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With the development of nuclear energy, the reprocessing of TcO/ReO has become a very difficult problem due to environmental issues such as high output, long life, and easy leakage. In this study, three extraction systems containing carbamic acid were introduced into the reprocessing of TcO/ReO for the first time. The results involving one of the three results show that -[,-di(2-ethylhexyl) aminocarbonylmethyl] glycine (D2EHAG) has ultrahigh selectivity for removal to TcO/ReO. When the extreme concentration ratio of SO and Cl to ReO of D2EHAG is 10,000:1, the distribution coefficient of ReO still reaches 12.73 and 2.67, respectively. Additionally, the most hydrophilic NO, when the extreme concentration ratio of NO and ReO is 1000:1, still has a distribution coefficient close to 2.33, which is more than the most reported MOF adsorption materials. Moreover, the reaction kinetics, stripping rate, and reuse rate were studied. After five cycles, the removal rate is still 98.12%, with a decrease of less than 0.7%. The system containing carbamic acid is a potential extraction removal system to remove TcO/ReO from nuclear radioactive wastewater.
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http://dx.doi.org/10.1021/acs.inorgchem.2c03708 | DOI Listing |
Dalton Trans
January 2025
Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China.
The co-extraction of pertechnetate (TcO) along with the uranyl ion (UO) is a problematic issue that complicates the Plutonium Uranium Reduction EXtraction (PUREX) process for reprocessing spent nuclear fuel. Unfortunately, research on the interactions of TcO with UO is very scarce. This work quantitatively investigated the interactions of TcO and its analog ReO with UO in acetonitrile with 0.
View Article and Find Full Text PDFChem Commun (Camb)
May 2024
Department of Chemistry, Oregon State University, Corvallis, OR-97331, USA.
Pertechnetate (TcO), reduced Tc, and actinides co-exist in spent nuclear fuel and legacy wastes. They co-transport in fuel reprocessing and waste disposal scenarios, necessitating an understanding of co-speciation. Here, we report five new molecular cluster/framework structures with pentameric and tetrameric uranyl building units decorated by TcO/ReO oxoanions, or fused with the reduced technetyl cation Tc(V)O.
View Article and Find Full Text PDFInorg Chem
January 2024
Department of Chemistry, Oregon State University, Corvallis, Oregon 97331, United States.
Spent nuclear fuel (SNF) contains transuranic and lanthanide species, which are sometimes recovered and repurposed. One particularly problematic fission product, TcO, hampers this recovery via coextraction with high valence metals, perhaps by complexation during aqueous reprocessing of SNF. There is limited molecular-level knowledge concerning the coordination chemistry between TcO or its well-known surrogate ReO and transuranic/lanthanide species.
View Article and Find Full Text PDFChemistry
February 2024
Department of Chemistry, Oregon State University, Corvallis, Oregon, 97331, USA.
Spent nuclear fuel contains heavy element fission products that must be separated for effective reprocessing for a safe and sustainable nuclear fuel cycle. Zr and Tc are high-yield fission products that co-transport in liquid-liquid extraction processes. Here we seek atomic-level information of this co-extraction process, as well as fundamental knowledge about Zr (and Hf ) aqueous speciation in the presence of topology-directing ligands such as pertechnetate (TcO ) and non-radioactive surrogate perrhenate (ReO ).
View Article and Find Full Text PDFChemistry
October 2023
College of Chemistry, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, Tianjin Normal University, Tianjin, 300387, China.