East Kilbride, United Kingdom
East Kilbride, United Kingdom

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Fletcher W.J.,University of Manchester | Zielhofer C.,University of Leipzig | Mischke S.,University of Iceland | Bryant C.,NERC Radiocarbon Facility | And 2 more authors.
Quaternary Geochronology | Year: 2017

In lake sediments where terrestrial macrofossils are rare or absent, AMS radiocarbon dating of pollen concentrates may represent an important alternative solution for developing a robust and high resolution chronology suitable for Bayesian modelling of age-depth relationships. Here we report an application of the heavy liquid density separation approach (Vandergoes and Prior, Radiocarbon 45:479–492, 2003) to Holocene lake sediments from karstic Lake Sidi Ali, Morocco. In common with many karstic lakes, a significant lake 14C reservoir effect of 450–900 yr is apparent, evidenced by paired dates on terrestrial macrofossils and either aquatic (ostracod) or bulk sediment samples. AMS dating of 23 pollen concentrates alongside laboratory standards (bituminous coal, anthracite, IAEA C5 wood) was undertaken. Concentrates were prepared using a series of sodium polytungstate (SPT) solutions of progressively decreasing density (1.9–1.15 g/cm3) accompanied by microscopic analysis of the resulting residues to allow quantification of the terrestrial pollen content. The best fractions (typically precipitating at 1.4–1.2 g/cm3) yielded dateable samples of 0.5–5 mg (from sediment samples of ∼15 g), with C content typically ∼50% by weight. Terrestrial pollen purity ranges from 29% to 88% (μ = 67%), reflecting the challenge of isolating pollen grains from common aquatic algae, e.g. Pediastrum and Botryococcus. A Poisson-process Bayesian depositional model incorporating radiocarbon (pollen and macrofossil) and 210Pb/137Cs data is employed. As all pollen samples incorporate some non-terrestrial organic matter, we assume an exponential outlier distribution treating each pollen concentrate datum as an old outlier and terminus post quem. This approach yields strong data-model agreement, and differences between the prior and posterior age distributions are furthermore consistent with theoretical offsets anticipated for the known reservoir ages and sample-specific terrestrial content. This application of the pollen concentrate dating approach reinforces the importance of microscopic inspection of the residues during the separation and sieving stages. Sample specific differences mean that the pollen concentrate preparation cannot be reduced to a simplistic “black box” protocol, and dating and subsequent age-model development must be supported by detailed analysis of the microfossil content of the sediments. © 2017 Elsevier B.V.


Garnett M.H.,NERC Radiocarbon Facility | Gulliver P.,NERC Radiocarbon Facility | Billett M.F.,University of Stirling
Ecohydrology | Year: 2016

Peatland streams typically contain high methane concentrations and act as conduits for the release of this greenhouse gas to the atmosphere. Radiocarbon analysis provides a unique tracer that can be used to identify the methane source, and quantify the time elapsed between carbon fixation and return to the atmosphere as CH4. Few studies - those that have focus largely on sites with bubble (ebullition) emissions - have investigated the 14C age of methane in surface waters because of the difficulty in collecting sufficient CH4 for analysis. Here, we describe new sampling methods for the collection of CH4 samples from CH4-oversaturated peatland streams for radiocarbon analysis. We report the results of a suite of tests, including using methane 14C standards and replicated field measurements, to verify the methods. The methods are not restricted to ebullition sites, and can be applied to peatland streams with lower methane concentrations. We report the 14C age of methane extracted from surface water samples (~4-13l) at two contrasting locations in a temperate raised peat bog. Results indicate substantial spatial variation with ages ranging from ~400 (ditch in afforested peatland) to ~3000years BP (bog perimeter stream). These contrasting ages suggest that methane in stream water can be derived from a wide range of peat depths. This new method provides a rapid (10-15min per sample) and convenient approach, which should make 14CH4 dating of surface water more accessible and lead to an increased understanding of carbon cycling within the soil-water-atmosphere system. © 2015 The Authors. Ecohydrology published by John Wiley & Sons Ltd. © 2016 John Wiley & Sons, Ltd.


Clark K.E.,University of Oxford | Hilton R.G.,Durham University | West A.J.,University of Southern California | Malhi Y.,University of Oxford | And 5 more authors.
Geochemistry, Geophysics, Geosystems | Year: 2013

Mountain rivers play a key role in the delivery of particulate organic carbon (POC) to large river systems and the ocean. Due to the extent of its drainage area and runoff, the Amazon River is one of Earth's most important biogeochemical systems. However, the source of POC eroded from the humid region of the Eastern Andes and the input of fossil POC from sedimentary rocks (POCfossil) remains poorly constrained. Here we collected suspended sediments from the Kosñipata River during flood events to better characterize Andean POC, measuring the nitrogen to organic carbon ratio (N/C), stable carbon isotopes (δ13Corg) and radiocarbon (Δ14Corg). Δ14Corg values ranged from -711‰ to -15‰, and significant linear trends between Δ14Corg, N/C and δ13C org suggested that this reflects the mixing of POCfossil with very young organic matter (Δ14Corg ~ 50‰) from the terrestrial biosphere (POCnon-fossil). Using N/C and Δ14Corg in an end-member mixing analysis, we quantify the fraction of POCfossil (to within 0.1) and find that it contributes a constant proportion of the suspended sediment mass (0.37 ± 0.03%) and up to 80% of total POC. In contrast, the relative contribution of POCnon-fossil was variable, being most important during the rising limb and peak discharges of flood events. The new data shed light on published measurements of "old" POC (low Δ14Corg) in Andean-fed tributaries of the Amazon River, with their Δ 14Corg and δ13Corg values consistent with variable addition of POCfossil. The findings suggest a greater persistence of Andean POC in the lowland Amazon than previously recognized. © 2013. American Geophysical Union. All Rights Reserved.


Hilton R.G.,Durham University | Galy V.,Woods Hole Oceanographic Institution | Gaillardet J.,CNRS Paris Institute of Global Physics | Dellinger M.,CNRS Paris Institute of Global Physics | And 6 more authors.
Nature | Year: 2015

Soils of the northern high latitudes store carbon over millennial timescales (thousands of years) and contain approximately double the carbon stock of the atmosphere. Warming and associated permafrost thaw can expose soil organic carbon and result in mineralization and carbon dioxide (CO 2) release. However, some of this soil organic carbon may be eroded and transferred to rivers. If it escapes degradation during river transport and is buried in marine sediments, then it can contribute to a longer-term (more than ten thousand years), geological CO 2 sink. Despite this recognition, the erosional flux and fate of particulate organic carbon (POC) in large rivers at high latitudes remains poorly constrained. Here, we quantify the source of POC in the Mackenzie River, the main sediment supplier to the Arctic Ocean, and assess its flux and fate. We combine measurements of radiocarbon, stable carbon isotopes and element ratios to correct for rock-derived POC. Our samples reveal that the eroded biospheric POC has resided in the basin for millennia, with a mean radiocarbon age of 5,800 ± 800 years, much older than the POC in large tropical rivers. From the measured biospheric POC content and variability in annual sediment yield, we calculate a biospheric POC flux of teragrams of carbon per year from the Mackenzie River, which is three times the CO 2 drawdown by silicate weathering in this basin. Offshore, we find evidence for efficient terrestrial organic carbon burial over the Holocene period, suggesting that erosion of organic carbon-rich, high-latitude soils may result in an important geological CO 2 sink. © 2015 Macmillan Publishers Limited. All rights reserved.


PubMed | NERC Radiocarbon Facility, University of Stockholm, University Paris - Sud, Woods Hole Oceanographic Institution and 2 more.
Type: Journal Article | Journal: Nature | Year: 2015

Soils of the northern high latitudes store carbon over millennial timescales (thousands of years) and contain approximately double the carbon stock of the atmosphere. Warming and associated permafrost thaw can expose soil organic carbon and result in mineralization and carbon dioxide (CO2) release. However, some of this soil organic carbon may be eroded and transferred to rivers. If it escapes degradation during river transport and is buried in marine sediments, then it can contribute to a longer-term (more than ten thousand years), geological CO2 sink. Despite this recognition, the erosional flux and fate of particulate organic carbon (POC) in large rivers at high latitudes remains poorly constrained. Here, we quantify the source of POC in the Mackenzie River, the main sediment supplier to the Arctic Ocean, and assess its flux and fate. We combine measurements of radiocarbon, stable carbon isotopes and element ratios to correct for rock-derived POC. Our samples reveal that the eroded biospheric POC has resided in the basin for millennia, with a mean radiocarbon age of 5,800 800 years, much older than the POC in large tropical rivers. From the measured biospheric POC content and variability in annual sediment yield, we calculate a biospheric POC flux of 2.2(+1.3)(-0.9) teragrams of carbon per year from the Mackenzie River, which is three times the CO2 drawdown by silicate weathering in this basin. Offshore, we find evidence for efficient terrestrial organic carbon burial over the Holocene period, suggesting that erosion of organic carbon-rich, high-latitude soils may result in an important geological CO2 sink.


Lawson M.,University of Manchester | Lawson M.,ExxonMobil | Polya D.A.,University of Manchester | Boyce A.J.,Scottish Universities Environmental Research Center | And 3 more authors.
Geochimica et Cosmochimica Acta | Year: 2016

Biogeochemical processes that utilize dissolved organic carbon are widely thought to be responsible for the liberation of arsenic from sediments to shallow groundwater in south and southeast Asia. The accumulation of this known carcinogen to hazardously high concentrations has occurred in the primary source of drinking water in large parts of densely populated countries in this region. Both surface and sedimentary sources of organic matter have been suggested to contribute dissolved organic carbon in these aquifers. However, identification of the source of organic carbon responsible for driving arsenic release remains enigmatic and even controversial. Here, we provide the most extensive interrogation to date of the isotopic signature of ground and surface waters at a known arsenic hotspot in Cambodia. We present tritium and radiocarbon data that demonstrates that recharge through ponds and/or clay windows can transport young, surface derived organic matter into groundwater to depths of 44 m under natural flow conditions. Young organic matter dominates the dissolved organic carbon pool in groundwater that is in close proximity to these surface water sources and we suggest this is likely a regional relationship. In locations distal to surface water contact, dissolved organic carbon represents a mixture of both young surface and older sedimentary derived organic matter. Ground-surface water interaction therefore strongly influences the average dissolved organic carbon age and how this is distributed spatially across the field site. Arsenic mobilization rates appear to be controlled by the age of dissolved organic matter present in these groundwaters. Arsenic concentrations in shallow groundwaters (<20 m) increase by 1 μg/l for every year increase in dissolved organic carbon age compared to only 0.25 μg/l for every year increase in dissolved organic carbon age in deeper (>20 m) groundwaters. We suggest that, while the rate of arsenic release is greatest in shallow aquifer sediments, arsenic release also occurs in deeper aquifer sediments and as such remains an important process in controlling the spatial distribution of arsenic in the groundwaters of SE Asia. Our findings suggest that any anthropogenic activities that alter the source of groundwater recharge or the timescales over which recharge takes place may also drive changes in the natural composition of dissolved organic carbon in these groundwaters. Such changes have the potential to influence both the spatial and temporal evolution of the current groundwater arsenic hazard in this region. © 2016 The Authors.


Lawson M.,University of Manchester | Polya D.A.,University of Manchester | Boyce A.J.,Scottish Universities Environmental Research Center | Bryant C.,NERC Radiocarbon Facility | And 3 more authors.
Environmental Science and Technology | Year: 2013

Microbially mediated reductive processes involving the oxidation of labile organic carbon are widely considered to be critical to the release of arsenic into shallow groundwaters in South and Southeast Asia. In areas where there is significant pumping of groundwater for irrigation the involvement of surface-derived organic carbon drawn down from ponds into the underlying aquifers has been proposed but remains highly controversial. Here we present isotopic data from two sites with contrasting groundwater pumping histories that unequivocally demonstrate the ingress of surface pond-derived organic carbon into arsenic-containing groundwaters. We show that pond-derived organic carbon is transported to depths of up to 50 m even in an arsenic-contaminated aquifer in Cambodia thought to be minimally disturbed by groundwater pumping. In contrast, in the extensively exploited groundwaters of West Bengal, we show that pond-derived organic carbon is transported in shallow groundwater to greater depths, in excess of 100 m in the aquifer. Intensive pumping of groundwaters may potentially drive secular increases in the groundwater arsenic hazard in this region by increasing the contribution of bioavailable pond-derived dissolved organic carbon drawn into these aquifer systems and transporting it to greater depths than would operate under natural flow conditions. © 2013 American Chemical Society.


Adams J.L.,UK Center for Ecology and Hydrology | Tipping E.,UK Center for Ecology and Hydrology | Bryant C.L.,NERC Radiocarbon Facility | Helliwell R.C.,James Hutton Institute | And 3 more authors.
Science of the Total Environment | Year: 2015

The riverine transport of particulate organic matter (POM) is a significant flux in the carbon cycle, and affects macronutrients and contaminants. We used radiocarbon to characterise POM at 9 riverine sites of four UK catchments (Avon, Conwy, Dee, Ribble) over a one-year period. High-discharge samples were collected on three or four occasions at each site. Suspended particulate matter (SPM) was obtained by centrifugation, and the samples were analysed for carbon isotopes. Concentrations of SPM and SPM organic carbon (OC) contents were also determined, and were found to have a significant negative correlation. For the 7 rivers draining predominantly rural catchments, PO14C values, expressed as percent modern carbon absolute (pMC), varied little among samplings at each site, and there was no significant difference in the average values among the sites. The overall average PO14C value for the 7 sites of 91.2pMC corresponded to an average age of 680 14C years, but this value arises from the mixing of differently-aged components, and therefore significant amounts of organic matter older than the average value are present in the samples. Although topsoil erosion is probably the major source of the riverine POM, the average PO14C value is appreciably lower than topsoil values (which are typically 100pMC). This is most likely explained by inputs of older subsoil OC from bank erosion, or the preferential loss of high-14C topsoil organic matter by mineralisation during riverine transport. The significantly lower average PO14C of samples from the River Calder (76.6pMC), can be ascribed to components containing little or no radiocarbon, derived either from industrial sources or historical coal mining, and this effect is also seen in the River Ribble, downstream of its confluence with the Calder. At the global scale, the results significantly expand available information for PO14C in rivers draining catchments with low erosion rates. © 2015 Elsevier B.V.


Vihermaa L.E.,University of Glasgow | Waldron S.,University of Glasgow | Garnett M.H.,NERC Radiocarbon Facility | Newton J.,Scottish Universities Environmental Research Center
Biogeosciences | Year: 2014

Knowing the rate at which carbon is cycled is crucial to understanding the dynamics of carbon transfer pathways. Recent technical developments now support measurement of the 14C age of evaded CO2 from fluvial systems, which provides an important "fingerprint" of the source of C. Here we report the first direct measurements of the 14C age of effluxed CO2 from two small streams and two rivers within the western Amazonian Basin. The rate of degassing and hydrochemical controls on degassing are also considered. We observe that CO2 efflux from all systems except for the seasonal small stream was 14C-depleted relative to the contemporary atmosphere, indicating a contribution from "old" carbon fixed before ∼ 1955 AD. Further, "old" CO2 was effluxed from the perennial stream in the rainforest; this was unexpected as here connectivity with the contemporary C cycle is likely greatest. The effluxed gas represents all sources of CO2 in the aquatic system and thus we used end-member analysis to identify the relative inputs of fossil, modern and intermediately aged C. The most likely solutions indicated a contribution from fossil carbon sources of between 3 and 9% which we interpret as being derived from carbonate weathering. This is significant as the currently observed intensification of weather has the potential to increase the future release of old carbon, which can be subsequently degassed to the atmosphere, and so renders older, slower C cycles faster. Thus 14C fingerprinting of evaded CO2 provides understanding which is essential to more accurately model the carbon cycle in the Amazon Basin. © 2014 Author(s).

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