Andrew Strzelecki

Los Alamos National Laboratory

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Xiaofeng Guo

Washington State University

Hongwu Xu

Los Alamos National Laboratory

Artas Migdisov

Los Alamos National Laboratory

Di Wu

Washington State University

Hakim Boukhalfa

Los Alamos National Laboratory

Nicolas Dacheux

Institut de Chimie Séparative de Marcoule

Cody B. Cockreham

Washington State University

Robert P. Currier

Los Alamos National Laboratory

Robert Roback

Los Alamos National Laboratory

Vitaliy G. Goncharov

Washington State University

Cooperative Institutions

Los Alamos National Laboratory

Washington State University

Government of the United States of America

Université de Montpellier

CEA Marcoule

École Nationale Supérieure de Chimie de Montpellier

Centre National de la Recherche Scientifique

Institut de Chimie Séparative de Marcoule

Argonne National Laboratory

Commissariat à l'Énergie Atomique et aux Énergies Alternatives

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Crystal chemistry and thermodynamic properties of zircon structure-type materials

American Mineralogist (2023)

Andrew Strzelecki Xiaodong Zhao Paul Estevenon Hongwu Xu Nicolas Dacheux

Abstract Zircon-class ternary oxide compounds have an ideal chemical formula of ATO4, where A is commonly a lanthanide and an actinide, with T = As, P, Si, or V. Their structure (I41/amd) accommodates a diverse chemistry on both A- and T-sites, giving rise to more than 17 mineral end-members of five different mineral groups, and in excess of 45 synthetic end-members. Because of their diverse chemical and physical properties, the zircon structure-type materials are of interest to a wide variety of fields and may be used as ceramic nuclear waste forms and as aeronautical environmental barrier coatings, to name a couple. To support advancement of their applications, many studies have been dedicated to the understanding of their structural and thermodynamic properties. The emphasis in this review will be on recent advances in the structural and thermodynamic studies of zircon structure-type ceramics, including pure end-members [e.g., zircon (ZrSiO4), xenotime (YPO4)] and solid solutions [e.g., ErxTh1–x(PO4)x(SiO4)1–x]. Specifically, we provide an overview on the crystal structure, its variations and transformations in response to non-ambient stimuli (temperature, pressure, and radiation), and its correlation to thermophysical and thermochemical properties.

Crystal Chemistry

10.2138/am-2022-8632

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Citations (5)

Selective hydrothermal extraction of lanthanides: Mimicking natural ore-forming processes [Slides]

Artaches Migdissov Andrew Strzelecki Hakim Boukhalfa Kirsten Sauer Haylea Nisbet

Rare Earth Elements (REE) consumption in the US was 20,000 metric ton in 2018. China controls 97% of the global REE market. The aims for new technology are to 1. Avoid investing in extraction of cheap LREE, extract M/HREE only → increase the value of the intermediate/final product, 2. Exclude extraction and concentration of U and Th → avoid investment in rad remediation, and 3. Maximize environmental friendliness of the technology. Hints from nature can aid in achieving these amis.

Investment

Tonne

Rare-earth element

Consumption

10.2172/1601603

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Citations (1)

An experimental study of the solubility of rare earth chloride salts (La, Nd, Er) in HCl bearing water vapor from 350 to 425 °C

Geochimica et Cosmochimica Acta (2021)

Christopher Alcorn Kirill A. Velizhanin Andrew Strzelecki Haylea Nisbet Robert P. Currier

Sublimation

Boiling point

Saturation (graph theory)

Enthalpy of sublimation

10.1016/j.gca.2021.06.011

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Citations (6)

Uranium partitioning between apatite and hydrothermal fluids at 150–250 °C

Chemical Geology (2024)

R. I. Gabitov Artas Migdisov Ángel Jiménez-Arroyo Hongwu Xu Xiaofeng Guo

Uranium ore

10.1016/j.chemgeo.2024.122277

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Citations (0)

Kinetics of Pyrolysis and Thermal Evolution of Negev Desert Lithologies

ACS Earth and Space Chemistry (2025)

Cody B. Cockreham Xianghui Zhang Andrew Strzelecki Chris J. Benmore Christopher Campe

The Negev desert in Israel is home to large quantities of organic-rich, shallow marine sedimentary lithologies that could potentially accommodate the disposal of spent nuclear fuel. Previous thermal analyses of Negev carbonates have focused on industrially relevant considerations such as natural gas and oil extraction or pyrolysis for recovering hydrocarbon fuels. This study addresses thermal evolution of the Negev organic-rich carbonate, siliceous, and phosphorite rocks and associated chemical, mineralogical, and microstructural changes that may occur under prolonged thermal loading in the vicinity of spent nuclear fuel disposal systems. Our employed methods include high-temperature X-ray diffraction, high-temperature infrared spectroscopy, and thermal analysis integrating thermogravimetry, differential scanning calorimetry, and mass spectrometry. Further, we apply iterative iso-conversional model-free methods to derive kinetic parameters for thermal decomposition of the Negev organic-rich carbonate rocks from 200 to 550 °C. Our results have provided mechanistic insights into the thermal evolution encompassing water desorption, decomposition of organic matter, and decarbonation of carbonate phases.

Thermogravimetry

Lithology

10.1021/acsearthspacechem.4c00218

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Unravelling the origins of shale nanoporosity using small-angle neutron scattering (SANS)

Fuel (2025)

Chelsea W. Neil Rex P. Hjelm Andrew Strzelecki Michael C. Cheshire Jon Burger

Small-Angle Scattering

10.1016/j.fuel.2025.134578

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Crystal Chemistry and Thermodynamics of HREE (Er, Yb) Mixing in a Xenotime Solid Solution

ACS Earth and Space Chemistry (2022)

Andrew Strzelecki Margaret Reece Xiaodong Zhao Wendy Yu Chris J. Benmore

Rare earth elements (REEs), the 15 naturally occurring lanthanides plus yttrium and scandium, are ubiquitously used in modern life as they are critical components of many advanced devices and technologies. However, the demand for REEs is not equal, with the heavy rare earth elements (HREEs) having a higher demand. Xenotime (HREEPO4) is an important HREE ore mineral and globally is an economical source of HREE. Most of the crystallographic and thermodynamic properties of xenotime endmembers have been elucidated by calorimetric, solubility, and high-pressure studies. Yet, in natural systems, endmembers are rarely encountered, and instead, REE solid solutions are more commonly observed. In this work, we characterize the crystal chemistry, thermodynamics of HREE mixing, and high-temperature material behaviors and thermochemistry of a synthetic erbium (Er)–ytterbium (Yb) binary xenotime solid solution (Er(x)Yb(1–x)PO4) using a suite of experimental techniques, including X-ray fluorescence spectroscopy, synchrotron X-ray powder diffraction implemented with Rietveld analysis, Fourier transform infrared spectroscopy coupled with attenuated total reflectance, Raman spectroscopy, thermogravimetric analysis coupled with differential scanning calorimetry, and high-temperature oxide melt drop solution calorimetry. Our results shed light on the formation of natural xenotimes and lay the foundation for their industrial applications as thermal coating materials.

Rietveld Refinement

Scandium

Ytterbium

10.1021/acsearthspacechem.2c00052

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Citations (16)

Thermodynamics of molybdenum trioxide encapsulated in zeolite Y

AIChE Journal (2021)

Xianghui Zhang Andrew Strzelecki Cody B. Cockreham Vitaliy G. Goncharov Houqian Li

Abstract Zeolites with encapsulated transition metal species are extensively applied in the chemical industry as heterogenous catalysts for favorable kinetic pathways. To elucidate the energetic insights into formation of subnano‐sized molybdenum trioxide (MoO 3 ) encapsulated/confined in zeolite Y (FAU) from constituent oxides, we performed a systematic experimental thermodynamic study using high‐temperature oxide melt solution calorimetry as the major tool. Specifically, the formation enthalpy of each MoO 3 /FAU is less endothermic than corresponding zeolite Y, suggesting enhanced thermodynamic stability. As Si/Al ratio increases, the enthalpies of formation of MoO 3 /FAU with identical loading (5 Mo‐wt%) tend to be less endothermic, ranging from 61.1 ± 1.8 (Si/Al = 2.9) to 32.8 ± 1.4 kJ/mol TO 2 (Si/Al = 45.6). Coupled with spectroscopic, structural and morphological characterizations, we revealed intricate energetics of MoO 3 –zeolite Y guest–host interactions determined by the Si/Al ratio and the subtle redox and/or local structural evolutions of encapsulated MoO 3 .

Endothermic process

Molybdenum trioxide

Molybdenum disulfide

Molybdenum oxide

Chemical Stability

Exothermic reaction

10.1002/aic.17464

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Citations (5)

High-Temperature Thermodynamics of Cerium Silicates, A-Ce₂Si₂O₇, and Ce_4.67(SiO₄)₃O

ACS Earth and Space Chemistry (2020)

Andrew Strzelecki Kyle W. Kriegsman Paul Estevenon Vitaliy G. Goncharov Jianming Bai

Lanthanide disilicates and oxyapatites have potential roles in high-temperature applications as thermal (TBC) and environmental barrier coatings (EBC) or possible alteration phases in geological nuclear waste repositories. However, those Ce3+-bearing silicates have only been limitedly studied. In this work, we performed detailed structural and thermodynamic investigations on A-Ce2Si2O7 (tetragonal, P41) and Ce4.67(SiO4)3O (hexagonal, P63/m). The high-temperature structural behaviors and coefficients of thermal expansion were determined by in situ high-temperature synchrotron X-ray diffraction (HT-XRD) implemented with Rietveld analysis and thermogravimetric analysis coupled with differential scanning calorimetry (TGA-DSC). A-Ce2Si2O7 was found to be stable in N2 and air up to ∼1483 K with an isotropic thermal expansion along the a- and c-axes (αa = 12.3 × 10–6 K–1 and αc= 12.4 × 10–6 K–1). Ce4.67(SiO4)3O had a slow partial oxidation between 533 and 873 K to a new nonstoichiometric phase Ce3+1.67-xCe4+xCe3+3(SiO4)3O1+0.5x, followed by a thermal decomposition to CeO2 and SiO2 at ∼1000 K in air. By using high temperature oxide melt solution calorimetry at 973 K with lead borate as the solvent, the standard enthalpy of formation was determined for A-Ce2Si2O7 (−3825.1 ± 6.0 kJ/mol) and Ce4.67(SiO4)3O (−7391.3 ± 9.5 kJ/mol). These thermodynamic parameters were compared with those of CeO2, CeSiO4, and other silicate oxyapatites for examining their chemical stability in high-temperature environments relevant for aeronautical applications, mineral formation, and nuclear fuel cycle.

Thermogravimetric analysis

Rietveld Refinement

Orthosilicate

Tetragonal crystal system

10.1021/acsearthspacechem.0c00231

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Citations (26)

Fluocerite as a precursor to rare earth element fractionation in ore-forming systems

Nature Geoscience (2022)

Andrew Strzelecki Artas Migdisov Hakim Boukhalfa Kirsten Sauer Kathryn G. McIntosh

Rare-earth element

Lutetium

Fluorite

10.1038/s41561-022-00921-6

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Citations (19)