Metallic Technetium Sequestration in Nickel Core/Shell Microstructure during Fe(OH)2 Transformation with Ni doping

Wang, Guohui; Kim, Dong-Sang; Olszta, Matthew J.; Bowden, Mark E.; Schreiber, Daniel K.; Saslow, Sarah A.; Um, Wooyong; Riley, Brian J.; Wang, Jing; Kruger, Albert A.

doi:10.1016/j.jhazmat.2021.127779

Metallic Technetium Sequestration in Nickel Core/Shell Microstructure during Fe(OH)2 Transformation with Ni doping

Journal Article · 05 March 2022 · Journal of Hazardous Materials

DOI:https://doi.org/10.1016/j.jhazmat.2021.127779· OSTI ID:1872431

Wang, Guohui ^[1]; ^[1]; ^[1]; Bowden, Mark E. ^[1]; Schreiber, Daniel K. ^[1]; ^[1]; Um, Wooyong ^[1]; ^[1]; ^[1]; Kruger, Albert A. ^[2]

BATTELLE (PACIFIC NW LAB)
OFFICE RIVER PROTECTION

This study investigates the impacts of Ni doping on technetium-99 (Tc) sequestration in aqueous solutions through transformation of Fe(OH)2(s) to iron spinel (magnetite) under alkaline conditions. Extensive solid characterization was performed for the mineral phases produced, as well as the Tc/Ni speciation and distribution within these phases. X-ray diffraction results show that iron spinel was the dominant mineral product without detectable Ni incorporation. The doped Ni ions mainly precipitated as fine Fe/Ni oxide/hydroxide particles, including strongly reduced nanometer?sized spheroidal Ni-rich and metallic Ni phases. High-resolution analytical scanning transmission electron microscopy using energy dispersive X-ray spectroscopy and electron energy loss spectroscopy on the produced solid samples (focused ion beam-prepared specimens) revealed three Tc distribution domains dominated by nanocrystals and, especially, a Tc-rich metallic phase. Instances of metallic Tc were specifically found in spheroidal, Ni-rich and metallic nanoparticles exhibiting a core/shell microstructure that suggests strong reduction and sequential precipitation of Ni-Tc-Ni. Mass balance analysis showed nearly 100% Tc removal from the 4.8 × 10-4 M Tc solutions. The finding of the metallic Tc encapsulation indicates that Tc sequestration through Ni-doped Fe(OH)2(s)?to?iron spinel transformation process likely provides an alternative treatment pathway for Tc removal and could be combined into further waste treatment approaches.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1872431

Report Number(s):: PNNL-SA-146435

Journal Information:: Journal of Hazardous Materials, Vol. 425

Country of Publication:: United States

Language:: English

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