INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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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 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
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
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催化材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2020
·
IF 2.463
Xueyu Wang,Xiaoyang Hu,Lianjun Song,Xiuying Yang,Qian Xiao,Haowei Xu,Songdong Ding
The two DOTA-tetraamide ligands, DOTAM- n -butyl (1,4,7,10-tetrakis[( N - n -butyl; carbamoyl)methyl]-1,4,7,10-tetraazacyclododecane) and DOTAM-benzyl (1,4,7,10- tetrakis[( N -benzylcarbamoyl)methyl]-1,4,7,10-tetraazacyclododecane), were synthesized and characterized by MS, NMR and FTIR spectra. In acid solution, DOTAM- n -butyl was liable to be protonated. FTIR, 1 H NMR, ESI-MS spectra and X-ray diffraction analyses revealed that the nitrogen atoms of cyclen ring combined two protons to form a cation with two positive charges. The protonated DOTAM- n -butyl had strong extraction ability and good selectivity for ReO 4 − . It was extracted by means of the substitution of one ReO 4 − for one NO 3 − in the 1:2 complex of DOTAM- n -butyl with HNO 3 . The solvent extraction and X-ray crystallography demonstrated an anion-exchange extraction model. Meanwhile, X-ray crystal structure analyses of ligand complexes with HReO 4 or HNO 3 also indicated that ReO 4 − or NO 3 − ions were located in the gap between the upper and lower protonated ligands through multiple hydrogen bonds and electrostatic interactions.
研究领域:
化学
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放射化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2016
·Vol. 40
·期 8
·7027-7033
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IF 3.277
Jie Zhang,Shaofeng Liu,Antai Li,Hongqi Ye,Zhibo Li
N,N′-Bis(2,6-R-phenyl)-2,6-pyridinedicarboxamides (L: R = Cl, L1; R = F, L2; R = H, L3; R = Me, L4; R = Et, L5; R = iPr, L6) were designed as neutral ligands, and the corresponding nickel complexes LNiBr2 (Ni1–Ni6) were synthesized as precatalysts for ethylene oligomerization. All new ligands were fully characterized by NMR, and FT-IR spectroscopy, and elemental analysis, while the nickel complexes were examined using FT-IR spectroscopy and elemental analysis. The coordination mode of the ligand with nickel in complexes Ni5 and Ni6 was tridentate (O^N^O), as established by single crystal X-ray diffractions. All the nickel complexes Ni1–Ni6 were tested for ethylene oligomerization with different alkylaluminum compounds as cocatalysts, and diethylaluminum chloride (Et2AlCl) was proved to be the most effective. Upon activation with Et2AlCl, all nickel complexes showed high catalytic activity (up to 7.55 × 105 g mol−1 (Ni) h−1 atm−1) with good selectivity for α-C4.
研究领域:
化学
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材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Long Li,Xuanhao Huang,Xiaoyang Hu,Xingyue Liu,Rui Li,Hang Zhou,Fengfeng Li,Fangxiang Luo,Qingjiang Pan,Songdong Ding
Efficient and selective extraction of pertechnetate (TcO 4 − ) from nitric acid medium has become a significant challenge, especially in the presence of a large excess of interfering anions. By employing a combined strategy involving H-bonding and electrostatic interaction, a highly selective extraction of TcO 4 − can be achieved. The present work reports three homologous amine-diamide ligands with different alkyl chain lengths on the amine N atom of 2,2′-(metylimino)bis( N , N -dioctylacetamide) (MIDOA), 2,2′-(butylimino)bis( N , N -dioctylacetamide) (BIDOA) and 2,2′-(octylimino)bis( N , N -dioctylacetamide) (OIDOA), and their extraction behaviors for TcO 4 − /ReO 4 − in HNO 3 solution are also investigated by using n -dodecane as a diluent. It has been shown that all of them exhibit excellent extractability and high selectivity to TcO 4 − /ReO 4 − . Their extractability and phase disengagement follow the order of OIDOA > BIDOA > MIDOA, revealing a greater extractability and rapider phase disengagement for the amine-diamide ligand with longer chain substituents on the amine N atom. Both slope analysis and loading capacity test indicate the formation of 1:1 metal/ligand extracted complex, which is also confirmed by the analyses of single-crystal X-ray diffraction (SC-XRD), electrospray ionization mass (ESI-MS), Fourier transform infrared (FT-IR), and X-ray photoelectron spectroscopy (XPS). The extraction of TcO 4 − /ReO 4 − by the amine-diamide ligand follows the anion exchange extraction model and is a spontaneous and endothermic process. Furthermore, a competing extraction test was also conducted and demonstrates excellent extractability and high selectivity to TcO 4 − /ReO 4 − .
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
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zeqian Zhang,Hongshan Wu,Qiming Chen,Xiaowei Li,Yimin Cai,Lihua Yuan,Wen Feng
Efficient and selective palladium (Pd) recovery from high-level liquid waste (HLLW) constitutes a crucial task for both precious resource recovery and environmental remediation, but remains challenging to achieve high efficiency, sufficient selectivity, and fast kinetics. Herein, we report a new pyrazinamide ligand (denoted as PA) as the first example of employing pyrazine-based ligand for Pd 2 + separation with impressive efficiency. Using an ionic liquid C 8 mimNTf 2 as diluent, the developed pyrazinamide-ionic liquid (PA-IL) extraction system exhibited attractive merits for Pd 2+ separation such as a wide range of workable acidities from 0.2 M to 5 M HNO 3 , ultra-fast extraction kinetics with equilibrium time of 3 min, and good Pd 2+ selectivity over 16 ions coexisting in simulated HLLW and other non-metallic anions. Slope analysis indicated that the extraction mechanism involves the cation exchange of C 8 mim + and the coextraction of NO 3 - anions in the course of Pd 2+ extraction. Results from a set of spectroscopic investigations and single crystal X-ray diffraction analysis suggest the formation of complexes with stoichiometry of both 1:1 and 2:1 (PA/Pd 2+ ) in solution and in solid state, of which the formation of 2:1 complex is the most thermodynamically favored according to DFT theoretical calculations. This work provides a highly promising pyrazinamide-based extraction system for efficient and selective Pd 2+ separation from HLLW, and brings more understanding about the complexation and coordination behaviors between N-based ligands and Pd 2+ ions.
研究领域:
化学工程
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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
Journal of Inorganic and Organometallic Polymers and Materials
·
2016
·Vol. 27
·期 1
·176-185
·
IF 1.308
Sun Junjun,Lin Hongyan,Chang Zhihan,Wang Xiuli,Liu Guocheng
Four new inorganic–organic hybrid supramolecular architectures constructed from octamolybdates (Mo 8 O 26 ) and different bis-pyridyl-bis-amide ligands, (3-dpye = N,N ′-bis(3-pyridinecarboxamide)-1,2-ethane, 4-dpye = N,N ′-bis(4-pyridinecarboxamide)-1,2-ethane, 3-dpyp = N,N ′-bis(3-pyridinecarboxamide)-1,3-propane, 4-dpyp = N,N ′-bis(4-pyridinecarboxamide)-1,3-propane): (3-H 2 dpye)(γ-Mo 8 O 26 ) 0.5 ( 1 ) and (4-H 2 dpye)[(4-dpye)(γ-Mo 8 O 26 )] 0.5 ·2H 2 O ( 2 ) and [(3-H 2 dpyp) 2 (β-Mo 8 O 26 )]·2H 2 O ( 3 ) [(4-H 2 dpyp) 2 (β-Mo 8 O 26 )]·2H 2 O ( 4 ), have been hydrothermally prepared and structurally characterized by single crystal X-ray diffraction analyses. Compound 1 exhibits a 3D 6-connected supramolecular framework assembled from 1D γ-Mo 8 O 26 inorganic chains and 3-H 2 dpye molecules. Compound 2 consists of an uncommon 1D γ-Mo 8 O 26 –4-dpye inorganic–organic hybrid chain connected by Mo–N bond, which are extended by 4-H 2 dpye molecules to a 3D 3,8-connected supramolecular framework. Compounds 3 and 4 show 3D 6,6-connected supramolecular framework and 2D 3,6-connected supramolecular layer based on β-Mo 8 O 26 anions and 3/4-H 2 dpyp molecules via hydrogen bonds, respectively. The different bis-pyridyl-bis-amide ligands, isomers of octamolybdates and hydrogen bonding interactions in the title compounds show great effects on the final supramolecular networks. The electrochemical, electrocatalytic and photocatalytic activities of compounds 1–4 have been investigated.
研究领域:
无机化学
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材料科学
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DOI
高影响因子
CRYSTENGCOMM
·
2013
·Vol. 15
·期 36
·7274-7284
·
IF 3.879
Xiu-Li Wang,Fang-Fang Sui,Hong-Yan Lin,Chuang Xu,Guo-Cheng Liu,Ju-Wen Zhang,Ai-Xiang Tian
Six new transition metal coordination polymers, namely, [Co(1,2-BDC)(L)1.5(H2O)] (1), [Co(1,3-BDC)(L)(H2O)2]·H2O (2) [Co(5-AIP)(L)0.5(H2O)]·2H2O (3), [Cu(1,2-BDC)(L)] (4), [Cu(1,3-BDC)(L)(H2O)]·3H2O (5), and [Cu2(5-AIP)2(L)2(H2O)]·6H2O (6) (L = N,N′-di(3-pyridyl)octanediamide, 1,2-H2BDC = 1,2-benzenedicarboxylic acid, 1,3-H2BDC = 1,3-benzenedicarboxylic acid, 5-H2AIP = 5-aminoisophthalic acid), have been hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction. In compound 1, the adjacent CoII ions are connected by L ligands to form a 1D chain with an alternating arrangement of L ligands and Co2L2 dinuclear loops. The 1,2-BDC anions coordinate with one CoII ion in a bis(monodentate) chelate mode. Complex 2 shows a 2D (44) grid network with the sql topology, which consists of the 1D zigzag [Co–L]n chain and 1D linear [Co-1,3-BDC]n chain. When 5-H2AIP is used in compound 3, an interesting 2D terraced-type layer based on 1D [Co-5-AIP]2n ladder-like chains and μ2-bridging L ligands with 3,4-connected {62.10}{6} topology is formed. Under the similar conditions to compound 1, except that the cobalt(II) salt is replaced by a copper(II) salt, a 2D wave-like network 4 with 2,4-connected {64.8.10}{6} topology is obtained. Compound 5 displays a 3D coordination polymeric architecture based on 1D [Cu-1,3-BDC]n chains and [Cu–L]n chains, which represents an intriguing 3-fold interpenetrating framework with CdSO4-type topology. When 1,3-BDC is replaced by 5-AIP, another 3-fold interpenetrating 3D CdSO4-type coordination framework for compound 6 is obtained, which is constructed from three types of 1D chains: [La–Cu–Lc]n chain, [Lb–Cu–Lb]n chain and [Cu-5-AIP]n chain. The adjacent 1D chains for 1 and 2D layers for compounds 2, 3 and 4 are further extended by hydrogen bonding interactions to 3D supramolecular frameworks. The effect of dicarboxylates and central metals on the structures of the title complexes has been discussed. Furthermore, the electrochemical behaviors and solid state fluorescent properties for compounds 1–6 are investigated.
研究领域:
化学
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材料科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Sun Zuowei,Fang Hu,Mei Mingjie,Fu Haiyan,Xue Weichao,Xu Jiaqi,Li Ruixiang,Chen Hua,Zheng Xueli
An innovative bitopic phosphoramidite ligand L was proficiently synthesized and subsequently employed in coordination with two distinct metal species (Ag I and Rh I ), leading to the construction of a heterometallic coordination polymer. The catalyst showcased remarkable performance in the hydroformylation of long-chain alkenes, displaying high activity and selectivity with a minimum yield of 90% for aldehydes. Operating as a heterogeneous catalyst, it not only demonstrated outstanding efficacy in facile separation from the product but also maintained a low rhodium loss per catalytic cycle. The catalyst exhibited exceptional stability, remaining high activity and selectivity over 10 successive reuses. Moreover, the RhAgL catalysts exhibit notable isomerization effects on alkenes, which promote the preferential formation of branched aldehydes in the resulting product. The straightforward synthetic strategy employed in preparing this highly effective catalyst introduced an innovative concept for heterogeneous catalysis, offering promising prospects for advancing industrial processes. This remarkable performance indicates the catalyst's potential for sustainable and efficient chemical transformations, highlighting its significance in driving advancements in catalytic technology for a variety of applications in industry. Graphical Abstract
研究领域:
化学
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催化材料
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工业化学
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DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2025
·
IF 1.6
Ren Peng,Yang Yang,Liu Dai,Guan Cheng-peng,Huang Pin-wen,Qi Ming
A novel extraction process utilizing THEE-BisDGA ligand has been developed for the rapid and efficient recovery of trivalent lanthanide elements (La, Nd, Eu, and Dy) from uranium-containing acidic systems. The process rapidly achieves equilibrium within just 2 min and exhibits high distribution ratios. Notably, its extraction efficiency shows a positive correlation with the atomic number of the lanthanides. Significantly, the ligand demonstrates exceptional selectivity by excluding U(VI) extraction, thus enabling the targeted recovery of lanthanides. Back-extraction experiments confirm that 0.01 M HNO 3 can quantitatively strip lanthanides in three steps, highlighting its potential for industrial-scale separation and purification of valuable lanthanides. Moreover, density functional theory(DFT) calculations have confirmed that THEE-BisDGA exhibits superior selectivity for Ln(III) over U(VI), further reinforcing its effectiveness and applicability in advanced separation technologies.
研究领域:
化学工程
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无机化学
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分离科学
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材料科学
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核化学
✓ 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）