Geology topics

George R. Aiken

Publications and source records attributed to George R. Aiken.

At least 19 recordsLinked to original sources

USGS2023

Biogeochemical and hydrologic synergy control mercury fate in an arid land river-reservoir system

Reservoirs in arid landscapes provide critical water storage and hydroelectric power but influence the transport and biogeochemical cycling of mercury (Hg). Improved management of reservoirs to mitigate the supply and uptake of bioavailable methylmercury (MeHg) in aquatic food webs will benefit from a mechanistic understanding of inorganic divalent Hg (Hg( II )) and MeHg fate within and downstream of reservoirs. Here, we quantified Hg( II ), MeHg, and other pertinent biogeochemical constituents in water (filtered and associated with particles) at high temporal resolution from 2016–2020. This was done (1) at inflow and outflow locations of three successive hydroelectric reservoirs (Snake River, Idaho, Oregon) and (2) vertically and longitudinally within the first reservoir (Brownlee Reservoir). Under spring high flow, upstream inputs of particulate Hg (Hg( II ) and MeHg) and filter-passing Hg( II ) to Brownlee Reservoir were governed by total suspended solids and dissolved organic matter, respectively. Under redox stratified conditions in summer, net MeHg formation in the meta- and hypolimnion of Brownlee reservoir yielded elevated filter-passing and particulate MeHg concentrations, the latter exceeding 500 ng g −1 on particles. Simultaneously, the organic matter content of particulates increased longitudinally in the reservoir (from 9–29%) and temporally with stratified duration. In late summer and fall, destratification mobilized MeHg from the upgradient metalimnion and the downgradient hypolimnion of Brownlee Reservoir, respectively, resulting in downstream export of elevated filter-passing MeHg and organic-rich particles enriched in MeHg (up to 43% MeHg). We document coupled biogeochemical and hydrologic processes that yield in-reservoir MeHg accumulation and MeHg export in water and particles, which impacts MeHg uptake in aquatic food webs within and downstream of reservoirs.

Environmental Science: Processes & Impacts↗

USGS2019

Geochemical factors controlling dissolved elemental mercury and methylmercury formation in Alaskan wetlands of varying trophic status

Transformations of aqueous inorganic divalent mercury (Hg(II)i) to volatile dissolved gaseous mercury (Hg(0)(aq)) and toxic methylmercury (MeHg) governs mercury bioavailability and fate in northern ecosystems. This study quantified concentrations of aqueous mercury species (Hg(II)i, Hg(0)(aq), MeHg) and relevant geochemical constituents in pore waters of eight Alaskan wetlands that differ in trophic status (i.e., bog-to-fen gradient) to gain insight on processes controlling dark Hg(II)i reduction and Hg(II)i methylation. Regardless of wetland trophic status, positive correlations were observed between pore water Hg(II)i and dissolved organic carbon (DOC) concentrations. The concentration ratio of Hg(0)(aq) to Hg(II)i exhibited an inverse relationship to Hg(II)i concentration. A ubiquitous pathway for Hg(0)(aq) formation was not identified based on geochemical data, but we surmise that dissolved organic matter (DOM) influences mercury retention in wetland pore waters by complexing Hg(II)i and decreasing the concentration of volatile Hg(0)(aq) relative to Hg(II)i. There was no evidence of Hg(0)(aq) abundance directly limiting mercury methylation. The concentration of MeHg relative to Hg(II)i was greatest in wetlands of intermediate trophic status, and geochemical data suggest mercury methylation pathways vary between wetlands. Our insights on geochemical factors influencing aqueous mercury speciation should be considered in context of the long-term fate of mercury in northern wetlands.

Environmental Science & Technology↗

USGS2019

Evidence for conservative transport of dissolved organic carbon in major river basins in the Gulf of Maine Watershed

Transport and fate of dissolved organic carbon (DOC) in rivers are important aspects of the carbon cycle and the critical linkage between terrestrial, aquatic, and marine systems. Recent studies have quantified fluvial export to the marine environment in many systems, but in-stream losses of DOC are poorly constrained. This study compares DOC yields (kg C/ha) between the area-weighted averages of several tributaries within larger watersheds with the DOC yields of the larger watersheds to gain insight on in-stream losses in larger river systems. Four large watersheds, 22 tributaries to those watersheds, and 5 additional main stem locations in Maine were studied during 1 April to 15 November in 2011 through 2013. There were no significant differences in the area-weighted average DOC yield of the tributaries and the larger watersheds indicating little net in-stream loss in the main stems of the larger rivers. It is unlikely that inputs of DOC from un-gauged areas compensated for losses from gauged tributaries based on similarity in DOC yield longitudinally along the main stems of two of the rivers. In addition, wetland abundance, which is associated with higher DOC yield in this environment, did not consistently increase from tributaries to the larger watershed or longitudinally along the main stems. This geographic distribution of wetlands therefore also indicates that it is unlikely that inputs of DOC from un-gauged areas compensated for losses from gauged tributaries. These findings suggest that in-stream losses of DOC in these larger river systems are minimal and that the vast majority of DOC in major rivers in Maine is transported conservatively to the coastal ocean.

Maine↗

USGS2018

Dissolved organic carbon and nitrogen release from boreal Holocene permafrost and seasonally frozen soils of Alaska

Permafrost (perennially frozen) soils store vast amounts of organic carbon (C) and nitrogen (N) that are vulnerable to mobilization as dissolved organic carbon (DOC) and dissolved organic and inorganic nitrogen (DON, DIN) upon thaw. Such releases will affect the biogeochemistry of permafrost regions, yet little is known about the chemical composition and source variability of active-layer (seasonally frozen) and permafrost soil DOC, DON and DIN. We quantified DOC, total dissolved N (TDN), DON, and DIN leachate yields from deep active-layer and near-surface boreal Holocene permafrost soils in interior Alaska varying in soil C and N content and radiocarbon age to determine potential release upon thaw. Soil cores were collected at three sites distributed across the Alaska boreal region in late winter, cut in 15 cm thick sections, and deep active-layer and shallow permafrost sections were thawed and leached. Leachates were analyzed for DOC, TDN, nitrate (NO 3 − ), and ammonium (NH 4 + ) concentrations, dissolved organic matter optical properties, and DOC biodegradability. Soils were analyzed for C, N, and radiocarbon ( 14 C) content. Soil DOC, TDN, DON, and DIN yields increased linearly with soil C and N content, and decreased with increasing radiocarbon age. These relationships were significantly different for active-layer and permafrost soils such that for a given soil C or N content, or radiocarbon age, permafrost soils released more DOC and TDN (mostly as DON) per gram soil than active-layer soils. Permafrost soil DOC biodegradability was significantly correlated with soil Δ 14 C and DOM optical properties. Our results demonstrate that near-surface Holocene permafrost soils preserve greater relative potential DOC and TDN yields than overlying seasonally frozen soils that are exposed to annual leaching and decomposition. While many factors control the fate of DOC and TDN, the greater relative yields from newly thawed Holocene permafrost soils will have the largest potential impact in areas dominated by organic-rich soils.

Alaska↗

USGS2018

Comparison of the chemical composition of dissolved organic matter in three lakes in Minnesota

New information on the chemical composition of dissolved organic matter (DOM) in three lakes in Minnesota has been gained from spectral editing and two-dimensional nuclear magnetic resonance (NMR) methods, indicating the effects of lake hydrological settings on DOM composition. Williams Lake (WL), Shingobee Lake (SL), and Manganika Lake (ML) had different source inputs, and the lake water residence time (WRT) of WL was markedly longer than that of SL and ML. The hydrophobic organic acid (HPOA) and transphilic organic acid (TPIA) fractions combined comprised >50% of total DOM in these lakes, and contained carboxyl-rich alicyclic molecules (CRAM), aromatics, carbohydrates, and N-containing compounds. The previously understudied TPIA fractions contained fewer aromatics, more oxygen-rich CRAM, and more N-containing compounds compared to the corresponding HPOA. CRAM represented the predominant component in DOM from all lakes studied, and more so in WL than in SL and ML. Aromatics including lignin residues and phenols decreased in relative abundances from ML to SL and WL. Carbohydrates and N-containing compounds were minor components in both HPOA and TPIA and did not show large variations among the three lakes. The increased relative abundances of CRAM in DOM from ML, SL to WL suggested the selective preservation of CRAM with increased residence time.

Minnesota↗

USGS2018

Permafrost stores a globally significant amount of mercury

Changing climate in northern regions is causing permafrost to thaw with major implications for the global mercury (Hg) cycle. We estimated Hg in permafrost regions based on in situ measurements of sediment total mercury (STHg), soil organic carbon (SOC), and the Hg to carbon ratio (R HgC ) combined with maps of soil carbon. We measured a median STHg of 43 ± 30 ng Hg g soil −1 and a median R HgC of 1.6 ± 0.9 μg Hg g C −1 , consistent with published results of STHg for tundra soils and 11,000 measurements from 4,926 temperate, nonpermafrost sites in North America and Eurasia. We estimate that the Northern Hemisphere permafrost regions contain 1,656 ± 962 Gg Hg, of which 793 ± 461 Gg Hg is frozen in permafrost. Permafrost soils store nearly twice as much Hg as all other soils, the ocean, and the atmosphere combined, and this Hg is vulnerable to release as permafrost thaws over the next century. Existing estimates greatly underestimate Hg in permafrost soils, indicating a need to reevaluate the role of the Arctic regions in the global Hg cycle.

Geophysical Research Letters↗

USGS2018

Unifying concepts linking dissolved organic matter composition to persistence in aquatic ecosystems

The link between composition and reactivity of dissolved organic matter (DOM) is central to understanding the role aquatic systems play in the global carbon cycle; yet, unifying concepts driving molecular composition have yet to be established. We characterized 37 DOM isolates from diverse aquatic ecosystems, including their stable and radiocarbon isotopes (δ 13 C-dissolved organic carbon (DOC) and Δ 14 C-DOC), optical properties (absorbance and fluorescence), and molecular composition (ultrahigh resolution mass spectrometry). Isolates encompassed end-members of allochthonous and autochthonous DOM from sites across the United States, the Pacific Ocean, and Antarctic lakes. Modern Δ 14 C-DOC and optical properties reflecting increased aromaticity, such as carbon specific UV absorbance at 254 nm (SUVA 254 ), were directly related to polyphenolic and polycyclic aromatic compounds, whereas enriched δ 13 C-DOC and optical properties reflecting autochthonous end-members were positively correlated to more aliphatic compounds. Furthermore, the two sets of autochthonous end-members (Pacific Ocean and Antarctic lakes) exhibited distinct molecular composition due to differences in extent of degradation. Across all sites and end-members studied, we find a consistent shift in composition with aging, highlighting the persistence of certain biomolecules concurrent with degradation time.

Environmental Science & Technology↗

USGS2018

Evidence for major input of riverine organic matter into the ocean

The changes in the structure of XAD-8 isolated dissolved organic matter (DOM) samples along a river (Penobscot River) to estuary (Penobscot Bay) to ocean (across the Gulf of Maine) transect and from the Pacific Ocean were investigated using selective and two dimensional (2D) nuclear magnetic resonance (NMR) spectroscopy coupled with elemental and carbon isotope analysis. The results provide important insights into the nature of relatively stable structures in the river-to-ocean continuum and the enigma of the fate of terrestrial DOM in the marine system. First, lignin and carboxyl-rich alicyclic molecules (CRAMs), which are indistinguishable from mass spectrometry, were clearly differentiated with NMR spectroscopy. NMR unambiguously showed that CRAMs persisted along the river-to-ocean transect and in the Pacific Ocean, while lignin residues dramatically decreased in abundance from the river to the coastal ocean and the Pacific Ocean. The results challenge a previous conclusion that lignin-derived compounds are refractory and can accumulate in the coastal ocean. The loss of terrestrial plant-derived aromatic compounds such as lignin and tannin residues throughout the sequence of riverine, coastal, and open ocean DOM extracts could also partially explain the decreasing organic carbon recovery by XAD-8 isolation and the change in carbon stable isotope composition from riverine DOM (δ 13 C −27.6‰) to ocean DOM (δ 13 C −23.0‰) extracts. The observation, from advanced NMR, of similar CRAM molecules in XAD-8 isolated DOM samples from the Penobscot River to the Penobscot Bay and from the ocean refutes a previous conclusion that XAD-isolated DOM samples from seawater and river are distinctly different. The alicyclic structural features of CRAMs and their presence as the major structural units in DOM extracts from the Penobscot River to Gulf of Maine transect, together with the deduced old 14 C age of CRAMs in the ocean, imply that terrestrial CRAMs may persist on timescales long enough to be transported into the ocean.

Organic Geochemistry↗

USGS2017

High pressure size exclusion chromatography (HPSEC) determination of dissolved organic matter molecular weight revisited: Accounting for changes in stationary phases, analytical standards, and isolation methods

We reassessed the molecular weight of dissolved organic matter (DOM) determined by high pressure size exclusion chromatography (HPSEC) using measurements made with different columns and various generations of polystyrenesulfonate (PSS) molecular weight standards. Molecular weight measurements made with a newer generation HPSEC column and PSS standards from more recent lots are roughly 200 to 400 Da lower than initial measurements made in the early 1990s. These updated numbers match DOM molecular weights measured by colligative methods and fall within a range of values calculated from hydroxyl radical kinetics. These changes suggest improved accuracy of HPSEC molecular weight measurements that we attribute to improved accuracy of PSS standards and changes in the column packing. We also isolated DOM from wetlands in the Prairie Pothole Region (PPR) using XAD-8, a cation exchange resin, and PPL, a styrene-divinylbenzene media, and observed little difference in molecular weight and specific UV absorbance at 280 nm (SUVA 280 ) between the two solid phase extraction resins, suggesting they capture similar DOM moieties. PPR DOM also showed lower SUVA 280 at similar weights compared to DOM isolates from a global range of environments, which we attribute to oxidized sulfur in PPR DOM that would increase molecular weight without affecting SUVA 280 .

Environmental Science & Technology↗

USGS2017

Organic chemical characterization and mass balance of a hydraulically fractured well: From fracturing fluid to produced water over 405 days

A long-term field study (405 days) of a hydraulically fractured well from the Niobrara Formation in the Denver-Julesburg Basin was completed. Characterization of organic chemicals used in hydraulic fracturing and their changes through time, from the preinjected fracturing fluid to the produced water, was conducted. The characterization consisted of a mass balance by dissolved organic carbon (DOC), volatile organic analysis by gas chromatography/mass spectrometry, and nonvolatile organic analysis by liquid chromatography/mass spectrometry. DOC decreased from 1500 mg/L in initial flowback to 200 mg/L in the final produced water. Only ∼11% of the injected DOC returned by the end of the study, with this 11% representing a maximum fraction returned since the formation itself contributes DOC. Furthermore, the majority of returning DOC was of the hydrophilic fraction (60–85%). Volatile organic compound analysis revealed substantial concentrations of individual BTEX compounds (0.1–11 mg/L) over the 405-day study. Nonvolatile organic compounds identified were polyethylene glycols (PEGs), polypropylene glycols (PPG), linear alkyl-ethoxylates, and triisopropanolamine (TIPA). The distribution of PEGs, PPGs, and TIPA and their ubiquitous presence in our samples and the literature illustrate their potential as organic tracers for treatment operations or in the event of an environmental spill.

Environmental Science & Technology↗

USGS2017

Effects of sulfide concentration and dissolved organic matter characteristics on the structure of nanocolloidal metacinnabar

Understanding the speciation of divalent mercury (Hg(II)) in aquatic systems containing dissolved organic matter (DOM) and sulfide is necessary to predict the conversion of Hg(II) to bioavailable methylmercury. We used X-ray absorption spectroscopy to characterize the structural order of mercury in Hg(II)–DOM–sulfide systems for a range of sulfide concentration (1–100 μM), DOM aromaticity (specific ultraviolet absorbance (SUVA 254 )), and Hg(II)–DOM and Hg(II)–DOM–sulfide equilibration times (4–142 h). In all systems, Hg(II) was present as structurally disordered nanocolloidal metacinnabar (β-HgS). β-HgS nanocolloids were significantly smaller or less ordered at lower sulfide concentration, as indicated by under-coordination of Hg(II) in β-HgS. The size or structural order of β-HgS nanocolloids increased with increasing sulfide abundance and decreased with increasing SUVA 254 of the DOM. The Hg(II)–DOM or Hg(II)–DOM–sulfide equilibration times did not significantly influence the extent of structural order in nanocolloidal β-HgS. Geochemical factors that control the structural order of nanocolloidal β-HgS, which are expected to influence nanocolloid surface reactivity and solubility, should be considered in the context of mercury bioavailability.

Environmental Science & Technology↗

USGS2017

Biological and land use controls on the isotopic composition of aquatic carbon in the Upper Mississippi River Basin

Riverine ecosystems receive organic matter (OM) from terrestrial sources, internally produce new OM, and biogeochemically cycle and modify organic and inorganic carbon. Major gaps remain in the understanding of the relationships between carbon sources and processing in river systems. Here we synthesize isotopic, elemental, and molecular properties of dissolved organic carbon (DOC), particulate organic carbon (POC), and dissolved inorganic carbon (DIC) in the Upper Mississippi River (UMR) system above Wabasha, MN, including the main stem Mississippi River and its four major tributaries (Minnesota, upper Mississippi, St. Croix, and Chippewa Rivers). Our goal was to elucidate how biological processing modifies the chemical and isotopic composition of aquatic carbon pools during transport downstream in a large river system with natural and man-made impoundments. Relationships between land cover and DOC carbon-isotope composition, absorbance, and hydrophobic acid content indicate that DOC retains terrestrial carbon source information, while the terrestrial POC signal is largely replaced by autochthonous organic matter, and DIC integrates the influence of in-stream photosynthesis and respiration of organic matter. The UMR is slightly heterotrophic throughout the year, but pools formed by low-head navigation dams and natural impoundments promote a shift towards autotrophic conditions, altering aquatic ecosystem dynamics and POC and DIC composition. Such changes likely occur in all major river systems affected by low-head dams and need to be incorporated into our understanding of inland water carbon dynamics and processes controlling CO 2 emissions from rivers, as new navigation and flood control systems are planned for future river and water resources management.

Upper Mississippi River Basin↗

USGS2017

Spatial dependence of reduced sulfur in Everglades dissolved organic matter controlled by sulfate enrichment

Sulfate inputs to the Florida Everglades stimulate sulfidic conditions in freshwater wetland sediments that affect ecological and biogeochemical processes. An unexplored implication of sulfate enrichment is alteration of the content and speciation of sulfur in dissolved organic matter (DOM), which influences the reactivity of DOM with trace metals. Here, we describe the vertical and lateral spatial dependence of sulfur chemistry in the hydrophobic organic acid fraction of DOM from unimpacted and sulfate-impacted Everglades wetlands using X-ray absorption spectroscopy and ultrahigh-resolution mass spectrometry. Spatial variation in DOM sulfur content and speciation reflects the degree of sulfate enrichment and resulting sulfide concentrations in sediment pore waters. Sulfur is incorporated into DOM predominantly as highly reduced species in sulfidic pore waters. Sulfur-enriched DOM in sediment pore waters exchanges with overlying surface waters and the sulfur likely undergoes oxidative transformations in the water column. Across all wetland sites and depths, the total sulfur content of DOM correlated with the relative abundance of highly reduced sulfur functionality. The results identify sulfate input as a primary determinant on DOM sulfur chemistry to be considered in the context of wetland restoration and sulfur and trace metal cycling.

Florida↗

USGS2017

Relative contributions of copper oxide nanoparticles and dissolved copper to Cu uptake kinetics of Gulf killifish (Fundulus grandis) embryos

The toxicity of soluble metal-based nanomaterials may be due to the uptake of metals in both dissolved and nanoparticulate forms, but the relative contributions of these different forms to overall metal uptake rates under environmental conditions are not quantitatively defined. Here, we investigated the linkage between the dissolution rates of copper(II) oxide (CuO) nanoparticles (NPs) and their bioavailability to Gulf killifish ( Fundulus grandis ) embryos, with the aim of quantitatively delineating the relative contributions of nanoparticulate and dissolved species for Cu uptake. Gulf killifish embryos were exposed to dissolved Cu and CuO NP mixtures comprising a range of pH values (6.3–7.5) and three types of natural organic matter (NOM) isolates at various concentrations (0.1–10 mg-C L –1 ), resulting in a wide range of CuO NP dissolution rates that subsequently influenced Cu uptake. First-order dissolution rate constants of CuO NPs increased with increasing NOM concentration and for NOM isolates with higher aromaticity, as indicated by specific ultraviolet absorbance (SUVA), while Cu uptake rate constants of both dissolved Cu and CuO NP decreased with NOM concentration and aromaticity. As a result, the relative contribution of dissolved Cu and nanoparticulate CuO species for the overall Cu uptake rate was insensitive to NOM type or concentration but largely determined by the percentage of CuO that dissolved. These findings highlight SUVA and aromaticity as key NOM properties affecting the dissolution kinetics and bioavailability of soluble metal-based nanomaterials in organic-rich waters. These properties could be used in the incorporation of dissolution kinetics into predictive models for environmental risks of nanomaterials.

Environmental Science & Technology↗

USGS2017

Mobilization of mercury and arsenic from a carbonate-hosted ore deposit, central Idaho, U.S.A.

The Cinnabar and Fern mine sites in central Idaho are primary source areas for elevated mercury and arsenic entering the South Fork of the Salmon River, which provides critical spawning habitat for bull trout and Chinook salmon. Mercury mineralization is hosted by carbonate rocks, which generate waters dominated by Ca2+ and HCO3 - at pH 7 to 9. A synoptic sampling was conducted on headwater tributaries to determine geologic background concentrations and quantify trace metal concentrations in stream water associated with historical mining. Geologic background concentrations in unfiltered Cinnabar Creek water were 8 - 14 ng Hg L-1 and 4.8 - 9.5 µg As L-1. Immediately downstream from the mine site, concentrations increased to 257 ng Hg L-1 and 20.6 µg As L-1. Groundwater inflow diluted these concentrations by approximately half before the confluence of Cinnabar Creek with Sugar Creek. As expected, mercury and arsenic concentrations increased downstream in Sugar Creek below the confluence with Cinnabar Creek. However, the final downstream reach on Sugar Creek showed an increase in unfiltered mercury, methylmercury, and iron concentrations relative to the upstream reach. This increase is associated with historical mining activity in a mineralized area of carbonate rock that intersects the reach.

Idaho↗

USGS2016

Dissolved organic matter composition of Arctic rivers: Linking permafrost and parent material to riverine carbon

Recent climate change in the Arctic is driving permafrost thaw, which has important implications for regional hydrology and global carbon dynamics. Permafrost is an important control on groundwater dynamics and the amount and chemical composition of dissolved organic matter (DOM) transported by high-latitude rivers. The consequences of permafrost thaw for riverine DOM dynamics will likely vary across space and time, due in part to spatial variation in ecosystem properties in Arctic watersheds. Here we examined watershed controls on DOM composition in 69 streams and rivers draining heterogeneous landscapes across a broad region of Arctic Alaska. We characterized DOM using bulk dissolved organic carbon (DOC) concentration, optical properties, and chemical fractionation and classified watersheds based on permafrost characteristics (mapping of parent material and ground ice content, modeling of thermal state) and ecotypes. Parent material and ground ice content significantly affected the amount and composition of DOM. DOC concentrations were higher in watersheds underlain by fine-grained loess compared to watersheds underlain by coarse-grained sand or shallow bedrock. DOC concentration was also higher in rivers draining ice-rich landscapes compared to rivers draining ice-poor landscapes. Similarly, specific ultraviolet absorbance (SUVA 254 , an index of DOM aromaticity) values were highest in watersheds underlain by fine-grained deposits or ice-rich permafrost. We also observed differences in hydrophobic organic acids, hydrophilic compounds, and DOM fluorescence across watersheds. Both DOC concentration and SUVA 254 were negatively correlated with watershed active layer thickness, as determined by high-resolution permafrost modeling. Together, these findings highlight how spatial variations in permafrost physical and thermal properties can influence riverine DOM.

Global Biogeochemical Cycles↗

USGS2016

Spatial and temporal patterns of dissolved organic matter quantity and quality in the Mississippi River Basin, 1997–2013

Recent studies have found insignificant or decreasing trends in time-series dissolved organic carbon (DOC) datasets, questioning the assumption that long-term DOC concentrations in surface waters are increasing in response to anthropogenic forcing, including climate change, land use, and atmospheric acid deposition. We used the weighted regressions on time, discharge, and season (WRTDS) model to estimate annual flow-normalized concentrations and fluxes to determine if changes in DOC quantity and quality signal anthropogenic forcing at 10 locations in the Mississippi River Basin. Despite increases in agriculture and urban development throughout the basin, net increases in DOC concentration and flux were significant at only 3 of 10 sites from 1997 to 2013 and ranged between −3.5% to +18% and −0.1 to 19%, respectively. Positive shifts in DOC quality, characterized by increasing specific ultraviolet absorbance at 254 nm, ranged between +8% and +45%, but only occurred at one of the sites with significant DOC quantity increases. Basinwide reductions in atmospheric sulfate deposition did not result in large increases in DOC either, likely because of the high buffering capacity of the soil. Hydroclimatic factors including annual discharge, precipitation, and temperature did not significantly change during the 17-year timespan of this study, which contrasts with results from previous studies showing significant increases in precipitation and discharge over a century time scale. Our study also contrasts with those from smaller catchments, which have shown stronger DOC responses to climate, land use, and acidic deposition. This temporal and spatial analysis indicated that there was a potential change in DOC sources in the Mississippi River Basin between 1997 and 2013. However, the overall magnitude of DOC trends was not large, and the pattern in quantity and quality increases for the 10 study sites was not consistent throughout the basin.

Hydrological Processes↗

USGS2016

Climate change and dissolved organic carbon export to the Gulf of Maine

Ongoing climate change is affecting the concentration, export (flux), and timing of dissolved organic carbon (DOC) exported to the Gulf of Maine (GoM) through changes in hydrologic regime. DOC export was calculated for water years 1950 through 2013 for 20 rivers and for water years 1930 through 2013 for 14 rivers draining to the GoM. DOC export was also estimated for the 21st century based on climate and hydrologic modeling in a previously published study. DOC export was calculated by using the regression model LOADEST to fit seasonally adjusted concentration discharge (C-Q) relations. Our results are an analysis of the sensitivity of DOC export to changes in hydrologic conditions over time since land cover and vegetation were held constant over time. Despite large interannual variability, all rivers had increasing DOC export during winter and these trends were significant ( p < 0.05) in 10 out of 20 rivers for 1950 to 2013 and in 13 out of 14 rivers for 1930 to 2013. All rivers also had increasing annual export of DOC although fewer trends were statistically significant than for winter export. Projections for DOC export during the 21st century were variable depending on the climate model and greenhouse gas emission scenario that affected future river discharge through effects on precipitation and evapotranspiration. The most consistent result was a significant increase in DOC export in winter in all model-by-emission scenarios. DOC export was projected to decrease during the summer in all model-by-emission scenarios, with statistically significant decreases in half of the scenarios.

Maine↗