Separations
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2025
·Vol. 12
·期 5
·106
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IF 2.7
Xiaoyun Guo,Junli Wang,Yao Liu,Haojun Zhao,Hui Wang,Wentao Wang,Baole Li,Taihong Yan
Developing a new efficient separation ligand based on the “CHON” principle to address the limitations of phosphorus containing extractants in nuclear fuel reprocessing can help further simplify the process flow and reduce the amount of secondary waste. Building upon this critical need, a novel ligand was developed through a strategic application of the Hard and Soft Acids and Bases (HSAB) theory, integrating a soft donor nitrogen atom into the linear architecture of bis-diglycolamide. This groundbreaking ligand, named N,N′-bis[2-(2-(N,N-dioctylcarbamoyl)ethoxy)ethylacetamido]-N″-diethylenetriamine (TOMDEA-BisDGA), has demonstrated remarkable potential in the extraction of Pu(IV). The study unveils that the ligand demonstrates remarkable selectivity and separation efficiency towards Pu(IV) ions while maintaining an exceptionally low extraction capacity for U(VI) across a wide acidity spectrum of 0.1~6 mol/L. To explain the structure properties of complex formed by the ligand and Pu(IV), a systematic analysis was performed, including slope analysis, proton nuclear magnetic resonance (NMR) titration, and Fourier-transform infrared (FT-IR) spectroscopy. This study explores the coordination and separation behavior of diglycolamide ligands with actinide. This work is expected to provide important information and theoretical bases upon which advanced design and optimization of ligands for high-performance processes for the separation of plutonium might be carried out. Such findings will contribute to the understanding of actinide chemistry and further the design of improved separation methods for nuclear applications.
研究领域:
核化学
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配体设计
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放射化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Zhenzhen Wang,Encheng Liu,Zhonghua Sun,Zhihui Zhang,Mingyang He,Qun Chen,Junfeng Qian
Formic acid (FA) is of great significance given its extensive applications in various industrial fields. At present, methanol carbonylation is the main industrial production process of FA. However, this process uses two kinds of raw materials from fossil fuels and emits a large amount of CO 2 . Alternatively, converting CO 2 into FA can not only achieve the production of value-added chemicals but also effectively address environmental issues caused by CO 2 emission. To improve the low reactivity of CO 2 , homogeneous and heterogeneous catalytic systems have been widely evaluated, among which heterogeneous catalytic systems are attracting ever-increasing attention owing to their great industrialization prospects. However, some of these heterogeneous catalysts suffer from low catalytic performance. Herein, PdAu alloy nanoparticles anchored on amine-functionalized hierarchical porous carbon (PdAu/HPC-AP) were constructed to drive efficient converting of CO 2 into FA. Characterization and testing results demonstrated that the introduced Au atoms caused lattice distortion and charge redistribution on the surface of the bimetallic catalyst, facilitating the adsorption and activation of reaction molecules. Furthermore, the modification of HPC with an appropriate amount of amine ligands was found important to the chemical adsorption of CO 2 and the dispersion of PdAu NPs. The Pd 60 Au 40 /HPC-AP catalyst with the optimum synergy of alloy and ligand demonstrated excellent activity for the target reaction with a TOF value of 486 h –1 at 100 °C. Moreover, it can even catalyze the reaction at room temperature with a TOF value of 13 h –1 .
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2018
·
IF 3.306
Wen Xu,Xiaofeng Dai,Teng Zhang,Tao Wang
Copper complex conductive inks inevitably contains water which is derived from chemicals and humid air. The dual effects of water on the performance of copper complex conductive inks with amines as ligands were investigated for the first time. On one hand, excess water caused the deterioration of copper complexes by interacting with amines to produce high concentration of OH − , yielding basic salt, hydroxide or oxide precipitate, which shortened the shelf life of copper inks. The degree of deterioration was related to the amine’s coordination ability and alkalinity. On the other hand, trace water could accelerate the thermal decomposition of copper complexes, promote the nucleation of copper, and yield smaller particles to form copper films with denser structure and lower resistivity. The blending of 2-ethylhexylamine (EtHex) and 2-amino-2-methyl-1-propanol (AMP) as ligands to copper formate (Cuf) could balance the dual effects of water on copper complex conductive inks. It was found that Cuf-EtHex-AMP (with 95 mol% EtHex in blended ligands) ink showed strong water resistance. The shelf life of the blended complex ink with additional 2 wt% water was still more than 2 months. The additional water enabled the formation of highly conductive copper films at low heating temperature. The resistivity of the copper film from the blended complex ink with additional 2 wt% water stored for 2 months only increased a little compared to that from the newly prepared ink (from 9.70 μΩ·cm to 14.42 μΩ·cm), which could meet the general requirements of printed electronics.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Minggang Hu,Xiaochen Wang,Can Wang,Hongtao Chu,Xinfeng Song,Guohua Dong,Jiyuan Zhang,Jin Xing
In this study, a new and simple method for synthesizing boron complexes was presented. The boron complexes with C 2 -symmetric ligands were prepared from in situ generated tertiary amine by the reaction of salicylaldehyde with primary amine in the presence of sodium borohydride. The boron complexes were characterized by 1 H and 13 C NMR spectroscopy, elemental analysis, and mass spectrometry. The crystal structures of complexes 1 and 2 were determined by single crystal X-ray diffraction method. The complex is a mononuclear boron complex with a tertiary amine ligand. The boron center is tetracoordinated with a distorted tetrahedral geometry. Catalytic activities of the boron complexes in the reduction of dyes, was investigated using sodium borohydride as a reducing agent. Complexes 1 and 2 were effective catalysts for degradation of dyes. Kinetic studies reveal that the reduction of methylene blue is of the first order. Free radical scavenging activities of the boron complexes have been tested using DPPH, ABTS and hydroxyl radicals, respectively. The result shows that the boron complexes have effective antioxidant activity.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
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
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核化学与放射化学
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DOI
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
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2019
·
IF 1.685
Jun Wang,Jinyi Liu,Tianyu Lan,Liduo Chen,Libo Wang
Two new hyperbranched bispyridylamine ligands and multinuclear chromium complexes were synthesized with 1.0 G hyperbranched macromolecules, 2-chloropyridine, 2-chloro-4-methylpyridine and CrCl3(THF)3 as raw materials. The structures of hyperbranched ligands and chromium complexes were characterized by UV, FT-IR, 1H NMR, ESI-MS, and elemental analysis. These hyperbranched chromium complexes were evaluated as catalyst precursors by using MAO as activator in the oligomerization of ethylene. Effects of reaction temperature, reaction pressure, Al/Cr molar ratio, concentration of catalyst, solvent, and the structure of catalysts on the catalytic activity and product selectivity were investigated. The oligomerization results showed that with increase of reaction temperature, reaction pressure, and Al/Cr molar ratio, the catalytic activity increased and then decreased; the catalytic activity continuously decreased as the amount of catalyst increased. The products were mainly based on C6 and C8. Under optimized conditions, the catalytic system of hyperbranched NNN/Cr(III)/MAO led to activity of 1.26 × 105 g/(mol·Cr·h) and 63.34% selectivity for C6 and C8.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2015
·
IF 2.173
Haiyang Liu,Xiaoshuang Li,Feng Liu,Ying Tan,Yuyang Jiang
This paper discusses the synthesis of the amide ligand N,N-diisopropyl quinoline-2-carboxamide from quinoline-2-carboxylic acid and diisopropylamine. The prepared ligand was utilized in the palladium catalyzed Suzuki cross-coupling reaction in ethanol-water 1:1 (v/v). The reaction exhibited high catalytic efficiency with low Pd loading (0.05 mol %) under mild reaction conditions (at 60–90 °C under air atmosphere). In this study, the catalyst was successfully used in coupling reactions between various aryl halides with phenylboronic acid to obtain desired products in excellent yields. Spectrometric methods of 1 H NMR, 13 C NMR, and HR-MS were used to characterize this amide ligand, and its binding properties toward the Pd center were also investigated in detail via HR-MS measurements.
研究领域:
有机化学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Yimin Cai,Seraj A. Ansari,Kuirong Fu,Beichen Zhu,Haoyang Ma,Lixi Chen,Steven D. Conradson,Song Qin,Haiying Fu,Prasanta K. Mohapatra,Lihua Yuan,Wen Feng
Selective extraction of highly radiotoxic actinides(III) is an important and challenging task in nuclear wastewater treatment . Many proposed ligands containing S or P atoms have drawbacks including high reagent consumption and possible secondary pollution after incineration. The present work reports five novel pillar[5]arene-based extractants that are anchored with picolinamide substituents of different electronic nature by varying spacer. These ligands reveal highly efficient separation of actinides(III) over lanthanides(III). Specifically, almost all of these ligands could extract Am(III) over Eu(III) selectively at around pH 3.0 (SF Am/Eu > 11) with fast extraction kinetics. Variation of the pyridine nitrogen basicity via changing para-substitution leads to an increase in the distribution ratios by a factor of over 300 times for Am(III) with an electron-withdrawing group compared to those with an electron donating group. Investigation of complexation mechanism by slope analysis, NMR, IR, EXAFS , and DFT techniques indicates that each ligand binds two metal ions by pyridine nitrogen and amide oxygen. Finally, these ligands do not show obvious decrease in both extraction and separation ability after being exposed to 250 kGy absorbed gamma radiation . These results demonstrate the potential application of pillar[5]arene-picolinamides for actinide(III) separation.
研究领域:
化学
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核废料处理
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2021
·
IF 4.759
Houmei Liu,Pian Jin,Mi Jiang,Yu Duan,Guozheng Zhu,Hui Yu,Hongdeng Qiu
In this work, for the first time five amine-ligands including mono-amine, di-amine, tri-amine, secondary and tertiary amine, were functionalized on mesoporous micro-silicas and developed as stationary phases for hydrophilic interaction liquid chromatography (HILIC). The investigations about the retention mechanisms, effects of different chromatographic conditions and stability were systematically conducted. Three kinds of polar and hydrophilic compounds (saccharides, sulfonamides, nucleosides and nucleobases) were selected as probe molecules to evaluate their separation performances. Among the five stationary phases, only aminopropyl-bonded silica has already gained wide developments and applications. Whereas, there are no related researches about the other four to be utilized as separation media. By a series of chromatographic evaluations, the results revealed the other four mesoporous micro-silica materials functionalized with di-amine, tri-amine, secondary and tertiary amine, had great potential to be explored as novel stationary phases of HILIC. Particularly, the two stationary phases functionalized with di-amine and tri-amine exhibited outstanding separation and retention abilities. This work offered some insights on the understanding of retention in HILIC mode and provided us possibility to explore other amine-based HILIC stationary phases.
研究领域:
分析化学
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色谱科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL RESEARCH
·
2019
·
IF 0.67
Jun Wang,Jinyi Liu,Liduo Chen,Tianyu Lan,Libo Wang
A series of nickel complexes containing bispyridylamine ligands is synthesized and characterized by UV-Vis, FTIR, 1H NMR, ESI-MS, and elemental analysis. All nickel complexes activated with methylaluminoxane exhibited moderate activity for ethylene oligomerization (5.30 × 104 to 2.54 × 105 g/(mol·Ni·h)), producing oligomers in the range C4–C18. The effects of reaction temperature, reaction pressure, Al/Ni molar ratio, and solvent type on the catalytic activity and product selectivity are also investigated. The resulting products are mainly low-carbon olefins (C4 and C6). Under the optimized conditions, the complex with R1 = C4H9 formed by the reaction of the corresponding ligand R1 = C4H9 with NiCl2·6H2O showed a higher catalytic activity of 2.54 × 105 g/(mol·Ni·h) compared to the complex with R2 = C6H13 and R3 = C6H11 using toluene as the solvent. Moreover, the selectivity for the C4 and C6 oligomers can reach up to 82%.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Yubing Hu,Yan Wang,Yulian Wang,Wei Li,Jinli Zhang,You Han
In order to develop a cut-price, high-efficiency non-mercuric catalyst for acetylene hydrochlorination reaction, several kinds of supported Cu-based catalysts containing phosphoramide ligands have been synthesized by wet impregnation method. The outstanding catalytic activity was obtained over 15 %Cu10 %HMPA/SAC catalyst with acetylene conversion of 87.25 % in the test conditions of T =180 °C, GHSV (C 2 H 2 ) =180 h −1 and V (HCl): V (C 2 H 2 ) = 1.2. The catalyst with optimal HMPA ligand also exhibited splendid stability in 100 h lifetime test. The analysis for XRD, TEM, TGA, ICP, H 2 -TPR and XPS indicated that HMPA ligand can improve Cu species dispersion, restrain coke deposition, suppress loss of loading Cu, and stabilize valence state of active Cu species. Due to electron transfer mechanism, steady coordination structure between Cu and HMPA led to favorable properties of Cu-based catalyst, which was further proved by FT-IR, Raman spectra, O 1s XPS spectra integrated with DFT calculations.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2013
·Vol. 130
·期 2
·1399-1405
·
IF 1.395
Jiajie Wu,Jiachun Feng
A novel hindered amine ligand, mono-2,2,6,6-tetramethyl-4-piperidyl-succinate (MTPS), has been designed to chelate europium(III) ion with 1,10-phenanthroline (Phen) as a coligand to prepare polymer photostabilizer. The luminescent property of the stabilizer and its efficiency of protecting polymer matrix from photodegradation have also been investigated. Under UV excitation, the stabilizer has red light emission in both ethanol solution and polypropylene (PP) matrix. The PP sheets containing the stabilizer display significantly improved photostability, which may be attributed to MTPS which scavenges radical, as well as Phen which makes the complex dissipate the absorbed ultraviolet light in a harmless manner. These preliminary results demonstrate that the introduction of the stabilizer can endow polymer matrices not only excellent photoluminescent properties but also improved photostability. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 1399-1405, 2013
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）