Adsorption of terbium (III) on DGA and LN resins: Thermodynamics, isotherms, and kinetics

Holiski, Connor K.; Payne, Rachel; Wang, Meng-Jen (Vince); Sjoden, Glenn E.; Mastren, Tara

doi:10.1016/j.chroma.2024.465211

Adsorption of terbium (III) on DGA and LN resins: Thermodynamics, isotherms, and kinetics

Journal Article · Thu Jul 25 00:00:00 EDT 2024 · Journal of Chromatography

DOI:https://doi.org/10.1016/j.chroma.2024.465211· OSTI ID:2475654

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University of Utah, Salt Lake City, UT (United States); University of Utah
University of Utah, Salt Lake City, UT (United States)
University of Utah, Salt Lake City, UT (United States); University of Nevada, Las Vegas, NV (United States)

Two commercially available extraction chromatography (EXC) resins containing N,N,N’,N’-tetra-n-octyldiglycolamide (DGA Resin, Normal, 50 – 100 μm) and Bis(2-ethylhexyl) phosphate (LN Resin, 100 – 150 μm) were used as adsorbents to study fundamental adsorption properties such as thermodynamic values, equilibrium isotherms, and kinetic uptake models for terbium(III) adsorption. Weight distribution ratios (D_w) for terbium on DGA and LN resins were measured using a [¹⁶⁰Tb]Tb³⁺ radiometric tracer in nitric acid as a function of acidity, temperature, initial analyte concentration, and equilibrium time. The D_w values showed increasing binding affinity for DGA resin at high nitric acid concentrations and decreasing binding affinity for LN resins. Thermodynamic studies for DGA and LN resins revealed that the Gibbs free energy (ΔG) increased consistently with temperature. To model equilibrium data, increasingly higher parameter equilibrium isotherm models (Henry (1) < Langmuir, Freundlich (2) < Redlich-Peterson (3) < Fritz-Schluender (4)) were compared on their root mean squared errors (RMSE) and adjusted determination coefficients to determine the most applicable model. In all cases, the empirical four-parameter Fritz-Schluender isotherm demonstrated a superior fit. Similar comparisons for reaction-based kinetic models (Pseudo-first-order < Pseudo-second-order < Pseudo-n-order) revealed that the higher-order PNO model yielded a superior fit of kinetic data for both resins. Furthermore, in some cases, adsorption isotherms and kinetic models could also be modeled by a lower-order model with minimal change in error parameters. Weber-Morris plots revealed that two linear sections are observed for each resin, where the first linear segment is attributed to fast (film diffusion) adsorption of terbium, followed by slower intraparticle diffusion of terbium through the pores as the rate-limiting step. Based on the Weber-Morris plot, both film and intraparticle diffusion are involved in controlling the kinetic rate of adsorption for DGA and LN resins.

View Accepted Manuscript (DOE)

Research Organization:: University of Utah, Salt Lake City, UT (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Office of Isotope R&D and Production (IRP)

Grant/Contract Number:: SC0020955

OSTI ID:: 2475654

Alternate ID(s):: OSTI ID: 2439328

Journal Information:: Journal of Chromatography, Journal Name: Journal of Chromatography Vol. 1732; ISSN 0021-9673

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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