Huizhou Liu

Chinese Academy of Sciences, Peping, Beijing, China

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Publications (193)333.99 Total impact

  • [Show abstract] [Hide abstract]
    ABSTRACT: A novel adsorbent, polyethylenimine-functionalized poly(vinyl alcohol) (PVA-PEI) magnetic microspheres, was prepared by a process involving: (1) synthesis of magnetic poly(vinyl acetate) microspheres (PVAc) using modified suspension polymerization, (2) preparation of PVA magnetic microspheres by methanolysis of PVAc and (3) two-step reaction with epichlorohydrin and polyethylenimine to yield amino groups. Magnetic measurement illustrated that the PVA-PEI microspheres were superparamagnetic, with a high saturated magnetization of 36.7 emu/g. Once generated, the PVA-PEI microspheres were used as adsorbent to remove Cr(VI) from an aqueous solution. The results demonstrated that the optimized pH value was observed at 2.0. The adsorption rate was extremely fast and the equilibrium was reached within 8 min. The adsorption isotherms of the adsorbent were preferably fitted to the Langmuir model, with the maximum adsorption capacity of 88.4 mg/g at 25 °C. Thermodynamic parameters indicated the spontaneous and exothermic nature of adsorption. In addition, the Cr(VI) ions were successfully eluted by a 0.1 mol/L NaOH solution, with the desorption efficiency of over 99%, and the adsorbent exhibited a good reusability. These results implied that the PVA-PEI microspheres should be considered as a potential adsorbent to remove Cr(VI) from wastewater.
    Chemical Engineering Journal. 01/2015; 262:101–108.
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    ABSTRACT: Hydrothermal carbon spherules (HCSs) can be loaded with a variety of metal nanoparticles for various applications. In this work, three types of HCSs were prepared from saccharides (mono-, di- and poly-saccharides) by a modified hydrothermal method taking glucose, sucrose and starch as sources, respectively. The deposition of Au nanoparticles onto them can be realized through a regular adsorption process. For comparison, HCSs made from mono-saccharides glucose (HCSs-M) has a higher adsorption capacity for Au(III) from aqueous acidic chloride media. The adsorption behaviors for AuCl4- by HCSs-M were investigated systematically. It shows a high selectivity for Au(III) towards Pd(II), Pt(VI), Rh(III) and some relevant base metals Fe(III), Co(II), Cu(II) and Ni(II). An extra reductant glycine can not only significantly improve the adsorption capacities and selectivity, but also accelerate the adsorption rate. Langmuir isotherm model and the 2nd-order kinetics model can properly describe the adsorption behaviors of AuCl4-. The adsorption mechanism of Au(III) by HCSs was confirmed by XPS, XRD, TG, FTIR, SEM and TEM techniques. It demonstrates that AuCl4- has been reduced to Au0 deposited onto HCSs. On the basis of this, a reduction-deposition coupled mechanism was proposed. The current research illustrates a prospect for HCSs to be used as effective adsorbents for selective adsorption separation of Au(III) from chloride media. It also demonstrates a possibility to integrate the selective recovery of gold from a complex industrial waste stream and the fabrication of functional carbon materials through loading with gold nanoparticles.
    J. Mater. Chem. A. 11/2014;
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    ABSTRACT: A novel Heck reaction catalyst consisting of a palladium(II) complex of meso-tetra(p-hydroxyphenyl)porphyrin (MTP) and cross-linked chloromethylated polystyrene microspheres (PMs) was successfully prepared via covalent ether bonds between the chloride groups in the PMs and the hydroxyl groups in MTP. The catalyst was characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and inductively coupled plasma atomic emission spectroscopy (ICP-AES). This polystyrene-supported palladium-complex was an efficient heterogeneous catalyst for cross-coupling of aryl iodides with ethyl acrylate. The reaction of iodobenzene and ethyl acrylate under N2 at 100 °C and a catalyst concentration of 0.1% gave a gas chromatography product yield of 99.8%, which is much higher than that achieved using a free palladium(II) complex of MTP as the catalyst (41.3%). The catalyst was recycled up to six times without significant loss of catalytic activity. These results suggest that the immobilized palladium(II)–MTP catalyst has potential applications in synthetic and industrial chemistry.
    Particuology. 11/2014;
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    ABSTRACT: Many papers have reported that salt ions can exert a great influence on the self-assembly behavior of PEO-PPO copolymers in the aqueous solution. Whereas the mechanism through which salt ions influence the self-assembly behavior of PEO-PPO copolymers is unclear and the dispute is mainly focused on whether the salt ions have a direct interaction with PEO-PPO copolymers. In this paper, the interaction of sodium and potassium ions with PEO-PPO copolymer was investigated by using FTIR, Raman and 23Na NMR spectroscopy. Experimental results reveal that direct interactions between salt cations and PEO-PPO macromolecular chains indeed occur in appropriate conditions. The present work highlights the role of cations in the self-assembly process of PEO-PPO copolymer.
    Vibrational Spectroscopy 10/2014; · 1.75 Impact Factor
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    ABSTRACT: Monodisperse orthorhombic-phase rare earth fluorides nano-/microcrystals with a special shape of disk-stacked cylinder have been synthesized via a facile phase transfer assisted solvo-thermal route, where an acid-base-coupled extractant has been employed to transfer hydrofluoric acid into an oil phase as a fluoride source. The synthetic parameters have been optimized and a possible formation mechanism has also been proposed. More importantly, the adopted acid-base-coupled extractant in this route can be recycled. Surveying all of the lanthanides from La to Lu, most of the heavy rare earths, such as Tb, Dy, Ho, Er, Tm and Yb, can form LnF3 nanocrystals with the similar morphologies. Furthermore, Ln(3+)-doped YF3 (Ln=Tb, Yb/Er) nanocrystals have also been synthesized, and their down-conversion and up-conversion (980nm) luminescent properties were examined. The current approach could be extended to synthesize other metal fluorides nanoparticles.
    Journal of Colloid and Interface Science 09/2014; 436:171–178. · 3.55 Impact Factor
  • Colloids and Surfaces A Physicochemical and Engineering Aspects 09/2014; 457:160–168. · 2.11 Impact Factor
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    ABSTRACT: We explore whether it is possible to use 2D correlation spectrum to characterize intermolecular interactions between two solutes dissolved in the same solution when one substance does not possesses any characteristic peak. We demonstrate that the interaction can be manifested by characteristic cross peaks in 2D asynchronous correlated spectrum. The above cross peaks reflect the subtle spectral variations on the characteristic peak of another solute under intermolecular interaction. On the other hand, 2D synchronous spectrum is not suitable to characterize intermolecular interaction since the cross peaks contain irremovable interfering parts. The terbium-chloride/benzamide/methanol system is used to demonstrate that this approach is applicable in the real chemical system.
    Journal of Molecular Structure 07/2014; 1069:127–132. · 1.40 Impact Factor
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    ABSTRACT: BACKGROUND Adsorption is believed to be an effective and green technology for the removal and recovery of rare earths (III) from dilute solution.RESULTSA novel hybrid gel, abbreviated as ALG-PGA, has been prepared through crosslinking calcium alginate (ALG) and γ-poly glutamic acid (PGA), and its adsorption behavior towards whole rare earths (III) has been examined. Taking Nd(III) as a representative element, the adsorption capacity, kinetics, reusability, selectivity and mechanism have been investigated. Cation exchange is proposed as a possible adsorption mechanism. Doping PGA molecules into calcium alginate beads can significantly enhance the adsorption capacity and the selectivity of rare earths from non-rare earths. The maximum adsorption capacity obtained for Nd(III) was 1.65 mmol g−1. Reutilization of ALG-PGA gel was confirmed for up to eight consecutive sorption–desorption cycles with no damage to the gel.CONCLUSION The prepared biosorbent, ALG-PGA, was biocompatible and cost effective with a good adsorption ability for Nd(III), and provides a new approach to the recovery of rare earths (III) from rare earths-containing wastewater. © 2013 Society of Chemical Industry
    Journal of Chemical Technology & Biotechnology 07/2014; 89(7). · 2.50 Impact Factor
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    ABSTRACT: Gas-assisted three-liquid-phase extraction (GATE), which has the advantages of both three-liquid-phase extraction and solvent sublation, is a novel separation technique for separation and concentration of two organic compounds into different phases in one step. This highly effective and economically applicable method has been developed for separating emodin and rhein from herbal extract. In a GATE system composed of butyl acetate/PEG4000/ammonium sulphate aqueous solution, influence of various parameters including gas flow rate, flotation time, salt concentration, initial volume of PEG and butyl acetate were investigated. Within 50 min of 30 ml · min− 1 nitrogen flow, removal ratio of emodin and rhein from aqueous phase could be over 99% and 97%, respectively. Mass fraction of emodin in the BA phase and rhein in the PEG phase could reach 97% and 95%, respectively. It is demonstrated that gas bubbling is effective for partitioning of emodin and rhein into butyl acetate and PEG phase respectively, and dispersed PEG and butyl acetate could be captured in the aqueous solution. Experimental results show that GATE could be an effective and economical technology for concentration and separation of co-existed products in medicinal plants. Graphic abstract The figure is schematic diagram of gas-assisted three-liquid-phase extraction system. The flotation column is made of glass, is equipped with a G4 sintered glass sparger (pore size 3-4 μm). The inner diameter of the column is 36 mm and the length is 450 mm. There are three coexisting phases in the column, i.e. organic phase, polymer phase and aqueous phase (containing ammonium sulphate solution and simulated herbal exact). Three ports are open at different parts along the column to obtain samples of the three phases. In the process of gas bubbling, emodin and rhein initially contained in the aqueous phase are extracted into organic phase and polymer phase, respectively.
    Chinese Journal of Chemical Engineering 06/2014; · 0.92 Impact Factor
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    ABSTRACT: SignificanceBubbles can be used to greatly improve the speed of magnetic separation and overcome the limitation of magnetic force on the capture distance, making low-field magnetic separation highly efficient and easily scalable. This novel method leads to the development of a medium-free continuous gas-assisted magnetic separator on small pilot scale using low-field permanent magnet. This separator is demonstrated highly efficient for recovery of proteins-loaded magnetic nanoparticles from large volume bio-suspension. © 2014 American Institute of Chemical Engineers AIChE J, 2014
    AIChE Journal 06/2014; · 2.58 Impact Factor
  • Separation and Purification Technology 06/2014; 131:94–101. · 2.89 Impact Factor
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    ABSTRACT: Graphical abstract Three-liquid-phase systems for removal of Al, Fe, Si and separation from rare earths (HREs-heavy rare earths, MREs-middle rare earths, LREs-light rare earths).
    Separation and Purification Technology 04/2014; 127:97–106. · 2.89 Impact Factor
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    ABSTRACT: A novel amino-functionalized magnetic cellulose composite was prepared by a process involving: (1) synthesis of magnetic silica nanoparticles using the co-precipitation method followed by the hydrolysis of sodium silicate, (2) coating with cellulose through the regeneration of cellulose dissolved in 7 wt% NaOH/12 wt% urea aqueous solvent, (3) grafting of glycidyl methacrylate using cerium initiated polymerization and (4) ring-opening reaction of epoxy groups with ethylenediamine to yield amino groups. Once generated, the resulting composite was tested for its ability to remove Cr(VI) from an aqueous solution in batch experiments. The results demonstrated that Cr(VI) adsorption was highly pH dependent. The optimized pH value was 2.0. The adsorption isotherms of the adsorbent fit the Langmuir model, with the maximum adsorption capacity of 171.5 mg/g at 25 °C. The adsorption rate was considerably fast, and the adsorption reached equilibrium within 10 min. The obtained thermodynamic parameters showed that the adsorption of Cr(VI) onto the adsorbent was an exothermic and spontaneous process. In addition, the Cr(VI) ions could be effectively desorbed using a 0.1 mol/L NaOH solution and the adsorbent exhibited a good reusability. The composite material should be a promising adsorbent for Cr(VI) removal, with the advantages of high adsorption capacity, rapid adsorption rate and convenient recovery under magnetic field.
    Chemical Engineering Journal 04/2014; 241:175–183. · 3.47 Impact Factor
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    ABSTRACT: Dried orange juice residue marketed as cattle food was converted into an economical and environmentally benign sorbent through chemical loading with zirconium(IV). Its adsorption properties for vanadium(V) and chromium(VI) from synthetic and actual waste water were investigated. The adsorption of V(V) is strongly dependent on solution pH, and the maximum separation coefficient (bV/Cr = 45) between V(V) and Cr(VI) takes place at pH 2.85. The anion exchange or nucleophilic substitution reaction between OH� and metal oxo-anions was proposed as the main adsorption mechanism. Langmuir adsorption and pseudo-second-order rate equations can describe well the adsorption of V(V) onto the gel. The maximum adsorption capacities for V(V) and Cr(VI) were estimated as 1.003 and 0.288 mmol/g, respectively. The adsorbed vanadium was effectively desorbed using a diluted NaOH solution. The negligible interference of coexisting anions, such as nitrates and chlorides, durability, reproducibility of the gel, and the column adsorption test through the mixture of V(V) and Cr(VI) followed by elution make the Zr(IV)-SOW a promising sorbent for the recovery of a small quantity of vanadium from chromium(VI)- containing effluent. Finally, a preliminary attempt to selectively enrich V(V) from the real dilute industrial effluent that contains Cr(VI) using the present gel has been carried out, and it was confirmed to be successfully achieved.
    Chemical Engineering Journal 03/2014; 248:79-88. · 3.47 Impact Factor
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    ABSTRACT: The present study prepared a size-controllable, uniform, and surfactant-free emulsification to investigate the zeta potential (ζ potential) of the solvent effect. The results showed that the ratio of electrophoretic mobility changed with droplet diameter, and the correct factor of the ζ potential was determined. The effect of functional groups on the ζ potential was further studied in the presence of an organic hydrophilic solvent. The study characterized the effects of pH, ionic strength, and ionic type on the ζ potential and indicated that the solvents were able to modulate the local electrochemical environment, thus leading to the redistribution of interface charges.
    Langmuir 02/2014; · 4.38 Impact Factor
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    Xuetuan Wei, Mingfang Luo, Huizhou Liu
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    ABSTRACT: The bifunctional coating with antithrombotic and antimicrobial activity was developed using nattokinase (NK) and nanosilver (AgNPs). Firstly, the adsorption interactions between NK and AgNPs were confirmed, and the composite particles of NK-AgNPs were prepared by adsorption of NK with AgNPs. At 5FU/mL of NK concentration, the saturation adsorption capacity reached 24.35FU/mg AgNPs with a high activity recovery of 97%, and adsorption by AgNPs also enhanced the heat stability and anticoagulant effect of NK. Based on the electrostatic force driven layer-by-layer self-assembly, the NK-AgNPs were further assembled with polyethylenimine (PEI) to form coating. UV-vis analysis showed that the self-assembly process was regular, and atom force microscopy analysis indicated that NK-AgNPs were uniformly embedded into the coating. The NK-AgNPs-PEI composite coating showed potent antithrombotic activity and antibacterial activity. This study developed a novel strategy to construct the bifunctional coating with antithrombotic and antimicrobial properties, and the coating material showed promising potential to be applied in the medical device.
    Colloids and surfaces B: Biointerfaces 01/2014; 116C:418-423. · 4.28 Impact Factor
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    ABSTRACT: Neutral organophosphates have been used for the extraction and separation of rare earths, usually with the addition of an extra salting-out reagent to achieve the necessary high ionic strength. In this work, we propose a novel approach to extraction from rare earth solutions with fairly high concentrations without an extra salting-out reagent. The distribution behaviors of La, Pr, and Nd in a nitrate solution extracted with di-(2-ethylhexyl) 2-ethylhexyl phosphonate (DEHEHP) in kerosene under the action of a self-salting-out effect were investigated, including the extraction mechanism, extracted species, extraction isotherms, and effects of acidity and temperature. The obtained results show that the extraction species probably is RE(NO3)3·1.5DEHEHP according to the slope analysis method and the saturation extraction method. Considering the other coexisting light rare earths, such as Ce and Sm, the separation factors were also examined through a comparison of the two commercial extractants P350 and TBP. The extraction selectivity for DEHEHP under the action of the self-salting-out effect is much higher than that of TBP but just slightly below that of P350. Finally, it can be concluded that the current system using DEHEHP as an extractant under the action of the self-salting-out effect shows good prospects for the purification of La from other light rare earths.
    Industrial & Engineering Chemistry Research. 01/2014; 53(4):1598–1605.
  • Chemical Engineering Journal 12/2013; 234:338-345. · 3.47 Impact Factor
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    ABSTRACT: In this study, gas-assisted superparamagnetic extraction (GASE) with potential large-scale application was proposed for selective separation of multicomponent proteins. Magnetic poly(glycidyl methacrylate)–iminodiacetic acid–Zn2+ microspheres (MPMs) for selective separation of bovine serum albumin (BSA) and bovine hemoglobin (BHb) are selected as a model. The feasibility of flotation for concentrating BHb-loaded MPMs from dilute mixed proteins solution was proved. The well-concentrated solution of BHb-loaded MPMs could be achieved by simple adjustment of pH values and ionic strength in low regions, without additive detergent. Impurity BSA had the effects of improving the flotability of BHb-loaded MPMs, acting as foaming agent, but decreasing the enrichment ratio in the GASE process. The flotation conditions and the selective adsorption ones showed strong consistency. Under the optimal conditions, the enrichment ratio of 39 and recovery percentage of 98% was obtained within 1.3 min. Furthermore, the enrichment ratio could be further improved by added flotation steps.
    Industrial & Engineering Chemistry Research. 11/2013; 52(46):16314–16320.
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    ABSTRACT: The present work puts forward a new strategy to achieve group separation of light, middle, and heavy rare-earth ions by liquid–liquid–liquid three-phase systems. Experimental results indicated that heavy rare-earth ion, Yb(III), can be selectively extracted into the organic top phase, while middle rare-earth ion, Eu(III), and light rare-earth ion, La(III), can be enriched, respectively, into PEG-rich middle phase and (NH4)2SO4-rich bottom aqueous phase of Cyanex272/PEG/(NH4)2SO4–H2O three-liquid-phase system. Various influences of aqueous pH, (NH4)2SO4 concentrations, complexing agents, polymers, and their added amount on three-liquid-phase separation of La, Eu, and Yb were investigated. Besides, a possible partitioning mechanism for three rare-earth ions was discussed. The present work highlights the possibility of employing the discrepancy in selective partitioning behaviors of different rare-earth ions (such as La, Ce, Eu, Gd, Yb, and Lu) into different liquid layers of three-liquid-phase system to achieve one-step group separation of light, middle, and heavy rare-earth ions. In comparison with traditional organic-aqueous biphasic extraction for group separation of rare-earth ions, which require multiple steps of pH adjustments and repeated separation, the three-liquid-phase approach exhibits obvious advantages for future industrial application.
    Industrial & Engineering Chemistry Research 04/2013; 52(17):5997–6008. · 2.24 Impact Factor

Publication Stats

1k Citations
333.99 Total Impact Points

Institutions

  • 1999–2014
    • Chinese Academy of Sciences
      • • Key Laboratory of Green Process and Engineering
      • • State Key Laboratory of Biochemical Engineering
      Peping, Beijing, China
  • 2002–2013
    • Northeast Institute of Geography and Agroecology
      • • State Key Laboratory of Biochemical Engineering
      • • Key Laboratory of Green Process and Engineering
      Peping, Beijing, China
  • 2008–2009
    • Beijing University of Chemical Technology
      Peping, Beijing, China
  • 2004
    • Peking University
      • Department of Chemistry
      Beijing, Beijing Shi, China
  • 2001
    • Technical Institute of Physics and Chemistry
      Peping, Beijing, China