Thermodynamic assessment of the neptunium–oxygen system: Mass spectrometric studies and thermodynamic modelling

Smith, Anna; Colle, Jean‐Yves; Beneš, O.; Konings, R.J.M.; Sundman, Bo; Guéneau, C.

doi:10.1016/j.jct.2016.07.040

Cited by 9 publications

(5 citation statements)

References 50 publications

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“…A large amount of literature is available and can be found in earlier reviews, including data on highly radiotoxic oxides 77,80,303 . Most recently, in the field of fast reactors for transmutation, Smith et al have published a thermodynamic study of the Np–O system, which included KEMS measurements and thermodynamic modeling 304 . Refractory ceramic oxides are also important for other nuclear issues such as nuclear waste immobilization, fuel cladding, and severe accident containment.…”

Section: Novel Applications Of Kemsmentioning

confidence: 99%

“…have published a thermodynamic study of the Np-O system, which included KEMS measurements and thermodynamic modeling. 304 Refractory ceramic oxides are also important for other nuclear issues reprocessing. 310,311 Stolyarova et al 312 have recently reported thermodynamic data and vaporization behavior of Cs, Sr, and Ba compounds relevant to nuclear safety.…”

Section: Oxide Fuelsmentioning

confidence: 99%

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Knudsen effusion mass spectrometry: Current and future approaches

Jacobson,

Colle,

Stolyarova

et al. 2024

Rapid Comm Mass Spectrometry

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RationaleKnudsen effusion mass spectrometry (KEMS) has been a powerful tool in physical chemistry since 1954. There are many excellent reviews of the basic principles of KEMS in the literature. In this review, we focus on the current status and potential growth areas for this instrumental technique.MethodsWe discuss (1) instrumentation, (2) measurement techniques, and (3) selected novel applications of the technique. Improved heating methods and temperature measurement allow for better control of the Knudsen cell effusive source. Accurate computer models of the effusive beam and its introduction to the ionizer allow optimization of such parameters as sensitivity and removal of background signals. Computer models of the ionizer allow for optimized sensitivity and resolution. Additionally, data acquisition systems specifically tailored to a KEMS system permit improved quantity and quality of data.ResultsKEMS is traditionally utilized for thermodynamic measurements of pure compounds and solutions. These measurements can now be strengthened using first principles and model‐based computational thermochemistry. First principles can be used to calculate accurate Gibbs energy functions (gefs) for improving third law calculations. Calculated enthalpies of formation and dissociation energies from ab initio methods can be compared to those measured using KEMS. For model‐based thermochemistry, solution parameters can be derived from measured thermochemical data on metallic and nonmetallic solutions. Beyond thermodynamic measurements, KEMS has been used for many specific applications. We select examples for discussion: measurements of phase changes, measurement/control of low‐oxygen potential systems, thermochemistry of ultrahigh‐temperature ceramics, geological applications, nuclear applications, applications to organic and organometallic compounds, and thermochemistry of functional room temperature materials, such as lithium ion batteries.ConclusionsWe present an overview of the current status of KEMS and discuss ideas for improving KEMS instrumentation and measurements. We discuss selected KEMS studies to illustrate future directions of KEMS.

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Section: Novel Applications Of Kemsmentioning

confidence: 99%

Section: Oxide Fuelsmentioning

confidence: 99%

Knudsen effusion mass spectrometry: Current and future approaches

Jacobson,

Colle,

Stolyarova

et al. 2024

Rapid Comm Mass Spectrometry

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“…Phase diagrams: U–O (adapted with permission from refs and , Copyright 2007 ASM International); Th–O (adapted with permission from refs and , Copyright 1969 Elsevier B.V.); Np–O (reprinted with permission from ref , Copyright 2016 Elsevier Ltd.) and Pu–O (adapted with permission from refs and , Copyright 2017 John Wiley & Sons, Inc. and Copyright 2009, ASM International, respectively).…”

Section: Thermodynamic Propertiesmentioning

confidence: 99%

Thermodynamics of Fluorite-Structured Oxides Relevant to Nuclear Energy: A Review

Shelyug

Navrotsky

2021

ACS Earth Space Chem.

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Fluorite structured materials have shown their applicability in various fields both on and off Earth. In particular, these oxides find extensive application in nuclear energy and the use of actinides in space and planetary settings, thermal and environmental barrier coatings, aerospace applications, catalysts, fuel cells, and batteries. Research done on thermodynamic data collection should be structured to facilitate its use in predictive calculations. In this review, we bring together several decades of experimental thermodynamic analysis of fluorite-based oxides with an emphasis on their relevance to all stages of the nuclear fuel cycle. This review is relatively short in the interest of offering an accessible perspective, especially for scientists early in their careers in nuclear science.

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“…Whereas Figure 3. Binary-phase diagrams of uranium and oxygen (left), 31 neptunium and oxygen (middle), 51 and plutonium and oxygen (right). 52 OH and propylene oxide as gelation initiators.…”

Section: Synthesis Of Actinide Oxide Nanomaterialsmentioning

confidence: 99%

“…Binary-phase diagrams of uranium and oxygen (left), neptunium and oxygen (middle), and plutonium and oxygen (right) . Reprinted and modified with permissions from refs ,, . Copryight 2013 Taylor & Francis.…”

Section: Introductionmentioning

confidence: 99%

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

et al. 2019

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The chemistry of actinide molecules and materials has shown remarkable conceptual advancements in the past decade illustrating their unique reactivity profiles, when compared with lanthanides and transition elements, but there are still some challenging questions on the intriguing stability of low valent states and the significant role of 5f orbitals in bonding and reactivity of actinides. The distinctive electronic flexibility of actinide centers makes them potential catalysts for heterogeneous molecular transformations because of the kinetic lability of their coordination states and facile switching among oxidaton states. Actinide-enabled chemical transformations such as the six-electron reduction of dinitrogen into two reactive ammonia molecules or four-electron oxidation of water into oxygen under mild conditions are promising pathways in the quest of high-efficiency heterogeneous catalysts. This Review provides a comprehensive account on actinide-mediated catalytic transformation of small molecules such as CO, CO2, N2, O2, H2O, CH4, HCl, and NH3. The emphasis is placed on the emerging phenomena in actinide-based solid catalysts and controlled synthesis of nanostructured actinide materials as pristine and substrate-grown phases. The mechanistic investigations highlight the influence of the 5f electrons in multielectron transfer reactions and the propensity of actinide centers to achieve higher oxidation states that defines the surface termination in actinide oxides. Finally, the status and perspectives of actinide-containing materials beyond the nuclear fuel applications is discussed, underlining their exciting chemistry and unexplored potential toward alternative catalytic energy production processes.

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Thermodynamic assessment of the neptunium–oxygen system: Mass spectrometric studies and thermodynamic modelling

Cited by 9 publications

References 50 publications

Knudsen effusion mass spectrometry: Current and future approaches

Knudsen effusion mass spectrometry: Current and future approaches

Thermodynamics of Fluorite-Structured Oxides Relevant to Nuclear Energy: A Review

Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules

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