An assessment of contamination pickup on ground robotic vehicles for nuclear surveying application.

Ground robotic vehicles are often deployed to inspect areas where radioactive floor contamination is a prominent risk. However, the accuracy of detection could be adversely affected by enhanced radiation signal through self-contamination of the robot occurring over the course of the inspection. In this work, it was hypothesised that a six-legged robot could offer advantages over the more conventional ground robotic devices such as wheeled and tracked rovers. To investigate this, experimental contamination testing and computational Monte Carlo simulation techniques (GEANT4) were employed to understand how radioactive contamination pick-up on three different robotic vehicles would affect their detection accuracy. Two robotic vehicles were selected for comparison with the hexapod robot based on their type of locomotion; a wheeled rover and a tracked rover. With the aid of a non-toxic fluorescent tracer dust, the contamination received by the all three vehicles when traversing a contaminated area was initially compared through physical inspection using high definition cameras. The parametric results from these tests where used in the computational study carried out in GEANT4. A cadmium zinc telluride detector was simulated at heights ranging from 10 to 50 cm above each contaminated vehicle, as if it were mounted on a plinth. Assuming a uniform activity of 60 Bq cm-2on all contaminated surfaces, the results suggested that due to the hexapod's small ground-contacting surface area and geometry, radiation detection rates using an uncollimated detector are likely to be overestimated by between only 0.07%-0.12%, compared with 3.95%-8.43% and 1.75%-14.53% for the wheeled and tracked robot alternatives, respectively.

The kinetics and mechanism of the uranium hydride - water vapour system under ambient conditions.

This work investigated the reaction of uranium hydride powder with saturated water vapour at 25 °C. Two corrosion experiments were conducted one with deionised water (H2O) and one with deuterated water (D2O). The kinetics of the reaction were measured through gas generation method while concurrent residual gas analysis (RGA) allowed better understanding of the oxidation mechanism governing the system. From the analysis, it was found that the kinetics of the reaction are robust initially, followed by quasi-linear decelerating regime indicative of a 'shrinking core' type oxidation behaviour. The extent of the reaction (conversion to UO2) was lower in comparison to other works. The reaction remained incomplete bolstering the case of UH3 persistence in legacy wastes. Through interpretation of the gas analysis data, a mechanism for the uranium hydride water reaction was suggested.

A review of the reaction rates of uranium corrosion in water.

This work conducts a review on the kinetics of the uranium and water reaction system by gathering all available kinetic data and across a wide range of reaction conditions. Temperature and pressure dependent kinetic equations that describe the reaction are derived for the uraniumwater vapour and uranium-liquid water systems. Detailed tables which provide information about the reaction conditions and other parameters for each rate point are constructed. From evaluation of the tables, the effects of underlying parameters on the reaction kinetics are discussed. It is suggested that these parameters contribute to the reported discrepancies between reaction rate values under similar conditions. Better prediction of the corrosion rate and rate behaviour can be achieved by combining the kinetic rate equations with the effect of these underlying parameters.

Radiological comparison of a FDNPP waste storage site during and after construction.

The clean-up effort that is occurring across the region affected by the 2011 Fukushima Daiichi Nuclear Power Plant accident is unprecedented in its magnitude as well as the financial cost that will eventually result. A major component of this remediation is the stripping of large volumes of material from the land surface, depositing this into large waste storage bags before placing these 1 cubic meter bags into specially constructed stores across Fukushima Prefecture. In this work, using an unmanned aerial vehicle to perform radiological surveys of a site, the time-resolved distribution of contamination during the construction of one of these waste storage sites was assessed. The results indicated that radioactive material was progressively leaching from the store into the surrounding environment. A subsequent survey of the site conducted eight months later revealed that in response to this survey and remedial actions, the contamination issue once existing on this site had been successfully resolved. Such results highlight the potential of low-altitude unmanned aerial systems to easily and rapidly assess site-wide changes over time - providing highly-visual results; therefore, permitting for prompt remedial actions to be undertaken as required. Use of UAV radiation mapping and airborne photogrammetry to produce a time-resolved assessment of remediation efforts within a Fukushima temporary storage facility.

Validation of a novel radiation mapping platform for the reduction of operator-induced shielding effects.

With extensive remediation currently ongoing because of the Fukushima Daiichi Nuclear Power Plant accident, there exists the even greater need to provide a system with which the distribution of radiation (specifically radiocesium) can be rapidly determined across extensive areas, yet at high (metre or sub-metre) spatial resolutions. Although a range of potential survey methods have been utilised (e.g. fixed-wing aircraft, helicopter, vehicular and more-recently unmanned aerial vehicle) to characterise the distribution of radiological contamination, ground-based (on-foot) methods that employ human operatives to traverse sites of interest remains one of the primary methods through which to perform routine radiological site surveys. Through the application of a newly-developed platform carried as a backpack-contained unit, it was possible to map sites at twice the rate previously possible-reducing not only the exposure time of the operator to ionising radiation, but also dramatically reducing the level of radiation attenuation (introduced by the operator) onto the detector. Like magnetometry platforms used during geological ore prospecting, this system was similarly boom-based, extending sideways away from the central operator. While conventional radiological survey platforms require a correction be performed on the data to account for the carrier (aircraft, vehicle or human) interception and attenuation incident radiation-this system is shown to not require such a retrospective correction.

In-situ, time resolved monitoring of uranium in BFS:OPC grout. Part 2: Corrosion in water.

To reflect potential conditions in a geological disposal facility, uranium was encapsulated in grout and submersed in de-ionised water for time periods between 2-47 weeks. Synchrotron X-ray Powder Diffraction and X-ray Tomography were used to identify the dominant corrosion products and measure their dimensions. Uranium dioxide was observed as the dominant corrosion product and time dependent thickness measurements were used to calculate oxidation rates. The effectiveness of physical and chemical grout properties to uranium corrosion and mobilisation is discussed and Inductively Coupled Plasma Mass Spectrometry was used to measure 238U(aq) content in the residual water of several samples.

Source identification of uranium-containing materials at mine legacy sites in Portugal.

Whilst prior nuclear forensic studies have focused on identifying signatures to distinguish between different uranium deposit types, this paper focuses on providing a scientific basis for source identification of materials from different uranium mine sites within a single region, which can then be potentially used within nuclear forensics. A number of different tools, including gamma spectrometry, alpha spectrometry, mineralogy and major and minor elemental analysis, have been utilised to determine the provenance of uranium mineral samples collected at eight mine sites, located within three different uranium provinces, in Portugal. A radiation survey was initially conducted by foot and/or unmanned aerial vehicle at each site to assist sample collection. The results from each mine site were then compared to determine if individual mine sites could be distinguished based on characteristic elemental and isotopic signatures. Gamma and alpha spectrometry were used to differentiate between samples from different sites and also give an indication of past milling and mining activities. Ore samples from the different mine sites were found to be very similar in terms of gangue and uranium mineralogy. However, rarer minerals or specific impurity elements, such as calcium and copper, did permit some separation of the sites examined. In addition, classification rates using linear discriminant analysis were comparable to those in the literature.

Application of airborne photogrammetry for the visualisation and assessment of contamination migration arising from a Fukushima waste storage facility.

Airborne systems such as lightweight and highly portable unmanned aerial vehicles (UAVs) are becoming increasingly widespread in both academia and industry - with an ever-increasing range of applications, including (but not limited to), air quality sampling, wildlife monitoring and land-use mapping. In this work, high-resolution airborne photogrammetry obtained using a multi-rotor system operating at low survey altitudes, is combined with ground-based radiation mapping data acquired at an interim storage facility for wastes removed as part of the large-scale Fukushima clean-up program. The investigation aimed to assess the extent to which the remediation program at a specific site has contained the stored contaminants, as well as present a new methodology for rapidly surveying radiological sites globally. From the three-dimensional rendering of the site of interest, it was possible to not only generate a powerful graphic confirming the elevated radiological intensity existing at the location of the waste bags, but also to also illustrate the downslope movement of contamination due to species leakage from the large 1m3 storage bags. The entire survey took less than 1 h to perform, and was subsequently post-processed using graphical information software to obtain the renderings. The conclusions within this study not only highlight the usefulness of incorporating three-dimensional renderings within radiation mapping protocols, but also conclude that current methods of monitoring these storage facilities in the long term could be improved through the integration of UAVs within the standard protocol.

In-situ, time resolved monitoring of uranium in BFS:OPC grout. Part 1: Corrosion in water vapour.

Uranium encapsulated in grout was exposed to water vapour for extended periods of time. Through synchrotron x-ray powder diffraction and tomography measurements, uranium dioxide was determined the dominant corrosion product over a 50-week time period. The oxide growth rate initiated rapidly, with rates comparable to the U + H2O reaction. Over time, the reaction rate decreased and eventually plateaued to a rate similar to the U + H2O + O2 reaction. This behaviour was not attributed to oxygen ingress, but instead the decreasing permeability of the grout, limiting oxidising species access to the metal surface.

High-resolution radiation mapping to investigate FDNPP derived contaminant migration.

As of March 2016, five years will have passed since the earthquake and ensuing tsunami that crippled the Fukushima Daiichi Nuclear Power Plant on Japan's eastern coast, resulting in the explosive release of significant quantities of radioactive material. Over this period, significant time and resource has been expended on both the study of the contamination as well as its remediation from the affected environments. Presented in this work is a high-spatial resolution foot-based radiation mapping study using gamma-spectrometry at a site in the contaminated Iitate Village; conducted at different times, seventeen months apart. The specific site selected for this work was one in which consistent uniform agriculture was observed across its entire extent. From these surveys, obtained from along the main northwest trending line of the fallout plume, it was possible to determine the rate of reduction in the levels of contamination around the site attributable to the natural decay of the radiocesium, remediation efforts or material transport. Results from the work suggest that neither the natural decay of radiocesium nor its downward migration through the soil horizons were responsible for the decline in measured activity levels across the site, with the mobilisation of contaminant species likely adhered to soil particulate and the subsequent fluvial transport responsible for the measurable reduction in activity. This transport of contaminant via fluvial methods has already well studied implications for the input of contaminant material entering the neighbouring Pacific Ocean, as well as the deposition of material along rivers within previously decontaminated areas.

Impact of high CO2 on the geochemistry of the coralline algae Lithothamnion glaciale.

Coralline algae are a significant component of the benthic ecosystem. Their ability to withstand physical stresses in high energy environments relies on their skeletal structure which is composed of high Mg-calcite. High Mg-calcite is, however, the most soluble form of calcium carbonate and therefore potentially vulnerable to the change in carbonate chemistry resulting from the absorption of anthropogenic CO2 by the ocean. We examine the geochemistry of the cold water coralline alga Lithothamnion glaciale grown under predicted future (year 2050) high pCO2 (589 µatm) using Electron microprobe and NanoSIMS analysis. In the natural and control material, higher Mg calcite forms clear concentric bands around the algal cells. As expected, summer growth has a higher Mg content compared to the winter growth. In contrast, under elevated CO2 no banding of Mg is recognisable and overall Mg concentrations are lower. This reduction in Mg in the carbonate undermines the accuracy of the Mg/Ca ratio as proxy for past temperatures in time intervals with significantly different carbonate chemistry. Fundamentally, the loss of Mg in the calcite may reduce elasticity thereby changing the structural properties, which may affect the ability of L. glaciale to efficiently function as a habitat former in the future ocean.

Low altitude unmanned aerial vehicle for characterising remediation effectiveness following the FDNPP accident.

On the 12th of March 2011, The Great Tohoku Earthquake occurred 70 km off the eastern coast of Japan, generating a large 14 m high tsunami. The ensuing catalogue of events over the succeeding 12 d resulted in the release of considerable quantities of radioactive material into the environment. Important to the large-scale remediation of the affected areas is the accurate and high spatial resolution characterisation of contamination, including the verification of decontaminated areas. To enable this, a low altitude unmanned aerial vehicle equipped with a lightweight gamma-spectrometer and height normalisation system was used to produce sub-meter resolution maps of contamination. This system provided a valuable method to examine both contaminated and remediated areas rapidly, whilst greatly reducing the dose received by the operator, typically in localities formerly inaccessible to ground-based survey methods. The characterisation of three sites within Fukushima Prefecture is presented; one remediated (and a site of much previous attention), one un-remediated and a third having been subjected to an alternative method to reduce emitted radiation dose.

An investigation into heterogeneity in a single vein-type uranium ore deposit: Implications for nuclear forensics.

Minor element composition and rare earth element (REE) concentrations in nuclear materials are important as they are used within the field of nuclear forensics as an indicator of sample origin. However recent studies into uranium ores and uranium ore concentrates (UOCs) have shown significant elemental and isotopic heterogeneity from a single mine site such that some sites have shown higher variation within the mine site than that seen between multiple sites. The elemental composition of both uranium and gangue minerals within ore samples taken along a single mineral vein in South West England have been measured and reported here. The analysis of the samples was undertaken to determine the extent of the localised variation in key elements. Energy Dispersive X-ray spectroscopy (EDS) was used to analyse the gangue mineralogy and measure major element composition. Minor element composition and rare earth element (REE) concentrations were measured by Electron Probe Microanalysis (EPMA). The results confirm that a number of key elements, REE concentrations and patterns used for origin location do show significant variation within mine. Furthermore significant variation is also visible on a meter scale. In addition three separate uranium phases were identified within the vein which indicates multiple uranium mineralisation events. In light of these localised elemental variations it is recommended that representative sampling for an area is undertaken prior to establishing the REE pattern that may be used to identify the originating mine for an unknown ore sample and prior to investigating impact of ore processing on any arising REE patterns.

An Investigation on the Persistence of Uranium Hydride during Storage of Simulant Nuclear Waste Packages.

Synchrotron X-rays have been used to study the oxidation of uranium and uranium hydride when encapsulated in grout and stored in de-ionised water for 10 months. Periodic synchrotron X-ray tomography and X-ray powder diffraction have allowed measurement and identification of the arising corrosion products and the rates of corrosion. The oxidation rates of the uranium metal and uranium hydride were slower than empirically derived rates previously reported for each reactant in an anoxic water system, but without encapsulation in grout. This was attributed to the grout acting as a physical barrier limiting the access of oxidising species to the uranium surface. Uranium hydride was observed to persist throughout the 10 month storage period and industrial consequences of this observed persistence are discussed.

The use of unmanned aerial systems for the mapping of legacy uranium mines.

Historical mining of uranium mineral veins within Cornwall, England, has resulted in a significant amount of legacy radiological contamination spread across numerous long disused mining sites. Factors including the poorly documented and aged condition of these sites as well as the highly localised nature of radioactivity limit the success of traditional survey methods. A newly developed terrain-independent unmanned aerial system [UAS] carrying an integrated gamma radiation mapping unit was used for the radiological characterisation of a single legacy mining site. Using this instrument to produce high-spatial-resolution maps, it was possible to determine the radiologically contaminated land areas and to rapidly identify and quantify the degree of contamination and its isotopic nature. The instrument was demonstrated to be a viable tool for the characterisation of similar sites worldwide.

Comparison between magnetic force microscopy and electron back-scatter diffraction for ferrite quantification in type 321 stainless steel.

Several analytical techniques that are currently available can be used to determine the spatial distribution and amount of austenite, ferrite and precipitate phases in steels. The application of magnetic force microscopy, in particular, to study the local microstructure of stainless steels is beneficial due to the selectivity of this technique for detection of ferromagnetic phases. In the comparison of Magnetic Force Microscopy and Electron Back-Scatter Diffraction for the morphological mapping and quantification of ferrite, the degree of sub-surface measurement has been found to be critical. Through the use of surface shielding, it has been possible to show that Magnetic Force Microscopy has a measurement depth of 105-140 nm. A comparison of the two techniques together with the depth of measurement capabilities are discussed.

Nuclear waste viewed in a new light; a synchrotron study of uranium encapsulated in grout.

How do you characterise the contents of a sealed nuclear waste package without breaking it open? This question is important when the contained corrosion products are potentially reactive with air and radioactive. Synchrotron X-rays have been used to perform micro-scale in-situ observation and characterisation of uranium encapsulated in grout; a simulation for a typical intermediate level waste storage packet. X-ray tomography and X-ray powder diffraction generated both qualitative and quantitative data from a grout-encapsulated uranium sample before, and after, deliberately constrained H2 corrosion. Tomographic reconstructions provided a means of assessing the extent, rates and character of the corrosion reactions by comparing the relative densities between the materials and the volume of reaction products. The oxidation of uranium in grout was found to follow the anoxic U+H2O oxidation regime, and the pore network within the grout was observed to influence the growth of uranium hydride sites across the metal surface. Powder diffraction analysis identified the corrosion products as UO2 and UH3, and permitted measurement of corrosion-induced strain. Together, X-ray tomography and diffraction provide means of accurately determining the types and extent of uranium corrosion occurring, thereby offering a future tool for isolating and studying the reactions occurring in real full-scale waste package systems.

Lightweight aerial vehicles for monitoring, assessment and mapping of radiation anomalies.

The Fukushima Daiichi nuclear power plant (FDNPP) incident released a significant mass of radioactive material into the atmosphere. An estimated 22% of this material fell out over land following the incident. Immediately following the disaster, there was a severe lack of information not only pertaining to the identity of the radioactive material released, but also its distribution as fallout in the surrounding regions. Indeed, emergency aid groups including the UN did not have sufficient location specific radiation data to accurately assign exclusion and evacuation zones surrounding the plant in the days and weeks following the incident. A newly developed instrument to provide rapid and high spatial resolution assessment of radionuclide contamination in the environment is presented. The device consists of a low cost, lightweight, unmanned aerial platform with a microcontroller and integrated gamma spectrometer, GPS and LIDAR. We demonstrate that with this instrument it is possible to rapidly and remotely detect ground-based radiation anomalies with a high spatial resolution (<1 m). Critically, as the device is remotely operated, the user is removed from any unnecessary or unforeseen exposure to elevated levels of radiation.

Nanoscale zero-valent iron: future prospects for an emerging water treatment technology.

For the past 15 years, nanoscale metallic iron (nZVI) has been investigated as a new tool for the treatment of contaminated water and soil. The technology has reached commercial status in many countries worldwide, however is yet to gain universal acceptance. This review summarises our contemporary knowledge of nZVI aqueous corrosion, manufacture and deployment, along with methods to enhance particle reactivity, stability and subsurface mobility. Reasons for a lack of universal acceptance are also explored. Key factors include: concerns over the long-term fate, transformation and ecotoxicity of nZVI in environmental systems and, a lack of comparable studies for different nZVI materials and deployment strategies. It is highlighted that few investigations to date have examined systems directly analogous to the chemistry, biology and architecture of the terrestrial environment. Such emerging studies have highlighted new concerns, including the prospect for remobilisation of heavy metals and radionuclides over extended periods. The fundamental importance of being able to accurately predict the long-term physical, chemical and biological fate of contaminated sites following nZVI treatment is emphasised and, as part of this, a universal empirical testing framework for nZVI is suggested.

Reduction of carbon dioxide on jet spray formed titanium dioxide surfaces.

The photocatalytic reduction of carbon dioxide (CO(2)) on jet spray formed titanium dioxide (TiO(2)) was studied using light-emitting diode (LED) illumination centred at a wavelength of 388 nm. In addition, the photocatalytic reduction of CO(2) under soft X-ray irradiation was also studied. Specifically, the experiments examined the reduction of CO(2) in a gaseous and liquid-gas system using residual gas analysis mass spectrometry. A photochemical reduction of CO(2) was observed over a course of 250 min, with transformation to a major product, C(2)H(3)O(-) (ethenolate), until equilibrium was reached. The product was observed to be surface stabilised, with it reverting back to CO(2) over the course of 100 min without illumination. A proposed free radical mechanism is presented for the formation of this product. A similar effect to that of UV illumination is also observed to occur under the influence of soft X-rays, which presents a potentially significant alternative method for the activation of TiO(2).