Isotopic Signatures and Outputs of Lead from Coal Fly Ash Disposal in China, India, and the United States.

Despite extensive research and technology to reduce the atmospheric emission of Pb from burning coal for power generation, minimal attention has been paid to Pb associated with coal ash disposal in the environment. This study investigates the isotopic signatures and output rates of Pb in fly ash disposal in China, India, and the United States. Pairwise comparison between feed coal and fly ash samples collected from coal-fired power plants from each country shows that the Pb isotope composition of fly ash largely resembles that of feed coal, and its isotopic distinction allows for tracing the release of Pb from coal fly ash into the environment. Between 2000 and 2020, approx. 236, 56, and 46 Gg Pb from fly ash have been disposed in China, India, and the U.S., respectively, posing a significant environmental burden. A Bayesian Pb isotope mixing model shows that during the past 40 to 70 years, coal fly ash has contributed significantly higher Pb (∼26%) than leaded gasoline (∼7%) to Pb accumulation in the sediments of five freshwater lakes in North Carolina, U.S.A. This implies that the release of disposed coal fly ash Pb at local and regional scales can outweigh that of other anthropogenic Pb sources.

Legacy of Coal Combustion: Widespread Contamination of Lake Sediments and Implications for Chronic Risks to Aquatic Ecosystems.

Elevated concentrations of toxic elements in coal ash pose human and ecological health risks upon release to the environment. Despite wide public concerns about water quality and human health risks from catastrophic coal ash spills and chronic leaking of coal ash ponds, coal ash disposal has only been partially regulated, and its impacts on aquatic sediment quality and ecological health have been overlooked. Here, we present a multiproxy approach of morphologic, magnetic, geochemical, and Sr isotopic analyses, revealing unmonitored coal ash releases over the past 40 to 70 years preserved in the sediment records of five freshwater lakes adjacent to coal-fired power plants across North Carolina. We detected significant sediment contamination and potential chronic ecological risks posed by the occurrence of hundreds of thousands of tons of coal ash solids mainly resulting from high-magnitude stormwater runoff/flooding and direct effluent discharge from coal ash disposal sites. The proximity of hundreds of disposal sites to natural waterways across the U.S. implies that such contamination is likely prevalent nationwide and expected to worsen with climate change.

Evaluation and Integration of Geochemical Indicators for Detecting Trace Levels of Coal Fly Ash in Soils.

Coal combustion residuals (CCRs), in particular, coal fly ash, are one of the major industrial solid wastes in the U.S., and due to their high concentrations of toxic elements, they could pose environmental and human health risks. Yet detecting coal fly ash in the environment is challenging given its small particle size. Here, we explore the utility and sensitivity of using geochemical indicators (trace elements, Ra nuclides, and Pb stable isotopes), combined with physical observation by optical point counting, for detecting the presence of trace levels of coal fly ash particles in surface soils near two coal-fired power plants in North Carolina and Tennessee. Through experimental work, mixing models, and field data, we show that trace elements can serve as a first-order detection tool for fly ash presence in surface soils; however, the accuracy and sensitivity of detection is limited for cases with low fly ash proportion (i.e., <10%) in the soil, which requires the integration of more robust Ra and Pb isotopic tracers. This study revealed the presence of fly ash particles in surface soils from both the recreational and residential areas, which suggests the fugitive emission of fly ash from the nearby coal-fired power plants.

Mid-Pleistocene climate transition drives net mass loss from rapidly uplifting St. Elias Mountains, Alaska.

Erosion, sediment production, and routing on a tectonically active continental margin reflect both tectonic and climatic processes; partitioning the relative importance of these processes remains controversial. Gulf of Alaska contains a preserved sedimentary record of the Yakutat Terrane collision with North America. Because tectonic convergence in the coastal St. Elias orogen has been roughly constant for 6 My, variations in its eroded sediments preserved in the offshore Surveyor Fan constrain a budget of tectonic material influx, erosion, and sediment output. Seismically imaged sediment volumes calibrated with chronologies derived from Integrated Ocean Drilling Program boreholes show that erosion accelerated in response to Northern Hemisphere glacial intensification (∼ 2.7 Ma) and that the 900-km-long Surveyor Channel inception appears to correlate with this event. However, tectonic influx exceeded integrated sediment efflux over the interval 2.8-1.2 Ma. Volumetric erosion accelerated following the onset of quasi-periodic (∼ 100-ky) glacial cycles in the mid-Pleistocene climate transition (1.2-0.7 Ma). Since then, erosion and transport of material out of the orogen has outpaced tectonic influx by 50-80%. Such a rapid net mass loss explains apparent increases in exhumation rates inferred onshore from exposure dates and mapped out-of-sequence fault patterns. The 1.2-My mass budget imbalance must relax back toward equilibrium in balance with tectonic influx over the timescale of orogenic wedge response (millions of years). The St. Elias Range provides a key example of how active orogenic systems respond to transient mass fluxes, and of the possible influence of climate-driven erosive processes that diverge from equilibrium on the million-year scale.

Phasing of millennial-scale climate variability in the Pacific and Atlantic Oceans.

New radiocarbon and sedimentological results from the Gulf of Alaska document recurrent millennial-scale episodes of reorganized Pacific Ocean ventilation synchronous with rapid Cordilleran Ice Sheet discharge, indicating close coupling of ice-ocean dynamics spanning the past 42,000 years. Ventilation of the intermediate-depth North Pacific tracks strength of the Asian monsoon, supporting a role for moisture and heat transport from low latitudes in North Pacific paleoclimate. Changes in carbon-14 age of intermediate waters are in phase with peaks in Cordilleran ice-rafted debris delivery, and both consistently precede ice discharge events from the Laurentide Ice Sheet, known as Heinrich events. This timing precludes an Atlantic trigger for Cordilleran Ice Sheet retreat and instead implicates the Pacific as an early part of a cascade of dynamic climate events with global impact.

Sediment controls dynamic behavior of a Cordilleran Ice Stream at the Last Glacial Maximum.

The uncertain response of marine terminating outlet glaciers to climate change at time scales beyond short-term observation limits models of future sea level rise. At temperate tidewater margins, abundant subglacial meltwater forms morainal banks (marine shoals) or ice-contact deltas that reduce water depth, stabilizing grounding lines and slowing or reversing glacial retreat. Here we present a radiocarbon-dated record from Integrated Ocean Drilling Program (IODP) Site U1421 that tracks the terminus of the largest Alaskan Cordilleran Ice Sheet outlet glacier during Last Glacial Maximum climate transitions. Sedimentation rates, ice-rafted debris, and microfossil and biogeochemical proxies, show repeated abrupt collapses and slow advances typical of the tidewater glacier cycle observed in modern systems. When global sea level rise exceeded the local rate of bank building, the cycle of readvances stopped leading to irreversible retreat. These results support theory that suggests sediment dynamics can control tidewater terminus position on an open shelf under temperate conditions delaying climate-driven retreat.

Evidence for unmonitored coal ash spills in Sutton Lake, North Carolina: Implications for contamination of lake ecosystems.

Coal combustion residuals (CCRs, also known as "coal ash") contain high concentrations of toxic and carcinogenic elements that can pose ecological and human health risks upon their release into the environment. About half of the CCRs that are generated annually in the U.S. are stored in coal ash impoundments and landfills, in most cases adjacent to coal plants and waterways. Leaking of coal ash ponds and CCR spills are major environmental concerns. One factor which may impact the safety of CCRs stored in impoundments and landfills is the storage area's predisposition to flooding. The southeastern U.S., in particular, has a large number of coal ash impoundments located in areas that are vulnerable to flooding. In order to test for the possible presence of CCR solids in lake sediments following Hurricane Florence, we analyzed the magnetic susceptibility, microscopic screening, trace element composition, and strontium isotope ratios of bottom sediments collected in 2015 and in 2018 from Sutton Lake in eastern North Carolina and compared them to a reference lake. The results suggest multiple, apparently previously unmonitored, CCR spills into Sutton Lake from adjacent CCR storage sites. The enrichment of metals in Sutton Lake sediments, particularly those with known ecological impact such as As, Se, Cu, Sb, Ni, Cd, V, and Tl, was similar to or even higher than those in stream sediments impacted by the Tennessee Valley Authority (TVA) in Kingston, Tennessee, and the Dan River, North Carolina coal ash spills, and exceeded ecological screening standards for sediments. High levels of contaminants were also found in leachates extracted from Sutton Lake sediments and co-occurring pore water, reflecting their mobilization to the ambient environment. These findings highlight the risks of large-scale unmonitored spills of coal ash solids from storage facilities following major storm events and contamination of nearby water resources throughout the southeastern U.S.

Magnetic susceptibility measurements to detect coal fly ash from the Kingston Tennessee spill in Watts Bar Reservoir.

An estimated 229,000 m(3) of coal fly ash remains in the river system after dredging to clean-up the 2008 Tennessee Valley Authority (TVA) spill in Kingston, Tennessee. The ash is heterogeneous with clear, orange and black spheres and non-spherical amorphous particles. Combustion produces iron oxides that allow low field magnetic susceptibility (χ(LF)) and percent frequency dependent susceptibility (χ(FD)%) to be used to discriminate between coal fly ash and sediments native to the watershed. Riverbed samples with χ(LF) greater than 3.0 × 10(-6) m(3)/kg, have greater than 15% ash measured by optical point counting. χ(LF) is positively correlated with total ash, allowing ash detection in riverbed sediments and at depth in cores. The ratio of ash sphere composition is altered by river transport introducing variability in χ(LF). Measurement of χ(LF) is inexpensive, non-destructive, and a reliable analytical tool for monitoring the fate of coal ash in this fluvial environment.