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Separation and Purification Technology
Elsevier Science B.V.
Separation and Purification Technology

Elsevier Science B.V.

1383-5866

Separation and Purification Technology/Journal Separation and Purification TechnologySCIEIISTP
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    Covalent organic polymers for aqueous and organic solvent nanofiltration

    Akbar Asadi TashvighNieck E. Benes
    8页
    查看更多>>摘要:Here we present the preparation of a novel positively charged covalent organic polymer (COP) based nanofiltration membrane. The porous COP selective layer grows on top of a polybenzimidazole (PBI) support from coupling reaction of 1,3,5-tris(bromomethyl)benzene and 4,4'-dipyridyl in alkaline conditions. Chemical and morphological analyses confirm the formation of a thin layer of COP (less than 50 nm), which is also evidenced by its high water permeance and salt retentions. Moreover, it is shown that COP membranes can form hydrogen bonds with HNO3, leading to a tighter membrane pore size that increases the NaCl retention from 46% to 75% without significantly losing its permeance. Further, the composite membranes demonstrated exceptional solvent and pH stabilities. The COP membranes showed a molecular weight cut off between 400 and 1000 g mol~(-1) together with pure solvent permeances of 0.91, 2.4, 3.3, 7.1 and 9.5 Lm~(-2)h~(-1)bar~(-1) toward dimethylformamide (DMF), ethanol, acetone, methanol an acetonitrile, respectively. The remarkable performance together with the stability in harsh environments make the newly developed COP membranes an attractive candidate for extreme nanofiltration.

    Efficient visible-light-driven photoreduction of U(VI) by carbon dots modified porous g-C3N4

    Zhongran DaiShang ZhaoJunjie Lian
    9页
    查看更多>>摘要:The efficient removal of uranium from radioactive wastewater is of great significance for the ecological environment safety and sustainable development of nuclear energy. Herein, the carbon dots modified porous graphitic carbon nitride (CNCD) was fabricated and used for photoreduction of U(VI) under visible LED light irradiation. The removal rate of U(VI) by CNCD-2 could reach more than 95 % over a wide range of U(VI) concentration. In addition, the CNCD-2 showed excellent selectivity and recyclability for photoreduction of U(VI). Further mechanism studies showed that the high photocatalysis activity of CNCD-2 was attributed to the effective separation of photoinduced electron-hole pairs, strong visible light absorption capacity and narrow bandgap. The U(VI) was activated by both photoinduced e" and ·O2~- in the process of photoreduction, and then immobilized by transforming it to metastudtite ((UO2)O2 · 2H2O). These results indicate that the CNCD is a promising material for remediation of uranium-containing wastewater under visible light irradiation.

    CO2 separation from biogas with ionic liquid-based hybrid solvents: From properties to process

    Nan WangChunyan MaNannan Ye
    10页
    查看更多>>摘要:In this work, ionic liquids (ILs)-based hybrid solvents, consisting of 1-butyl-3-methylimidazolium acetate (BMAC)-propylene carbonate (PC), were developed for CO2 separation from biogas. The impacts of IL mass fraction and temperature on the absorption capacity, viscosity, and density were studied. Feed gases, including pure CO2, pure CH4, and synthetic biogas, were tested, and the results were evaluated and compared. Thermodynamic modeling was used to represent the newly measured results together with literature data, and a systematic process simulation and evaluation were conducted. The measurements show an enhanced CO2 solubility with an increased BMAC mass fraction and decreased temperature. An increased viscosity was observed with increasing BMAC mass fraction and decreasing temperature. In addition, the type of feed gas holds a neglectable effect on CO2 and CH4 absorption capacities. To find an optimal mass fraction of BMAC-PC and quantify the performance, in the process simulation and evaluation, two types of regeneration blocks, i.e., air-blow regeneration and thermal regeneration, were involved. It shows that the process with thermal regeneration block requires less energy and lower capture cost than the process with the air-blow regeneration, which indicates a superior affinity to thermal regeneration when BMAC is presented in the solvent system. Also, the decrease in PC content firstly decreases and then increases the energy demand, and the minimum energy demand of 23.4 kW can be found with w_(IL) = 0.3, which reduces by 33.5% compared to pure PC. Similarly, the minimum capture cost of 68 $/ton-CO2 can be found with w_(IL) = 0.3, representing a 21% reduction from the case with pure PC. The further analysis concludes a major reduction in the utility cost by 48%.

    Deep removal of phosphorus and synchronous preparation of high-strength gypsum from phosphogypsum by crystal modification in NaCl-HCl solutions

    Qingjun GuanYing SuiWeijian Yu
    13页
    查看更多>>摘要:Phosphogypsum (PG) is a bulk solid waste that is generated during the production of wet-process phosphoric acid. Presently, the impurities (especially co-crystalline phosphorus impurities) and low value-added recycling products restrict the utilization of PG. In this study, the complete deconstruction of co-crystalline phosphorus encapsulated in gypsum lattices was realized through phase transformation from PG to α-hemihydrate gypsum (α-HH) in NaCl solutions, which was the key to efficiently eliminating phosphorus impurities from PG. Simultaneously, the addition of HCl into NaCl solutions could fully dissolve the phosphates released from gypsum lattices and distinctly increase the phosphorus leaching efficiency. Moreover, synergistic regulation of crystal morphology and particle size of α-HH was obtained in NaCl-HCl solutions by crystal seed induction, and regular large-grained α-HH with small specific surface areas was prepared, which weakened the phosphorus adsorption on the product surfaces and further improved the leaching efficiency. Importantly, the prepared α-HH were high-strength gypsum with high added value. Consequently, deep phosphorus removal (>99%) and synchronous preparation of high-strength gypsum (>30 MPa) with high added value from PG was achieved bv regulating the phase transition from PG to α-HH and controlling the α-HH morphology and size by crystal seed induction in mixed solutions of NaCl and HCl under mild conditions. This work provides instructive guidance for efficient impurity removal and high value-added utilization of industrial byproduct gypsum at low cost.

    Robust preparation of braid-reinforced hollow fiber membrane covered by PVDF nanofibers and PVDF/SiO2 micro/nanospheres for highly efficient emulsion separation

    Jingjing YanChangfa XiaoChun Wang
    12页
    查看更多>>摘要:The PVDF nanofibers and the PVDF/silica (SiO2) micro/nanospheres were deposited simultaneously on the outer surface of a rotating PVDF braided tube by electro spinning and electrospraying to fabricate a new type of enhanced hollow fiber membrane. By adjusting the content of SiO2 in electrospraying solution, the micro/nanospheres with different morphology were obtained to optimize the performance of the prepared membranes. When 2 wt% SiO2 was added, the deposited micro/nanospheres mainly took loose porous PVDF aggregates as the skeleton and SiO2 particles as the filler to construct the micro/nano structure on the membrane surface like that on the lotus leaf surface. Therefore, the membrane surface exhibited superoleophilicity (θo = 0°) and underoil superhydrophobicity (θ_(uow) = 154°). In addition, the deposited micro/nanospheres can effectively weakened the stacking between the deposited nanofibers. The resultant membrane not only had the high permeability with pure oil flux of 8557 L·m~(-2)·h~(-1), but also possessed the excellent oil-water separation performance with separation efficiency of 99.70%. Meanwhile, it also showed the outstanding tensile strength of 79.40 MPa. The preparation method was simple and easy to operate, which would provide more possibilities for the preparation of hollow fiber membranes with efficient separation performance to the water-in-oil emulsion.

    Boosting the CO2/N2 selectivity of MMMs by vesicle shaped ZIF-8 with high amino content

    Yan DaiRui DingZiheng Li
    9页
    查看更多>>摘要:The amino functionalization of MOFs has been verified to be effective in improving the selective permeation of CO2. However, the introduction of amino groups into ZIF-8 by mixed ligands strategy is hard to achieve due to the high steric hindrance of benzene ring in 2-aminobenzimidazole ligand, resulting in insufficient content of amino groups. Therefore, in this work, polystyrene-acrylate (PSA) template is proposed to provide abundant adsorption and reaction sites for the rapid synthesis of NH2-ZIF-8 with high content of 2-aminobenzimidazole. Furthermore, the incomplete etching strategy is used to construct PSA modified hollow NH2-ZIF-8 nanospheres (PHNZ). Importantly, the thickness of PSA layer and the hollow size are adjusted by the etching time, as revealed by the SEM and TEM images. In this PHNZ, the modified PSA can provide good interface compatibility between PHNZ and Pebax matrix to enhance the CO2 selectivity, while the hollow structure can reduce the mass transfer resistance and improve the gas permeability. Moreover, the introduced amino groups can enhance the CO2 affinity of PHNZ and further improve the CO2/N2 selectivity of the PHNZ-based mixed matrix membranes (MMMs). Benefiting from the synergy of good interface compatibility and enhanced CO2 affinity from the amino groups, the PHNZ/Pebax MMMs present greatly improved CO2/N2 selectivity in contrast with pure Pebax and NH2-ZIF-8 based membranes. Besides, as the etching time increases, the PHNZ-2 and PHNZ-3 based MMMs present a higher CO2 permeability than that of NH2-ZIF-8 based MMM, revealing the significance of the hollow structure. The PHNZ-2/Pebax MMM with filler loading of 10 wt% expresses the best gas separation performance with the CO2 permeability of 121.9 Barrer and CO2/N2 selectivity of 96.6, respectively, showing an increase of 54.7 % and 98.0 % in contrast with pure Pebax membrane. Meanwhile, this CO2 separation performance is far beyond the Robeson upper bound in 2008 and close to the McKeown upper bound in 2019, demonstrating that the proposed PHNZ displays a promising and competitive potential in MMM based CO2 capture.

    Vanadium trioxide mediated peroxymonosulfate for fast metronidazole oxidation: Stepwise oxidation of vanadium for donating electrons

    Jiao ShenFeng ChengYichi Chen
    11页
    查看更多>>摘要:In this study, vanadium trioxide (V2O3) was adopted to activate PMS via a Fenton-like reaction to degrade metronidazole (MNZ). The V2O3-PMS system can almost completely degrade MNZ at 30 min with 42.4% TOC removal. Comparative tests reveal that V2O3 stands out among a variety of heterogeneous catalysts, including metallic oxides and carbon materials. Sulfate radicals (SO4~(·-)) and hydroxyl radicals (·OH) derived from PMS decomposition are major reactive oxygen species, based on quenching tests, electron spin resonance (ESR) analysis, the steady-state concentrations of radicals ([SO4~(·-)]_(ss) = 5.1 × 10~~(-13) M and [·OH]_(ss) = 4.0 × 10~~(-14) M), and kinetics model. The process of stepwise electron transfer from vanadium species to PMS to produce reactive radicals was proved by small-molecule simulation experiments and pickling experiments of vanadium oxides. Possible pathways of MNZ degradation were proposed based on the results of LC-MS and Fukui function, including two stages of the hydroxylation and bond cleavage of nitro and the subsequent ring-opening. This study reveals the high reusability and practicability of the V2O3-PMS system over a relatively wide pH range, which puts forward a new vision on V2O3 induced Fenton-like reactions and a new reference method for the removal of medical organic contaminants in water.

    Fe~(3+)/Fe~(2+) cycle promoted peroxymonosulfate activation with addition of boron for sulfamethazine degradation: Efficiency and the role of boron

    Zihao LiZhuoyu BuMinhui Hou
    15页
    查看更多>>摘要:Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe~(2+) enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe~(2+)/PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe~(2+)/PMS (B/Fe~(2+)/PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that ·OH and SO~(4+)~ played important role and Fe(IV), ~1O2 and O2~(·-) also participated in SMT removal. The addition of boron could enhance the role of'OH and SO4~(·-) in SMT removal in Fe~(2+)/PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe~(2+). Possible SMT degradation pathway was proposed. B/Fe~(2+)/PMS process could efficiently remove SMT at low Fe~(2+) dosage and neutral pH. B/Fe~(2+)/PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe~(2+)/PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others' works also demonstrated the present study process was a promising strategy for antibiotics removal.

    Biomimetic Janus photothermal membrane for efficient interfacial solar evaporation and simultaneous water decontamination

    Yaxin ShangConglei XuBeibei Li
    10页
    查看更多>>摘要:Solar-driven water evaporation has been regarded as a promising technology to generate clean water due to the abundance and environmental friendliness of solar energy resources. However, the limited clean water production and limitation in tailored solar-driven system (SDS) have impeded its practical application. Herein, inspired by Lemna minor, a biomimetic, hierarchically structured, photothermal membrane (b-HPM) comprising Ti3C2Tx MXene and oxidized carbon nanotubes cross-linkage is designed. The hydrophilic bottom layer of b-HPM with macropores helps promote water transportation whilst the hydrophobic mesoporous upper layer accelerates solar/contaminant absorption and inhibits heat loss. Such-acquired Janus membrane not only improves the water transfer rate to reach 1.66 kg m~(-2)h~(-1) but also harvests excellent evaporation efficiency of 99.73% deriving from the direct solar light energy (92.58%) and ambient environment (7.15%) under one-sun illumination. Impressively, PPCP removal of > 99% in raw wastewater, and no pollutants were found in the distilled water. More encouragingly, b-HPM enables a high evaporation rate and contaminant removal efficiency in real waterbody with long-term utilization based upon experimental and theoretical calculation results. Our designed SDS synergizes the merits of facile preparation, high light utilization efficiency, high-rate clean water generation, stability and robust performance, holding great promise in solving freshwater shortage and remedying water pollution under natural sunlight.

    Ascorbic acid enhanced the zero-valent iron/peroxymonosulfate oxidation: Simultaneous chelating and reducing

    Peng XuLei WangXin Liu
    11页
    查看更多>>摘要:The activation of peroxymonosulfate (PMS) with zero-valent iron (Fe(0)) generates reactive oxygen species that can effectively degrade aromatic organic contaminants. However, the low conversion rate from Fe(III) to Fe(II) and the aggregation of iron sludge restrict its wide application. In this study, a wrater-soluble vitamin, ascorbic acid (H2A), was combined with the conventional Fe(0)/PMS system to enhance the degradation of benzoic acid (BA). The removal efficiency of BA in the H2A/Fe(0)/PMS system was improved by 59.4% compared with the conventional Fe(0)/PMS system under the optimal conditions of 0.03 g/L Fe(0), 0.4 mM PMS, 0.1 mM H2A and initial pH of 4.5. This result was mainly credited to the excellent reducing and chelating ability of H2A, which promoted the generation of reactive oxygen species by accelerating the reduction of Fe(III) and forming Fe(III)-ascorbate complexes. Alcohol quenching and electron spin resonance (ESR) experiments demonstrated that the main reactive oxygen species for the degradation of BA in the H2A/Fe(0)/PMS system were ·OH and SO4~(·-) Scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS) analyzed the surface chemistry and phase transformation of fresh and used Fe(0). Based on the above experimental analysis, the degradation mechanism of BA in the H2A/Fe/PMS system was systematically explored. Common water matrix including Cl~-, HCO3~-, NO3~- and humic acid inhibited the degradation of BA, while SO4~(2-) had negligible impacts. In addition, the degradation performance of the H2A/Fe(0)/PMS system in natural water environment and its degradation of various pollutants were also investigated. In summary, this study provides new insights for enhanced removal of refractory organics by improving the conventional Fe(0)/PMS system.