Stuart Hankin

Movement of a tritium plume in shallow groundwater at a legacy low-level radioactive waste disposal site in eastern Australia.

Between 1960 and 1968 low-level radioactive waste was buried in a series of shallow trenches near the Lucas Heights facility, south of Sydney, Australia. Groundwater monitoring carried out since the mid 1970s indicates that with the exception of tritium, no radioactivity above typical background levels has been detected outside the immediate vicinity of the trenches. The maximum tritium level detected in ground water was 390 kBq/L and the median value was 5400 Bq/L, decay corrected to the time of disposal. Since 1968, a plume of tritiated water has migrated from the disposal trenches and extends at least 100 m from the source area. Tritium in rainfall is negligible, however leachate from an adjacent and fill represents a significant additional tritium source. Study data indicate variation in concentration levels and plume distribution in response to wet and dry climatic periods and have been used to determine pathways for tritium migration through the subsurface.

Uranium and other contaminant migration in groundwater at a tropical Australian Uranium Mine

Hydrogeochemical modelling (utilising the modelling tools MODFLOW, MT3D and HARPHRQ) has been used in conjunction with laboratory-based experiments and a field monitoring program to investigate the fate of uranium and other contaminants in excess water sprayed on a 33 ha region of the Ranger Uranium Mine (RUM), northern Australia. The results indicate that uranium is retained in the surficial layer of the lateritic soils of the area. Conservative contaminants are not retained by the soils and are transported into the groundwater. Subsequently, they migrate relative to the groundwater flow rate towards the river system down hydraulic gradient of the irrigation area.

Groundwater residence time in a dissected and weathered sandstone plateau: Kulnura–Mangrove Mountain aquifer, NSW, Australia

Groundwater residence time in the Kulnura–Mangrove Mountain aquifer was assessed during a multi-year sampling programme using general hydrogeochemistry and isotopic tracers (H2O stable isotopes, δ13CDIC, 3H, 14C and 87Sr/86Sr). The study included whole-rock analysis from samples recovered during well construction at four sites to better characterise water–rock interactions. Based on hydrogeochemistry, isotopic tracers and mineral phase distribution from whole-rock XRD analysis, two main groundwater zones were differentiated (shallow and deep). The shallow zone contains oxidising Na–Cl-type waters, low pH, low SC and containing 3H and 14C activities consistent with modern groundwater and bomb pulse signatures (up to 116.9 pMC). In this shallow zone, the original Hawkesbury Sandstone has been deeply weathered, enhancing its storage capacity down to ∼50 m below ground surface in most areas and ∼90 m in the Peats Ridge area. The deeper groundwater zone was also relatively oxidised with a tendency towards Ca–HCO3-type waters, although with higher pH and SC, and no 3H and low 14C activities consistent with corrected residence times ranging from 11.8 to 0.9 ka BP. The original sandstone was found to be less weathered with depth, favouring the dissolution of dispersed carbonates and the transition from a semi-porous groundwater media flow in the shallow zone to fracture flow at depth, with both chemical and physical processes impacting on groundwater mean residence times. Detailed temporal and spatial sampling of groundwater revealed important inter-annual variations driven by groundwater extraction showing a progressive influx of modern groundwater found at >100 m in the Peats Ridge area. The progressive modernisation has exposed deeper parts of the aquifer to increased NO3− concentrations and evaporated irrigation waters. The change in chemistry of the groundwater, particularly the lowering of groundwater pH, has accelerated the dissolution of mineral phases that would generally be inactive within this sandstone aquifer triggering the mobilisation of elements such as aluminium in the aqueous phase.

Evaporative isotope enrichment as a constraint on reach water balance along a dryland river

Abstract Deuterium and oxygen-18 enrichment in river water during its transit across dryland region is found to occur systematically along evaporation lines with slopes of close to 4 in 2H–18O space, largely consistent with trends predicted by the Craig–Gordon model for an open-water dominated evaporating system. This, in combination with reach balance assessments and derived runoff ratios, strongly suggests that the enrichment signal and its variability in the Barwon–Darling river, Southeastern Australia is acquired during the process of evaporation from the river channel itself, as enhanced by the presence of abundant weirs, dams and other storages, rather than reflecting inherited enrichment signals from soil water evaporation in the watershed. Using a steady-state isotope mass balance analysis based on monthly 18O and 2H, we use the isotopic evolution of river water to re-construct a perspective of net exchange between the river and its contributing area along eight reaches of the river during a drought period from July 2002 to December 2003, including the duration of a minor flow event. The resulting scenario, which uses a combination of climatological averages and available real-time meteorological data, should be viewed as a preliminary test of the application rather than as a definitive inventory of reach water balance. As expected for a flood-driven dryland system, considerable temporal variability in exchange is predicted. While requiring additional real-time isotopic data for operational use, the method demonstrates potential as a non-invasive tool for detecting and quantifying water diversions, one that can be easily incorporated within existing water quality monitoring activities.

Assessing Connectivity Between an Overlying Aquifer and a Coal Seam Gas Resource Using Methane Isotopes, Dissolved Organic Carbon and Tritium

Coal seam gas (CSG) production can have an impact on groundwater quality and quantity in adjacent or overlying aquifers. To assess this impact we need to determine the background groundwater chemistry and to map geological pathways of hydraulic connectivity between aquifers. In south-east Queensland (Qld), Australia, a globally important CSG exploration and production province, we mapped hydraulic connectivity between the Walloon Coal Measures (WCM, the target formation for gas production) and the overlying Condamine River Alluvial Aquifer (CRAA), using groundwater methane (CH4) concentration and isotopic composition (δ13C-CH4), groundwater tritium (3H) and dissolved organic carbon (DOC) concentration. A continuous mobile CH4 survey adjacent to CSG developments was used to determine the source signature of CH4 derived from the WCM. Trends in groundwater δ13C-CH4 versus CH4 concentration, in association with DOC concentration and 3H analysis, identify locations where CH4 in the groundwater of the CRAA most likely originates from the WCM. The methodology is widely applicable in unconventional gas development regions worldwide for providing an early indicator of geological pathways of hydraulic connectivity.

Trench 'bathtubbing' and surface plutonium contamination at a legacy radioactive waste site.

Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (∼12 Bq/L of 239+240Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest 239+240Pu soil activity was 829 Bq/kg in a shallow sample (0–1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the ‘bathtub’ effect.

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor.

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes. Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of (3)H that were significantly higher (up to ∼700 Bq L(-1)) than local background levels (0-10 Bq L(-1)). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout (3)H but its influence did not reach as far as the disposal trenches. The elevated (3)H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate (3)H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate (3)H variability for any sampled tree at this site. The results demonstrate successful use of (3)H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.

Identification of sources and processes in a low-level radioactive waste site adjacent to landfills: groundwater hydrogeochemistry and isotopes

Multiple tracer-element and isotope approaches were applied at a 1960s-era low-level radioactive waste burial site located in the Lucas Heights area on the southwest urban fringe of Sydney, Australia. The site is situated among other municipal and industrial (solid and liquid) waste disposal sites causing potential mixing of leachates. Local rainfall contains marine-derived major ion ratios that are modified during infiltration depending on waste interactions. The local geology favours the retention of contaminants by ion-exchange processes within the clay-rich soils and the shale layer underlying the burial site. Local soils experience periodic infiltration and wetting fronts that can fully saturate the waste trenches (bathtub effect) while surrounding soils are mostly unsaturated with discontinuous perched lenses. Within the trenches, the degradation of organic matter results in localised methanogenesis, as suggested by enriched δ2H and δ13CDIC values in adjacent subsurface water. Movement of contaminants from the trenches is indicated by Na+, Br− and I− concentrations, variations in 87Sr/86Sr, enriched δ13CDIC values and evolution of δ34S of dissolved sulfate in perched water bodies above the shale. Although transport is limited by the low transmissivity of the clay-rich soils, migration and mixing processes are indicated by the variation of concentrations with distance from the trenches, disappearance of δ2H enrichments, mixing with other sources of Sr and sulfate isotope fractionations. The depth distribution of waste-derived contaminants (specifically 3H and Be) between the perched water surrounding the trenches, and the underlying shale and sandstone layers, indicates limited downward transport of contaminants. Past removal of the shale layer in an adjacent site, Harringtons Quarry, has facilitated the mixing of some municipal waste leachates (characterised by circum-neutral pH, high alkalinity, low sulfate, high 3H, high Be, enriched δ2H and δ13CDIC) into the underlying groundwater system as suggested by high TDS, Cl−/Br− ratios, Be and 3H found in deeper wells. This study demonstrates the applicability of using trace elements, stable- and radio-isotopes to document the existing geochemistry and the contaminant transport from the waste trenches. The multiple tracer approach addresses the complexities of transport at the site and differentiates various municipal, industrial and radioactive waste sources.

Seasonal total methane depletion in limestone caves

Methane concentration in caves is commonly much lower than the external atmosphere, yet the cave CH4 depletion causal mechanism is contested and dynamic links to external diurnal and seasonal temperature cycles unknown. Here, we report a continuous 3-year record of cave methane and other trace gases in Jenolan Caves, Australia which shows a seasonal cycle of extreme CH4 depletion, from ambient ~1,775 ppb to near zero during summer and to ~800 ppb in winter. Methanotrophic bacteria, some newly-discovered, rapidly consume methane on cave surfaces and in external karst soils with lifetimes in the cave of a few hours. Extreme bacterial selection due to the absence of alternate carbon sources for growth in the cave environment has resulted in an extremely high proportion 2–12% of methanotrophs in the total bacteria present. Unexpected seasonal bias in our cave CH4 depletion record is explained by a three-step process involving methanotrophy in aerobic karst soil above the cave, summer transport of soil-gas into the cave through epikarst, followed by further cave CH4 depletion. Disentangling cause and effect of cave gas variations by tracing sources and sinks has identified seasonal speleothem growth bias, with implied palaeo-climate record bias.

Chemical characterisation and source identification of atmospheric aerosols in the Snowy Mountains, south-eastern Australia

Characterisation of atmospheric aerosols is of major importance for: climate, the hydrological cycle, human health and policymaking, biogeochemical and palaeo-climatological studies. In this study, the chemical composition and source apportionment of PM2.5 (particulate matter with aerodynamic diameters less than 2.5μm) at Yarrangobilly, in the Snowy Mountains, SE Australia are examined and quantified. A new aerosol monitoring network was deployed in June 2013 and aerosol samples collected during the period July 2013 to July 2017 were analysed for 22 trace elements and black carbon by ion beam analysis techniques. Positive matrix factorisation and back trajectory analysis and trajectory clustering methods were employed for source apportionment and to isolate source areas and air mass travel pathways, respectively. This study identified the mean atmospheric PM2.5 mass concentration for the study period was (3.3±2.5)μgm-3. It is shown that automobile (44.9±0.8)%, secondary sulfate (21.4±0.9)%, smoke (12.3±0.6)%, soil (11.3±0.5)% and aged sea salt (10.1±0.4)% were the five PM2.5 source types, each with its own distinctive trends. The automobile and smoke sources were ascribed to a significant local influence from the road network and bushfire and hazard reduction burns, respectively. Long-range transport are the dominant sources for secondary sulfate from coal-fired power stations, windblown soil from the inland saline regions of the Lake Eyre and Murray-Darling Basins, and aged sea salt from the Southern Ocean to the remote alpine study site. The impact of recent climate change was recognised, as elevated smoke and windblown soil events correlated with drought and El Niño periods. Finally, the overall implications including potential aerosol derived proxies for interpreting palaeo-archives are discussed. To our knowledge, this is the first long-term detailed temporal and spatial characterisation of PM2.5 aerosols for the region and provides a crucial dataset for a range of multidisciplinary research.