INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xiao Xiao,Long Li,Zhuang Wang,Qiao Yu,Xuanhao Huang,Xingyue Liu,Qingjiang Pan,Songdong Ding
Five amine-diamide ligands (DAMIA) with varying alkyl chain lengths and steric hindrances are developed for selective extraction of Am3+ over Eu3+ in high-acidity HNO3 solution with the aim of understanding the structure–activity relationship. The ability of these ligands to extract metal ions is closely related to their basicity. The weaker the basicity is, the stronger the extraction ability is. The substituent on the aminic N has more significant effect on the extraction ability than that on the amidic N. Among the five ligands, the DAMIA containing five branched 2-ethylhexyl substituents demonstrates the highest extraction ability and selectivity at molar acidity level. Slope analysis suggests the formation of a 1:1 metal/ligand extracted species, which is also supported by the results obtained from the UV–vis spectrophotometric titration. Furthermore, the analyses of Fourier transform infrared (FT-IR), time-resolved laser-induced fluorescence spectroscopy (TRLFS), and X-ray photoelectron spectroscopy (XPS) for the extracted complex indicate that one Eu3+ ion may be nine-coordinated by one ligand molecule in a tridentate manner via two amide O atoms and one tertiary amine N atom and three bidentate NO3– ions. There is no H2O molecule in the inner coordination sphere of central Eu3+. Additionally, based on the studies of solvent extraction and complexation, the extraction of metal ions follows the neutral complexation extraction model, and the corresponding thermodynamic parameters (ΔH, ΔS, and ΔG) are also presented.
研究领域:
化学
·
核化学与放射化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2017
·Vol. 313
·期 2
·309-318
·
IF 1.282
Wang Zhipeng,Huang Huang,Ding Songdong,Hu Xiaoyang,Zhang Lirong,Liu Ying,Song Lianjun,Chen Zhili,Li Shimeng
Abstract Two diglycolamide homologs, N,N,N′,N′ -tetraoctyl-3,6-dioxaoctane diamide (DOODA) and N,N,N′,N′ -tetraoctyl-3,6,9-trioxaundecane diamide (TOUDA), were synthesized. Their extraction behaviors of Am 3+ and Eu 3+ were investigated and compared with those of N,N,N′,N′ -tetraoctyl-3-oxapentane diamide (TODGA). The extraction ability toward Am 3+ and Eu 3+ decreased with increasing etheric oxygen number in the extractant structure. In contrast to TODGA, an very interesting inversion on the selectivity occurred for DOODA and TOUDA, which were more favor of extracting Am 3+ than Eu 3+ . The maximum SF
Am/Eu of 3.5 for DOODA can be achieved at 3.0 mol/L HNO 3 . The stoichiometries of extracted species and extraction thermodynamic parameters were also presented. Graphical Abstract
研究领域:
化学
·
核化学与放射化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lanlan He,Xueyu Wang,Qiuju Li,Xiao Xiao,Fengfeng Li,Fangxiang Luo,Qingjiang Pan,Songdong Ding
Two novel water-soluble aromatic bisdiglycolamides (BisDGAs) of SO 3 -TEX( m )-BisDGA (sodium bis((2-(2-(diethylamino)− 2-oxoethoxy)acetamido)methyl)benzenesulfonate) and SO 3 -TEX( p )-BisDGA (sodium 2,5-bis((2-(2-(diethylamino)− 2-oxoethoxy)acetamido)methyl)benzenesulfonate) were synthesized and used as masking agents for the selective extraction and separation of Am 3+ over Eu 3+ in HNO 3 solutions by N,N,N′,N′,N′′,N′′ -hexaoctylnitrilotriacetamide (NTAamide( n -Oct)) in n -dodecane. Their influences on the separation effect of Am 3+ over Eu 3+ were investigated and compared with that of a water-soluble aliphatic bisdiglycolamide of N,N,N′′′,N′′′ -tetraethyl- N′,N′′ -ethidene bisdiglycolamide (TEE-BisDGA) reported by our previous work. SO 3 -TEX( m )-BisDGA and SO 3 -TEX( p )-BisDGA exhibit significantly better masking effects than TEE-BisDGA. The masking selectivity for Eu 3+ over Am 3+ follows the order of SO 3 -TEX( m )-BisDGA > SO 3 -TEX( p )-BisDGA > TEE-BisDGA. During the extraction process, the three BisDGA masking agents form the 1:2 complexes, while the NTAamide ( n -Oct) extractant forms the 1:1 complexes with Am 3+ and Eu 3+ . Meanwhile, the conditional stability constants (log β ) for the three masking agents with Eu 3+ were calculated using the least squares method, which are also in line with those obtained from fluorescence spectrometry (FS). By means of FS, time-resolved laser-induced fluorescence spectrometry (TRLFS), Fourier Transform infrared spectrometry (FT-IR), conductivity, and electrospray ionization mass spectrometry (ESI-MS) analyses, the composition of the complex of Eu 3+ with water-soluble BisDGAs (L) was determined to be [Eu(NO 3 ) 2 (H 2 O)∙2L](NO 3 ). Furthermore, a batch simulation of multistage countercurrent extraction with 12-stage extraction, 4-stage scrubbing and 8-stage stripping was carried out and demonstrates a highly efficient separation of Am 3+ over Lns 3+ with the recovery rates above 99.9 % for all metal ions in the simulated feed solution, and with the decontamination factors more than 500 between Am 3+ and most of the lanthanide ions.
研究领域:
化学
·
核化学与放射化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
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