Dominic Larivière

Analytical Chemistry, Flow Chemistry, Green Chemistry

31.54

Publications

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    ABSTRACT: Nowadays, rare earth elements (REEs) and their compounds are critical for the rapidly growing advanced technology sectors and clean energy demands. However, their separation and purification still remain challenging. Among different extracting agents used for REE separation, the diglycolamide (DGA)-based materials have attracted increasing attention as one of the most effective extracting agents. In this contribution, a series of new and element-selective sorbents were generated through derivatisation of the diglycolamide ligand (DGA), grafted to mesoporous silica and tested for the separation of rare earth elements. It is shown that, by tuning the ligand bite angle and its environment, it is possible to improve the selectivity towards specific rare earth elements.
    No preview · Article · Dec 2015 · RSC Advances
  • Charles Labrecque · Julien Légaré Lavergne · Dominic Larivière
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    ABSTRACT: A procedure for the effective separation and determination of the most abundant actinides relevant to the nuclear industry (U, Th, Np, Pu and Am) was developed based on cloud point extraction (CPE) using H2DEH[MDP] (P,P-di-(2-ethylhexyl) methanediphosphonic acid) as a ligand. The extractability of actinides with varying concentrations of nitric acid and hydrochloric acid were assessed. The robustness of the method was demonstrated for environmental matrices such as reference materials and spiked liquid samples for the quantification of the gross actinide content. This analytical strategy may replace traditional sample preparation techniques used in radiological methods for gross measurements of radioactivity, and may act as a rapid screening tool in emergency situations. The developed method is a greener alternative to common radiochemical sample preparation techniques such as co-precipitation or evaporation. The formation of a small-volume surfactant-rich phase containing the complexed actinides enables rapid, highly selective and great enrichment of the analytes in this phase. The proposed method shows good extraction and separation yield compared to existing methods, since the surfactant-rich phase is soluble in water and can therefore be redispersed quantitatively in a medium compatible with mass spectrometry while providing fast isolation of the actinide content. Separation of actinides can be achieved after by wet ashing of the surfactant-rich phase obtained by CPE if coupled to the proper radiochemical separation scheme.
    No preview · Article · Sep 2015 · Journal of Radioanalytical and Nuclear Chemistry
  • A. Habibi · B. Boulet · M. Gleizes · D. Larivière · G. Cote
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    ABSTRACT: Nuclear accidents occurred in latest years highlighted the difficulty to achieve, in a short time, the quantification of alpha and beta emitters. Indeed, most of the existing methods, though displaying excellent performances, can be very long, taking up to several weeks for some radioisotopes, such as (90)Sr. This study focuses on alpha and beta radioisotopes which could be accidentally released from nuclear installations and which could be measured by inductively coupled plasma mass spectrometer (ICP-MS). Indeed, a new and rapid separation method was developed for (234,235,236,238)U, (230,232)Th, (239,240)Pu, (237)Np, (241)Am and (90)Sr. The main objective was to minimize the duration of the separation protocol by the development of a unique radiochemical procedure with elution media compatible with ICP-MS measurements. Excellent performances were obtained with spiked river water samples. These performances are characterized by total yields exceeding 80% for all monitored radionuclides, as well as good reproducibility (RSD≤10%, n=12). The proposed radiochemical separation (including counting time) required less than 7h for a batch of 8 samples. Copyright © 2015 Elsevier B.V. All rights reserved.
    No preview · Article · Apr 2015 · Analytica Chimica Acta
  • M. Delage · M. Lecavalier · D. Lariviere · C. Allen · L. Beaulieu

    No preview · Article · Dec 2014 · Radiotherapy and Oncology
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    Pablo J. Lebed · Iván Maisuls · Pablo M. Arnal · Dominic Larivière
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    ABSTRACT: As part of an ongoing effort to develop new radionuclides inorganic adsorbents with interesting characteristics for spent nuclear fuel reprocessing and disposal activities we studied four monodisperse colloidal core@shell and @shell materials designed around a silica core and a zirconia shell. The removal capacity and kinetic behaviour of uranium as well as the effect of aged materials on the extraction ability of U were investigated. We found that all materials tested were able to extract reasonably high amounts of U and reached a kinetic equilibrium in aproximately10 min. The extraction capacity was maintained in a low acidity media except for the crystalline core@shell samples which exhibited a decrease of 60 % in its extraction ability. Americium, plutonium, protactinium and polonium extractions showed diverse behaviour depending on the element and aqueous media conditions. Finally, the particles stability in aqueous media was studied through the analysis of silicon and zirconium presence in solution after 48 h. Our results indicated that the materials possess a reasonably high stability.
    Full-text · Conference Paper · Oct 2014
  • Charles Labrecque · Dominic Larivière
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    ABSTRACT: This article describes the development of a procedure for the bulk separation and determination of rare earth elements in soils by combining alkaline fusion, cloud point extraction, and inorganic mass spectrometry. The proposed cloud point extraction method uses a diglycolamide derivative as the chelating agent, which has a well-established affinity for rare earth elements. The method integrates bromine shielding to achieve efficient phase separation at highly acidic pH values. The methodology led to very low detection limits (0.2 to 30 ng/L), quantitative extraction (>97%) for soils, and a high preconcentration factor (up to 140). Decontamination factors were assessed for the most abundant elements, including trivalent ions such as Al3+ and Fe3+. A reduction in concentration of up to 180-fold was measured for some elements. Quantitative recoveries for most rare earth elements in highly acidic conditions were achieved and validated using sediment reference material (NIST-2709a). There was excellent agreement between the expected and measured concentrations for all 16 rare earth elements evaluated. The superior analytical figures of merit enabled rare earth element determination at ultra-trace levels in environmental samples.
    No preview · Article · Oct 2014 · Analytical methods
  • M-E Delage · M-E Lecavalier · D Lariviere · C Allen · L Beaulieu
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    ABSTRACT: Purpose: Structure and energy transfer mechanisms confer colloidal quantum dots (cQDs) interesting properties, among them their potential as scintillators. CdSe multi-shell cQDs in powder were investigated under photons irradiation. The purpose of this work is to characterize signal to dose linearity, stability with time and to quantify the dependence of their light output with beam energy.
    No preview · Article · Jun 2014 · Medical Physics
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    Pablo J Lebed · Dominic Larivière · Xiongxin Dai
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    ABSTRACT: In this contribution we report our efforts to produce a protactinium standard through purification of Pa-231 from uranium ores in order to obtain measurable quantities. Through this process we explore the full range of the analytical process: from comparing sample preparation methods such as microwave digestion and fusion, the characterization of protactinium retention in commercial solid phase extraction resins with breakthrough curves and the challenges of detection and measurement with alpha spectrometry and ICP-MS.
    Full-text · Conference Paper · Jun 2014
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    ABSTRACT: Analyse des bouteilles de la collection du Musée maritime du Québec.
    Full-text · Conference Paper · May 2014
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    ABSTRACT: The importance of rare‐earth elements in the global economy is booming as they are used in numerous advanced technologies. However, industrially, their extraction and purification remain tedious. Functional nanoporous hybrid materials, represented by D. Larivière, F. Kleitz, and co‐workers as an asteroid preferentially cycling around a rare‐earth planet, demonstrate enhanced affinity for the rare‐earths with a high level of reusability, which increases their marketable potential. The image emphasizes the selectivity and reusability of these new extraction materials towards rare‐earths, rather than gravitating around actinide and other metal contaminants.
    No preview · Article · May 2014 · Advanced Functional Materials
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    ABSTRACT: The importance of rare-earth elements (REEs) in the global economy is booming as they are used in numerous advanced technologies. Industrially, the extraction and purification of REEs involve multiple liquid–liquid extraction (LLE) steps as they exhibit very similar complexation properties with most common ligands. In order to substantially improve this process and provide a greener alternative to LLE, functional porous hybrid materials, demonstrating enhanced selectivity towards heavier REEs compared to commercially-available products, are proposed. In addition, because of the grafting procedure used in the synthesis, the proposed materials demonstrate a higher degree of reusability, increasing their marketable potential.
    No preview · Article · May 2014 · Advanced Functional Materials
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    ABSTRACT: An analytical procedure for determining the relative amounts of 60 Co and its 60 Ni daughter in a radioactive cobalt source by means of chromatographic separation and radiometric and mass spectrometric detection was developed, optimized and assessed through two round robin exercises for nuclear forensic investigations. Solid phase extraction (EXC) using Ni resin (Eichrom) and ion exchange (IEC) using Dowex-1X8 (Acros Organics) chromatographic approaches were considered for separating Co and Ni. Decontamination factors of 25 and 2.8 Â 10 6 were measured for EXC and IEC, respectively. Based on those results, only the IEC option was pursued. The effects of particle size, mass of resin, and degree of cross-linkage for decontamination performance were assessed, and the loading/eluting conditions were optimized. Canadian (CNSC, RPB, UL, RMC, AECL) and American (ANL) laboratories participated in two round robin exercises designed by the National Research Council of Canada to determine the suitability and limitations of the proposed methods. Age determination for freshly irradiated sources (<1 a) and for sources with high Ni content was challenging for the laboratories. Nevertheless, age estimates were obtained with sufficient accuracy for nuclear forensic purposes.
    Full-text · Article · Feb 2014 · Analytical methods
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    Pablo J Lebed · Sabrina Potvin · Dominic Larivière · Xiongxin Dai
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    ABSTRACT: Effective solid phase extraction separation methods of actinides and fission products are required in the control and evaluation of common or experimental nuclear spent fuel reprocessing strategies and environmental contaminated samples. In this study, we have developed a simpler sequential analytical separation scheme to isolate 237Np from U and Pu. Experimental design tools were used to achieve parameter optimization. We studied the contribution of critical factors such as the type of resin, acidity, sulfamic acid concentration and sample volume to actinide extraction with a multivariate approach. Following a sequential assembly approach, fractional factorial designs were used to select the best resin. Full factorial designs were used to evaluate the expected response for the chosen multifactorial space. After discarding a first order linear model, the designs were augmented and the response surface methodology was used to evaluate the response through the use of a quadratic model together with graphical and canonical analysis. Knowledge acquired from multiple actinide responses allowed us to find multi-criteria compromise solutions that were successfully applied for the separation of Np from Pu and U in complex matrices.
    Full-text · Article · Jan 2014 · Analytical methods
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    ABSTRACT: Cesium pre-concentration/separation was investigated using novel ammonium molybdophosphate (AMP)-based adsorbents supported on mesoporous silica (SBA-15). This combination is a viable strategy to produce reusable, highly effective and selective adsorbents to be used for remediation during radiological/nuclear events or radiological monitoring.
    Full-text · Article · Dec 2013 · New Journal of Chemistry
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    ABSTRACT: Purpose: To assess the dosimetry of Ra-226 in a two-year chronic ingestion study in laboratory maintained fathead minnow fed environmentally relevant levels of the isotope known to occur in gut contents of fish from a uranium mining area. Methods: Fish were established on reconstituted commercial fish food containing 10 mBq-10 Bq Ra-226.g(- 1) dry food. The fish were sampled at 1, 6, 18 and 24 months and the Ra-226 levels in the whole fish were directly determined using measurement performed using inorganic mass spectrometry. Pilot experiments using higher doses were also done during development of a liquid scintillation detection system which support some data. Results: The data show that after 1 month the levels of accumulation in the fish were below detection. At 6 months there was an activity dependent accumulation which was relatively higher in the low activity groups. By 18 and 24 months the radium was very low in all groups - well below 6 month levels suggesting considerable loss of radium from the fish. These data were confirmed in a small and shorter study using higher dietary activities. The highest dose calculated for any measurement point was 16 μGy.h(- 1) in the 6-month-old fish fed the diet containing 10 Bq.g(- 1). Conclusions: We conclude that environmentally relevant levels of Ra-226 have a maximum impact at early time-points when the fish are still growing. After that they appear to depurate accumulated radium. In terms of environmental impact, the maximum accumulation peaks at the age where fish could be spawning but is extremely low leading to μGy.year(- 1) doses even after exposure to the high activity diets.
    No preview · Article · Nov 2013 · International Journal of Radiation Biology
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    ABSTRACT: Fluorescent CdSe-CdS-Cd0.5Zn0.5S-ZnS core-shell colloidal quantum dots (cQDs) dispersed in aqueous and organic solvents have been prepared and used as scintillators for detecting ionizing radiation. Results demonstrate a linear relationship between emitted luminescence and dose-activity. These results suggest that cQDs alone could be used as liquid scintillators for specific environmental and medical applications.
    No preview · Article · Nov 2013 · Chemical Communications
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    ABSTRACT: A new cloud point extraction procedure has been developed for the quantification) of plutonium (IV) in environmental samples. The separation procedure can be either coupled to inductively coupled plasma mass spectrometry (ICP-MS) or alpha spectrometry for plutonium quantification. The method uses a combination of selective ligand (P,P di-(2-ethylhexyl) methanediphosphonic acid (H2DEH[MDP])) and micelle shielding by bromine formation to enable quantitative extraction of Pu in highly acidic solutions. Cross-optimization of all parameters (non-ionic and ionic surfactant, chelating agent, bromate, bromide and pH) led to optimal of the extraction conditions. Figures of merit of the method for the detection using alpha spectrometry and ICP-MS are reported (limit of detection, limit of quantification, minimal detectable activity and recovery). Quantitative extractions (> 95 %) were obtained for a wide variety of aqueous and digested samples (synthetic urine, waste water, drinking water, sea water and soil samples). The method features the first successful coupling between alpha spectrometry and cloud point extraction and was the first demonstration of CPE suitability with metaborate fusion as a sample preparation approach, all techniques used extensively in nuclear industries.
    No preview · Article · Sep 2013 · Analytical Chemistry
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    Pablo J Lebed · Sabrina Potvin · Dominic Larivière · Xiongxin Dai
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    ABSTRACT: Ultra-trace analysis of radionuclides, particularly actinides and fission products, is required for a number of important applications including nuclear forensics and radio-bioassay. In the field of environmental radio-analytical chemistry current 237Np separation protocols are mainly based on the use of TEVA EXC commercial where samples are usually loaded after reduction of Np to Np(IV) while Pu is in the non-retainable Pu(III) oxidation state. Traditionally, these time consuming separation methodologies are developed by monitoring the influence of one-variable-at-a-time on an experimental response. Although it is possible to obtain successful results, this approach presents disadvantages such as the increase in the number of necessary experiments and the lack of inclusion of the interactive effects among the variables studied with the consequence of an incomplete effect description over the response. Multivariate statistic techniques have proven to be valid tools in the pathway of simultaneous parameters optimization to achieve the maximum system performance. The aim of the present work is to show that it is possible to develop a much simpler time-saving analytical separation scheme to obtain 237Np samples free from 238U and 242Pu through the application of experimental design tools, mainly fractional and full factorial designs, and the response surface methodology (RSM). Knowledge acquired from multiple actinide responses allowed us to find multi-criteria compromise solutions that were successfully applied over complex matrices such as waste water and soil.
    Full-text · Conference Paper · Sep 2013
  • Carmel Mothersill · Richard Smith · Dominic Lariviere · Colin Seymour
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    ABSTRACT: Purpose: To assess the impact of environmentally relevant levels of ingested (226)Ra on a common freshwater fish species. Methods: Fathead minnow (Pimephales promelas, Rafinesque) were obtained at the first feeding stage and established on a commercial fish food diet containing (226)Ra in the activity range 10 mBq/g(-1), -10,000 mBq/g(-1). They remained on this diet for 24 months and were sampled invasively at 1,6,18 and 24 months to assess growth, biochemical indices and accumulated dose and non-invasively also at 12 and 15 months to assess growth. Results: Fish fed 10 and 100 mBq/g(-1) diet showed a small transitory deregulation of growth at 6 and 12 months. Fish fed higher activities showed less significant or insignificant effects. There was a trend at 18 months which was stronger at 24 months for the population distribution to change in all of the (226)Ra fed groups so that smaller fish were smaller and bigger fish were bigger than the controls. There were also significant differences in the ratios of protein:DNA at 24 months which were seen as a trend but were not significant at earlier time points. Conclusions: Fish fed a radium diet for 2 years show a small and transitory growth dysregulation at 6 and 12 months. The effects predominate at the lower activities suggesting hormetic or homeostatic adjustments. There was no effect on growth of exposure to the high activities (226)Ra. This suggests that radium does not have a serious impact on the ecology of the system and the level of radium that would be transferred to humans is very low. The results may be important in the assessment of long-term environmental impacts of (226)Ra exposure.
    No preview · Article · Jun 2013 · International Journal of Radiation Biology
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    ABSTRACT: A procedure has been developed for the cloud point extraction (CPE) of uranium (VI) using H2DEH[MDP] (P,P-di(2-ethylhexyl) methanediphosphonic acid) with inductively coupled plasma coupled to mass spectrometry (ICP-MS). The method is based on the modification of the cloud point temperature using cetyl trimethyl ammonium bromide (CTAB) and KI. Optimal conditions of extraction were found using a cross-optimization of every parameter (non-ionic and ionic surfactant concentrations, chelating agent concentration, pH and the extraction, and phase separation temperatures). Furthermore, the figures of merit of the methodology were assessed (limit of detection, limit of quantification, recovery, sensibility, and linear range) and are reported. Quantitative extraction (99±0.5%) was obtained in drinking water samples over a wide range of uranium concentrations. The approach was also validated using drinking (SCP EP-L-3 and SCP EP-H-3), and wastewater (SCP EU-L-3) certified materials. Interferences from most critical anions and cations were evaluated to determine the reliability of the method. The proposed method showed robustness since its performance is maintained over a wide range of pH and metal ion concentrations.
    No preview · Article · Mar 2013 · Talanta

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