Science Advances
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2024
·Vol. 10
·期 19
·
IF 11.7
Tingting Xu,Bin Wu,Wenmin Li,Yifan Li,Yanran Zhu,Fangmeng Sheng,Qiuhua Li,Liang Ge,Xingya Li,Huanting Wang,Tongwen Xu
Fast transport of monovalent ions is imperative in selective monovalent ion separation based on membranes. Here, we report the in situ growth of crown ether@UiO-66 membranes at a mild condition, where dibenzo-18-crown-6 (DB18C6) or dibenzo-15-crown-5 is perfectly confined in the UiO-66 cavity. Crown ether@UiO-66 membranes exhibit enhanced monovalent ion transport rates and mono-/divalent ion selectivity, due to the combination of size sieving and interaction screening effects toward the complete monovalent ion dehydration. Specifically, the DB18C6@UiO-66 membrane shows a permeation rate (e.g., K+) of 1.2 mol per square meter per hour and a mono-/divalent ion selectivity (e.g., K+/Mg2+) of 57. Theoretical calculations and simulations illustrate that, presumably, ions are completely dehydrated while transporting through the DB18C6@UiO-66 cavity with a lower energy barrier than that of the UiO-66 cavity. This work provides a strategy to develop efficient ion separation membranes via integrating size sieving and interaction screening and to illuminate the effect of ion dehydration on fast ion transport.
研究领域:
材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Shiyu Hou,Yiliang Tang,Tianle Zhu,Zheng-Hong Huang,Yingshu Liu,Ye Sun,Xiang Li,Fangxia Shen
In order to ensure regeneration property of adsorption materials in the air pollution purification system of the airtight cabin, such as submarine and space station, it is necessary to selectively separate semi-volatile organic compounds whose desorption is difficult. For this reason, the effects of pore size on the adsorption capacity and adsorption selectivity of toluene and naphthalene were investigated by both molecular simulation and experimental investigation. The ordered porous silica-based adsorbents with pore sizes ranging from 1.0 nm to 2.8 nm were constructed by simulation and were prepared by template synthesis method in this study. Both simulation and experiment show that the adsorption capacity of toluene and naphthalene firstly increased and then decreased with the increase of the pore size of adsorbents from 1.0 nm to 2.8 nm, and the pore diameter (1.3 nm) corresponding to the maximum adsorption amount of toluene was smaller than that (2.3 nm) of naphthalene. Simulation results show that the adsorption energy and adsorption stability of naphthalene are higher than those of toluene, and binary-component co-adsorption experiments also testified that toluene molecules could be replaced by naphthalene molecules. The optimum pore size for selective adsorption of naphthalene is 2.3 nm.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2016
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IF 3.299
Xinrui Zhang,Liyong Yuan,Zhifang Chai,Weiqun Shi
A novel tetradentate ligand combining hard O-donor and soft N-donors in the same molecule, N,N′-diethyl-N,N′-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen), was developed in our laboratory aiming at the group separation of actinides from lanthanides. Herein, the solvent extraction of UO 2 2+ by Et-Tol-DAPhen in 1-(trifluoromethyl)-3-nitrobenzene diluent was investigated in detail. The effects of contact time, Et-Tol-DAPhen concentration, acidity, and competing ions on the extraction were discussed, the extracted UO 2 2+ speciation was analysed, and the stripping of UO 2 2+ from organic phase was performed. The results clearly show that Et-Tol-DAPhen/1-(trifluoromethyl)-3-nitrobenzene provides a highly efficient extraction of UO 2 2+ from HNO 3 media with a fast extraction kinetics of less than 5 min and a large distribution ratio of more than 300. Moreover, the system shows excellent selectivity toward UO 2 2+ over Ln 3+ in a wide acidity range. Stripping experiments indicate that almost a complete back extraction of UO 2 2+ could be achieved via only one stage operation using 5% Na 2 CO 3 solution. Findings of the present work provide new data for assessing the feasibility of Et-Tol-DAPhen, as well as other new ligand with hard–soft donors combined in the same molecule, applied in the group separation of actinides over lanthanides.
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
SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Zhangxiang Lin,Pei Yuan,Yuanyuan Yue,Zhengshuai Bai,Haibo Zhu,Tinghai Wang,Xiaojun Bao
Selective separation and recovery of Co(II)/Mn(II) from purified terephthalic acid (PTA) production wastewater is very important to reduce the Co(II)/Mn(II) catalysts consumption and control the pollutant discharge. This work employed zeolites NaA, NaX, and HZSM-5 with different pore sizes and Na(I) contents to selectively separate and recover Co(II)/Mn(II) from PTA wastewater and to understand the adsorption mechanism. It is found that only NaA can exclusively adsorb Co(II)/Mn(II) through ion-exchange without adsorbing any aromatic organic compound (AOC); oppositely, HZSM-5 shows the highest adsorption capacity for AOCs but almost no adsorption for Co(II)/Mn(II); and NaX exhibits moderate adsorption capacities for both Co(II)/Mn(II) and AOCs. Moreover, pH can significantly impact the adsorption of both Co(II)/Mn(II) and AOCs due to the competitive adsorption between H(I) and Co(II)/Mn(II) and the electrostatic repulsion between AOCs and zeolites. The adsorption kinetics, isotherms, and thermodynamics were also investigated to lay a good basis for process development. Importantly, bench-scale experiments for simulating the industrial operation were carried out, and the results show that the adsorption capacity of the NaA particles for Co(II)/Mn(II) from the industrial PTA wastewater is 9.1/8.6 mg/g, respectively, without adsorbing any AOC. Therefore, an efficient strategy to selectively separate and recover Co(II)/Mn(II) from PTA wastewater was successfully developed.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2023
·Vol. 140
·期 40
·1-18
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IF 3
Wan Xu,Shengyuan Zhao,Huijuan Zhang,Fangfang Niu,Xingsheng Liu,Zhenbin Chen,Yuan Sun
With the continuous depletion of global rhenium resources, the separation and purification of rhenium (Re) from secondary resources became very important. Herein, an imprinted composite membrane with “flexible chain” thermo-responsive imprinted separation layer structure (Re-TIICM) was prepared to achieve selective separation and recovery of Re from secondary resources with complex composition. Re-TIICM's thermo-responsive imprinted separation layer occurred sol/gel phase transition by adjusting the temperature, which effectively mitigated the trade-off between selectivity and desorption. The structure and performance of Re-TIICM under optimum process conditions were tested and evaluated. The results showed that Re-TIICM exhibited a maximum adsorption capacity of 0.1036 mmol/g at 35°C, a separation degree of 4.37 (MnO 4 − as disturbing ions), and remained good adsorption capacity and selectivity after 9 adsorption/desorption cycles. When Re-TIICM was applied in secondary resources, the purity of Re increased from 35.412% to 70.208% after one adsorption/desorption cycle, showing a great potential for industrial applications.
研究领域:
材料科学
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环境工程
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冶金工程
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 51
·110417-110430
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IF 5.8
Du Xuan,Rashid Suraya Abdul,Abdullah Luqman Chuah,Rahman Norizah Abdul
Separation materials have received increasing attention given their broad applications in the management of environmental pollution. It is desired to balance the contradiction between high separation efficiency and selectivity of separation materials. The integration of ball-milled bone chars with electrospun membranes might achieve this balance. In this study, electrospun cellulose/chitosan/ball-milled bone char (CL/CS/MB) membranes were by well-dispersing ball-milled bone chars with nanoscale size (98.9–167.5 nm) and developed porosity (40.2–373.1 m 2 /g) in the electrospinning solvent. The synergistic integration of distributed MBs (5.4–31.5 wt.% of loading hydroxyapatite on the membrane matrix) allowed the efficient sorption of Pb(II) with fast kinetics (20.0 min), excellent capacity (219.9 mg/g at pH 5.0, T 298 K), and favorable selectivity coefficients (2.76–6.79). The formation of minerals was dominant for the selective sorption of Pb(II) by combining the spectral analysis and quantitative determination. The surface complexation with O-/reductive N-species, the cation exchange with inorganic Ca 2+ , the electrostatic attraction with deprotonated O − , and the cation-π coordination with the aromatic carbon via the π-electrons should be not ignored for the capture of Pb(II). This work demonstrated the feasibility of electrospun CL/CS/MB membranes as a promising candidate for the remediation of aquatic pollutants.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Kaicheng Zhang,Rongxin Lin,Ming Yan,Yilin Wu
Membrane-based technology with accurate-recognition and specific-transmission has been regarded as one of the most promising strategies in environmental protection and energy conservation. However, membrane technique still faces challenges of “trade-off effect” between high selectivity and permeation flux within organic-aqueous mixed matrix. Here, well-intergrown click-chemistry synergic MXene-functionalized flexible skeleton membranes has been prepared in this strategy, enabling size-exclusion&structure selectivity by uniform location array imprinting unit and transport performance towards specific medicinal molecules of artemisinin (Ars). The well-assembled ultrathin cascade-type MXene layer guarantees the narrow interlayer nanochannels and the flexible skeleton modified mesoporous SiO 2 nanoparticles provide active reaction platform for the construction of selective recognition space. The resulting membranes demonstrated outstanding selective separation performance with permeability factor that artesunate (Aru) /Ars and dihydro-artemisinin ( d -Ars) / Ars of 3.17 and 2.89 and permeation flux of 1173.25 L·m −2 ·h −1 ·bar −1 . Besides, combined with antibacterial durability, recycling performance, high separation performance in mobile phase stability of CMFMs, it is anticipated that this work hopefully opens a new avenue for efficient chiral separation to medicinal molecules, exhibiting broad potential for practical application.
研究领域:
环境科学
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材料科学
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药物化学
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DOI
PubMed
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
Separations
·
2025
·Vol. 12
·期 2
·24
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IF 2.7
Lilei Yang,Zhongwei Ding,Zhengtao Zhu,Weidong Zhang
Selective separation of hydroxylamine (HA) from metal ions to prepare high-purity HA remains a challenge. In this study, given that HA can react with carbonyl compounds, TTA (thenoyltrifluoroacetone) was screened as a carrier to prepare the polymer inclusion membrane (PIM), which was used to separate HA from metal and inorganic acid ions. The experimental results demonstrated that the PIM exhibited good selectivity for HA. During the PIM process, the proton gradient served as a driving force to transport NH2OH(I). The electrodialysis (ED) process was used to efficiently and continuously provide proton gradient without introducing other ions, which coupled with PIM to separate HA. Under the optimum conditions, the separation factors of NH2OH(I)/Na(I) and NH2OH(I)/K(I) were 30.81 and 35.11; the purity of HA was 99.4%, indicating that the PIM-ED process can be used for high-purity preparation of HA.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jiateng Shi,Junfeng Wang,Tao Dong,Jie Yan,Danfeng Jiang,Zengxi Li,Haitao Zhang
The ionic liquid tetrakis(decyl)ammonium dicyanamide ([TKN][Dca]) was investigated for the selective extraction of Co(II) from a simulated spent battery leachate, achieving efficient separation of Co(II) from Ni(II) and Li(I). [TKN][Dca] demonstrate a high Co(II) extraction efficiency in a 4 mol/L NaCl solution, without requiring pH adjustment. The separation factor ( β Co/Ni ) for [TKN][Dca] was determined to be 47433. Density functional theory (DFT) calculations and ESI-MS spectra revealed that the predominant anionic species involved in Co(II) extraction were [Co(Dca) 3-x Cl x ] − , with [Co(Dca)Cl 2 ] − and [Co(Dca) 2 Cl] − as the primary complexes. The strong coordination between the dicyanamide anion (Dca − ) and Co(II) enabled selective separation of Co(II) from the leachate. Co(II) was efficiently stripped from the loaded organic phase using Na 2 SO 4 , with the extraction efficiency after stripping comparable to that of fresh [TKN][Dca]. Furthermore, [TKN][Dca] exhibits excellent stability and maintained consistent performance over multiple extraction-stripping cycles, highlighting its potential for sustainable applications in metal separation fields.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Min Zheng,Mingzhen Shi,Xingbang Hu,Zhuoheng Tu,Youting Wu
Efficient separation and recovery of hydrogen chloride (HCl) from HCl tail gas containing impurities such as sulfur dioxide (SO 2 ) is very important from the viewpoint of economy and environment. However, due to the similar dissolution ability of SO 2 and HCl , most solvents, including organic solvents, ionic liquids and deep eutectic solvents (DESs), show low SO 2 /HCl selectivity near 1.0 and are thus incompetent to separate SO 2 /HCl. To address this, we firstly reported the task-specific design of a novel class of protic metal-based DESs (PM-DESs) containing hydrochloride, metal chloride and sulfolane, which have good SO 2 affinity but much inhibited HCl uptake, for the separation of HCl/SO 2 . The solubility data of SO 2 and HCl in PM-DESs were determined and correlated by Krichevsky-Пiinskaya (K-I) equation. Among these PM-DESs, N,N -dimethylaniline hydrochloride (DMA·HCl) + zinc chloride (ZnCl 2 ) + sulfolane exhibits satisfactory recyclability and selectivity up to 2.669 (100 kPa, 313.2 K), which is the highest value reported so far. Absorption of HCl/SO 2 (50/50) mixed gas was also tested, with a high SO 2 /HCl selectivity of 3.250 obtained. In addition, the NMR and FTIR spectroscopic characterizations paired with quantum chemistry calculation were utilized to investigate the absorption mechanism from the perspective of atomic level. The DESs developed in the present work have the potential to separate and recycle HCl from SO 2 owing to their good selectivity and desirable reversibility, and the strategy proposed in this work may offer new guidance for designing green media for HCl recovery.
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 Environmental Chemical Engineering
·
2025
·
IF 7.2
Qingrui Zeng,Ziang Jia,Xu Liu,Yiwen Fan,Yubo Pang,Jinping Cheng
The capture of CO 2 from ambient air (400 ppm) has become a critical issue in combating climate change. In this study, a novel recombinant 13X zeolite (RS13X) with an Faujasite (FAU) structure was synthesized by transforming discarded Linde type A (LTA)-structured 4 A molecular sieves through alkali fusion. This material was subsequently modified with hydrazine (HZ) vapor to produce HZ-RS13X, which significantly enhances the pore structure of RS13X, leading to excellent CO 2 adsorption performance across a range of concentrations. Specifically, HZ-RS13X demonstrates excellent adsorption capacities of 2.16 mmol/g at 400 ppm, 6.14 mmol/g at 10,000 ppm, and 7.89 mmol/g at 100,000 ppm, highlighting its efficacy for industrial CO 2 emissions. Additionally, HZ-RS13X excels in the selective separation of CO 2 from CH 4 and N 2 , exhibiting high ideal adsorbed solution theory (IAST) selectivity values of 335 for a CO 2 /N 2 mixture (10/80) and 260 for a CO 2 /CH 4 mixture (50/50). Characterization results, along with grand canonical Monte Carlo (GCMC) simulations, reveal that HZ vapor modification enhances CO 2 adsorption modes of RS13X beyond those achieved through conventional carbamate generation methods. HZ-RS13X offers substantial CO 2 capture potential across a wide range of concentrations, from atmospheric levels to industrial emissions, presenting a promising strategy for solid-state CO 2 capture.
研究领域:
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
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