Huizhou Liu

Chinese Academy of Sciences, Peping, Beijing, China

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Publications (221)532.35 Total impact

  • Xitong Sun · Qian Li · Liangrong Yang · Huizhou Liu
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    ABSTRACT: Two novel strongly basic magnetic adsorbents, quaternary ammonium-modified polystyrene and chitosan magnetic microspheres (Pst-MIMCl and CTS-GTMAC), were prepared using the in-situ coprecipitation and emulsion cross-linking methods under mild conditions, with the features of strong magnetic responsiveness and high quaternary ammonium group contents. The Cr(VI) adsorption/desorption properties and mechanisms of strongly and weakly basic magnetic adsorbents were compared through simulated wastewater. The strongly basic adsorbent exhibited low pH dependence, and the main adsorption mechanism was ion exchange. The weakly basic adsorbent exhibited high pH dependence, and the major adsorption mechanism was electrostatic attraction. Besides, the strongly basic adsorbent (0.3 mol/L NaOH + 0.3 mol/L NaCl) required higher desorption conditions than the weakly basic adsorbent (0.1 mol/L solution) owing to the difference of the desorption mechanisms. Furthermore, the removal selectivity of the strongly and weakly basic magnetic adsorbents was estimated by the chromium plating wastewater. The results demonstrated that the strongly basic magnetic adsorbents exhibited higher selectivity than the weakly basic magnetic adsorbents. In addition, the Pst-MIMCl was selected as the optimal magnetic adsorbent for Cr(VI) recovery from wastewater, with the advantages of strongly magnetic responsiveness, wide pH applicable range, high removal efficiency, high adsorption selectivity and good reusability.
    No preview · Article · Feb 2016 · RSC Advances
  • Na Sui · Kun Huang · Huizhou Liu
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    ABSTRACT: The relationship between the partitioning of rare-earth ions in polymer-based three-liquid-phase system (TLPS) of Cyanex 272/PEG 600/(NH4)2SO4-H2O and the change in volume ratios of PEG-rich middle phase to salt-rich bottom phase was investigated. It was found that the change in phase volume ratios might be attributed to the transfer of hydrated PEG molecules. Therefore, the partitioning of hydrated PEG is a main driving force for the partitioning of rare earths. The change in water content in PEG-rich phase should be taken into account for calculating partition coefficients of rare-earth ions. The traditional Diamond-Hsu model derived from Flory-Huggins theory considered only the partitioning of simple PEG molecules to calculate the partition coefficients of targets in polymer-based aqueous biphasic system, so that it could not reflect such influences from the change in phase volume ratios. The present work discusses the influences from the change of the concentrations of PEG and inorganic salt, Cyanex 272 concentration in top organic phase of TLPS, aqueous pH value and initial concentration of rare-earth ions, on the partitioning of rare-earth ions into PEG-rich middle phase of TLPS. Experimental results indicate that the partition coefficients of rare-earth ions have close relationship with the transfer of hydrated PEG molecules. The work implies that the partition behaviors of rare-earth ions in TLPS can be described more clearly based on the hydrogen-bond interaction of rare-earth ion with hydrated PEG molecules.
    No preview · Article · Feb 2016 · Colloids and Surfaces A Physicochemical and Engineering Aspects
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    ABSTRACT: A novel, bioadsorbent material of polyethylenimine-modified magnetic chitosan microspheres enwrapping magnetic silica nanoparticles (Fe3O4-SiO2-CTS-PEI) was prepared under relatively mild conditions. The characterization results indicated that the adsorbent exhibited high acid resistance and magnetic responsiveness. The Fe3O4 loss of the adsorbent was measured as 0.09% after immersion in pH 2.0 water for 24 h, and the saturated magnetization was 11.7 emu/g. The introduction of PEI obviously improved the adsorption capacity of Cr(VI) onto the adsorbent by approximately 2.5 times. The adsorption isotherms and kinetics preferably fit the Langmuir model and the pseudo-second-order model. The maximum adsorption capacity was determined as 236.4 mg/g at 25°C, which was much improved compared to other magnetic chitosan materials, and the equilibrium was reached within 60 to 120 min. The obtained thermodynamic parameters revealed the spontaneous and endothermic nature of the adsorption process. Furthermore, the Cr(VI)-adsorbed adsorbent could be effectively regenerated using a 0.1 mol/L NaOH solution, and the adsorbent showed a good reusability. Due to the properties of good acid resistance, strong magnetic responsiveness, high adsorption capacity, and relatively rapid adsorption rate, the Fe3O4-SiO2-CTS-PEI microspheres have a potential use in Cr(VI) removal from acidic wastewater.
    No preview · Article · Nov 2015 · Journal of Applied Polymer Science
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    ABSTRACT: In the protein separation, adsorption and desorption of target protein have been using different buffer condition. Different buffer will change the structure and activity of target protein in some cases. This work describes the use of different wavelength light for remote regulation of adsorption and desorption of target protein in the same buffer solutions. A dynamic system that captured and released protein in response to light is reported. Matrix gold nanoparticles and light-responsive affinity ligand comprising thrombin aptamer (APT15), polyethylene glycol linker, and azobenzene-modified complementary sequence were used. UV light induced a trans–cis isomerization of the azobenzene that destabilized the duplex of aptamer and azobenzene-modified complementary sequence, resulting in thrombin binding to aptamer sequence. Visible light irradiation resulted in DNA duplex rehybridization and thrombin released. Our work demonstrates that different light wavelengths effectively regulated the adsorption and desorption of thrombin in the same buffer, and this system also can capture and release prothrombin from plasma with different wavelength light. Furthermore, this method can be widely applied to a variety of different protein separation process.
    No preview · Article · Nov 2015 · Talanta
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    ABSTRACT: In this study, a method combined low-field magnetic separation (MS) with flotation, named as gas-assisted magnetic separation (GAMS), was applied for the removal of cadmium from wastewater. With bubbles’ assistance, the speed of magnetic separation can be greatly improved and the limitation of magnetic force on the capture distance can be overcome. Thus, GAMS is much more efficient and easily scalable than MS. In this work, ethanediamine-modified magnetic poly-(glycidyl methacrylate) microspheres (EMPs) were synthesized as the adsorbent for cadmium. And GAMS was used to separate the EMPs and Cd-loaded EMPs. The effects of pH, gas flow rate, concentration of Cd-loaded EMPs, loading volume, and ionic strength on GAMS were investigated. The results indicated that the EMPs and Cd-loaded EMPs could be rapidly and remotely removed from the solution with GAMS. And the separation time decreased with the increase of gas flow rate and NaCl concentration, but grew with the rise of pH value, loading volume, and concentration of the EMPs. This work showed the great potential of GAMS in the area of water treatment.
    No preview · Article · Nov 2015 · The Chemical Engineering Journal

  • No preview · Article · Oct 2015 · ACS Sustainable Chemistry & Engineering
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    ABSTRACT: A new approach called "asynchronous spectrum with auxiliary peaks (ASAP)" is proposed for generating a 2D asynchronous spectrum to investigate the intermolecular interaction between two solutes (P and Q) dissolved in the same solution. In the ASAP approach, a virtual substance S with an isolated peak assumed to be at νS is introduced, while the characteristic peaks of P and Q are actually observed at νP and νQ. The concentrations series of P, Q and S are specifically designed so that a spectral portion that has nothing to do with the intermolecular interaction between P and Q is completely removed from the 2D asynchronous spectrum. Auxiliary cross peaks around (νP, νS) and (νQ, νS) can be used to reveal spectral variation caused by intermolecular interaction, which cannot be observed on conventional cross peaks appearing around the spectral coordinates (νP, νP), (νP, νQ), (νQ, νP), (νQ, νQ). For example, variation of the absorptivity of P caused by an intermolecular interaction between P and Q can be probed from the auxiliary cross peaks around (νP, νS) when Q does not even have any characteristic peak in the observed spectral range.
    Full-text · Article · Oct 2015 · RSC Advances
  • Pan Sun · Kun Huang · Huizhou Liu
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    ABSTRACT: Extraction and separation of V and Cr in alkaline aqueous solutions have attracted extensive interests in recent years due to successful development of the Sub-molten Salt Method for treating the vanadium–chromium complex magnetite ores, such as those from Pan-Zhihua in China. However, vanadium products with high purity are hard to be obtained directly by traditional chemical precipitation and crystallization separation from the alkaline leaching solutions obtained from the Sub-molten Salt Method, due to the chemical similarity between V and Cr. In present work, a new strategy by liquid–liquid solvent extraction using acidified primary amine N1923-isooctanol system is suggested to extract and separate V from Cr and Si co-existing in the strongly alkaline aqueous solutions with initial pH values even above 12. Experimental results revealed that co-extraction of V and Cr can be effectively avoided if some special inorganic salts, such as sodium sulfate, are previously added into the alkaline aqueous solutions. The influence from the added amount of sodium sulfate, initial aqueous pH value, acidification percentage of primary amine N1923, operation phase ratio, and initial concentration ratio of V to Cr, on separation behaviors of V from Cr and Si were investigated. Extraction isotherms, kinetics and extraction mechanism of V from alkaline solutions were also discussed. Stripping of V from the loaded organic phase and recycling of the organic phase were evaluated. The present work highlights a new approach to separate V from the strongly alkaline leaching solutions containing Cr and Si, and it exhibits great potential for promoting development of the Sub-molten Salt Method to treat the High Chromium Vanadium–Titanium Magnetite.
    No preview · Article · Oct 2015 · Hydrometallurgy
  • Feng Pan · Song Gao · Huizhou Liu
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    ABSTRACT: Single crystals of three polymorphous compounds were synthesized started from two building blocks, [Fe(CN)6]3- and [Co(LN3O2)]2+ (L is a Schiff-base macrocyclic ligand derived from the condensation of 2,6-diacetylpyridine with 3,6-dioxaoctane-1,8-diamine) using a crystallization condition control. All three compounds consist of electroneutral skeletons made up of Fe6Co6 twelve-metal ring units, which is the smallest enclosed circle in their structures: 1 is comprised of 1D nanometer-diameter tubes possessing nanometer-sized tunnels (0.58 nm × 0.74 nm); 2 and 3 are based on piled-up 2D lamellar layers in the (6, 3) and (4, 4) networks, respectively. Magnetic studies indicate ferromagnetic interactions between cyanide-bridged cobalt(ii) and iron(iii) in each compound. This journal is
    No preview · Article · Sep 2015 · CrystEngComm
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    ABSTRACT: Na-ion batteries are becoming comparable to Li-ion batteries because of their similar chemical characteristics and abundant sources of sodium. However, the materials production should be cost-effective in order to meet the demand for large-scale application. Here, a series of nanosized high-performance cathode materials, Na3 (VO1-x PO4 )2 F1+2x (0≤x≤1), has been synthesized by a solvothermal low-temperature (60-120 °C) strategy without the use of organic ligands or surfactants. The as-synthesized Na3 (VOPO4 )2 F nanoparticles show the best Na-storage performance reported so far in terms of both high rate capability (up to 10 C rate) and long cycle stability over 1200 cycles. To the best of our knowledge, the current developed synthetic strategy for Na3 (VO1-x PO4 )2 F1+2x is by far one of the least expensive and energy-consuming methods, much superior to the conventional high-temperature solid-state method. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
    No preview · Article · Jul 2015 · Angewandte Chemie International Edition

  • No preview · Article · Jul 2015
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    ABSTRACT: In this paper, gas-assisted magnetic separation (GAMS), a technique that combines magnetic separation with flotation, was investigated for the potential large-scale separation of proteins. The GAMS process includes adsorption of target proteins and magnetic separation to recover protein-loaded magnetic particles from the dilute biosuspension with the assistance of bubbles. Microsized ethylenediamine-functionalized poly(glycidyl methacrylate) superparamagnetic microspheres (MPMs) and bovine serum albumin (BSA) were used as a model system. The feasibility of GAMS for capturing BSA-loaded MPMs from an appropriate medium was shown. High recovery of BSA-loaded MPMs was obtained by simple adjustment of the initial solution pH without extra detergents and antifoaming agents. The GAMS conditions were consistent with the adsorption conditions, and no proteins were desorbed from the MPMs during this process. Under the optimal conditions, the separation rate and recovery percentage reached 410 mL/min and 98% in 0.61 min, respectively. Conformational changes of BSA during the GAMS process were investigated by fluorescence spectroscopy and circular dichroism spectrometry.
    No preview · Article · Jul 2015
  • Jie Liu · Kun Huang · Huaizhi Wu · Huizhou Liu
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    ABSTRACT: Enrichment and recovery of valuable components in industrial waste waters by traditional liquid-liquid solvent extraction is not economic due to extremely low concentrations of those targets. Large-phase-ratio extraction exhibits potential advantages for recovery of small quantities of target components from large volume of aqueous solutions. In present work, a novel bubbling extraction tower is proposed towards performing solvent extraction at large aqueous-to-oil phase ratios. Organic extractants were covered onto surface of gas bubbles to form a layer of organic liquid membrane and the dispersed organic phase in tower could be small enough. The target components are extracted from aqueous feed solution onto the surface of the bubbles, and the enrichment ratios could be extremely high. We develop a feasible methodology to calculate tower height and operation phase ratios of the bubbling extraction tower, which is essential for future industrial scale-up. Experimental results in pilot test are highly consistent with calculations. This article is protected by copyright. All rights reserved.
    No preview · Article · Jun 2015 · AIChE Journal
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    ABSTRACT: Rapid and sensitive detection of thrombin has very important significance in clinical diagnosis. In this work, bare magnetic iron oxide nanoparticles (magnetic nanoparticles) without any modification were used as fluorescence quenchers. In the absence of thrombin, a fluorescent dye (CY3) labeled thrombin aptamer (named CY3-aptamer) was adsorbed on the surface of magnetic nanoparticles through interaction between a phosphate backbone of the CY3-aptamer and hydroxyl groups on the bare magnetic nanoparticles in binding solution, leading to fluorescence quenching. Once thrombin was introduced, the CY3-aptamer formed a G-quartet structure and combined with thrombin, which resulted in the CY3-aptamer being separated from the magnetic nanoparticles and restoration of fluorescence. This proposed assay took advantage of binding affinity between the CY3-aptamer and thrombin for specificity, and bare magnetic nanoparticles for fluorescence quenching. The fluorescence signal had a good linear relationship with thrombin concentration in the range of 1-60 nM, and the limit of detection for thrombin was estimated as low as 0.5 nM. Furthermore, this method could be applied for other target detection using the corresponding fluorescence labeled aptamer.
    No preview · Article · Apr 2015 · The Analyst
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    ABSTRACT: Phase separation dynamic processes in Three-Liquid-Phase System (TLPS), composed of organic oil (P507 extractant), water-soluble polymer (PEG2000), ammonium sulfate and water, with the change of mass composition of phase-forming components were investigated. It was found that dynamic separation of three-layered liquid phases in TLPS is in fact a course of dispersive polymer and organic oil droplets aggregated and separated out respectively from continuous salt aqueous bottom phase. Formation rate of organic oil phase was controlled mainly by coalescence rate of dispersed oil droplets, however rate-determining process for formation of polymer middle phase may change from drop sedimentation to coalescence or co-determined by both, when mass composition of the TLPS changed along different operation lines. With the formation of organic oil phase, it becomes another continuous phase, from which dispersive polymer droplets separated out and aggregated into a bulk phase gradually. Phase separation equilibrating time of TLPS, tE, depends on formation rate of the polymer middle phase and its equilibrium volume. A quantitative correlation of phase separation rate of TLPS with its physic-chemical properties was given. The present work promotes further understanding about influence from change in mass composition of phase-forming components in TLPS on three-phase separation dynamic processes.
    No preview · Article · Apr 2015 · Industrial & Engineering Chemistry Research
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    ABSTRACT: Room temperature sodium-ion batteries with much lower cost relative to lithium-ion batteries have attracted particular interest for large-scale electrical energy storage in the fields of renewable energies and smart grid. However, most reported cathode materials were synthesized through a conventional high-temperature solid-state method. In order to further save energy and reduce cost, here we show that a series of high-performance cathode materials, sodium vanadium polyanionic compounds, Na3(VO1-xPO4)2F1+2x (x = 0, 0.5 and 1), can been synthesized by a phase-transfer assisted solvo-thermal strategy at a rather low temperature (80 - 140 oC) in one simple step, where an acid-base-coupled extractant was used to attain the phase-transfer of phosphoric acid. More importantly, the used extractant in this route can be recycled. The as-synthesized materials (Na3(VPO4)2F3 and Na3(VOPO4)2F) exhibit a high Na storage capacity of ca. 120 mAh/g which is close to the theoretical capacity and excellent cycling performance. This study makes a significant step to extend this strategy in the synthesis of functional materials from simple binary to complex multicomponent compounds.
    No preview · Article · Mar 2015 · Chemical Communications
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    ABSTRACT: In this work, a novel IL-based synergistic extraction system utilizing the ionic liquid tricaprylmethylammonium nitrate ([A336][NO3]) and the commercial extractant Di(2-ethylhexyl) 2-ethylhexyl phosphonate (DEHEHP) was developed for the extraction of rare earth (RE) nitrates. Pr(III) was used as a model RE and the effects of key factors, i.e. the ratio of [A336][NO3] to DEHEHP, the acidity of feed solutions, and the concentration of a salting-out reagent, were systematically studied. Our results demonstrate that the mixture of [A336][NO3] and DEHEHP had an obviously synergistic extraction effect for the extraction of Pr(III). The maximum synergistic enhancement coefficient of 3.44 was attained at XA = 0.4 (v%). Alternatively, mixture of [A336][Cl] and DEHEHP hardly extracted Pr(III) from chloride media. Moreover, we investigated the Pr(III) extraction mechanism and demonstrated that Pr(III) can be extracted as the neutral complexation species Pr(NO3)3﹒xDEHEHP and the ion-type species [A336]y﹒Pr(NO3)3+y. These extraction processes can effectively hamper the release of organic cation-ligands into the aqueous phase. The synergistic extraction effect is mainly derived from the enhanced solubility of the extracted species in the ionic liquid phase. The extraction behaviors of Pr(III) could be properly described by Langmuir and pseudo-second-order rate equations. Increased temperature was unfavorable for the extraction reaction but greatly improved the extraction rate. Interestingly, the mixed IL extraction system has an obviously synergistic extraction effect for light REs (LREs, La - Eu), but an anti-synergistic effect for heavy REs (HREs, Gd - Lu, Y), thus, indicating that our synergistic extraction system is helpful for the separation of LREs from HREs. In addition, the high selectivity between REs and non-REs suggested that the recovery of REs from a complicated high-salt leachate could be highly possible. It demonstrates that the IL-based synergistic extraction strategy developed in this work is promising and sustainable, and as a result, the development of an IL-based synergistic extraction process for the recovery of REs is straightforwardly envisaged.
    Preview · Article · Mar 2015 · Green Chemistry
  • Junmei Zhao · Qiaoyu Hu · Yingbo Li · Huizhou Liu
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    ABSTRACT: Ionic liquid (IL)-based extraction is a promising and environmentally benign separation technology. To develop sustainable extraction technologies, quaternary ammonium-based IL extraction strategy is attractable. In this work, the separation of vanadium(V) from chromium(VI) by pure tricaprylmethylammonium nitrate ([A336][NO3]) and organic acidified primary amine N1923 ([RNH3][NO3]) was systematically investigated. The optimal proportion of [A336][NO3] and [RNH3][NO3] was studied and results showed that the mixed [A336][NO3] and [RNH3][NO3] exhibited an obvious synergistic-effect for V(V). The extraction of V(V) was strongly dependent on the acidity of the aqueous phase and reaches maximum at pH 2.5-3, while the maximum separation coefficient (βV/Cr) was located at about pH 9.0. Moreover, βV/Cr could be improved through adjusting the molar concentration ratio of V/Cr. The interference of coexisting anions (nitrates, chlorides, sulfate and phosphate) on the extraction of V(V) was examined and the results showed that PO43−, NO3− and Cl− had negative effects at various degrees except for SO42−. The V(V) extraction behaviors could be properly described by Langmuir and pseudo-second-order rate equations. The maximum extraction capacity for V(V) was estimated as 1.877 mmol/g at 303 K. Increased temperature had little effect on the extraction capacity, but greatly improved the extraction rate. The typical anion exchange mechanism between NO3− and V4O124− (or V3O93−) was proposed for the current extraction system. The IL phase could be renewed through stripping the loaded vanadium by a 0.5 M NaNO3 solution. This work demonstrated that quaternary ammonium IL containing a commercial organic extractant is an efficient and sustainable IL-based extraction strategy for the separation of vanadium from chromium, and as a result, the development of an IL-based extraction process is straightforwardly envisaged.
    No preview · Article · Mar 2015 · The Chemical Engineering Journal
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    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.
    No preview · Article · Feb 2015 · The Chemical Engineering Journal
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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.
    Preview · Article · Nov 2014

Publication Stats

5k Citations
532.35 Total Impact Points

Institutions

  • 1999-2015
    • Chinese Academy of Sciences
      • • State Key Laboratory of Biochemical Engineering
      • • Institute of Process Engineering
      • • Key Laboratory of Green Process and Engineering
      Peping, Beijing, China
    • Academia Sinica
      T’ai-pei, Taipei, Taiwan
  • 2007
    • Nanyang Technological University
      Tumasik, Singapore
  • 2001
    • Technical Institute of Physics and Chemistry
      Peping, Beijing, China
  • 1995
    • Peking University
      • Department of Chemistry
      Beijing, Beijing Shi, China