Article
Chemistry, Inorganic & Nuclear
Zi-Rong Ye, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Hong-Qing Wang, Wei-Qun Shi
Summary: Designing ligands with efficient actinide/lanthanide separation performance is crucial for the disposal of radioactive waste and the recovery of minor actinides. This study investigated the selective back-extraction of Am(III) over Eu(III) using hydrophilic hydroxylated triazolyl-based ligands. The results showed that Am-N bonds have more covalent character compared to Eu-N bonds. The ligand with the best selectivity for Am(III)/Eu(III) was found to have the largest difference in covalency between Am-N and Eu-N bonds.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Xia-Ping Lei, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Chang-Ming Nie, Wei-Qun Shi
Summary: Separation of trivalent actinide and lanthanide is a major challenge in nuclear waste treatment. Recent research has shown that ligands modified with amide groups have excellent separation performance. The present study investigates the extraction behaviors of Am(III) and Eu(III) using different ligands with varying levels of preorganization. The results demonstrate that ligands with a completely preorganized structure exhibit the strongest extraction ability and highest selectivity, while those with a more flexible skeleton have weaker extraction ability and lower selectivity. This study provides valuable information for designing efficient ligands for An(III)/Ln(III) separation using a preorganization strategy.
DALTON TRANSACTIONS
(2022)
Article
Multidisciplinary Sciences
Hailong Zhang, Ao Li, Kai Li, Zhipeng Wang, Xiaocheng Xu, Yaxing Wang, Matthew V. Sheridan, Han-Shi Hu, Chao Xu, Evgeny V. Alekseev, Zhenyi Zhang, Pu Yan, Kecheng Cao, Zhifang Chai, Thomas E. Albrecht-Schonzart, Shuao Wang
Summary: The separation of americium from lanthanides in used nuclear fuel is crucial for the sustainable development of nuclear energy. Researchers have developed a nanoscale polyoxometalate cluster that selectively coordinates hexavalent actinides over trivalent lanthanides, allowing for efficient and rapid separation. This method, which utilizes membrane filtration, is organic-free and requires minimal energy input.
Article
Chemistry, Inorganic & Nuclear
Zi-Rong Ye, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Hong-Qing Wang, Wei-Qun Shi
Summary: This study focused on the separation of Am(III)/Eu(III) using four hydrophilic sulfonated ligands based on the phenanthroline and bipyridine framework. The tetrasulfonated ligand with a bipyridine framework showed the strongest complexing ability for metal ions, while the disulfonated ligand exhibited the highest selectivity for Am(III)/Eu(III). Thermodynamic analysis confirmed the selectivity of the hydrophilic sulfonated ligands towards Am(III) over Eu(III). Compared to hydrophobic nonsulfonated ligands, these hydrophilic sulfonated ligands demonstrated better complexing ability and selectivity for Am(III)/Eu(III) separation.
INORGANIC CHEMISTRY
(2021)
Article
Engineering, Chemical
Jun Liu, Baihua Chen, Yunnu Liu, Jun Ma, Xingliang Li, Yanqiu Yang
Summary: The article presents a novel tridentate ligand ETPhenAm with selective extraction properties for americium and curium, demonstrating promising experimental results and potential applications.
SEPARATION AND PURIFICATION TECHNOLOGY
(2021)
Article
Engineering, Environmental
Xiao-Fan Yang, Yang Liu, Wu-Qing Tao, Shuai Wang, Peng Ren, Su-Liang Yang, Li-Yong Yuan, Hong-Bin Tang, Zhi-Fang Chai, Wei-Qun Shi
Summary: In this study, several lipophilic N,N'-dialkyl-N,N'-diphenyl-2,9-diamide-1,10-phenanthroline (R-Ph-DAPhen) ligands were synthesized and utilized for the selective separation of Am(III) from Eu(III) in 1-octanol. The solvent extraction results confirmed the separation effect of these ligands for Am (III) over Eu(III) in both 1-octanol and TBP/1-octanol systems. Spectroscopic analysis revealed that the ligands can simultaneously form 1:1 and 1:2 complexes with Ln(III), depending on the molar ratio of metal ion to ligand. Density functional theory (DFT) calculations showed that these R-PhDAPhen ligands exhibit a strong affinity for An(III) compared to Ln(III), and 1-octanol weakens their extraction ability for both lanthanides and actinides.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Inorganic & Nuclear
Yao Zou, Jian-Hui Lan, Li-Yong Yuan, Cong-Zhi Wang, Qun-Yan Wu, Zhi-Fang Chai, Peng Ren, Wei-Qun Shi
Summary: In this study, four hydrophilic sulfonated and phosphorylated ligands L1, L2, L3, and L4 based on the bipyridine and phenanthroline backbones were designed, and their structures, neutral complexes [ML(NO3)3] (M = Am, Eu), and thermodynamic properties of complexing reactions were studied through density functional theory. According to the changes of the Gibbs free energy for the back-extraction reactions, the phenanthroline-based ligands L2 and L4 showed stronger complexing capacity for both Am(III) and Eu(III) ions, while the phosphorylated ligand L3 with the bipyridine framework exhibited the highest Am(III)/Eu(III) selectivity. This study provides theoretical insights into the separation of actinide(III)/lanthanide(III) using hydrophilic sulfonated and phosphorylated N-donor ligands.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Yao Zou, Jian-Hui Lan, Li-Yong Yuan, Cong-Zhi Wang, Qun-Yan Wu, Zhi-Fang Chai, Peng Ren, Wei-Qun Shi
Summary: In this study, three new nitrogen-donor ligands were designed and their complexes with Am(III) and Eu(III) ions were investigated using density functional theory. The results showed that the third ligand, L3, had the strongest complexation capacity, while the first ligand, L1, exhibited the highest Am(III)/Eu(III) selectivity in octanol/water solutions.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Chao Xu, Tingting Liu, Qian Liu, Suliang Yang, Dingming Li, Guoxin Tian
Summary: The similarity of coordination chemistry between Am(III) and Eu(III) and two homologous tridentate ligands, DEHAPA and DMAPA, was revealed through structural and spectroscopic analysis of complexes ML'(3) (org), ML3 (aq), and ML3 (s).
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Xia-Ping Lei, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Chang-Ming Nie, Wei-Qun Shi
Summary: The study investigates the effect of substituents on the interaction between Et-Tol-DAPhen ligands and Am(III)/Eu(III) ions. The electronic structures of the complexes are minimally affected by the substituents. However, thermodynamic results indicate that ligands with electron-withdrawing groups improve metal ion extraction ability, while ligands with electron-donating groups show the best Am(III)/Eu(III) selectivity.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Liwei Yan, Ankur Saha, Wei Zhao, Jennifer F. Neal, Yusheng Chen, Amar H. Flood, Heather C. Allen
Summary: This study investigates the role of ion binding and ion hydration in the self-assembly of cyanosurf molecules at aqueous interfaces. The results show that ion binding triggers the self-organization of cyanosurf into monolayers at the water-air interface, and hydration affects the binding and ordering of the interface.
Article
Biochemical Research Methods
Hayden R. Anderson, Wei L. Reeves, Andrew T. Bockus, Paolo Suating, Amy G. Grice, Madeleine Gallagher, Adam R. Urbach
Summary: We have developed a novel insulin derivative that exhibits high nanomolar affinity for the synthetic receptor cucurbit[7]uril (Q7), potentially enabling the development of continuous insulin detection methods for diabetes management.
BIOCONJUGATE CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Jose Munoz, Edurne Redondo, Martin Pumera
Summary: This study explores 3D-printed nanocomposite carbon electrodes as unconventional responsive interfaces for electrically reading bistable molecular switches. Two different 3D-printed responsive interfaces have been devised using surface engineering to define two electrical states driven by either electrical or optical stimuli.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Duck Hyun Kim, Yun Kyung Lee, Jin Hur, Hee-Jin Yoo, Kyung-Seok Ko, Jae Min Lee, Dong-Chan Koh, Kwang-Sik Lee, Kun Cho
Summary: This study analyzed the characteristics of NOM in water from cold and hot mineral springs in South Korea and proposed a method for evaluating the water quality characteristics in different regions of South Korea.
Article
Chemistry, Physical
Mark. N. Kobrak, Dmytro Nykypanchuk, Camiel H. C. Janssen
Summary: Mixtures of trihexylamine and cyclic carboxylic acids were used as solvents for extracting zinc salts from water. The choice of zinc salt anions represented a range of solvation properties, and their influence on extraction was investigated. Small-angle x-ray scattering was used to study the liquid structure. The results showed that extraction was strongly affected by the Hofmeister effect, but the local liquid structure was not sensitive to the solvation properties of the anions. Unlike similar studies, the strength of the Hofmeister effect did not change with the composition of the mixtures. (c) 2023 Elsevier B.V. All rights reserved.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Gregory P. Horne, Stephen P. Mezyk, Bruce J. Mincher, Christopher A. Zarzana, Cathy Rae, Richard D. Tillotson, Nicholas C. Schmitt, Richard D. Ball, Joakim Ceder, Marie-Christine Charbonnel, Philippe Guilbaud, George Saint-Louis, Laurence Berthon
RADIATION PHYSICS AND CHEMISTRY
(2020)
Review
Chemistry, Multidisciplinary
Manuel Miguirditchian, Vincent Vanel, Cecile Marie, Vincent Pacary, Marie-Christine Charbonnel, Laurence Berthon, Xavier Heres, Marc Montuir, Christian Sorel, Marie-Jordane Bollesteros, Sylvain Costenoble, Christine Rostaing, Michel Masson, Christophe Poinssot
SOLVENT EXTRACTION AND ION EXCHANGE
(2020)
Article
Chemistry, Multidisciplinary
Andreas Geist, Laurence Berthon, Marie-Christine Charbonnel, Udo Muellich
SOLVENT EXTRACTION AND ION EXCHANGE
(2020)
Editorial Material
Chemistry, Multidisciplinary
Mark R. Antonio, Mark P. Jensen
SOLVENT EXTRACTION AND ION EXCHANGE
(2021)
Article
Chemistry, Multidisciplinary
Laurence Berthon, Amaury Paquet, Georges Saint-Louis, Philippe Guilbaud
Summary: This study characterized the structure of complex organic solutions based on N,N,N',N'-tetraoctyldiglycolamide (TODGA) used in actinide separation processes, showing the influence of different factors on the formation of complexes during the metal extraction process.
SOLVENT EXTRACTION AND ION EXCHANGE
(2021)
Article
Chemistry, Multidisciplinary
Erin R. Bertelsen, Mark R. Antonio, Mark P. Jensen, Jenifer C. Shafer
Summary: The PUREX process, which involves recycling plutonium and uranium from used nuclear fuel, has been extensively researched for over 70 years, and little room is left for further discoveries. By using advanced electroanalytical methods, molecular-level insights into the back-extraction of Pu(IV) have been reported.
SOLVENT EXTRACTION AND ION EXCHANGE
(2022)
Article
Chemistry, Multidisciplinary
Clemence Berger, Ella Moreau, Cecile Marie, Dominique Guillaumont, Audrey Beillard, Laurence Berthon
Summary: The use of tri-alkylcarbamides as novel extractants shows higher capability in co-extracting uranium(VI) and plutonium(IV), with very high separation factors at lower nitric acid concentration. However, the addition of branched alkyl chains can decrease the distribution ratios and separation factors, as well as lower the viscosity of the solvent.
SOLVENT EXTRACTION AND ION EXCHANGE
(2022)
Article
Chemistry, Physical
D. Sheyfer, Michael J. Servis, Qingteng Zhang, J. Lal, T. Loeffler, E. M. Dufresne, A. R. Sandy, S. Narayanan, Subramanian K. R. S. Sankaranarayanan, R. Szczygiel, P. Maj, L. Soderholm, Mark R. Antonio, G. B. Stephenson
Summary: This study explores the applicability of critical phenomena theory in understanding the phase behavior of liquid-liquid extraction. The results show that different samples exhibit remarkably similar critical behavior, indicating that the phase transitions in liquid-liquid extraction rely on fewer variables than assumed. The extractant plays a key role in the separation process, while other solution components and their concentrations only affect the critical temperature but not the nature of the critical fluctuations.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Multidisciplinary
Ke Yuan, Mark R. Antonio, Eugene S. Ilton, Zhongrui Li, Udo Becker
Summary: Under reducing conditions, U(V) is the dominant species on the magnetite surface, and its existence is limited. By polarizing the magnetite electrode using electrochemical methods, mixed-valence U(V)/U(VI) species can be obtained, which may hinder the presence of tetravalent U.
ACS EARTH AND SPACE CHEMISTRY
(2022)
Review
Chemistry, Applied
Gauthier J-P Deblonde, Alexandre Chagnes, Gerard Cote
Summary: This review highlights the importance of hydrometallurgical processes for strategic industrial sectors and compares traditional separation methods with emerging ones. It also reviews the progress made on separation methods over the past two decades and identifies the challenges faced by hydrometallurgists in academia and the industry.
SEPARATION AND PURIFICATION REVIEWS
(2023)
Article
Chemistry, Physical
Daniel Massey, Christopher D. Williams, Junju Mu, Andrew J. Masters, Ryuhei Motokawa, Noboru Aoyagi, Yuki Ueda, Mark R. Antonio
Summary: By using an improved force field to conduct molecular dynamics simulations, we have discovered that metallic complexes in organic solvents form complex fluids with intricate structures, mainly consisting of cis isomers. With increasing metal concentration, more clustering occurs and the chemical equilibrium shifts toward the cis isomer. These isomeric effects may play a role in liquid-liquid extraction and can improve flow sheet modeling.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Alexandre Artese, Sandrine Dourdain, Nathalie Boubals, Thomas Dumas, Pier Lorenzo Solari, Denis Menut, Laurence Berthon, Philippe Guilbaud, Stephane Pellet-Rostaing
Summary: The study revealed that the different separation factors of two bifunctional extractants towards uranium and zirconium, which differ only by the grafting of an alkyl chain, are mainly controlled by their supramolecular self-assembly.
SOLVENT EXTRACTION AND ION EXCHANGE
(2022)
Article
Chemistry, Multidisciplinary
Lucas Mangold, Hubert Halleux, Sebastien Leclerc, Aurelien Moncomble, Gerard Cote, Alexandre Chagnes
Summary: Titanium chemistry in aqueous acidic media has been extensively studied, with the discovery of hydrolyzed species and the existence of titanium oxo-clusters for large concentration of titanium(iv). Furthermore, the presence of polynuclear hydrolyzed species at very low Ti(iv) concentration has been evidenced. UV-visible absorbance spectra and TD-DFT calculations have shown improved matches when considering polynuclear species. Additionally, the study of phosphoric acid solutions containing titanium(iv) identified different complexes and formulated a general complexation scheme for a wide range of acid concentration.
Article
Chemistry, Multidisciplinary
Ashleigh Kimberlin, Dominique Guillaumont, Sylvie Arpigny, Beatrice Cames, Philippe Guilbaud, Georges Saint-Louis, Hitos Galan, Laurence Berthon
Summary: This study investigates the use of diglycolamide extractants in nuclear fuel reprocessing by examining the effects of radiolysis and hydrolysis on solution chemistry, under different conditions. The presence of nitric acid provides slight protection for TODGA, while 1-octanol may have a sensitizing effect. The study also identifies the complexation behavior of lanthanide ions with degradation products, shedding light on the complex chemistry of these systems.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
Erin R. Bertelsen, Nolan C. Kovach, Brian G. Trewyn, Mark R. Antonio, Jenifer C. Shafer
JOURNAL OF MATERIALS CHEMISTRY C
(2020)
