Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine-N,N′,N′′,N′′-tetraacetic acid
| العنوان: | Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine-N,N′,N′′,N′′-tetraacetic acid |
|---|---|
| المؤلفون: | Santa Jansone-Popova, Peter R. Zalupski, Travis S. Grimes, Colt R. Heathman, Vyacheslav S. Bryantsev, Alexander S. Ivanov |
| المصدر: | Dalton Transactions. 47:1092-1105 |
| بيانات النشر: | Royal Society of Chemistry (RSC), 2018. |
| سنة النشر: | 2018 |
| مصطلحات موضوعية: | Coordination sphere, 010405 organic chemistry, Chemistry, Ligand, Potentiometric titration, Protonation, 010402 general chemistry, 01 natural sciences, Medicinal chemistry, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, Amide, Diethylenetriamine, Proton affinity, Acetamide |
| الوصف: | The novel metal ion complexant N-butyl-2-acetamide-diethylenetriamine-N,N′,N′′,N′′-tetraacetic acid (DTTA-BuA) uses an amide functionalization to increase the total ligand acidity and attain efficient 4f/5f differentiation in low pH conditions. The amide, when located on the diethylenetriamine platform containing four acetate pendant arms maintains the octadentate coordination sphere for all investigated trivalent f-elements. This compact coordination environment inhibits the protonation of LnL− complexes, as indicated by lower K111 constants relative to the corresponding protonation site of the free ligand. For actinide ions, the enhanced stability of AnL− lowers the K111 for americium and curium beyond the aptitude of potentiometric detection. Density functional theory computations indicate the difference in the back-donation ability of Am3+ and Eu3+ f-orbitals is mainly responsible for stronger proton affinity of EuL− compared to AmL−. The measured stability constants for the formation of AmL− and CmL− complexes are consistently higher, relative to ML− complexes with lanthanides of similar charge density. When compared with the conventional aminopolycarboxylate diethylenetriamine pentaacetic acid (DTPA), the modified DTTA-BuA complexant features higher ligand acidity and the important An3+/Ln3+ differentiation when deployed on a liquid–liquid distribution platform. |
| تدمد: | 1477-9234 1477-9226 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::b1d5ce63929c1802fc447259dc04cb2b https://doi.org/10.1039/c7dt04104g |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....b1d5ce63929c1802fc447259dc04cb2b |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 14779234 14779226 |
|---|