Mineral-specific heterogeneous neptunium sorption onto geological repository rocks in oxic and anoxic conditions and various temperatures

Konevnik, Yu V.; Zakharova, E. V.; Shiryaev, A. A.; Olds, T. A.; Burns, P. C.

doi:10.1016/j.chemgeo.2020.119654

Mineral-specific heterogeneous neptunium sorption onto geological repository rocks in oxic and anoxic conditions and various temperatures

Journal Article · Sun May 03 00:00:00 EDT 2020 · Chemical Geology

DOI:https://doi.org/10.1016/j.chemgeo.2020.119654· OSTI ID:1800402

Konevnik, Yu V. ^[1]; Zakharova, E. V. ^[2]; Shiryaev, A. A. ^[2]; Olds, T. A. ^[3]; ^[3]

Russian Academy of Sciences (RAS), Moscow (Russian Federation); OSTI
Russian Academy of Sciences (RAS), Moscow (Russian Federation)
Univ. of Notre Dame, IN (United States)

Neptunium poses challenges for radioactive wastes management due to its long half-life and ingrowth from americium decay, as well as its high mobility in water in its oxidized forms. Np(V)-bearing aqueous solutions were contacted with polished and crushed gneiss and dolerite from the Yeniseisky site, Russia, which is under consideration as a location for an underground repository, both in oxic and anoxic conditions at 20 and 90 °C. Neptunium sorption on crushed gneiss and dolerite in oxic conditions at 20 °C was quite low, but increased substantially in anoxic conditions. Autoradiography on samples treated at 20 °C revealed that sorbed Np was associated mostly with dark colored iron-bearing minerals, and solvent extraction indicated partial reduction of Np(V) to Np(IV). Sorption of Np from aqueous solutions contacted with dolerite and gneiss at 90 °C was in all cases higher than at the lower temperature. Autoradiography of polished rock samples treated in anoxic conditions at 90 °C revealed that Fe-bearing minerals had 3–4 orders of magnitude more Np sorbed on them than the quartz and feldspar grains. X-ray photoelectron spectroscopy indicated this sorbed Np was present as NpO₂. This study supports the concept that the geologic conditions present at the planned repository site will retard Np migration.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-07ER15880

OSTI ID:: 1800402

Alternate ID(s):: OSTI ID: 1703140

Journal Information:: Chemical Geology, Journal Name: Chemical Geology Vol. 545; ISSN 0009-2541

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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