Airborne gamma-ray mapping using fixed-wing vertical take-off and landing (VTOL) uncrewed aerial vehicles.

Low-cost uncrewed aerial vehicles (UAVs) are replacing manned aircraft for airborne radiation mapping applications such as nuclear accident response scenarios or surveying ore deposits and mine sites because of their cost-effectiveness and ability to conduct surveys at lower altitude compared to manned counterparts. Both multi-rotor UAVs and fixed-wing UAVs are well established technologies for aerial radiation mapping applications, however, both also have drawbacks: multi-rotor UAVs are very limited in flight time and range, and fixed-wing UAVs usually require facilities for take-off and landing. A compromise solution is introduced in this work, using a fixed-wing vertical take-off and landing (VTOL) UAV that combines the flexibility of a multi-rotor UAV with the range and flight time of a fixed-wing UAV. The first implementation of a VTOL with radiation mapping capabilities is presented, based on a commercial WingtraOne UAV augmented with CsI scintillator and CZT semiconductor gamma spectrometers. The radiation mapping capabilities of the prototype are demonstrated in a case study, mapping the distribution of radionuclides around the South Terras legacy uranium mine in the south of England, United Kingdom, and the results are compared with previous studies using multi-rotor and manned aircraft to survey the same area.

A highly scalable and autonomous spectroscopic radiation mapping system with resilient IoT detector units for dosimetry, safety and security.

Technologies utilizing radiological materials across power generation, defence, industry, research and medicine have increased the global inventory of highly active and hazardous materials. Consequently, an amplified threat exists of illicitly obtained materials being used as part of hostile acts. The potential for intentional releases occurs alongside risks from natural disasters or facility accidents. In any such event, it is crucial to rapidly assess the release composition and extent of response and remediation activities. Therefore, the deployment of an effective, resilient and autonomous radiation monitoring network is pivotal both during and after an incident. Underpinning this assessment is a detailed understanding of the pre-event or background, radiation levels, the knowledge of which is also essential in assessing a population's dosimetric exposure to, and impact from anthropogenic and naturally occurring/varying sources of ionizing radiation. Presented here is a fully operational cloud-based spectroscopic radiation mapping platform comprising IoT modules compatible with cellular networks, without modification, in over 180 countries. Combined with locally roaming vehicles, a continuous multi-pass radiological characterization of an urban environment was performed. Such IoT devices are deployable as either individual sensors for specific localized temporal events or integrated over a greater time period (and area) to represent a larger static sensor. Over several months of continued operation, more than 1000 000 individual location-referenced gamma-ray spectra were collected and securely uploaded, in real-time, to an online cloud database and automatically characterized via a custom multi-step workflow. Fine-scale local variations in the radiological fingerprint of a 1 km × 1 km urban area were subsequently rendered in near-real-time to an interactive secure online graphical dashboard for temporal, spatial and spectral interrogation by the user. Considerations for the automated 'elastic' handling of ever-expanding volumes of input data have been carried out, facilitating propagation and expansion of the system's database without human input.

Characterisation of rare earth elements and toxic heavy metals in coal and coal fly ash.

Due to increasing demand for rare earth elements (REE), growing concerns over their sustainability, and domination of their supply by China, coal fly ash has recently emerged as a viable target for REE recovery. With billions of tonnes in repositories and still more being generated across the globe, it is necessary to develop environmentally friendly and economical extraction technologies for the recovery of the REEs from coal fly ash, and to consider the environmental implications of such a recovery process. This study reports characterisation of Nigerian simulant coal fly ash, and investigates the distribution and leaching of the REEs and U, Th, As, Cr, Cd and Pb from these materials using ethanoic acid. Significant amounts (14% to 31%) of the REEs were recovered in the acid-soluble fraction of a sequential extraction procedure using ethanoic acid. While the greatest amounts of U (53% to 62%) and Th (89% to 96%) were recovered in the stable residual fraction, significant amounts (3% to 13%) of U were recovered in the acid-soluble fraction. As was the most enriched element in the mobile acid-soluble fraction (46% to 60%), followed by Cd (15% to 34%). These results demonstrate that REEs contained within coal fly ash - especially those sourced from coal-fired power plants burning coal at temperatures between 700 °C and 1100 °C - can be recovered through an environmentally friendly procedure using the cost-effective heap leaching method, with ethanoic acid or the more cheaply-available vinegar as lixiviant. These results are also valuable for cost evaluation of rare earths recovery from coal fly ash generated by fluidised bed combustion coal fired power plants, and the development of methodologies for coal fly ash management.

Miniaturised Low-Cost Gamma Scanning Platform for Contamination Identification, Localisation and Characterisation: A New Instrument in the Decommissioning Toolkit.

Formerly clandestine, abandoned and legacy nuclear facilities, whether associated with civil or military applications, represent a significant decommissioning challenge owing to the lack of knowledge surrounding the existence, location and types of radioactive material(s) that may be present. Consequently, mobile and highly deployable systems that are able to identify, spatially locate and compositionally assay contamination ahead of remedial actions are of vital importance. Deployment imposes constraints to dimensions resulting from small diameter access ports or pipes. Herein, we describe a prototype low-cost, miniaturised and rapidly deployable 'cell characterisation' gamma-ray scanning system to allow for the examination of enclosed (internal) or outdoor (external) spaces for radioactive 'hot-spots'. The readout from the miniaturised and lead-collimated gamma-ray spectrometer, that is progressively rastered through a stepped snake motion, is combined with distance measurements derived from a single-point laser range-finder to obtain an array of measurements in order to yield a 3-dimensional point-cloud, based on a polar coordinate system-scaled for radiation intensity. Existing as a smaller and more cost-effective platform than presently available, we are able to produce a millimetre-accurate 3D volumetric rendering of a space-whether internal or external, onto which fully spectroscopic radiation intensity data can be overlain to pinpoint the exact positions at which (even low abundance) gamma-emitting materials exist.

Radioactive Source Localisation via Projective Linear Reconstruction.

Radiation mapping, through the detection of ionising gamma-ray emissions, is an important technique used across the nuclear industry to characterise environments over a range of length scales. In complex scenarios, the precise localisation and activity of radiological sources becomes difficult to determine due to the inability to directly image gamma photon emissions. This is a result of the potentially unknown number of sources combined with uncertainties associated with the source-detector separation-causing an apparent 'blurring' of the as-detected radiation field relative to the true distribution. Accurate delimitation of distinct sources is important for decommissioning, waste processing, and homeland security. Therefore, methods for estimating the precise, 'true' solution from radiation mapping measurements are required. Herein is presented a computational method of enhanced radiological source localisation from scanning survey measurements conducted with a robotic arm. The procedure uses an experimentally derived Detector Response Function (DRF) to perform a randomised-Kaczmarz deconvolution from robotically acquired radiation field measurements. The performance of the process is assessed on radiation maps obtained from a series of emulated waste processing scenarios. The results demonstrate a Projective Linear Reconstruction (PLR) algorithm can successfully locate a series of point sources to within 2 cm of the true locations, corresponding to resolution enhancements of between 5× and 10×.

Structural and compositional characteristics of Fukushima release particulate material from Units 1 and 3 elucidates release mechanisms, accident chronology and future decommissioning strategy.

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.

Project IPAD, a database to catalogue the analysis of Fukushima Daiichi accident fragmental release material.

The 2011 accident at Japan's Fukushima Daiichi Nuclear Power Plant released a considerable inventory of radioactive material into the local and global environments. While the vast majority of this contamination was in the form of gaseous and aerosol species, of which a large component was distributed out over the neighbouring Pacific Ocean (where it was subsequently deposited), a substantial portion of the radioactive release was in particulate form and was deposited across Fukushima Prefecture. To provide an underpinning understanding of the dynamics of this catastrophic accident, alongside assisting in the off-site remediation and eventual reactor decommissioning activities, the 'International Particle Analysis Database', or 'IPAD', was established to serve as an interactive repository for the continually expanding analysis dataset of the sub-mm ejecta particulate. In addition to a fully interrogatable database of analysis results for registered users (exploiting multiple search methods), the database also comprises an open-access front-end for members of the public to engage with the multi-national analysis activities by exploring a streamlined version of the data.

Project Gatekeeper: An Entrance Control System Embedded Radiation Detection Capability for Security Applications.

Threat assessments continue to conclude that terrorist groups and individuals as well as those wanting to cause harm to society have the ambition and increasing means to acquire unconventional weapons such as improvised nuclear explosive devices and radiological disposal devices. Such assessments are given credence by public statements of intent by such groups/persons, by reports of attempts to acquire radioactive material and by law enforcement actions which have interdicted, apprehended or prevented attempts to acquire such material. As a mechanism through which to identify radioactive materials being transported on an individual's person, this work sought to develop a detection system that is of lower-cost, reduced form-factor and more covert than existing infrastructure, while maintaining adequate sensitivity and being retrofittable into an industry standard and widely utilised Gunnebo Speed Gate system. The system developed comprised an array of six off-set Geiger-Muller detectors positioned around the gate, alongside a single scintillator detector for spectroscopy, triggered by the systems inbuilt existing IR proximity sensor. This configuration served to not only reduce the cost for such a system but also allowed for source localisation and identification to be performed. Utilising the current setup, it was possible to detect a 1 µSv/h source carried into the Speed Gate in all test scenarios, alongside locating and spectrally analysing the material in a significant number.

Compositional and structural analysis of Fukushima-derived particulates using high-resolution x-ray imaging and synchrotron characterisation techniques.

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation x-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site - north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume - bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium (134Cs, 135Cs and 137Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.

Radiation Mapping and Laser Profiling Using a Robotic Manipulator.

The use of a robotic arm manipulator as a platform for coincident radiation mapping and laser profiling of radioactive sources on a flat surface is investigated in this work. A combined scanning head, integrating a micro-gamma spectrometer and Time of Flight (ToF) sensor were moved in a raster scan pattern across the surface, autonomously undertaken by the robot arm over a 600 × 260 mm survey area. A series of radioactive sources of different emission intensities were scanned in different configurations to test the accuracy and sensitivity of the system. We demonstrate that in each test configuration the system was able to generate a centimeter accurate 3D model complete with an overlaid radiation map detailing the emitted radiation intensity and the corrected surface dose rate.

Corrigendum: Radiological Mapping of Post-Disaster Nuclear Environments Using Fixed-Wing Unmanned Aerial Systems: A Study From Chornobyl.

[This corrects the article DOI: 10.3389/frobt.2019.00149.].

Evaluation of Scintillator Detection Materials for Application within Airborne Environmental Radiation Monitoring.

In response to the Fukushima Daiichi Nuclear Power Plant accident, there has occurred the unabated growth in the number of airborne platforms developed to perform radiation mapping-each utilising various designs of a low-altitude uncrewed aerial vehicle. Alongside the associated advancements in the airborne system transporting the radiation detection payload, from the earliest radiological analyses performed using gas-filled Geiger-Muller tube detectors, modern radiation detection and mapping platforms are now based near-exclusively on solid-state scintillator detectors. With numerous varieties of such light-emitting crystalline materials now in existence, this combined desk and computational modelling study sought to evaluate the best-available detector material compatible with the requirements for low-altitude autonomous radiation detection, localisation and subsequent high spatial-resolution mapping of both naturally occurring and anthropogenically-derived radionuclides. The ideal geometry of such detector materials is also evaluated. While NaI and CsI (both elementally doped) are (and will likely remain) the mainstays of radiation detection, LaBr3 scintillation detectors were determined to possess not only a greater sensitivity to incident gamma-ray radiation, but also a far superior spectral (energy) resolution over existing and other potentially deployable detector materials. Combined with their current competitive cost, an array of three such composition cylindrical detectors were determined to provide the best means of detecting and discriminating the various incident gamma-rays.

Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material.

Here we report the results of multiple analytical techniques on sub-mm particulate material derived from Unit 1 of the Fukushima Daiichi Nuclear Power Plant to provide a better understanding of the events that occurred and the environmental legacy. Through combined x-ray fluorescence and absorption contrast micro-focused x-ray tomography, entrapped U particulate are observed to exist around the exterior circumference of the highly porous Si-based particle. Further synchrotron radiation analysis of a number of these entrapped particles shows them to exist as UO2-identical to reactor fuel, with confirmation of their nuclear origin shown via mass spectrometry analysis. While unlikely to represent an environmental or health hazard, such assertions would likely change should break-up of the Si-containing bulk particle occur. However, more important to the long-term decommissioning of the reactors at the FDNPP (and environmental clean-upon), is the knowledge that core integrity of reactor Unit 1 was compromised with nuclear material existing outside of the reactors primary containment.

Iron-based nanoparticles prepared from yerba mate extract. Synthesis, characterization and use on chromium removal.

Iron-based nanoparticles were synthesized by a rapid method at room temperature using yerba mate (YM) extracts with FeCl3 in different proportions. Materials prepared from green tea (GT) extracts were also synthesized for comparison. These materials were thoroughly characterized by chemical analyses, XRD, magnetization, SEM-EDS, TEM-SAED, FTIR, UV-Vis, Raman, Mössbauer and XANES spectroscopies, and BET area analysis. It was concluded that the products are nonmagnetic iron complexes of the components of the extracts. The applicability of the materials for Cr(VI) (300 µM) removal from aqueous solutions at pH 3 using two Cr(VI):Fe molar ratios (MR), 1:3 and 1:0.5, has been tested. At Cr(VI):Fe MR = 1:3, the best YM materials gave complete Cr(VI) removal after two minutes of contact, similar to that obtained with commercial nanoscale zerovalent iron (N25), with dissolved Fe(II), and with a likewise prepared GT material. At a lower Cr(VI):Fe MR (1:0.5), although Cr(VI) removal was not complete after 20 min of reaction, the YM nanoparticles were more efficient than N25, GT nanoparticles and Fe(II) in solution. The results suggest that an optimal Cr(VI):Fe MR ratio could be reached when using the new YM nanoparticles, able to achieve a complete Cr(VI) reduction, and leaving very low Cr and Fe concentrations in the treated solutions. The rapid preparation of the nanoparticles would allow their use in removal of pollutants in soils and groundwater by direct injection of the mixture of precursors.

Radiological Mapping of Post-Disaster Nuclear Environments Using Fixed-Wing Unmanned Aerial Systems: A Study From Chornobyl.

In the immediate aftermath following a large-scale release of radioactive material into the environment, it is necessary to determine the spatial distribution of radioactivity quickly. At present, this is conducted by utilizing manned aircraft equipped with large-volume radiation detection systems. Whilst these are capable of mapping large areas quickly, they suffer from a low spatial resolution due to the operating altitude of the aircraft. They are also expensive to deploy and their manned nature means that the operators are still at risk of exposure to potentially harmful ionizing radiation. Previous studies have identified the feasibility of utilizing unmanned aerial systems (UASs) in monitoring radiation in post-disaster environments. However, the majority of these systems suffer from a limited range or are too heavy to be easily integrated into regulatory restrictions that exist on the deployment of UASs worldwide. This study presents a new radiation mapping UAS based on a lightweight (8 kg) fixed-wing unmanned aircraft and tests its suitability to mapping post-disaster radiation in the Chornobyl Exclusion Zone (CEZ). The system is capable of continuous flight for more than 1 h and can resolve small scale changes in dose-rate in high resolution (sub-20 m). It is envisaged that with some minor development, these systems could be utilized to map large areas of hazardous land without exposing a single operator to a harmful dose of ionizing radiation.

A study of dynamic nanoscale corrosion initiation events using HS-AFM.

Atomic force microscopes (AFMs) are capable of high-resolution mapping of structures and the measurement of mechanical properties on nanometre scales within gaseous, liquid and vacuum environments. The contact mode high-speed AFM (HS-AFM) developed at Bristol Nano Dynamics Ltd. operates at speeds that are orders of magnitude faster than conventional AFMs, and is capable of capturing multiple frames per second. This allows for direct observation of dynamic events in real-time, with nanometre lateral resolution and subatomic height resolution. HS-AFM is a valuable tool for the imaging of nanoscale corrosion initiation events, such as metastable pitting, grain boundary (GB) dissolution and short crack formation during stress corrosion cracking (SCC). Within this study HS-AFM was combined with SEM and FIB milling to produce a multifaceted picture of localised corrosion events occurring on thermally sensitised AISI 304 stainless steel in an aqueous solution of 1% sodium chloride (NaCl). HS-AFM measurements were performed in situ by imaging within a custom built liquid cell with parallel electrochemical control. The high resolution of the HS-AFM allowed for measurements to be performed at individual reaction sites, i.e. at specific GB carbide surfaces. Topographic maps of the sample surface allowed for accurate measurements of the dimensions of pits formed. Using these measurements it was possible to calculate, and subsequently model, the volumes of metal reacting with respect to time, and so the current densities and ionic fluxes at work. In this manner, the local electrochemistry at nanoscale reaction sites may be reconstructed.

Experimental leaching of massive sulphide from TAG active hydrothermal mound and implications for seafloor mining.

Seafloor massive sulphide samples from the Trans-Atlantic Geotraverse active mound on the Mid-Atlantic Ridge were characterised and subjected to leaching experiments to emulate proposed mining processes. Over time, leached Fe is removed from solution by the precipitation of Fe oxy-hydroxides, whereas Cu and Pb leached remained in solution at ppb levels. Results suggest that bulk chemistry is not the main control on leachate concentrations; instead mineralogy and/or galvanic couples between minerals are the driving forces behind the type and concentration of metals that remain in solution. Dissolved concentrations exceed ANZECC toxicity guidelines by 620 times, implying the formation of localised toxicity in a stagnant water column. Moreover, concentrations will be higher when scaled to higher rock-fluid ratios and finer grain sizes proposed for mining scenarios. The distance at which dilution is achieved to meet guidelines is unlikely to be sufficient, indicating a need for the refinement of the mining process.

Development and validation of a high-resolution mapping platform to aid in the public awareness of radiological hazards.

The distribution, quantification and exposure-related effects of radiation in the environment, arising from both natural and anthropogenic sources, is of great (and growing) concern for global populations. Recent events at the Fukushima Daiichi Nuclear Plant (FDNPP) have further highlighted the importance of developing radiation mapping technologies that not only contribute to the continued assessment of contamination, but can serve as an educational tool for members of the public regarding both its behaviour and extent. With an even greater number of people possessing smart-phone technology, a lightweight and portable 'connected system' has been developed to demonstrate to users the calibrated radioactive dose rate in an area, viewable in real-time through a dedicated phone application. As well as allowing for system users to be alerted where variations in dose rate are experienced, the combined results from multiple systems are viewable through a custom-built desktop application-permitting the output obtained via any number of units to be similarly displayed in real-time. A successful initial trialling of the system is described at a former tin mine in Cornwall (south-west England)-known to exhibit low, but identifiable radiation anomalies in discrete areas. Additional applications outside of its educational usage are also discussed.

Examination of Surface Deposits on Oldbury Reactor Core Graphite to Determine the Concentration and Distribution of 14C.

Pile Grade A graphite was used as a moderator and reflector material in the first generation of UK Magnox nuclear power reactors. As all of these reactors are now shut down there is a need to examine the concentration and distribution of long lived radioisotopes, such as 14C, to aid in understanding their behaviour in a geological disposal facility. A selection of irradiated graphite samples from Oldbury reactor one were examined where it was observed that Raman spectroscopy can distinguish between underlying graphite and a surface deposit found on exposed channel wall surfaces. The concentration of 14C in this deposit was examined by sequentially oxidising the graphite samples in air at low temperatures (450°C and 600°C) to remove the deposit and then the underlying graphite. The gases produced were captured in a series of bubbler solutions that were analysed using liquid scintillation counting. It was observed that the surface deposit was relatively enriched with 14C, with samples originating lower in the reactor exhibiting a higher concentration of 14C. Oxidation at 600°C showed that the remaining graphite material consisted of two fractions of 14C, a surface associated fraction and a graphite lattice associated fraction. The results presented correlate well with previous studies on irradiated graphite that suggest there are up to three fractions of 14C; a readily releasable fraction (corresponding to that removed by oxidation at 450°C in this study), a slowly releasable fraction (removed early at 600°C in this study), and an unreleasable fraction (removed later at 600°C in this study).

XPS Study of Ion Irradiated and Unirradiated UO2 Thin Films.

XPS determination of the oxygen coefficient kO = 2 + x and ionic (U(4+), U(5+), and U(6+)) composition of oxides UO2+x formed on the surfaces of differently oriented (hkl) planes of thin UO2 films on LSAT (Al10La3O51Sr14Ta7) and YSZ (yttria-stabilized zirconia) substrates was performed. The U 4f and O 1s core-electron peak intensities as well as the U 5f relative intensity before and after the (129)Xe(23+) and (238)U(31+) irradiations were employed. It was found that the presence of uranium dioxide film in air results in formation of oxide UO2+x on the surface with mean oxygen coefficients kO in the range 2.07-2.11 on LSAT and 2.17-2.23 on YSZ substrates. These oxygen coefficients depend on the substrate and weakly on the crystallographic orientation. On the basis of the spectral parameters it was established that uranium dioxide films AP2,3 on the LSAT substrates have the smallest kO values, and from the XRD and EBSD results it follows that these samples have a regular monocrystalline structure. The XRD and EBSD results indicate that samples AP5-7 on the YSZ substrates have monocrystalline structure; however, they have the highest kO values. The observed difference in the kO values was probably caused by the different nature of the substrates: the YSZ substrates provide 6.4% compressive strain, whereas (001) LSAT substrates result only in 0.03% tensile strain in the UO2 films. (129)Xe(23+) irradiation (92 MeV, 4.8 × 10(15) ions/cm(2)) of uranium dioxide films on the LSAT substrates was shown to destroy both long-range ordering and uranium close environment, which results in an increase of uranium oxidation state and regrouping of oxygen ions in uranium close environment. (238)U(31+) (110 MeV, 5 × 10(10), 5 × 10(11), 5 × 10(12) ions/cm(2)) irradiations of uranium dioxide films on the YSZ substrates were shown to form the lattice damage only with partial destruction of the long-range ordering.