Absorption spectroscopy for the quantitative prediction of lanthanide concentrations in the 3LiCl–2CsCl eutectic at 723 K

Schroll, Cynthia A.; Lines, Amanda M.; Heineman, William R.; Bryan, Samuel A.

doi:10.1039/c6ay01520d

Cited by 42 publications

(37 citation statements)

References 34 publications

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“…Rare‐earth metal‐doped GQDs, on the other hand, can be conveniently excited by a common 808 nm NIR laser, ensuring their versatility and larger tissue imaging depth. Other absorption peaks for Nd‐GQDs at 521, 576, 731, 739 nm can be attributed to multiple f 5 – f 5 transitions [ 46 ] while for Tm‐GQDs at ≈685 nm peak can be assigned to the electronic transitions of 3 H 6 ground state to the 3 F 2,3 higher energy states [ 47 ] (Figure 3a). While the pristine GQDs [ 9 ] developed in our previous work show mainly broad visible emission with high quantum yield, upon doping with neodymium/thulium trivalent ions, substantial highly characteristic NIR fluorescence emerges.…”

Section: Resultsmentioning

confidence: 99%

Rare‐Earth Metal Ions Doped Graphene Quantum Dots for Near‐IR In Vitro/In Vivo/Ex Vivo Imaging Applications

Hasan

González-Rodríguez

Lin

et al. 2020

Advanced Optical Materials

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Near‐infrared (NIR) emitting biocompatible nanomaterials are desired in biotechnology as higher penetration depth fluorescence imaging probes. In this work, novel NIR‐emissive Nd3+‐doped or Tm3+‐doped biocompatible graphene quantum dots (GQDs) are developed via scalable, single‐step bottom‐up synthesis. Water‐soluble Nd‐GQDs/Tm‐GQDs with average diameters of 5.6–8.2 nm possess crystalline graphene lattice with <1 atomic percent of Nd/Tm and exhibit NIR fluorescence at ≈1060/≈925 nm attributed to the intrinsic transitions of Nd3+/Tm3+. High biocompatibility with >80% cell viability at 1 mg mL−1 for Nd‐GQDs and 0.25 mg mL−1 for Tm‐GQDs makes them well‐suited for bioimaging. In vitro, both GQD types exhibit efficient internalization with their intracellular emission maximized at 6 h. The pH‐dependence of this emission can serve as plethora of diagnostic applications. GQDs enable in vivo NIR imaging in live sedated NCr nude mice with IV administration: their NIR emission maximized at 6 h post‐injection is primarily detected in intestine, kidneys, liver, and spleen, however, diminishing to none at 48 h. Ex vivo organ/slice imaging shows significant Tm‐GQD fluorescence signatures in the aforementioned organs/slices. This capability of NIR fluorescence imaging in cells, tissues, and real‐time detection in live animals makes biocompatible rare‐earth metal‐doped GQDs an attractive new candidate for in vitro/in vivo/ex vivo theranostics.

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Section: Resultsmentioning

confidence: 99%

Rare‐Earth Metal Ions Doped Graphene Quantum Dots for Near‐IR In Vitro/In Vivo/Ex Vivo Imaging Applications

Hasan

González-Rodríguez

Lin

et al. 2020

Advanced Optical Materials

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“…The observed trends in diffusion coefficient data are based on the "hopping" mechanism of diffusion through ionic media. This work expands our concerted effort to systematically advance methods for quantitative electrochemical and spectroscopic measurement of lanthanides [29][30][31][32] and actinides within pyroprocessing 29-31 and other nuclear fuel reprocessing flowsheet applications including aqueous separation and detection of lanthanide and transition metal fission products. …”

mentioning

confidence: 99%

Electrochemistry of Europium(III) Chloride in 3 LiCl – NaCl, 3 LiCl – 2 KCl, LiCl – RbCl, and 3 LiCl – 2 CsCl Eutectics at Various Temperatures

Schroll

Chatterjee

Levitskaia

et al. 2017

J. Electrochem. Soc.

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Here we report the effect of changing the eutectic melt composition on the electrochemical properties of europium(III) chloride under pyroprocessing conditions. Stoichiometry of electron-transfer, redox potentials and diffusion coefficients were determined using various electrochemical and spectroelectrochemical techniques in four different eutectic mixtures (3 LiCl -NaCl, 3 LiCl -2 KCl, LiCl -RbCl, and 3 LiCl -2 CsCl) while varying the temperature of the melt. It was determined that Eu 3+ undergoes a one electron reduction to Eu 2+ in each melt at all temperatures evaluated. Within each of the melts a positive shift in the redox potential as well as an increase in the diffusion coefficient for Eu 3+ was observed as the temperature increased. Also observed was a positive shift in the redox potential and increase in the diffusion coefficient for Eu 3+ as the weighted average of the cationic radii the melt composition decreased. Pyroprocessing is one of the newest techniques for spent nuclear fuel reprocessing in which the separation is accomplished electrochemically in molten salt media at temperatures of >500• C. 1-3 Some of the advantages of pyroprocessing over the more traditional liquidliquid extraction techniques are that there is no organic solvent that is susceptible to radiolysis, 4,5 lack of pure plutonium product which provides less likelihood for proliferation, 6 generation of the U-Pu alloy product is ready for immediate fabrication into new fuel rods 7 and the ability to do a group separation of all actinides.8 There are also engineering related advantages such as amenability to scaling to the needs of the facility 9 and making the refinement vessel more compact. 10,11The most important information needed to understand pyroprocessing is accurate thermodynamic data for each of the analytes that may be found in used nuclear fuel in each of the possible eutectic melt compositions. We have chosen to investigate europium(III) chloride because it is a non-radioactive analog to the actinides which makes it safer to work with, it has the least negative redox potential of the lanthanides, and it undergoes a change in its absorption spectrum when it is reduced from Eu 3+ to Eu 2+ . 12 Prior research has been performed using europium(III) chloride and evaluating its thermodynamic properties in different melts, such as LiCl, 13 In this work we systematically evaluated the redox potentials and diffusion coefficients for europium(III) chloride using differential pulse voltammetry and cyclic voltammetry in three different eutectic salt compositions over a range of temperatures. The experiments were performed from 673 K to 1173 K in 3 LiCl -NaCl, LiCl -RbCl and 3 LiCl -2 CsCl. This data along with the results from our previous * Electrochemical Society Member.z E-mail: heinemwr@ucmail.uc.edu; sam.bryan@pnl.gov reports (Electrochemistry of Europium in 3 LiCl -2 KCl from 643 to 1123 K 29 and Spectroelectrochemistry of Europium in 3 LiCl -NaCl, 3 LiCl -2 KCl, LiCl -RbCl, and 3 LiCl −2 CsCl at 873 K 30 ) were analyzed ...

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“…Because of its highly complex chemistry and the opportunity to enable advanced fuel processing and recycle, pyrochemical processing represents a key area in which the integration of optical process monitoring technology can support significant process development (Schroll et al 2016). Utilizing optical monitoring (e.g., UV-vis absorbance or Raman spectroscopy) during bench-scale process development can enable drastic reductions in the time to deploy pyrochemical processes.…”

Section: Pyrochemical Systemsmentioning

confidence: 99%

Innovative Separations Research and Development Needs for Advanced Fuel Cycles

Moyer¹,

Lumetta

Bruffey³

et al. 2022

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Absorption spectroscopy for the quantitative prediction of lanthanide concentrations in the 3LiCl–2CsCl eutectic at 723 K

Abstract: The absorption spectra of single-component mixtures of six lanthanide chloride salts were obtained in the molten salt eutectic 3LiCl–2CsCl at 723 K, and used to build multivariate regression models to predict concentrations of multi-component mixtures of these metals in solution.

Cited by 42 publications

References 34 publications

Rare‐Earth Metal Ions Doped Graphene Quantum Dots for Near‐IR In Vitro/In Vivo/Ex Vivo Imaging Applications

Rare‐Earth Metal Ions Doped Graphene Quantum Dots for Near‐IR In Vitro/In Vivo/Ex Vivo Imaging Applications

Electrochemistry of Europium(III) Chloride in 3 LiCl – NaCl, 3 LiCl – 2 KCl, LiCl – RbCl, and 3 LiCl – 2 CsCl Eutectics at Various Temperatures

Innovative Separations Research and Development Needs for Advanced Fuel Cycles

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