Sedimentary evidence for changes in the pollution status of Taihu in the Jiangsu region of eastern China

As part of a study using lake sediments to determine the extent and causes of human impacts to lakes along an east–west transect following the Yangtse River, sediment cores were taken from Taihu in eastern China. Previous studies have focussed on the impacts of direct inputs of pollutants from municipal and industrial wastewater but little work has been undertaken on trends in atmospheric deposition from the many industrial sources surrounding the lake. Analysis of the Taihu sediment cores for atmospheric pollutant indicators such as trace metals, magnetic parameters and spheroidal carbonaceous particles (SCPs) show the lake has become increasingly contaminated over the last 40–50 years. Sediment levels of atmospherically deposited pollutants are currently similar to some of the more contaminated lakes in Europe. Further, sediment nitrogen, phosphorus and geochemical analyses confirm the dramatic increase in eutrophication at the site and periods of recent soil erosion in the catchment.     

Environmental records of carbonaceous fly-ash particles from fossil-fuel combustion

Analysis of fly-ash particles in lake sediments has become increasingly important in studies of environmental pollution and lake acidification history. Most fly-ash studies have concerned black spheroidal carbonaceous particles (SCP)(>5 m) produced from oil and coal combustion. This review paper provides a summary of this technique and its application, and focusses on our investigations in Sweden between 1979 and 1993. It consists of five parts: i) preparation and analysis methods, ii) historical trends in atmospheric deposition, iii) geographical surveys of atmospheric deposition, iv) sediment dating, and v) studies of sedimentation processes in lakes. Methods for preparation and analyses of SCP have been developed and applied to investigations using sediment, soil and snow samples. Stratigraphic trends of SCP concentrations in lake-sediment cores reflect the consumption history of fossil fuels. A characteristic temporal SCP pattern, with a marked concentration increase beginning after the 1940's and a peak in the early 1970's, has been recognized in most Swedish lakes and elsewhere in Europe. A survey of SCP concentrations in surface sediments of >100 lakes covering Sweden demonstrated that polluted areas in southern Sweden had >100 times higher SCP concentrations than clean areas in the north. The spatial distribution of SCP over Sweden is similar to the deposition pattern of long-range transported airborne pollutants, such as excess sulphate monitored by network stations. SCP also accumulate in soils, and soil analyses can be used for determining the integrated historical deposition of SCP at the local or regional scale. Finally, SCP have been used for indirect dating of sediment cores and as a marker to assess sediment distribution patterns within lake basins.     

Within-basin profile variability and cross-correlation of lake sediment cores using the spheroidal carbonaceous particle record

Spheroidal carbonaceous particles (SCPs) from the high temperature combustion of fossil-fuels are stored in lake sediments and provide an unambiguous record of industrially derived atmospheric contamination. It has been assumed that a single sediment core provides an accurate representation of SCP accumulation but to date there have been no studies to determine within-lake variability of the SCP sediment record. This paper describes the SCP profiles of ten sediment cores taken from the deep water area of Loch Coire nan Arr, a remote lake in north-west Scotland, UK. Although each core shows the basic SCP profile used for sediment dating in the UK there is considerable variation between cores. The conversion of SCP concentrations to cumulative percentages resolves a great deal of this variation with the result that more accurate cross-correlation and hence date allocation is possible, especially in the post-1945 section of the cores. However, significant departures from the usual SCP profile still reduce the effectiveness of this approach. It is concluded that: (i) SCP profiles from single cores from the deepest areas of the lake usually provide an accurate representation of the historical record of atmospherically deposited pollutants and that inter-core variability or noise does not affect the temporal interpretation of that profile, and (ii) comparisons of total SCP inventories are a better way of comparing historical deposition between sites as the impact of temporary variability is considerably reduced.     

Factors affecting sulfur incorporation into lake sediments: paleoecological implications

This paper discusses the use of S as a paleolimnological tracer of limnetic sulfate concentration. A positive relationship (p<0.05) was found between limnetic sulfate and sediment S concentrations for the Great Lakes, English Lakes, and lakes from the Adirondack and Northern New England regions. There is a positive correlation (p<0.05) between C and S concentration in sediment across all regions studied. The importance of C in affecting S content in sediment was also examined by a series of cores taken at different water depths in Big Moose Lake (Adirondacks). There was a strong relationship between C and S among cores with sediment from deeper water having higher C and S concentrations (r ²=0.99). Sulfur from the shallower cores had greater concentrations of chromium-reducible S (pyrite), while cores from deeper waters had a greater proportion of organic S fractions including C-bonded S and ester sulfates.For assessing historical changes in S accumulation in sediments, enrichment factors were calculated for the PIRLA lakes. Pre-1900 net sediment accumulation rates of S were very similar across all regions. Sulfur enrichment was greatest in Adirondack sediment which had total post-1900 S accumulation of 1.1 to 7.4 times pre-1900 S accumulation. Sediment from Northern New England (NNE) generally had lower S concentration than Adirondack sediments and S enrichment factors ranged from 1.2 to 2.1. Sediment from the Northern Great Lakes States region had similar S concentration and distribution with depth to NNE sediment. In two Northern Florida lakes, sediment showed little variation in S concentration with depth, but in two other lakes from the same region, there was higher S concentration in deeper layers. Lakes which had the greatest enrichment factors also exhibited the most marked changes in C:S ratios. Ratios of C:N showed little variation (10.6 to 26.1) among the PIRLA lakes. A first order model indicated slow decomposition within these organic rich sediments.Elemental concentrations and ratios of sediment from a variety of lakes and reservoirs were complied. Maximum and minimum elemental ratios for all the data were 28 to 8.1 for C:N, 0.81 to 0.11 for C:H, and 675 to 12.5 for C:S, respectively. For the C:S ratios in all regions except the Great Lakes, the maximum ratio was less than 231. Both the maximum and minimum amount of N and H concentration of organic matter is related to biotic processes. The minimum concentration of S is regulated not only by nutrient demands but also by non-assimilatory processes.Sulfur incorporation into sediments is a function of a complex of factors, but limnetic sulfate concentration and organic matter content play a major role in regulating the S content of sediment. Further quantification of S incorporation pathways will aid in the paleolimnological interpretation of sediment S profiles. Such information is also important in assessing how S sediment pools will respond to decreases in limnetic sulfate concentration which may occur with decreases in inputs from acidic deposition.This is the eighth of a series of papers to be published by this journal which is a contribution to the Paleoecological Investigation of Recent Lake Acidification (PIRLA) project. Drs. D.F. Charles and D.R. Whitehead are guest editors for this series.     

Lake-Sediment Evidence for Local and Remote Sources of Atmospherically Deposited Pollutants on Svalbard

Twenty-one lakes along the west coast of Svalbard were cored between 28 July and 14 August 1995. Five cores were ²¹⁰Pb dated and analysed for spheroidal carbonaceous particles (SCPs), indicators of deposition from fossil-fuel combustion sources, and trace metals. Surface and pre-industrial levels of five cores were analysed for 10 polychlorinated biphenyl (PCB) isomers and 16 polycyclic aromatic hydrocarbon (PAH) compounds, whilst all 21 surface sediments were analysed for SCPs. Temporal and spatial trends in the atmospheric deposition of pollutants were identified. Whilst temporal patterns of deposited pollutants may have been truncated due to concentrations falling below the limits of detection, spatial patterns showed elevated levels of SCP, PAH, PCB, and possibly Pb within 60–70 km of Isfjord. Tenndammen (U), the closest site to Longyearbyen, showed the highest levels of contamination for all pollutants. Differences in the deposition patterns of PAH and PCB are thought to be due to local sources of PAH from coal combustion whilst PCB sources are remote. It is concluded that the impact from atmospheric deposition on Svalbard is due to a combination of spatially limited local sources superimposed on a broad-scale, long-range pattern.     

The Holocene–Anthropocene transition in lakes of western Spitsbergen,Svalbard (Norwegian High Arctic): climate change and nitrogen deposition

Lake sediments from four small lakes on western Spitsbergen (Svalbard Archipelago, Norwegian High Arctic) preserve biostratigraphic and isotopic evidence for a complex suite of twentieth century environmental changes. At Lake Skardtjørna and Lake Tjørnskardet on Nordenskiöldkysten, there is a marked diatom floristic change coupled to increased diatom concentrations beginning around 1920. At Lake Istjørna and Lake Istjørnelva, 25 km southwest of Longyearbyen, both diatom total valve and chrysophyte stomatocyst concentrations have increased dramatically since the beginning of the 1900s. The early twentieth century changes are probably related to climate warming after the Little Ice Age. However, the most pronounced changes in diatom assemblages seem to have occurred in the last few decades. At the same time, nitrogen stable isotopes in sediment organic matter in two of the lakes became progressively depleted by ~2‰, which is consistent with diffuse atmospheric inputs from anthropogenic sources and attendant fertilization. These data suggest that climate change and nitrogen deposition may be acting together in driving these lakes towards new ecological states that are unique in the context of the Holocene.     

Historical trace metal loading to a large river recorded in the sediments of Lake St. Croix,USA

The global cycling of anthropogenic trace metals intensified during the twentieth century, impacting aquatic systems throughout the world. There are, however, few quantitative records showing the history of this contamination in large rivers. Here we present a well-dated sedimentary record of trace metal accumulation in Lake St. Croix, a natural riverine lake on the St. Croix River (Minnesota and Wisconsin, USA), revealing the history of heavy metal inputs to the river over the past 200 years. Concentrations of Hg, Pb, Ag, Cd, Cr and Zn and stable Pb isotopes were measured in eight ²¹⁰Pb-dated sediment cores collected from profundal depositional areas throughout the lake. Time trends of trace metal concentrations and accumulation rates differed greatly between the upper lake (above Valley Creek) and the lower lake, reflecting contrasting sediment sources along the flow axis of the lake. For most of the study period (1800–2000 AD), sediment deposited throughout the lake derived almost exclusively from the suspended sediment load carried by the main-stem river into the lake. From 1910 through 1970, however, large inputs of eroded soils and stream channel sediments from side-valley tributaries resulted in greatly increased sediment and trace metal accumulation in the lower lake. Anthropogenic accumulation rates of Hg, Pb, Cd, Zn, and Ag in the upper lake correlate well with those from Square Lake, a small, relatively undisturbed nearby lake that has received trace metal inputs almost exclusively via atmospheric deposition. The similarity of these records suggests that atmospheric deposition was primarily responsible for trace metal accumulation trends in upper Lake St. Croix. Trace metal accumulation in the lower lake was also strongly influenced by atmospherically derived inputs, but metal contributions from native soils were important, as well, during the period of elevated sediment inputs from side-valley tributaries. Concentrations and accumulation rates of trace metals in both upper and lower lake sediments have decreased substantially since the 1970s due to decreased atmospheric inputs and sediment loadings, but accumulation rates remain well above pre-settlement values. Metal inputs to Lake St. Croix have been far lower than those to nearby Lake Pepin, located on the Mississippi River downstream of the Minneapolis-St. Paul metropolitan area, but there nevertheless remains a clear record of anthropogenic impact on the relatively pristine St. Croix River.     

Controls on loss-on-ignition variation in cores from two shallow lakes in the northeastern United States

Loss-on-ignition analysis of Quaternary lake sediments provides an inexpensive and easy way to investigate past environmental changes. The mass loss on ignition at 550 °C (LOI) from lake sediment cores may vary because of temporal changes in: (1) sediment composition controlled by factors such as productivity, inorganic inputs, and decomposition; and (2) the patterns of sediment accumulation controlled by factors such as basin morphology and water level. Climatic changes can alter both. Here, modern surface samples and transects of sediment cores, collected across small (<10 ha), shallow (<4 m) lakes in the northeastern United States, show that LOI varies little (2–5%) across the deep portions of these small lakes at a given time. Large changes in LOI occur only at the transition into the littoral (shallow) zone. LOI variations in sediment cores that exceed 2–5%, therefore, appear to represent meaningful environmental changes. However, because of the many possible controls, changes in the LOI of a single core are often hard to interpret. Multiple cores increase the interpretability. At lakes studied here, similar LOI trends among several cores confirm that some LOI changes resulted from basin-wide shifts in sediment composition. Differences among cores, however, developed during the early- and mid-Holocene and indicate that the edge of the littoral zone moved towards the centers of the lakes during two periods of low lake levels, at ca. 11 000–8000 and ca. 5400–3000 cal yr B.P. The basin-wide balance of sediment sources controlled the LOI from deep-water sediments, but sedimentation patterns, which changed as lake levels changed, were also important. LOI differences among cores may therefore help identify past lake-level changes in other lakes.     

Landscape-scale patterns of sediment sulfur accumulation in Swedish lakes

Sulfur has played a central role in the acidification of many lakes in Scandinavia and other regions. As part of the research into sulfur cycling, numerous studies have analyzed the sediment record in order to develop insights into past in-lake cycling of sulfur, particularly in the context of reconstructing past deposition rates. Although many of these studies have shown that it is not easy to interpret the sediment record in terms of past sulfur deposition rates, analyses of sulfur in sediment still provide valuable information on the response of lakes to anthropogenic sulfur deposition. Here, we have analyzed sulfur in top and bottom samples from short surface cores (25–35 cm, representing ≥250 years) as well as bulk cores from ∼110 lakes located throughout Sweden, which were collected during 1986, as well as in more-detailed profiles from six lakes. The lakes with the highest surface sediment concentrations (9–24 mg S g⁻¹ dry mass) and the highest calculated inventories of ‘excess’ sulfur (20–180 g S m⁻²) are found in southern Sweden and around one industrial area along the northeastern coast where sulfur deposition rates and lake-water concentrations have been highest. For many lakes in the central and northern inland region it is common that the sediment cores exhibit either no enrichment or even a decline in sulfur concentrations in near-surface sediments, which we suggest was the pre-pollution norm for lakes. Although interpreting sulfur sediment profiles is problematic for reconstructing deposition, a more-comprehensive spatial sampling approach shows that there is a good geographic agreement between sulfur deposition, lake-water chemistry and sediment sulfur accumulation.     

Stratigraphy of total metals in PIRLA sediment cores

Sediment cores from 30 low-alkalinity lakes in northern New England (NE), New York (NY), the northern Great Lakes States (NGLS) of Minnesota, Michigan, and Wisconsin, and Florida (FL) have been dated by ²¹⁰Pb and analyzed for water and organic content, eight major elements (Al, Ti, Fe, Mn, Ca, Mg, Na, K) plus four trace metals (Pb, Zn, Cu, and V). Variations in the percentages of major elements through time are dominated by long-term independent variations in the abundance of SiO₂, FeO, and to a lesser extent Ca and Al. Additional variations are caused by varying proportions of inorganic matter. Major variations in chemistry are generally unrelated to documented distrubances in the watersheds; most disturbances are minor fires or selective logging.Accelerated accumulation of Pb from atmospheric sources into sediment first occurs in sediment dated between 1800 and 1850 in NY and NE, slightly later in the NGLS region, and about 1900 in FL. Modern accumulation rates in all areas are comparable (ca. 1 to 4 g cm^–2 yr^–1). Accumulation rates of Pb in some lakes have declined significantly from 1975 to 1985. Atmospheric deposition of anthropogenic Zn and Cu is also indicated by generally increasing accumulation rates in sediment cores, but the record is not as clear nor are chemical profiles in all lakes parallel to the trends in atmospheric emissions inferred on the basis of fossil fuel consumption, smelting, and other industrial activities. Inter-lake variations in profiles of Cu and Zn are large. Vanadium accumulation rates increase by the 1940s in NY and NE, but not until the 1950s in the NGLS region. This timing correlates with regional trends in the combustion of fuel oil, a major source of atmospheric V.Acidification of some of the lakes is suggested by decreases in the concentration and accumulation rates of Mn, Ca, and Zn in recent sediment, relative to other elements of catchment origin. The decreases generally occur slightly before the onset of acidification as indicated by diatoms. Increased sediment accumulation rates for Fe may indicate the acidification of watershed soils. The use of the accumulation rate of TiO₂ as an indicator of rates of erosion and for normalization of trace metal accumulation rates is in question for lakes where the flux of TiO₂ from the atmosphere varies and is a significant fraction of the total flux of TiO₂ to the sediment.This is the thirteenth of a series of papers to be published by this journal which is a contribution of the Paleoecological Investigation of Recent Lake Acidification (PIRLA) project. Drs. D. F. Charles and D. R. Whitehead are guest editors for this series.     

Sediment Stratigraphy and Heavy Metal Fluxes to Reservoirs in the Southern Pennine Uplands, UK

Reservoir sediments are rarely used as environmental archives because of the potential for sediment disturbance by fluctuating water levels. However, rapid rates of sedimentation, proximity to urban centres and often the existence of management records, may make them potentially important resources for reconstructing recent, anthropogenically-derived environmental change. This project assesses the potential of reservoir sedimentary records for reconstructing past atmospheric and drainage basin fluxes of heavy metals (manganese, iron, nickel, copper, zinc and lead) in the southern Pennines, UK. Five reservoirs were selected on the basis of management history and drainage basin characteristics. Multi-parameter analysis showed sediments to be replicable across the ȁ8accumulating zone’ with reasonably consistent rates of sedimentation. Water level fluctuations were not found to detrimentally affect sediment records in the deepwater area of the reservoirs. In fact, spheroidal carbonaceous particle (SCP) profiles show trends in inputs that closely reflect major changes in industrialisation, indicating the reservoir sediments to be excellent records of particulate inputs. Only lead (Pb) and zinc (Zn) were significantly enriched in the reservoir sediment in comparison to background levels. Manganese (Mn), iron (Fe) and to a limited degree, copper (Cu), appeared to be affected by post-deposition mobility. Preliminary calculations of Pb fluxes indicate that over 80% of the current Pb input to the reservoirs is from Pb deposited onto drainage basin soils in the past, rather than from direct atmospheric deposition or natural background inputs. In Howden reservoir, for example, the total Pb flux to deepwater sediment cores in 2000 was 119 mg m⁻² a⁻¹. Of this, an estimated 99 mg m⁻² a⁻¹ was from anthropogenically-derived Pb, initially deposited onto drainage basin soils and subsequently entering the reservoir via erosion and leaching processes. There is, therefore, no indication that the flux of Pb to the aquatic system is declining in response to reductions in Pb deposition. The ecotoxicological effects of the high and continuing Pb flux to these reservoirs, despite recent decreases in atmospheric deposition, is an area requiring further investigation.     

Sources and chronology of fifteen elements in the sediments of lakes affected by metal deposition in a mining area

Sources and chronologies of metal contamination were studied in sediment cores of three lakes of the Rouyn-Noranda mining area (Québec, Canada) affected by atmospheric deposition of anthropogenic contaminants. One of the three lakes also received acid mine drainage. The sediments were dated using ²¹⁰Pb and ¹³⁷Cs and analysed for stable Pb isotope ratios and for total concentrations of 15 elements (Ag, Al, Au, Ca, Cu, Cd, Fe, Hg, Mn, Ni, P, Pb, S, Ti, Zn). Stable lead isotopic signatures helped to determine the quantitative contributions of different industrial Pb sources to our sampling sites. This source apportionment showed the dominant influence of the Rouyn-Noranda copper smelter in airborne Pb emissions for the decades following 1926, when industrialization began in the region. The smelter source had a low ratio of ²⁰⁶Pb/²⁰⁷Pb ranging between 0.90 and 1.05, as typical of the Abitibi Archean sulphides. The relationships between element (metal) sedimentary fluxes and anthropogenic Pb fluxes allowed us to infer the origin of the anthropogenic source. These relationships strongly suggest that the copper smelter was (and may still be) an atmospheric source of Cd, Cu, Pb, Zn, Ag and Hg to the surrounding lakes. Our study indicates that the efforts made by the Rouyn-Noranda copper smelter to reduce airborne emissions of metals have been translated in reduced atmospheric metal loadings to the surrounding lakes.     

Lake Sediment Core Records of Sulphur Accumulation and Sulphur Isotopic Composition in Central Ontario, Canada Lakes

Stable isotopic compositions and concentrations of total sedimentary sulphur (S) were determined in cores from 6 lakes in the acid-sensitive Muskoka-Haliburton region of south-central Ontario. The isotopic composition of S in deep sediment (> ~ 20 cm) was approximately constant in all lakes, and indicated a pre-industrial δ ³⁴S value between +4.0 and +5.3‰, which is similar to current bulk deposition. Similarly, total S concentrations in deep sediment were relatively low (1.9–5 mg S g⁻¹ dwt) and approximately constant with depth within cores. All lakes exhibited up-core increases in total S and decreases in δ ³⁴S at a depth corresponding to the beginning of industrialization in the Great Lakes region ( ~ 1900), resulting in a generally reciprocal depth pattern between total S concentration and δ ³⁴S ratios. While initial shifts in total S and δ ³⁴S were likely due to enhanced SO₄ reduction of newly available anthropogenic SO₄, both the magnitude and pattern of up-core S enrichment and shifts in δ ³⁴S varied greatly among lakes, and did not match changes in S deposition post 1900. Differences between lakes in total S and δ ³⁴S were not related to any single hydrologic (e.g., residence time) or physical (e.g., catchment-area-to-lake area ratio) lake characteristic. This work indicates that sediment cores do not provide consistent records of changes in post-industrial S deposition in this region, likely due to redox-related mobility of S in upper sediment.     

A whole-basin, mass-balance approach to paleolimnology

Lake sediments record the flux of materials (nutrients, pollutants, particulates) through a lake system both qualitatively, as changes in the composition of geochemical and biological tracers, as well as quantitatively, through changes in their rate of burial. Burial rates provide a direct link to contemporary (neo-) limnological studies as well as management efforts aimed at load reductions, but are difficult to reconstruct accurately from single cores owing to the spatial and temporal variability of sediment deposition in most lakes. The accurate determination of whole-lake burial rates from analysis of multiple cores, though requiring more effort per lake, can help resolve such problems and improve our understanding of sediment heterogeneity at multiple scales. Partial solutions to these problems also include focusing corrections based on ²¹⁰Pb flux, co-evaluation of concentration profiles, trend analysis using multiple lakes, and trend replication based on a small number of cores from the same lake. Recent multi-core studies demonstrate that no single core site faithfully records the whole-lake time-resolved input of materials, but that as few as five well-placed cores can provide a reliable record of whole-lake sediment flux for morphometrically simple basins. Lake-wide sediment fluxes can be coupled with reconstructed outflow losses to calculate historical changes in watershed and atmospheric loading of nutrients, metals, and other constituents. The ability of paleolimnology to accurately assess the sedimentary flux and extend the period of reference into the distant past represents an important contribution to the understanding of biogeochemical processes and their response to human and natural disturbance.     

The temporal record and sources of atmospherically deposited fly-ash particles in Lake Akagi-konuma,a Japanese mountain lake

Fly-ash particles comprising spheroidal carbonaceous particles (SCP) and inorganic ash spheres (IAS), produced from industrial fossil-fuel combustion, are found in lake sediments throughout the world where they provide an historical record of atmospheric pollutant deposition. These particles have been widely used to assess the temporal and spatial distribution of industrial atmospheric pollution in both freshwater and terrestrial environments in Europe and the USA. However, there have been very few palaeolimnological fly-ash studies undertaken in Japan and none in Japanese mountain lakes. Here, we present the historical SCP and IAS records from a radiometrically dated sediment core taken from Lake Akagi-konuma (36°31′ 54″N, 139°11′ 32″E; elevation 1,470 m) located 100 km north-west of Tokyo. Meteorological data and back trajectory analyses confirm potential sources both within Japan and further afield in China and South Korea. SCP contamination began in the 1950s and increased rapidly to a peak in the mid-1980s. It is thought this represents contamination of Japanese origin, principally oil-fired power stations within 150 km of the lake. The profile of IAS, almost solely coal-derived, shows a rapid increase in the 1970s, in contrast to the record of coal consumption in Japan. The IAS record is therefore thought to reflect long-range transport from coal combustion sources in eastern China which started to expand in the 1970s. This raises concerns over the potential impact on Japanese mountain areas from recent rapid increases in, and predicted acceleration of, emissions from this industrial process. The scale of SCP contamination recorded in Lake Akagi-konuma is equivalent to moderately impacted mountain lakes in Europe, but is at the upper end of the range for remote lakes in the western United States.     

The sedimentary record of spheroidal carbonaceous fly-ash particles in shallow Danish lakes

Spheroidal carbonaceous particles (SCP) from combustion of oil and coal have been quantified in cores from top sediments of Danish shallow lakes. Chronologies were provided by ²¹⁰Pb-dating supplemented by measurements of other radionuclides (¹³⁷Cs, ¹³⁴Cs, ²⁴¹Am). All cores show indications of sediment mixing but most still retain a characteristic SCP record. Deposition rates of SCP were low until the 1920s, increased strongly after World War II, reached maximum levels around 1970 and decreased thereafter. These results were used to infer a new chronology for a sediment core from a shallow lake, from which a ²¹⁰Pb chronology had previously been published.SCP inventories are positively correlated with ²¹⁰Pb inventories and dry matter accumulated since 1900, suggesting that absolute SCP accumulation rates may be more influenced by sedimentary processes than by atmospheric fluxes. The concentrations of SCP in surface sediments of the six lakes do, however, correlate with regional SO₂ emissions.     

Identifying sources of organic matter in sediments of shallow lakes using multiple geochemical variables

We analyzed ²¹⁰Pb-dated sediment cores from four relatively shallow lakes (z_max < 10 m) in the Upper Ocklawaha River Basin, Florida, USA to compare primary producer community structure before and after anthropogenic impacts. We measured physical and chemical sediment variables including density, organic matter (OM), water-soluble phosphorus, polyphosphate (Poly-P), total P (TP), total carbon to total nitrogen mass ratios of OM (TC:TN), biogenic silica (diatoms, sponge spicules), total amorphous silica, and stable carbon and nitrogen isotope ratios of bulk OM. Principal component analysis showed that diatom biogenic silica, TC:TN, Poly-P and TP displayed discernible stratigraphic changes associated with the shift in the primary producer community. We applied k-means cluster analysis to these variables to identify macrophyte-derived, transitional, and phytoplankton-derived sediments. Our approach provides an objective method for identifying sediment sources that may be applied to shallow lakes in other regions. The four study lakes shifted from a macrophyte-dominated state to a transitional state before major anthropogenic disturbances, and became phytoplankton-dominated after ~1950.     

Recent changes in diatom-inferred pH, heavy metals, and spheroidal carbonaceous particles in lake sediments near an oil refinery at Mongstad, Western Norway

Sediments from two naturally acid lakes have been used to investigate whether there is any local impact of atmospheric pollution from an oil refinery at Mongstad in Western Norway. The refinery started production in 1975 and expanded in 1987. One lake was selected as a reference site as it only receives long-range transported air pollution, whereas a second lake was selected as it was expected to receive both long-range transported and local air pollution from the refinery. Heavy metal (Pb, Ni and Zn) and spheroidal carbonaceous particle (SCP) (> 5 µm in diameter) concentrations and accumulation rates have been estimated and lake-water pH has been reconstructed by weighted averaging and weighted averaging partial least squares regression and calibration from the fossil diatom assemblages.Heavy metals that are in the size range for which atmospheric residence time is greatest do not show any enhanced levels in the sediments after 1975 that could be associated with local impacts from the refinery. SCPs in the sediments that are in the size range thought to be effectively removed by dry deposition, and thus have a more local deposition pattern, show an increase after 1975 and an additional large increase after 1987 that can be explained by impacts from the local oil refinery. After 1975 the SCP diameter distribution changed from being dominated by SCPs with a small diameter in the range 5-10 µm to SCPs with larger diameters. The SO₂ emission from the oil refinery seems to have had no significant effect on lake pH. The reconstructed lake pH history is complex, possibly related to land-use changes and long-range transported air pollution.     

Isotope record of anthropogenic lead pollution in lake sediments of Florida, USA

We examined the anthropogenic lead (Pb) burden that accumulated in sediment of lakes in the southeastern USA during the last ~150 years. Mining, smelting, agriculture, and fossil-fuel combustion are known to have contributed to Pb pollution in lakes of other regions. Few studies, however, have examined Pb sequestered in lakes of the southeastern USA, particulary peninsular Florida, which is subject to less continental atmospheric influence than other regions of the eastern USA. We obtained sediment cores from Little Lake Jackson and Little Lake Bonnet in Highlands County, Florida and used Pb isotopes in the records to identify principal sources of Pb contamination. The sediment records showed that changes in Pb concentration and isotope ratios correspond temporally with gasoline consumption in the USA, as well as with changes in lead ores used to produce leaded gasoline. Lead concentrations in the study lakes showed temporal variations that were similar to those found in peat records from east-central Florida. Isotope trends were similar to the mean USA atmospheric Pb deposition record, and to Pb isotope records from Bermuda and Atlantic corals. We modeled the isotopic composition of the anthropogenic Pb in lake sediments and found that the overall trend is controlled by Pb that was released during leaded gasoline combustion. There is, however, additional Pb at each site that comes from sources that are not fully represented by the natural, background Pb. Lead isotope ratios and Pb/arsenic (As) ratios provide evidence that Pb deposition in lakes during the middle 1900s might have been influenced by lead arsenate applications to golf courses, a source that is often ignored in Pb isotope studies. Isotope evidence confirms, however, that following cessation of commercial lead arsenate use in the 1960s, atmospheric alkyl lead was again the primary influence on Pb in sediments of the study lakes.     

The spatial and temporal distribution of fossil-fuel dervied pollutants in the sediment record of Lake Baikal, east Siberia

Spatial and temporal patterns of spheroidal carbonaceous particles (SCP) extracted from lake sediments provide an unambiguous record of the distributions of fossil-fuel derived pollutants. When applied to sediment cores taken from Lake Baikal spatial patterns show good agreement with the distribution of industry, with the highest concentrations found in the southern basin nearest to Irkutsk. SCP were found to occur in all cores from all areas of the lake in contrast to metal results where anthropogenically enhanced deposition was only demonstrable in the southern basin. SCP distribution within the sediments of Lake Baikal is seen to be distinctly regional and therefore long distance transport is not thought to be an important pathway for these pollutants. Temporal patterns of SCP show trends that reflect the development of industry in the area since the 1940s. Settling rates in the 1600 m water column suggest that the SCP sediment record may be approximately an order of magnitude more sensitive to depositional changes than that of trace metals.