SEPARATION AND PURIFICATION TECHNOLOGY
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2014
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IF 3.065
Huang Huang,Songdong Ding,Dongping Su,Ning Liu,Jieru Wang,Mengling Tan,Jianen Fei
N , N , N ′, N ′, N ″, N ″-hexaoctylnitrilotriacetamide (NTAamide(C8)) and N,N,N ′ ,N ′ ,N ″ ,N ″-hexabutylnitrilotriacetamide (NTAamide(C4)) were synthesized for selective solvent extraction of Th(IV) from U(VI) and lanthanides(III) (Lns(III)) and for coordination between Th(IV) and NTAamide, respectively. NTAamide(C8) exhibits excellent extraction power and selectivity toward Th(IV) over U(VI) and Lns(III) in a wide range of acidity from 0.1 to 10.0 M HNO 3 . Very high SF Th/M in the range between 2.5 × 10 2 and 10 × 10 3 was observed. Slope analysis shows that Th(IV), U(VI) and Lns(III) were all extracted as mono-solvated species at 3.0 M HNO 3 . The thermodynamic parameters describing the extraction of Th(IV) indicate that the process is endothermic and spontaneous at 298 K. The single-crystal X-ray diffraction observations also establish that 1:1 complex is formed between NTAamide and thorium nitrate, which are in good accordance with the solvent extraction results, and NTAamide is coordinated with Th(IV) in a tetradentate coordination mode.
研究领域:
化学
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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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
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核化学与放射化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Chen Yuqing,Wu Xuan,Yan Taihong,Wang Wentao,Liu Junjie,Wang Hui
NTAamide(C8) exhibits high selectivity for the extraction of Pu(IV) across a wide range of nitric acid concentrations. To separate trace Pu(IV) from radioactive liquid stream generated during the PUREX process in spent nuclear fuel reprocessing, a novel silica-polymer-based adsorbent, NTAamide(C8)/SiO 2 -P, was synthesized via vacuum impregnation using NTAamide(C8) as the extractant and SiO 2 -P as the support. The adsorption performance of Pu(IV) were systematically evaluated. Batch experiments revealed that adsorption equilibrium was achieved within 2 h, with a maximum adsorption capacity of 143.2 mg/g for Pu(IV). The material demonstrated high selectivity for Pu(IV) and exhibited excellent radiation resistance and hydrolytic stability. The adsorption mechanisms were further elucidated using X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations, confirming the formation of 1:1 complexes between NTAamide(C8) and the metal ions. Column experiments using actual uranium product solution from the PUREX process verified the material's performance in trace Pu(IV) removal. After column treatment, the Pu content in the uranium product solution was reduced to below 10 Bq/gU, with no significant loss of uranium. These results demonstrate that NTAamide(C8)/SiO 2 -P is a promising adsorbent for the efficient and selective separation of Pu(IV) from radioactive liquid stream under a wide range of nitric acid concentrations.
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Zhuang Wang,Dongping Su,Ting Luo,Qiao Yu,Yiting Wang,Hang Zhou,Rui Li,Qing-Jiang Pan,Songdong Ding
High-purity thorium is essential for producing key radioactive nuclides, such as 233U and 225Ac. Currently, the primary challenge in preparing high-purity thorium is separating trace amounts of uranium and rare earth impurities from crude thorium products. To address this, an efficient NTAamide(n-Oct)@CG71M extraction resin was developed for isolating high-purity thorium in a nitric acid medium containing uranium and rare earth elements. Batch adsorption studies exhibit high selectivity and strong adsorbability for thorium over a relatively wide acidity range of 0.10–8.0 mol/L HNO3. The adsorption of thorium onto the resin conforms to pseudo-second-order kinetics and the Langmuir model, with a maximum Th(IV) adsorption capacity (qmax) of 79.9 mg/g. Thermodynamically, the process is exothermic and spontaneous, accompanied by an increase in the entropy. The NTAamide(n-Oct) extractant in the resin coordinates with Th(IV) via three oxygen atoms of the carbonyl groups and one tertiary amine nitrogen atom. Dynamic separation experiments confirmed that the NTAamide(n-Oct)@CG71M extraction resin can efficiently remove trace uranium impurities from commercial thorium nitrate reagents, yielding high-purity thorium nitrate (99.99%). Furthermore, the resin selectively separated thorium from simulated monazite HNO3 leach liquor with a 99.4% recovery rate and high-purity thorium (99.99%) while demonstrating good reusability. Overall, this efficient extraction resin provides reliable technical support for high-purity thorium nitrate preparation and shows significant application potential.
✓ 已验证
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2025
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IF 4.7
Xueyu Wang,Qiao Yu,Hang Zhou,Rui Li,Yanqiu Yang,Qingjiang Pan,Songdong Ding
The nitrilotriacetamide n-octyl derivative ligand (NTAamide(n-Oct)) is promising for minor actinide/lanthanide separation, yet periodic trends in its extraction and complexation across the lanthanide series remained unclear. This study systematically investigated its behavior with trivalent rare-earth ions (Ln3+, Y3+, and Sc3+) using solvent extraction, 1H NMR titration, UV–vis spectrophotometric titration, microcalorimetric titration, single-crystal X-ray diffractometry, ESI-MS, and FTIR. Key findings reveal opposing ionic radius dependencies. Solvent extraction showed that extraction efficiency negatively correlates with the ionic radius, decreasing with the ionic radius. Slope analysis indicated Sc3+ forms 1:2 metal–ligand extracted complexes, while other RE3+ ions form 1:1 complexes. Conversely, homogeneous and solid-state studies uniformly identified 1:2 stoichiometry for all RE3+ complexes, with complexation strength positively dependent on the ionic radius, increasing as the ionic radius decreases. Overall, the extraction and complexation ability trends of NTAamide(n-Oct) toward RE3+ exhibit opposing tendencies. Combined with the results of solvent extraction and complexation studies, the compositions of the complexes formed by NTAamide(n-Oct) with Sc3+ or other RE3+ are [ScL2](NO3)3 and [REL2][RE(NO3)6] (L = NTAamide(n-Oct)), respectively. Furthermore, an ion-pair extraction model is also proposed and discussed.
研究领域:
无机化学
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配位化学
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核化学
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分离科学
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稀土材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2017
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IF 3.359
Zhipeng Wang,Songdong Ding,Xiaoyang Hu,Shimeng Li,Dongping Su,Lirong Zhang,Ying Liu,Yongdong Jin
A novel water-soluble ligand of N,N,N‴,N‴ -tetraethyl- N ′ ,N ″-ethidene bisdiglycolamide (TEE-BisDGA) was synthesized and used as a masking agent for selective extraction of Am(III) over Eu(III) from HNO 3 solution by N,N,N ′, N ′ ,N ″ ,N ″-hexaoctylnitrilotriacetamide (NTAamide(C8)) in kerosene. Influences of acidity, concentration of water-soluble ligands and extractant as well as nitrate ions on the distribution ratios ( D ) and separation factors ( SF ) of Am(III) and Eu(III) were investigated. In the range of examined acidity from 0.001 to 0.2 mol/L, D Am and D Eu decreased with the increase of HNO 3 concentration. Using 0.1 mol/L NTAamide(C8) as an extractant, the maximum SF Am/Eu of 26 can be obtained in the presence of 0.01 mol/L TEE-BisDGA in aqueous phase with pH of 3.0, which was significantly higher than that case with no TEE-BisDGA. Job's method and mole ratio method were employed for extraction mechanism research. It has been shown that Am(III) and Eu(III) formed di-solvated species with TEE-BisDGA and mono-solvated species with NTAamide(C8), respectively. Moreover, the stability constants logβ values were obtained from UV–vis adsorption spectroscopic titration for Nd(III) complexes with TEE-BisDGA and N,N,N ′ ,N ′-tetraethyldiglycolamide (TEDGA), which indicated that TEDGA had a stronger complex ability than TEE-BisDGA.
研究领域:
化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）