Search

Plastics have become ubiquitous in the modern consumer economy. Unchecked production, failure to implement efficient recycling practices, and poorly defined global policy regarding production and disposal has led to a prevalent plastic problem. Over the past decade, microplastic pollution has emerged as a forefront concern of plastic in the global environment. As marine microplastic pollution becomes a predominant area of interest, it is important to understand microplastic sources, delivery pathways, and ultimate fate. Estuaries are key zones to monitor for microplastic pollution, due to their close proximity to source areas, and their natural ability to filter pollutants. The Galveston Bay watershed is located near the densely populated Houston, TX metro area and manufactures potentially half of the United States’ pre-production plastics. Using a Lagrangian particle-tracking method coupled with a validated 3D hydrodynamic model, we examined the transport behavior of microplastics, as well as export ability of the Galveston Bay estuary. Accounting for the variability of type and density of microplastics, multiple settling velocities were simulated to examine their effect on behavior. Four release sites were chosen near highly populated river connections. We found that settling velocity has significant impact on both local exposure time and retention time. Neutrally buoyant particles were flushed quickly out of the bay, while heavier particles migrated westward and spent far more time in the bay overall. Release location influenced percent of particles retained in bay, with a higher percent of particles still present from northern release locations than southern release locations after two years of simulation. The use of modelling studies to provide successful estimation of microplastic transport pathways and export efficiency of Galveston Bay will help contribute to a more robust understanding of microplastic behavior within estuarine environments.

The fate of soil organic carbon (SOC) in boreal forests is dependent on the integrative ecosystem response to climate change. For example, boreal forest productivity is often nitrogen (N) limited, and climate warming can enhance N cycling and primary productivity. However, the net effect of this feedback on the SOC reservoir and its longevity with climate change remain unclear due to difficulty in detecting small differences between large and variable carbon (C) fluxes needed to determine net changes in soil reservoirs. The diagenetic state of SOC – resulting from the physicochemical and biological transformations that alter the original biomolecular composition of detrital inputs to soil over time – is useful for tracing the net response of SOC at the timescales relevant to climate change not usually discernible from fluxes and stocks alone. Here, we test two hypotheses using a mesic boreal forest climate transect: (1) the SOC diagenetic state is maintained across this climosequence, and (2) the maintenance of the SOC diagenetic state is a consequence of coupled soil C and N cycling, signifying the role of enhanced N cycling supporting SOC inputs that maintain SOC stocks within the warmer-climate forests. Shifts in nonvascular to vascular plant inputs with climate observed in these and other boreal forests highlighted the need to carefully separate biogeochemical indicators of SOC source from those signifying diagenetic alteration. We thus evaluated and applied lignin biomarkers to assess the diagenetic alteration of SOC in these boreal forest organic soils and directly compared the lignin diagenetic state with that of soil organic nitrogen (SON) assessed through amino acid composition. The lignin diagenetic state remained constant across the climate transect, indicating a balance between the input and removal of lignin in these mesic boreal forests. When combined with previous knowledge of these forest ecosystems, including the diagenetic state of SON and direct measures of C fluxes and stocks, the results indicate a coupled increase in C and N cycling with climate warming that supports forest productivity and maintains SOC stocks. This balance could markedly shift as other factors begin to limit forest productivity (e.g., trace nutrients, water) with further climate change or affect forest nutrient allocation (e.g., forest age or compositional change). Further application of the approach presented here could be used to detect the limits of this and other ecosystem–climate feedbacks, by providing a tractable and parameterizable index of the lignin state across large spatial scales, necessary for ecosystem-scale parameterizations.

This study traces dissolved organic matter (DOM) in different water masses of the Arctic Ocean and its effect on the distributions of trace elements (TEs; Fe, Cu, Mn, Ni, Zn, Cd) using fluorescent properties of DOM and the terrigenous biomarker lignin. The Nansen, Amundsen, and Makarov Basins were characterized by the influence of Atlantic water and the fluvial discharge of the Siberian rivers with high concentrations of terrigenous DOM (tDOM). The Canada Basin and the Chukchi Sea were characterized by Pacific water, modified through contact with productive shelf sediments with elevated levels of marine DOM. Within the surface layer of the Beaufort Gyre, meteoric water (river water and precipitation) was characterized by low concentrations of lignin and terrigenous DOM fluorescence proxies as DOM is removed during freezing. High-resolution in situ fluorescence profiles revealed that DOM distribution closely followed isopycnals, indicating the strong influence of sea-ice formation and melt, which was also reflected in strong correlations between DOM fluorescence and brine contributions. The relationship of DOM and hydrography to TEs showed that terrigenous and marine DOM were likely carriers of dissolved Fe, Ni, Cu from the Eurasian shelves into the central Arctic Ocean. Chukchi shelf sediments were important sources of dCd, dZn, and dNi, as well as marine ligands that bind and carry these TEs offshore within the upper halocline (UHC) in the Canada Basin. Our data suggest that tDOM components represent stronger ligands relative to marine DOM components, potentially facilitating the long-range transport of TE to the North Atlantic. Key Points Dissolved Organic Matter (DOM) distribution in the Arctic Ocean is largely controlled by sea ice formation and melt processes DOM distribution in the Arctic Ocean reveals its potential as a tracer for halocline formation and freshwater source assignments Terrigenous and marine DOM are carriers of trace elements from shelves to the open Arctic Ocean, but terrigenous DOM represent stronger ligands

Hurricane Harvey was the wettest hurricane in US history bringing record rainfall and widespread flooding in Houston, TX. The resulting storm- and floodwaters largely emptied into the Galveston Bay. Surface water was collected from 10 stations during five cruises to investigate the concentrations and sources of 16 priority polycyclic aromatic hydrocarbons (PAHs), and relative abundances of PAH-degrading bacteria. Highest PAH levels (102-167 ng/L) were detected during the first sampling event, decreasing to 36-69 ng/L within a week. Four sites had elevated concentrations of carcinogenic benzo[a]pyrene that exceeded the Texas Standard for Surface Water threshold. The highest relative abundances of known PAH-degrading bacteria Burkholderiaceae, Comamonadaceae, and Sphingomonadales were detected during the first and second sampling events. PAH origins were about 60% pyrogenic, 2% petrogenic, and the remainder of mixed sources. This study improves our understanding on the fate, source, and distributions of PAHs in Galveston Bay after an extreme flooding event.

The use of aqueous film forming foams (AFFFs) as fire retardants is an critical point-source for per- and polyfluoroalkyl substances (PFASs) pollution into the aquatic environment. This study investigated PFASs pollution in the surface waters and biota (shellfish and fish) of Galveston Bay, following AFFFs use to extinguish a petrochemical fire (March 17th to 20th, 2019) of oil storage tanks at the International Terminals Company (ITC) in Deer Park (Houston, TX). The levels of up to twelve EPA priority PFASs were measured in surface waters and biota from March–November 2019. PFASs levels in surface waters showed mean total levels in March and April 2019 to be from 4× to ~300× higher than those measured in the following months. PFOS (perfluorooctanesulfonic acid) was the most abundant homolog measured at ≥66% of total PFASs. Maximal PFOS levels exceeded the State of Texas' water regulatory limit of 0.6 μg L−1 in 3% of the samples analyzed in March and April 2019. PFOS was also the most prominent homolog (≥66% of total PFASs) measured in eastern oysters (Crassostrea virginica), red drum (Sciaenops ocellatus), gafftopsail catfish (Bagre marinus), and spotted seatrout (Cynoscion nebulosus). A statistically significant elevation of PFOS body-burdens was measured in oysters and spotted seatrout in April and May 2019, respectively. A Hazard Ratio calculation for seafood safety suggests an advisory of 1–2 meals per week for gafftopsail catfish and red drum, and 2 meals per week for spotted seatrout to be protective for human exposure to PFOS. The levels in oysters indicated no immediate concerns for the dietary exposure of humans. Our results highlight a need for continual monitoring to assess the long-term fate and seafood advisories for PFASs.

Dissolved lignin phenols, chromophoric dissolved organic matter (DOM), and in situ fluorescence were determined in waters of the Laptev Sea and major Arctic basins, and they were compared with dissolved iron (dFe) distributions to elucidate the sources, molecular characteristics and distributions of iron-binding ligands in the Arctic Ocean . In the Transpolar Drift region (TPD), concentrations of dFe were positively correlated with concentrations of lignin phenols and multiple optical proxies of DOM composition and source. Strong relationships between dFe and visible and ultraviolet wavelength fluorescent DOM indicated that vascular plant and algal-derived DOM contributed to the dFe-ligand pool. These observations are consistent with previous studies suggesting the association of dFe with humic terrigenous and marine organic ligands. The primary sources of iron-binding ligands appear to be the riverine discharge of terrigenous DOM, marine organic matter produced on the shelves, and degradation products of plankton-derived organic matter in the shelf sediments . A stronger relationship between dFe and visible wavelength CDOM fluorescence than with lignin phenols suggested the presence of multiple terrigenous ligands, such as aromatic tannins. The aromatic nature of these terrigenous ligands was indicated by a strong relationship between dFe and the absorption coefficient at 254 nm. A strong negative correlation between the p-hydroxyl to vanillyl lignin phenols ratio and dissolved iron concentrations indicated recently-discharged terrigenous DOM (tDOM) was an important source of iron-binding ligands. Given the strong relationships of marine and terrigenous DOM with dissolved iron, iron-binding functional groups appear to occur in diverse molecules of multiple sources. Examples of such iron-binding functional groups included catechols and carboxylates found in lignins and tannins of terrigenous origins and carboxyl-rich alicyclic molecules (CRAM) of terrigenous and marine origins. The observed dFe distributions in the Arctic Ocean could not be explained by the presence of a single ligand type, but rather by a potpourri of ligand molecules of varying concentrations and binding strengths. This molecular diversity of ligands and associated binding strengths ultimately controls the distribution and transport of dFe in the Arctic Ocean and beyond.

Peatlands are impacted by climate and land-use changes, with feedback to warming by acting as either sources or sinks of carbon. Expert elicitation combined with literature review reveals key drivers of change that alter peatland carbon dynamics, with implications for improving models. The carbon balance of peatlands is predicted to shift from a sink to a source this century. However, peatland ecosystems are still omitted from the main Earth system models that are used for future climate change projections, and they are not considered in integrated assessment models that are used in impact and mitigation studies. By using evidence synthesized from the literature and an expert elicitation, we define and quantify the leading drivers of change that have impacted peatland carbon stocks during the Holocene and predict their effect during this century and in the far future. We also identify uncertainties and knowledge gaps in the scientific community and provide insight towards better integration of peatlands into modelling frameworks. Given the importance of the contribution by peatlands to the global carbon cycle, this study shows that peatland science is a critical research area and that we still have a long way to go to fully understand the peatland-carbon-climate nexus.

Extreme weather events such as tropical storms and hurricanes deliver large amounts of freshwater (stormwater and river discharge) and associated dissolved organic carbon (DOC) to estuaries and the coastal ocean, affecting water quality, and carbon budgets. Hurricane Harvey produced an unprecedented 1000-year flood event in 2017 that inundated the heavily urbanized and industrialized Houston/Galveston region (TX, United States). Within a week, storm-associated floodwater delivered 87 +/- 18 Gg of terrigenous dissolved organic carbon (tDOC) to Galveston Bay and the Gulf of Mexico continental shelves. In situ decay constants of 8.75-28.33 year(-1) resulted in the biomineralization of similar to 70% of tDOC within 1 month of discharge from the flood plain. The high removal efficiency of tDOC was linked to a diverse microbial community capable of degrading a wide repertoire of dissolved organic matter (DOM), and suggested hurricane-induced flood events affect net CO2 exchange and nutrient budgets in estuarine watersheds and coastal seas.

Hurricane Harvey (category four storm) made landfall along the coast of Texas (United States) and then stalled out over Texas and Louisiana, releasing 1.29 × 1011 m3 of precipitation over 5 days. This caused extensive flooding that elevated freshwater river discharge and land runoff into Galveston Bay and eventually into the Gulf of Mexico. The floodwaters delivered a significant influx of dissolved organic carbon (DOC), organic pollutants and nutrients along with terrestrial and freshwater associated microbes. Over the 24 days following the flooding event, samples were collected on five cruises across Galveston Bay from the mouth of the San Jacinto River (Houston, TX, United States) to the Gulf of Mexico. Parameters measured for this study include: water quality (temperature, salinity, pH, and dissolved oxygen), nutrients (NO3–, NO2–, NH4+, Pi, and HSiO3–), polycyclic aromatic hydrocarbons (PAHs), pharmaceuticals (cotinine, carbamazepine, carbamazepine-epoxide, and prednisone), biocide (imidacloprid), DOC, bacteria, and the eukaryotic community composition (16S and 18S rRNA genes). In the week after the flood event, bay-wide salinities decreased to 0–5 compared to the higher pre-Harvey salinities of 20–30 (recorded 5 days before the flood). Water treatment facilities and petrochemical plants were compromised due to the heavy flooding in the region. Increased concentrations of DOC, nutrients, PAHs, pharmaceuticals, and biocides were observed across Galveston Bay immediately following the storm. During the 4 weeks after Harvey, concentrations of DOC, nutrients, and organic pollutants began to decrease coinciding with rising salinities as the freshwater was flushed into the Gulf of Mexico and seawater began moving back into the Bay. Successive blooms of Chlorophyta, diatoms (Bacillariophyta), and dinoflagellates (Dinophyta) occurred similar to post-storm communities from past hurricanes that have impacted estuarine systems along the Gulf of Mexico. The bacterial community showed an increase in the abundance of bacteria associated with terrestrial soils and freshwater at the initial time point and then decreased over time and were replaced by their estuarine and marine relatives within the month following the hurricane. The eukaryotic community changed substantially following Harvey and did not recover to pre-Harvey conditions during our study period, suggesting a longer recovery time compared to the prokaryotes. Although the water quality parameters and prokaryotic community showed signs of returning to pre-Harvey conditions within the month following the flood event, long-term impacts need to be measured in the years following the flood.

The San Francisco Bay Estuary (SFBE) together with the Sacramento–San Joaquin River Delta is the second largest estuary in the United States and represents a highly dynamic ecosystem. From 2014 to 2016, we conducted three transects across a salinity gradient to investigate the roles of sources, hydrologic and seasonal changes on the DOM composition. Sampling started with a riverine endmember, through a vast area of marshes, wetlands, to the Golden Gate, the largest estuary in western North America. The winter transect at its maximum discharge allowed the study of DOM dynamics largely in the absence of photodegradation processes and low levels of algal production; the summer transect captured significant photodegradation and algal production; the spring transect revealed the signal of stored DOM from the snowmelt cold water flows. Multiple studies indicated that algal primary production alone cannot support the SFBE foodweb, and the wetlands could also serve to reduce DOM loadings coming off of the delta. Hence, other sources of organic matter must be considered, including autochthonous and allochthonous DOM. Terrestrial DOM export in SFBE were revealed by dissolved lignin dynamics. Optical proxies (UV-vis and fluorescence) were also used to study the photochemical and biological transformations of DOM.

Data from GEOTRACES cruises GN01 (HLY1502) and GN04 (PS94) have been archived at the Biological & Chemical Oceanography Data Management Office (BCO-DMO; https://www.bco-dmo.org/deployment/638807) and PANGAEA (https://www.pangaea.de/?q=PS94&f.campaign%5B%5D=PS94) websites, respectively. The inorganic carbon data are available at the NOAA Ocean Carbon Data System (OCADS ; doi :10.3334/CDIAC/OTG.CLIVAR_ARC01_33HQ20150809). In addition to these national data archives, the data used in this paper is available as a supplementary downloadable excel file; International audience; A major surface circulation feature of the Arctic Ocean is the Transpolar Drift (TPD), a current that transports river‐influenced shelf water from the Laptev and East Siberian Seas toward the center of the basin and Fram Strait. In 2015, the international GEOTRACES program included a high‐resolution pan‐Arctic survey of carbon, nutrients, and a suite of trace elements and isotopes (TEIs). The cruises bisected the TPD at two locations in the central basin, which were defined by maxima in meteoric water and dissolved organic carbon concentrations that spanned 600 km horizontally and ~25‐50 m vertically. Dissolved TEIs such as Fe, Co, Ni, Cu, Hg, Nd, and Th, which are generally particle‐reactive but can be complexed by organic matter, were observed at concentrations much higher than expected for the open ocean setting. Other trace element concentrations such as Al, V, Ga, and Pb were lower than expected due to scavenging over the productive East Siberian and Laptev shelf seas. Using a combination of radionuclide tracers and ice drift modeling, the transport rate for the core of the TPD was estimated at 0.9 ± 0.4 Sv (106 m3 s‐1). This rate was used to derive the mass flux for TEIs that were enriched in the TPD, revealing the importance of lateral transport in supplying materials beneath the ice to the central Arctic Ocean and potentially to the North Atlantic Ocean via Fram Strait. Continued intensification of the Arctic hydrologic cycle and permafrost degradation will likely lead to an increase in the flux of TEIs into the Arctic Ocean.

Karst basins (e.g., blueholes, sinkholes) accumulate well-preserved sedimentary successions that provide transformative paleoclimatic and paleoenvironmental information. However, the sedimentary processes within these basins are not yet fully understood. Here we present stable carbon isotopic values (δ13Corg) and C:N ratios of bulk organic matter in well-dated sediment cores from Blackwood Sinkhole (Abaco, The Bahamas) to investigate the changing flux of organic matter into the sinkhole during the late Holocene. The provenance of preserved organic matter changed through the late Holocene between three primary sources, as determined by three-endmember mixing modeling: wetland organic matter from the adjacent epikarst surface, authigenic primary productivity in the oligohaline meteoric lens, and terrestrial organic matter from the surrounding landscape. Expansion of wetlands on the adjacent epikarst surface played a critical role by increasing the flux of wetland organic matter to the sinkhole, especially during the last 1000 years. Hurricanes and regional rainfall may have mediated organic matter delivery to the benthos, either through hampering wetland development (prior to 1000 cal yr BP) or by changing dissolved nutrient concentrations available in the basin for primary producers. These results demonstrate that organic matter provenance in karst basins is not constant through time, and is significantly dependent upon both landscape vegetation on the epikarst surface and changing hydrographic conditions that impacts nutrient availability to primary producers.

Large-scale exopolymeric substances (EPS) formation was observed in contaminated surface waters of the Gulf of Mexico , after the Deepwater Horizon oil spill. The conditions under which EPS are produced can cause variations in their physico-chemical properties , affecting the fate of the oil through either emulsification or coagulation with particles, followed by aggregation and marine oil snow (MOS) sedimentation . Here, we report results from a four-day mesocosm experiment that examined EPS production, the change in the bulk chemical composition (mainly polysaccharides and proteins), as well as the partitioning into different size fractions (suspended particulate matter (SPM), colloidal fraction, and sinking MOS). The treatments included 1) natural coastal seawater (Control), 2) a water accommodated fraction of oil (WAF), 3) a chemically-enhanced WAF with addition of oil dispersant Corexit (CEWAF), and 4) a diluted CEWAF (DCEWAF). Generally, the presence of WAF stimulated more extracellular polysaccharide production, whereas the addition of Corexit promoted more protein production. Moreover, marine aggregates changed from a terrestrial signature (higher aromaticity, lower EPS content and more uniform monosaccharide distribution) in the early stages of the experiment, to a fresher autochthonous signature (less aromatic, higher EPS content and glucose-dominated monosaccharide distribution) in the later stage of the mesocosm experiment. Corexit promoted the association between oil and proteins, assisting to emulsify the oil in colloids and SPM and delay the settling of EPS and oil (MOS) for the duration of the mesocosm. Furthermore, when oil, especially Corexit-dispersed oil, was present, extracellular polysaccharides were preferentially incorporated into sinking MOS relative to proteins, as evidenced from a lower protein-C/carbohydrate-C ratio of the sinking MOS than those of SPM and colloidal fraction in WAF, CEWAF and DCEWAF, respectively. This is in contrast to a higher protein-C/carbohydrate-C ratio in the sinking marine snow than those of SPM and colloidal fraction in the control. Likely, microbially-mediated extracellular polysaccharides are the key component that anchors the mineral ballast until the aggregates become dense enough and overcome the buoyancy added to the aggregates as a result of their association with oil/Corexit. We conclude that interactions between Corexit and EPS components regulate petroleum hydrocarbon distribution between the water column and sinking MOS.

A novel ultra-high performance liquid chromatography-electrospray ionization-tandem mass spectrometry method was developed to enable the analysis of ultra-low levels of lignin phenols (100 fmol) in environmental samples. The method included a sample clean-up with a polymer sorbent based solid-phase extraction and reversed-phase chromatography that allowed separation of all lignin phenols with minimal interference from co-eluting matrix components. The application of

We discovered a 50-cm-thick peat deposit near Cape Rasmussen (65.2°S), in the maritime Antarctic. To our knowledge, while aerobic ‘moss banks’ have often been examined, waterlogged ‘peatlands’ have never been described in this region before. The waterlogged system is approximately 100 m2, with a shallow water table. Surface vegetation is dominated by Warnstorfia fontinaliopsis, a wet-adapted moss commonly found in the Antarctic Peninsula. Peat inception was dated at 2750 cal. BP and was followed by relatively rapid peat accumulation (~0.1 cm/year) until 2150 cal. BP. Our multi-proxy analysis then shows a 2000-year-long stratigraphic hiatus as well as the recent resurgence of peat accumulation, sometime after 1950 AD. The existence of a thriving peatland at 2700–2150 cal. BP implies regionally warm summer conditions extending beyond the mid-Holocene; this finding is corroborated by many regional records showing moss bank initiation and decreased sea ice extent during this time period. Recent peatland recovery at the study site (

Dissolved lignin phenols, chromophoric dissolved organic matter (CDOM) absorption, and fluorescence were analyzed along cross-slope mooring locations in the Barents, Laptev, and East Siberian Seas to gain a better understanding of terrigenous dissolved organic carbon (tDOC) dynamics in Arctic shelf seas and the Arctic Ocean. A gradient of river water and tDOC was observed along the continental shelf eastward into the East Siberian Sea. Correlations of carbon-normalized yields of lignin-derived phenols supplied by Siberian rivers with river water fractions and known water residence times yielded in situ decay constants of 0.18–0.58 yr−1. Calculations showed ∼50% of annual tDOC discharged by Siberian rivers was mineralized in estuaries and on Eurasian shelves per year indicating extensive removal of tDOC. Bioassay experiments and in situ decay constants indicated a reactivity continuum for tDOC. CDOM parameters and acid/aldehyde ratios of vanillyl (V) and syringyl (S) lignin phenols showed biomineralization was the dominant mechanism for the removal of tDOC. Characteristic ratios of p-hydroxy (P), S, and V phenols (P/V, S/V) also identified shelf regions in the Kara Sea and regions along the Western Laptev Sea shelf where formation of Low Salinity Halocline Waters (LSHW) and Lower Halocline Water (LHW) occurred. The efficient removal of tDOC demonstrates the importance of Eurasian margins as sinks of tDOC derived from the large Siberian Rivers and confirms tDOC mineralization has a major impact on nutrients budgets, air-sea CO2 exchange, and acidification in the Siberian Shelf Seas.

Hurricane Harvey was the wettest hurricane in US history bringing record rainfall and widespread flooding in Houston, TX. The resulting storm- and floodwaters largely emptied into the Galveston Bay. Surface water was collected from 10 stations during five cruises to investigate the concentrations and sources of 16 priority polycyclic aromatic hydrocarbons (PAHs), and relative abundances of PAH-degrading bacteria. Highest PAH levels (102-167 ng/L) were detected during the first sampling event, decreasing to 36-69 ng/L within a week. Four sites had elevated concentrations of carcinogenic benzo[a]pyrene that exceeded the Texas Standard for Surface Water threshold. The highest relative abundances of known PAH-degrading bacteria Burkholderiaceae, Comamonadaceae, and Sphingomonadales were detected during the first and second sampling events. PAH origins were about 60% pyrogenic, 2% petrogenic, and the remainder of mixed sources. This study improves our understanding on the fate, source, and distributions of PAHs in Galveston Bay after an extreme flooding event.

In the version of this Analysis originally published, the following affiliation for A. Lohila was missing: ‘Finnish Meteorological Institute, Climate System Research, Helsinki, Finland’. This affiliation has now been added, and subsequent affiliations renumbered accordingly, in the online versions of the Analysis.