Title: How humans alter dissolved organic matter composition in freshwater: relevance for the Earth’s biogeochemistry
Abstract Dissolved organic matter (DOM) is recognized for its importance in freshwater ecosystems, but historical reliance on DOM quantity rather than indicators of DOM composition has led to an incomplete understanding of DOM and an underestimation of its role and importance in biogeochemical processes. A single sample of DOM can be composed of tens of thousands of distinct molecules. Each of these unique DOM molecules has their own chemical properties and reactivity or role in the environment. Human activities can modify DOM composition and recent research has uncovered distinct DOM pools laced with human markers and footprints. Here we review how land use change, climate change, nutrient pollution, browning, wildfires, and dams can change DOM composition which in turn will affect internal processing of freshwater DOM. We then describe how human-modified DOM can affect biogeochemical processes. Drought, wildfires, cultivated land use, eutrophication, climate change driven permafrost thaw, and other human stressors can shift the composition of DOM in freshwater ecosystems increasing the relative contribution of microbial-like and aliphatic components. In contrast, increases in precipitation may shift DOM towards more relatively humic-rich, allochthonous forms of DOM. These shifts in DOM pools will likely have highly contrasting effects on carbon outgassing and more »
burial, nutrient cycles, ecosystem metabolism, metal toxicity, and the treatments needed to produce clean drinking water. A deeper understanding of the links between the chemical properties of DOM and biogeochemical dynamics can help to address important future environmental issues, such as the transfer of organic contaminants through food webs, alterations to nitrogen cycling, impacts on drinking water quality, and biogeochemical effects of global climate change. « less
Kaushal, Sujay S.; Likens, Gene E.; Pace, Michael L.; Reimer, Jenna E.; Maas, Carly M.; Galella, Joseph G.; Utz, Ryan M.; Duan, Shuiwang; Kryger, Julia R.; Yaculak, Alexis M.; et al(
, Biogeochemistry)
null
(Ed.)
Abstract Freshwater salinization is an emerging global problem impacting safe drinking water, ecosystem health and biodiversity, infrastructure corrosion, and food production. Freshwater salinization originates from diverse anthropogenic and geologic sources including road salts, human-accelerated weathering, sewage, urban construction, fertilizer, mine drainage, resource extraction, water softeners, saltwater intrusion, and evaporative concentration of ions due to hydrologic alterations and climate change. The complex interrelationships between salt ions and chemical, biological, and geologic parameters and consequences on the natural, social, and built environment are called Freshwater Salinization Syndrome (FSS). Here, we provide a comprehensive overview of salinization issues (past, present, and future), and we investigate drivers and solutions. We analyze the expanding global magnitude and scope of FSS including its discovery in humid regions, connections to human-accelerated weathering and mobilization of ‘chemical cocktails.’ We also present data illustrating: (1) increasing trends in salt ion concentrations in some of the world’s major freshwaters, including critical drinking water supplies; (2) decreasing trends in nutrient concentrations in rivers due to regulations but increasing trends in salinization, which have been due to lack of adequate management and regulations; (3) regional trends in atmospheric deposition of salt ions and storage of salt ions in soils and groundwater, andmore »(4) applications of specific conductance as a proxy for tracking sources and concentrations of groups of elements in freshwaters. We prioritize FSS research needs related to better understanding: (1) effects of saltwater intrusion on ecosystem processes, (2) potential health risks from groundwater contamination of home wells, (3) potential risks to clean and safe drinking water sources, (4) economic and safety impacts of infrastructure corrosion, (5) alteration of biodiversity and ecosystem functions, and (6) application of high-frequency sensors in state-of-the art monitoring and management. We evaluate management solutions using a watershed approach spanning air, land, and water to explore variations in sources, fate and transport of different salt ions ( e.g. monitoring of atmospheric deposition of ions, stormwater management, groundwater remediation, and managing road runoff). We also identify tradeoffs in management approaches such as unanticipated retention and release of chemical cocktails from urban stormwater management best management practices (BMPs) and unintended consequences of alternative deicers on water quality. Overall, we show that FSS has direct and indirect effects on mobilization of diverse chemical cocktails of ions, metals, nutrients, organics, and radionuclides in freshwaters with mounting impacts. Our comprehensive review suggests what could happen if FSS were not managed into the future and evaluates strategies for reducing increasing risks to clean and safe drinking water, human health, costly infrastructure, biodiversity, and critical ecosystem services.« less
Yancey, Colleen E.; Smith, Derek J.; Den Uyl, Paul A.; Mohamed, Osama G.; Yu, Fengan; Ruberg, Steven A.; Chaffin, Justin D.; Goodwin, Kelly D.; Tripathi, Ashootosh; Sherman, David H.; et al(
, Applied and Environmental Microbiology)
Rudi, Knut
(Ed.)
ABSTRACT Cyanobacterial harmful algal blooms (cyanoHABs) degrade freshwater ecosystems globally. Microcystis aeruginosa often dominates cyanoHABs and produces microcystin (MC), a class of hepatotoxins that poses threats to human and animal health. Microcystin toxicity is influenced by distinct structural elements across a diversity of related molecules encoded by variant mcy operons. However, the composition and distribution of mcy operon variants in natural blooms remain poorly understood. Here, we characterized the variant composition of mcy genes in western Lake Erie Microcystis blooms from 2014 and 2018. Sampling was conducted across several spatial and temporal scales, including different bloom phases within 2014, extensive spatial coverage on the same day (2018), and frequent, autonomous sampling over a 2-week period (2018). Mapping of metagenomic and metatranscriptomic sequences to reference sequences revealed three Microcystis mcy genotypes: complete (all genes present [ mcyA–J ]), partial (truncated mcyA , complete mcyBC , and missing mcyD–J ), and absent (no mcy genes). We also detected two different variants of mcyB that may influence the production of microcystin congeners. The relative abundance of these genotypes was correlated with pH and nitrate concentrations. Metatranscriptomic analysis revealed that partial operons were, at times, the most abundant genotype and expressed in situ ,more »suggesting the potential biosynthesis of truncated products. Quantification of genetic divergence between genotypes suggests that the observed strains are the result of preexisting heterogeneity rather than de novo mutation during the sampling period. Overall, our results show that natural Microcystis populations contain several cooccurring mcy genotypes that dynamically shift in abundance spatiotemporally via strain succession and likely influence the observed diversity of the produced congeners. IMPORTANCE Cyanobacteria are responsible for producing microcystins (MCs), a class of potent and structurally diverse toxins, in freshwater systems around the world. While microcystins have been studied for over 50 years, the diversity of their chemical forms and how this variation is encoded at the genetic level remain poorly understood, especially within natural populations of cyanobacterial harmful algal blooms (cyanoHABs). Here, we leverage community DNA and RNA sequences to track shifts in mcy genes responsible for producing microcystin, uncovering the relative abundance, expression, and variation of these genes. We studied this phenomenon in western Lake Erie, which suffers annually from cyanoHAB events, with impacts on drinking water, recreation, tourism, and commercial fishing.« less
Streams in the southeastern United States Coastal Plains serve as an essential source of energy and nutrients for important estuarine ecosystems, and dissolved organic matter (DOM) exported from these streams can have profound impacts on the biogeochemical and ecological functions of fluvial networks. Here, we examined hydrological and temperature controls of DOM during low-flow periods from a forested stream located within the Coastal Plain physiographic region of Alabama, USA. We analyzed DOM via combining dissolved organic carbon (DOC) analysis, fluorescence excitation–emission matrix combined with parallel factor analysis (EEM-PARAFAC), and microbial degradation experiments. Four fluorescence components were identified: terrestrial humic-like DOM, microbial humic-like DOM, tyrosine-like DOM, and tryptophan-like DOM. Humic-like DOM accounted for ~70% of total fluorescence, and biodegradation experiments showed that it was less bioreactive than protein-like DOM that accounted for ~30% of total fluorescence. This observation indicates fluorescent DOM (FDOM) was controlled primarily by soil inputs and not substantially influenced by instream production and processing, suggesting that the bulk of FDOM in these streams is transported to downstream environments with limited in situ modification. Linear regression and redundancy analysis models identified that the seasonal variations in DOM were dictated primarily by hydrology and temperature. Overall, high discharge and shallowmore »flow paths led to the enrichment of less-degraded DOM with higher percentages of microbial humic-like and tyrosine-like compounds, whereas high temperatures favored the accumulation of high-aromaticity, high-molecular-weight, terrestrial, humic-like compounds in stream water. The flux of DOC and four fluorescence components was driven primarily by water discharge. Thus, the instantaneous exports of both refractory humic-like DOM and reactive protein-like DOM were higher in wetter seasons (winter and spring). As high temperatures and severe precipitation are projected to become more prominent in the southeastern U.S. due to climate change, our findings have important implications for future changes in the amount, source, and composition of DOM in Coastal Plain streams and the associated impacts on downstream carbon and nutrient supplies and water quality.« less
Hounshell, Alexandria G.; Fegley, Stephen R.; Hall, Nathan S.; Osburn, Christopher L.; Paerl, Hans W.(
, Estuaries and Coasts)
Estuaries function as important transporters, transformers, and producers of organic matter (OM). Along the freshwater to saltwater gradient, the composition of OM is influenced by physical and biogeochemical processes that change spatially and temporally, making it difficult to constrain OM in these ecosystems. In addition, many of the environmental parameters (temperature, precipitation, riverine discharge) controlling OM are expected to change due to climate change. To better understand the environmental drivers of OM quantity (concentration) and quality (absorbance, fluorescence), we assessed both dissolved OM (DOM) and particulate OM (POM) spatially, along the freshwater to saltwater gradient and temporally, for a full year. We found seasonal differences in salinity throughout the estuary due to elevated riverine discharge during the late fall to early spring, with corresponding changes to OM quantity and quality. Using redundancy analysis, we found DOM covaried with salinity (adjusted r2 = 0.35, 0.41 for surface and bottom), indicating terrestrial sources of DOM in riverine discharge were the dominant DOM sources throughout the estuary, while POM covaried with environmental indictors of terrestrial sources (turbidity, adjusted r2 = 0.16, 0.23 for surface and bottom) as well as phytoplankton biomass (chlorophyll-a, adjusted r2 = 0.25, 0.14 for surface and bottom). Responses inmore »OM quantity and quality observed during the period of elevated discharge were similar to studies assessing OM quality following extreme storm events suggesting that regional changes in precipitation, as predicted by climate change, will be as important in changing the estuarine OM pool as episodic storm events in the future.« less
Rodríguez-Cardona, B. M.; Coble, A. A.; Wymore, A. S.; Kolosov, R.; Podgorski, D. C.; Zito, P.; Spencer, R. G. M.; Prokushkin, A. S.; McDowell, W. H.(
, Scientific Reports)
Abstract
The Central Siberian Plateau is undergoing rapid climate change that has resulted in increased frequency of forest fires and subsequent alteration of watershed carbon and nutrient dynamics. Across a watershed chronosequence (3 to >100 years since wildfire) we quantified the effects of fire on quantity and composition of dissolved organic matter (DOM), stream water nutrient concentrations, as well as in-stream nutrient uptake. Wildfires increased concentrations of nitrate for a decade, while decreasing concentrations of dissolved organic carbon and nitrogen (DOC and DON) and aliphatic DOM contribution for five decades. These post-wildfire changes in stream DOM result in lower uptake efficiency of in-stream nitrate in recently burned watersheds. Nitrate uptake (as uptake velocity) is strongly dependent on DOM composition (e.g. polyphenolics), ambient dissolved inorganic nitrogen (DIN), and DOC to DIN ratios. Our observations and experiments suggest that a decade-long pulse of inorganic nitrogen and a reduction of DOC export occur following wildfires in streams draining the Central Siberian Plateau. Increased fire frequency in the region is thus likely to both decrease DOM and increase nitrate delivery to the main stem Yenisei River, and ultimately the Arctic Ocean, in the coming decades.
Xenopoulos, Marguerite A., Barnes, Rebecca T., Boodoo, Kyle S., Butman, David, Catalán, Núria, D’Amario, Sarah C., Fasching, Christina, Kothawala, Dolly N., Pisani, Oliva, Solomon, Christopher T., Spencer, Robert G., Williams, Clayton J., and Wilson, Henry F.. How humans alter dissolved organic matter composition in freshwater: relevance for the Earth’s biogeochemistry. Retrieved from https://par.nsf.gov/biblio/10221574. Biogeochemistry . Web. doi:10.1007/s10533-021-00753-3.
Xenopoulos, Marguerite A., Barnes, Rebecca T., Boodoo, Kyle S., Butman, David, Catalán, Núria, D’Amario, Sarah C., Fasching, Christina, Kothawala, Dolly N., Pisani, Oliva, Solomon, Christopher T., Spencer, Robert G., Williams, Clayton J., and Wilson, Henry F..
"How humans alter dissolved organic matter composition in freshwater: relevance for the Earth’s biogeochemistry". Biogeochemistry (). Country unknown/Code not available. https://doi.org/10.1007/s10533-021-00753-3.https://par.nsf.gov/biblio/10221574.
@article{osti_10221574,
place = {Country unknown/Code not available},
title = {How humans alter dissolved organic matter composition in freshwater: relevance for the Earth’s biogeochemistry},
url = {https://par.nsf.gov/biblio/10221574},
DOI = {10.1007/s10533-021-00753-3},
abstractNote = {Abstract Dissolved organic matter (DOM) is recognized for its importance in freshwater ecosystems, but historical reliance on DOM quantity rather than indicators of DOM composition has led to an incomplete understanding of DOM and an underestimation of its role and importance in biogeochemical processes. A single sample of DOM can be composed of tens of thousands of distinct molecules. Each of these unique DOM molecules has their own chemical properties and reactivity or role in the environment. Human activities can modify DOM composition and recent research has uncovered distinct DOM pools laced with human markers and footprints. Here we review how land use change, climate change, nutrient pollution, browning, wildfires, and dams can change DOM composition which in turn will affect internal processing of freshwater DOM. We then describe how human-modified DOM can affect biogeochemical processes. Drought, wildfires, cultivated land use, eutrophication, climate change driven permafrost thaw, and other human stressors can shift the composition of DOM in freshwater ecosystems increasing the relative contribution of microbial-like and aliphatic components. In contrast, increases in precipitation may shift DOM towards more relatively humic-rich, allochthonous forms of DOM. These shifts in DOM pools will likely have highly contrasting effects on carbon outgassing and burial, nutrient cycles, ecosystem metabolism, metal toxicity, and the treatments needed to produce clean drinking water. A deeper understanding of the links between the chemical properties of DOM and biogeochemical dynamics can help to address important future environmental issues, such as the transfer of organic contaminants through food webs, alterations to nitrogen cycling, impacts on drinking water quality, and biogeochemical effects of global climate change.},
journal = {Biogeochemistry},
author = {Xenopoulos, Marguerite A. and Barnes, Rebecca T. and Boodoo, Kyle S. and Butman, David and Catalán, Núria and D’Amario, Sarah C. and Fasching, Christina and Kothawala, Dolly N. and Pisani, Oliva and Solomon, Christopher T. and Spencer, Robert G. and Williams, Clayton J. and Wilson, Henry F.},
}
