled unionid mussels given previous literature classified this species a molluscivore. We acquired black carp from commercial fishers and biologists, and examined digestive contents of 109 fish captured over 8 y from lentic and lotic habitats in the central and southern U.S.A. Digestive tract contents were preserved, and diet items inventoried. We identified 59 aquatic animal taxa (21 mollusks, 27 insects, and 11 other invertebrates) and various plant material including nuts and seeds; no fish were found. Approximately 45% of stomachs examined were empty or only contained flukes (Trematoda) that had infected mollusks before they were ingested. Nonempty stomachs contained snails (16.5%), bivalve mussels (22.8%), and insect larvae (net-spinning caddisflies, 15.6%; burrowing mayflies, 6.4%; and midges, 13.7%). Fish also consumed freshwater sponges (Porifera), moss animals (Bryozoa), crustaceans (Ostracoda and Decapoda), water mites (Acarina), and three worm phyla (Nematoda, Nemertea, Annelida). Seven taxa of unionid mussels were identified from shell fragments among the fish we examined, all of which are found in habitats with soft mud or sand/silt substrates. Diet of fish captured in lentic environments contained significantly higher richness than those captured in lotic environments. Individual black carp often contained large numbers of only one or two diet items that were assumed locally abundant and did not always crush the shells of mollusks. Most fish we examined consumed benthic prey, which supports the classification of black carp as a benthic foraging species. However, the presence of other aquatic taxa associated with pelagic or subsurface zones suggests black carp are opportunistic in their consumption of diet items and flexible in their feeding modes.

The American Midland Naturalist↗
USGS2018

High frequency data exposes nonlinear seasonal controls on dissolved organic matter in a large watershed

We analyzed a five year, high frequency time series generated by an in situ fluorescent dissolved organic matter (fDOM) sensor installed near the Connecticut River’s mouth, investigating high temporal resolution DOM dynamics in a larger watershed and longer time series than previously addressed. We identified a gradient between large, saturating summer fDOM responses to discharge and linear, subdued responses during colder months. Seasonal response patterns were not consistent with multiple linear regression. Alternatively, we binned measurements across the yearly cycle using environmental indices, such as temperature, and applied moving regression, a novel approach which produced superior fits to calendar day binning. Spatially averaged watershed soil temperature at 10 cm was the best overall index of discharge-fDOM response. DOM fractionation showed fDOM was primarily a surrogate for hydrophobic organic acid (HPOA) concentrations. HPOAs were highly correlated with discharge, but hydrophilics (HPIs) were not. Discharge dependent DOM concentrations driven by the HPOA fraction may be controlled by soil temperature and water table position relative to organic and mineral soil horizons. HPI concentrations were correlated with average watershed soil temperature at 10 cm but were rather stationary throughout the year, further indicating a consistent groundwater source for this nonfluorescent DOM. We present a resolved subseasonal empirical model of DOM concentrations and fluxes, showing that riverine DOM flux and quality depend heavily on seasonal terrestrial carbon dynamics and hydrologic flow paths. High frequency monitoring reveals readily discernible patterns demonstrating that upland biogeochemical signals are maintained even at this large watershed scale.

Environmental Science and Technology↗
USGS2008

Seasonal and spatial variability in dissolved organic matter quantity and composition from the Yukon River basin, Alaska

[1] The seasonal and spatial variability of dissolved organic matter (DOM) quantity and chemical composition were investigated in the Yukon River basin of Alaska, United States, and northwestern Canada. Dissolved organic carbon (DOC), chromophoric DOM (CDOM), and dissolved lignin phenols were measured across a range of source waters and the seasonal hydrograph. Strong relationships were determined between CDOM and both DOC and lignin phenols, highlighting the potential for deriving detailed spatial and temporal distributions of DOM composition from CDOM monitoring. Maximum concentrations of measured parameters were observed during the spring flush, when DOM had a remarkably high content of aromatic vascular plant material derived from surface soil and litter layers. A larger portion of riverine DOM was attributed to vascular plant sources than previously believed by utilizing representative vegetation leachates and a soil pore water as end‐members. In combination with recent studies highlighting export of young, labile DOM during the spring flush in northern high‐latitude river systems, our results suggest riverine DOM is less degraded and more labile than previously thought with clear ramifications for its biomineralization or photo‐oxidation in marine environments.

Global Biogeochemical Cycles↗
USGS2008

Relating carbon monoxide photoproduction to dissolved organic matter functionality

Aqueous solutions of humic substances (HSs) and pure monomeric aromatics were irradiated to investigate the chemical controls upon carbon monoxide (CO) photoproduction from dissolved organic matter (DOM). HSs were isolated from lakes, rivers, marsh, and ocean. Inclusion of humic, fulvic, hydrophobic organic, and hydrophilic organic acid fractions from these environments provided samples diverse in source and isolation protocol. In spite of these major differences, HS absorption coefficients (a) and photoreactivities (a bleaching and CO production) were strongly dependent upon HS aromaticity ( r 2 >0.90; n = 11), implying aromatic moieties are the principal chromophores and photoreactants within HSs, and by extension, DOM. Carbonyl carbon and CO photoproduction were not correlated, implying that carbonyl moieties are not quantitatively important in CO photoproduction. CO photoproduction efficiency of aqueous solutions of monomeric aromatic compounds that are common constituents of organic matter varied with the nature of ring substituents. Specifically, electron donating groups increased, while electron withdrawing groups decreased CO photoproductivity, supporting our conclusion that carbonyl substituents are not quantitatively important in CO photoproduction. Significantly, aromatic CO photoproduction efficiency spanned 3 orders of magnitude, indicating that variations in the CO apparent quantum yields of natural DOM may be related to variations in aromatic DOM substituent group chemistry.

Environmental Science and Technology↗
USGS2003

Interactions between dissolved organic matter and mercury in the Florida Everglades

Experiments were conducted using organic matter isolated from various surface waters in the Florida Everglades to study the interactions between dissolved organic matter (DOM) and Hg (II). Conditional distribution coefficients ( ), obtained using an equilibriurn dialysis ligand exchange method, were strongly affected by the Hg/DOM concentration ratio. Very strong interactions ( = 10 L kg -1 ), indicative of Hg-thiol bonds, were observed at Hg/DOM ratios below approximately 1 g Hg per mg DOM. Above approximately 10 g Hg per mg DOM much lower values ( L kg -1 ) were obtained. DOM-Hg interactions were also studied by HgS (log K ) dissolution and precipitation experiments. In the dissolution experiments, a significant amount of Hg was released from cinnabar in the presence of DOM, suggesting strong interactions. Conversely, precipitation of HgS was strongly inhibited in the presence of low concentrations ( 3 mg C/L) of DOM. In both the dissolution and precipitation experiments, organic matter rich in aromatic moities was more reactive with HgS than less aromatic fractions and sulfur-containing model compounds. These results suggest that DOM can influence the geochemistry of inorganic complexes of Hg in the Everglades, especially HgS, by strong Hg-DOM binding and colloidal stabilization.

Florida↗
USGS2001

Fulvic acid-sulfide ion competition for mercury ion binding in the Florida everglades

Negatively charged functional groups of fulvic acid compete with inorganic sulfide ion for mercury ion binding. This competition is evaluated here by using a discrete site-electrostatic model to calculate mercury solution speciation in the presence of fulvic acid. Model calculated species distributions are used to estimate a mercury-fulvic acid apparent binding constant to quantify fulvic acid and sulfide ion competition for dissolved inorganic mercury (Hg(II)) ion binding. Speciation calculations done with PHREEQC, modified to use the estimated mercury-fulvic acid apparent binding constant, suggest that mercury-fulvic acid and mercury-sulfide complex concentrations are equivalent for very low sulfide ion concentrations (about 10-11 M) in Everglades' surface water. Where measurable total sulfide concentration (about 10-7 M or greater) is present in Everglades' surface water, mercury-sulfide complexes should dominate dissolved inorganic mercury solution speciation. In the absence of sulfide ion (for example, in oxygenated Everglades' surface water), fulvic acid binding should dominate Everglades' dissolved inorganic mercury speciation.

Florida↗