Mechanisms and kinetics of citrate-promoted dissolution of a uranyl phosphate mineral

Ferguson, Brennan O.; Murdoch, Lawrence C.; Trumm, Michael; Liu, Fengjiao; Rao, Apparao M.; Powell, Brian A.

doi:10.1016/j.gca.2021.11.023

Mechanisms and kinetics of citrate-promoted dissolution of a uranyl phosphate mineral

Journal Article · Sat Nov 27 00:00:00 EST 2021 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2021.11.023· OSTI ID:1977155

Ferguson, Brennan O. ^[1]; Murdoch, Lawrence C. ^[2]; ^[3]; Liu, Fengjiao ^[2]; Rao, Apparao M. ^[2]; ^[2]

Clemson University, SC (United States); OSTI
Clemson University, SC (United States)
Karlsruhe Inst. of Technology (KIT) (Germany)

The formation of uranyl phosphate precipitates is a remediation strategy to limit the mobility of uranium in contaminated soils. However, exposure to organic ligands, like the plant exudate citrate, can remobilize the uranium. The purpose of this study is to provide a more thorough comprehension of citrate-promoted dissolution of a uranyl phosphate mineral, chernikovite [(H₃O)(UO₂)(PO₄)·3H₂O], by determining the extent of uranium release from chernikovite at a wide range of citrate concentrations. Here we have quantified the kinetics of dissolution and proposed potential mechanisms of chernikovite dissolution to gain a better understanding of the fate of uranyl phosphate precipitates in the environment. Batch dissolution and continuously stirred tank reactor (CSTR) experiments indicate that increasing citrate concentrations from 0.1 mM to 50 mM increases the concentration of dissolved uranium. However, at citrate concentrations of 10 mM and greater, the effectiveness of the ligand to enhance the dissolution decreases. Density functional theory modeling and Raman spectroscopy indicate a strong interaction between citrate and the uranyl ions at the surface of the uranyl phosphate. The interaction between citrate and uranyl suggests the formation of an alteration layer of uranyl-citrate surface complexes, which could impede uranium release at citrate concentrations of 10 mM or higher. Together, these results indicate that the citrate-promoted dissolution of chernikovite is a fast reaction that is hindered by a combination of surface saturation and a secondary-phase precipitation reaction at higher concentrations of citrate and reaction times greater than or equal to 72 min based on the hydraulic residence time of CSTR experiments. These findings improve our understanding of the stability of uranyl phosphate for use in sequestration of uranium groundwater plumes at contaminated sites.

View Accepted Manuscript (DOE)

Research Organization:: Clemson University, SC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0012530

OSTI ID:: 1977155

Alternate ID(s):: OSTI ID: 1836877

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 318; ISSN 0016-7037

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

Country of Publication:: United States

Language:: English

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58 GEOSCIENCES
CSTR
Continuously stirred tank reactor
chernikovite
citrate
dissolution kinetics
phosphate
solubility
uranium

Mechanisms and kinetics of citrate-promoted dissolution of a uranyl phosphate mineral

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