NdPO4 solubility and aqueous Neodymium speciation in supercritical fluids: An experimental study at 500–700 °C and 1.7 kbar

Banerjee, Debarati; Waters, Laura E.; Hurtig, Nicole C.; Gysi, Alexander P.; Harlov, Daniel; Zhu, Chen; Migdisov, Artaches

doi:10.1016/j.gca.2025.01.004

NdPO₄ solubility and aqueous Neodymium speciation in supercritical fluids: An experimental study at 500–700 °C and 1.7 kbar

Journal Article · Mon Jan 13 00:00:00 EST 2025 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2025.01.004· OSTI ID:2500905

Banerjee, Debarati ^[1]; Waters, Laura E. ^[1]; Hurtig, Nicole C. ^[1]; Gysi, Alexander P. ^[1]; Harlov, Daniel ^[2]; Zhu, Chen ^[3]; Migdisov, Artaches ^[4]

New Mexico Institute of Mining and Technology, Socorro, NM (United States)
Deutsches GeoForschungsZentrum GFZ Telegrafenberg, Potsdam (Germany); China University of Geosciences, Wuhan (China); University of Johannesburg (South Africa)
Indiana University, Bloomington, IN (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

A key aspect in the formation of rare earth elements (REE) deposits is the role of REE transport as aqueous REE complexes in supercritical hydrothermal solutions, where the nature of the aqueous complex is controlled by solution composition, temperature and pressure. Despite chloride being considered as one of the most abundant transporting ligands in magmatic-hydrothermal fluids, experimental investigations on the stability of aqueous REE chloride complexes are scarce above 300 °C. In this study, synthetic NdPO₄ crystals were reacted with non-saline and saline (0, 0.05 and 0.5 mNaCl), acidic (0.01 mHCl) aqueous solutions in a series of solubility experiments conducted at 500–700 °C and 1.7 kbar, where the solubilities were determined using a stable Nd isotope (¹⁴⁵Nd isotope spike) dilution technique. NdPO₄ solubility ranges between 28 ppm and 10,858 ppm, where solubility increases with both temperature and salinity. At 500 °C, log mNdPO₄ increases from –3.93 to –1.60 and there is a strong correlation between NdPO₄ solubility and NaCl concentrations (slope of 1.2 ± 0.3), indicating stabilization of the Nd chloride aqueous complexes with a stoichiometry corresponding to NdCl²⁺. At 600 °C, this correlation is weaker (slope of 0.4, log mNdPO₄ increases from –2.63 to –1.88) indicating the stabilization of both Nd chloride and hydroxyl species controlling solubility. At 700 °C, NdPO₄ solubility is largely independent of NaCl concentration indicating that solubility is controlled by Nd hydroxyl complexes, where stoichiometry suggests the neutral Nd(OH)₃⁰ species is dominant. The solubility product (Ksp) of NdPO4 is derived from experimental data with the relation: log K_sp = -41.81 – 0.057T – 20987/T, with T temperature in Kelvin. Comparison of the measured Nd phosphate solubility to thermodynamic predictions using the available Helgeson-Kirkham-Flowers equation of state parameters for aqueous Nd complexes indicate that predictions are up to three orders of magnitude lower compared to experimental observations. This discrepancy is most pronounced in saline solutions, suggesting that thermodynamic properties of the REE chloride species in supercritical fluids require revision. Numerical simulations of fluid-rock interaction between acidic, saline fluids and a Strange Lake felsic mineral assemblage demonstrates that NdPO₄ solubility predictions from models are four to six orders of magnitude lower than those calculated based on empirical fits from experiments, which suggests that acidic, saline fluids may play an important role in mobilizing large amounts of light REE from 450 to 700 °C.

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This content will become publicly available on Tue Jan 13 00:00:00 EST 2026

Research Organization:: New Mexico Institute of Mining and Technology, Socorro, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0022269

OSTI ID:: 2500905

Report Number(s):: DOE-NMT-0022269

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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NdPO4 solubility and aqueous Neodymium speciation in supercritical fluids: An experimental study at 500–700 °C and 1.7 kbar

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