Co-reporter:Yinyong AoJian Chen, Yue Wang, Hongbing Chen, Jiuqiang Li, Maolin Zhai
The Journal of Physical Chemistry B 2017 Volume 121(Issue 8) pp:
Publication Date(Web):January 26, 2017
DOI:10.1021/acs.jpcb.6b11395
Experimental study with DFT validation on the effect of radiation on 1-carboxymethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([HOOCCH2MIM][NTf2]) as a solvent and extractant in rapid homogeneous extraction of UO22+ was performed for the first time. The radiolytic products of the anions and cations of [HOOCCH2MIM][NTf2] were identified by 19F NMR and high-resolution ESI-MS, respectively, and they were attributed to a decrease in UO22+ partitioning. Experimental study with DFT validation for complexing reactions between [HOOCCH2MIM][NTf2] and radiolytic products proved that F– competition was one of the main reasons for the decrease in UO22+ partitioning. However, UO22+ partitioning in irradiated [HOOCCH2MIM][NTf2] can largely be recovered after thorough water washing because of the removal of radiolytic products of [NTf2]−.
Co-reporter:Yimeng Wang;Jingyi Qiu;Jing Peng;Jiuqiang Li
Journal of Materials Chemistry A 2017 vol. 5(Issue 24) pp:12393-12399
Publication Date(Web):2017/06/20
DOI:10.1039/C7TA02291C
We demonstrated a one-step synthesis method for a novel gel polymer electrolyte (named PDMP-Li GPE) based on 3-(dimethylamino) propyl methacrylate, poly(ethylene glycol) diacrylate and 1 M LiPF6 liquid electrolyte solution by a γ-radiation technique for lithium-ion batteries. The resultant PDMP-Li GPE exhibited good thermal stability, excellent mechanical strength and high ionic conductivity, and the highest ionic conductivity reached 8.88 × 10−3 S cm−1 at 25 °C. The LiFePO4/PDMP-Li GPE/graphite pouch-type cell exhibited more than 97% columbic efficiency and the capacity retention was about 86% after 50 cycles at 0.1C. With these outstanding characteristics, it is expected to be a promising candidate for the application in polymer lithium-ion batteries.
Co-reporter:Yicheng Wang, Jing Peng, Jiuqiang Li, Maolin Zhai
Radiation Physics and Chemistry 2017 Volume 130(Volume 130) pp:
Publication Date(Web):1 January 2017
DOI:10.1016/j.radphyschem.2016.09.009
•PVDF-g-PSSA IEM was prepared by preradiation grafting of ETSS and sequent hydrolysis.•The PVDF-g-PSSA IEM showed a high IEC (1.66 mmol g−1) at a GY of 80%.•The PVDF-g-PSSA IEM showed a high proton conductivity (58.2 mS/cm) at a GY of 80%.A new synthesis route for poly(vinylidene fluoride)-g-polystyrene sulfonic acid ion exchange membrane (PVDF-g-PSSA IEM) has been developed via preradiation-induced grafting of ethyl styrenesulfonate and sequent hydrolysis. A high grafting yield (GY) 120% for PETSS grafted onto PVDF could be obtained at a reaction time of 3 h and dose of 50 kGy. The structure of PVDF-g-PSSA IEM was testified by FTIR, XPS, TGA and SEM analysis. At the GY above 80%, the ion exchange capacity, water uptake and proton conductivity of the resultant PVDF-g-PSSA IEM exceeds Nafion 117 membrane. This work provides an environmental method for the preparation of the IEM used in fuel cell or water treatment.
Co-reporter:Siqi Liu, Min Xu, Tianlin Yu, Dong Han, Jing Peng, Jiuqiang Li, Maolin Zhai
Carbohydrate Polymers 2017 Volume 174(Volume 174) pp:
Publication Date(Web):15 October 2017
DOI:10.1016/j.carbpol.2017.06.012
•New cellulose based adsorbents for boron (III) was prepared by radiation grafting.•The adsorbent (CVN) reached an adsorption capacity of 12.4 mg g−1 at pH 6.•The adsorption process obeys the Langmuir isotherm model.•The uptake of boron (III) was enhanced in saline solutions.A novel cellulose-based microsphere containing glucamine groups, referred as CVN, was successfully synthesized by radiation-induced graft polymerization of 4-vinylbenzyl chloride onto cellulose microspheres and subsequent functionalization with N-methyl-d-glucamine. The adsorption by CVN for boron (III) from aqueous solutions was evaluated systematically by batch adsorption technique. Langmuir models could fit well with the adsorption behavior of CVN. The CVN adsorbents exhibited a high adsorption capacity up to 12.4 mg g−1 towards boron (III) over the wide pH range of 5–8. After the addition of chloride salts, the boron uptake of CVN was enhanced that was attributed to the compensation of the surface charge generated by boron (III) adsorption leading to favor the adsorption. At high concentrations of salts, the ionic strength and different salts have no effect on the adsorption of boron(III). This work provides a new sustainable, cost effective material as a promising specific adsorbent for the removal of boron (III) from saline solutions.
Co-reporter:Dong Han, Xingxiao Li, Jing Peng, Ling Xu, Jiuqiang Li, Huibo Li and Maolin Zhai
RSC Advances 2016 vol. 6(Issue 73) pp:69052-69059
Publication Date(Web):20 Jul 2016
DOI:10.1039/C6RA12239F
A new imidazolium-based polymeric ionic liquid (PC2vimBr) gel was prepared by γ-radiation induced polymerization and crosslinking of 1-vinyl-3-ethylimidazolium bromide and a functional crosslinker 3,3′-divinyl-1,1′(1,6-hexanediyl) diimidazolium dibromide. A high gel fraction of ca. 95% could be achieved under 40 kGy, and the equilibrium degree of swelling and mechanical properties could be adjusted by crosslinker content and absorbed dose. The highest fracture compressive strength of PC2vimBr could be as high as 0.21 MPa. PC2vimBr could strongly adsorb perrhenate (ReO4−) with an adsorption capacity as high as ca. 8.6 × 102 mg g−1 (Re/gel), following a Langmuir model by an ion exchange mechanism, which was confirmed by IR and XPS. Competitive adsorption with the electrolytes or sodium dodecyl benzene sulfonate showed that the PC2vimBr gel has good efficiency for ReO4− removal from a low concentration of electrolyte solution or laundry waste water. Considering ReO4− is the natural analogue of TcO4−, PC2vimBr may be used in decontamination of low level wastes such as laundry wastes. Interestingly, PC2vimBr would shrink strongly after adsorbing ReO4−, which is meaningful for volume reduction of radioactive wastes.
Co-reporter:Jian Chen, Yinyong Ao, Tingrui Lin, Xin Yang, Jing Peng, Wei Huang, Jiuqiang Li, Maolin Zhai
Polymer 2016 Volume 87() pp:73-80
Publication Date(Web):22 March 2016
DOI:10.1016/j.polymer.2016.01.069
•Tough polyacrylamide gel containing hydrophobic crosslinking was synthesized by radiation induced micelle polymerization.•The gel could keep intact after compressed to the strain of 0.9 and stretched to as long as 10 times of the original gel.•Double network polyacrylamide gel with a good cycle compression property was further synthesized by γ-radiation.Tough polyacrylamide gel containing hydrophobic crosslinking (HPAAm gel) was easily synthesized by γ-radiation induced micelle copolymerization and crosslinking of a hydrophobic monomer, stearyl acrylate (STA), and acrylamide. HPAAm gel could still keep intact after compressed to the strain of 0.9 while the corresponding polyacrylamide gel prepared by adding chemical crosslinker has been broken. Meanwhile, elongation at break of HPAAm gel could reach 1000%, which is also much higher than conventional polyacrylamide gels, indicating the high toughness of HPAAm gel. Furthermore, double network polyacrylamide hydrogel containing hydrophobic crosslinking (DN-HPAAm) was synthesized by incorporating another PAAm network into the prepared HPAAm gel. The resultant DN-HPAAm gel has much better compression strength (∼2 MPa) than HPAAm gel and a good cycle compression property.
Co-reporter:Shuojue Wang, Hui-Ling Ma, Jing Peng, Youwei Zhang, Jian Chen, Liangliang Wang, Ling Xu, Jiuqiang Li and Maolin Zhai
Dalton Transactions 2015 vol. 44(Issue 16) pp:7618-7625
Publication Date(Web):17 Mar 2015
DOI:10.1039/C5DT00101C
A novel polymeric ionic liquid gel (PIL gel) was simply synthesized by γ-radiation-induced polymerization of ionic liquid monomer 1-allyl-3-vinylimidazolium chloride and crosslinking at ambient temperature without any additives. By changing the radiation dose, the properties of the resulting gel including the gel fraction, crosslinking density and equilibrium degree of swelling were optimized. The resulting PIL gel exhibited a superior adsorption ability toward Cr(VI) in aqueous solutions with a broad pH range (1–7) through anion exchange. It was found that the adsorption kinetics followed the pseudo-second-order model. The adsorption of Cr(VI) by the PIL gel obeyed the Langmuir isotherm equation with a theoretical maximum adsorption capacity of 283 mg g−1, twice the highest value for ionic liquid-based adsorbents that have been reported. In addition, the PIL gel could be recovered using a NaCl solution or a NaOH solution without much decreasing the adsorption capacity. This work paves the way for the scale-up production of PIL gels using the radiation technique for potential application in heavy metal removal.
Co-reporter:Yinyong Ao, Weijin Yuan, Tianlin Yu, Jing Peng, Jiuqiang Li, Maolin Zhai and Long Zhao
Physical Chemistry Chemical Physics 2015 vol. 17(Issue 5) pp:3457-3462
Publication Date(Web):11 Dec 2014
DOI:10.1039/C4CP04294H
The quantitative analysis and identification of the radiolytic products of dicyclohexano-18-crown-6 (DCH18C6), 4′,4′′(5′′)-di-tert-butyldicyclohexano-18-crown-6 (DtBuCH18C6) and benzo-18-crown-6 (B18C6) in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([C4mim][NTf2]) ionic liquid after irradiation were performed for the first time. It was found that the yield for radiolytic destruction of DCH18C6 and DtBuCH18C6 was less than that for B18C6. The main radiolytic products were identified as substituted crown ethers formed between crown ether and active radicals such as methyl, trifluoromethyl, butyl, and [C4mim]˙ radicals generated during the irradiation of the crown ether–[C4mim][NTf2] system. The radiation effect on the Sr2+ partitioning of the crown ether–[C4mim][NTf2] system shows further that DCH18C6–[C4mim][NTf2] and DtBuCH18C6–[C4mim][NTf2] still have good extractability for Sr2+ after irradiation. The extraction ability of DCH18C6–[C4mim][NTf2] and DtBuCH18C6–[C4mim][NTf2] system for Sr2+ decreased by 14.4% and 18.2% even at 500 kGy, respectively.
Co-reporter:Xing Zhang;Liangliang Wang;Jing Peng;Pengfei Cao;Xiaosheng Cai;Jiuqiang Li
Advanced Materials Interfaces 2015 Volume 2( Issue 15) pp:
Publication Date(Web):
DOI:10.1002/admi.201500267
A novel high-performance flexible gel polymer electrolyte (FGPE) for supercapacitors is prepared by a freeze-drying method. In the presence of 1-butyl-3-methylimidazolium chloride (BMIMCl) ionic liquid, Li2SO4 can easily be added into poly(vinyl alcohol) (PVA) aqueous solution over a large concentration range. The resultant FGPE demonstrates considerably high ionic conductivity (37 mS cm−1) and a high fracture strain at 100% elongation at the optimal weight ratio of PVA:BMIMCl:Li2SO4 = 1:3:2.2. The supercapacitor fabricated with the resultant FGPE and activated carbon electrodes shows an electrode-specific capacitance of 136 F g−1 with a stable operating voltage of 1.5 V, a maximum energy density of 10.6 Wh kg−1, and a power density of 3400 W kg−1. Double supercapacitors in series can efficiently drive a light emitting diode (LED) bulb for over 5 min and the retention of the specific capacitance reaches 90% even after 3000 charge–discharge cycles. The ionic conductivity and charge–discharge behaviors of the resultant FGPE are not affected by bending up to 180°. The flexible supercapacitor device shows only a small capacitance loss of 18% after 1000 cycles of 135° bending.
Co-reporter:Jian Chen, Shuojue Wang, Jing Peng, Jiuqiang Li, and Maolin Zhai
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 17) pp:14894
Publication Date(Web):August 19, 2014
DOI:10.1021/am504102r
Water and soil pollution by organic pollutants from petrochemical plants has become one of the major environmental problems in recent years. Lipophilic polyelectrolyte gels with ionic groups dissociable in nonpolar organic solvents show an enhanced swelling ability in a corresponding media attributed to the electrostatic repulsion and osmotic pressure provided by dissociated ionic groups. Here, we synthesized new lipophilic polyelectrolyte gels based on an easily available electrolyte monomer, methacryloxyethyl dimethyloctane ammonium trifluoromethanesulfonimide (MODAT), and a lipophilic neutral monomer, dodecyl acrylate by radiation-induced polymerization and cross-linking. The resultant lipophilic polyelectrolyte gels could absorb plenty of organic solvents with dielectric constants lower than 20 and exhibited a high absorbing ability at a wide range of temperatures (0–40 °C). The maximum swelling degree could reach as high as 200 g/g in some media, such as 1,2-dichloroethane (199.4 g/g) and dichloromethane (204 g/g), which was much higher than that of the nonionic gel without the addition of MODAT. Moreover, the resultant lipophilic polyelectrolyte gels could release most of the absorbed solvents within several hours and then be reused. It is expected that this new type of lipophilic polyelectrolyte gels may be a suitable candidate as organic pollutant absorbents.Keywords: absorbing ability; lipophilic polyelectrolyte gels; organic solvents; radiation-induced polymerization and cross-linking; solvent retention; swelling
Co-reporter:Shuojue Wang, Junzi Liu, Liyong Yuan, Zhenpeng Cui, Jing Peng, Jiuqiang Li, Maolin Zhai and Wenjian Liu
Physical Chemistry Chemical Physics 2014 vol. 16(Issue 35) pp:18729-18735
Publication Date(Web):24 Jul 2014
DOI:10.1039/C4CP01905A
The application of room-temperature ionic liquids (RTILs) in nuclear spent fuel recycling requires a comprehensive knowledge of radiation effects on RTILs. Although preliminary studies indicate a relatively high radiation stability of RTILs, little attention is paid to the color change of RTILs, an obvious phenomenon of RTILs during irradiation. In this paper, we have investigated radiation-induced darkening and decoloration of 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BMIm][NTf2]), an ionic liquid representing the most popular class of RTILs, by means of UV-Vis analysis and time-dependent density functional theory calculations. Based on the experimental and computational results, it is proposed that the color change of [BMIm][NTf2] upon irradiation originates from the formation of double bonds in the aliphatic chains of pristine organic cations (or radiolytic products of RTILs) and various associated species containing these “double-bond products”. This work sheds light on the understanding of the radiation-induced color change of RTILs.
Co-reporter:Yinyong Ao, Hanyang Zhou, Weijin Yuan, Shuojue Wang, Jing Peng, Maolin Zhai, Jianyong Wang, Ziqiang Zhao, Long Zhao and Yuezhou Wei
Dalton Transactions 2014 vol. 43(Issue 14) pp:5580-5585
Publication Date(Web):13 Jan 2014
DOI:10.1039/C3DT53297F
Helium ion (He+) beam produced by a heavy ion linear accelerator was used to simulate α-rays for studying the radiation effect on 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ionic liquid ([C4mim][NTf2]). The water-soluble radiolytic products of [C4mim][NTf2] under He+ beam irradiation were analysed, and it was found that they were similar to those by γ-ray irradiation, but their amount was much less than that by γ-ray irradiation, which was attributed to the recombination of [C4mim][NTf2] radical cations in track by high linear energy transfer (LET) radiations of the He+ beam. The extracting behaviour of Dy3+ using irradiated [C4mim][NTf2] in combination with alkylated bis-triazinyl-pyridine (CA-BTP) was assessed, and found that the influence of He+ beam on the extraction was less than that of γ-ray irradiation. In addition, radiolytic products have a different influence on Dy3+ extraction at different doses; Dy3+ partitioning decreases at 50 kGy due to the protonation of CA-BTP and the inhibition of cation exchange mechanism by radiation-formed hydrogen ions. The abnormal increase of Dy3+ partitioning at 100 kGy is mainly attributed to the precipitation formed between Dy3+ and radiolytic products (F− and SO32−).
Co-reporter:Weijin Yuan, Yinyong Ao, Long Zhao, Maolin Zhai, Jing Peng, Jiuqiang Li and Yuezhou Wei
RSC Advances 2014 vol. 4(Issue 93) pp:51330-51333
Publication Date(Web):02 Oct 2014
DOI:10.1039/C4RA08308C
Approaches were established for assessing the influence of radiation effect on the extractability of the 2,6-di(5,6-diisobutyl-1,2,4-triazin-3-yl)pyridine (isobutyl-BTP)/1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([C2mim][NTf2]) extraction system. The substituted compounds formed between isobutyl-BTP and radicals of [C2mim][NTf2], especially imidazolium cation radicals, were responsible for maintaining the partial extraction ability for Dy3+ even at 500 kGy.
Co-reporter:Cancan Li;Guojie Wang;Hongyi Gao;Jiuqiang Li
Journal of Applied Polymer Science 2014 Volume 131( Issue 6) pp:
Publication Date(Web):
DOI:10.1002/app.39998
ABSTRACT
Poly(dimethylaminoethyl methacrylate) hydrogels containing cholic acid (PDMAEMA–CA) were synthesized by radiation crosslinking. The introduction of 10 and 20 mol% cholic acid (CA) into the poly(dimethylaminoethyl methacrylate) (PDMAEMA) hydrogel decreased the maximum swelling ratio (SR) of the gel from 40 to 6 and 5, respectively. The incorporation of CA with dimethylaminoethyl methacrylate led to a decrease in the lower critical swelling temperature of the gel from 44 to 42°C but did not exert big influence on the ion-stimulus-responsive properties of the gel. However, the pH sensitivity of the PDMAEMA–CA gel was quite different from that of PDMAEMA gel. The SR of PDMAEMA gel decreased at pH 2.5, whereas the SRs of the PDMAEMA–CA gels showed a convex-upward function of pH; that is, SR of the PDMAEMA–10% CA gel first increased (pH 1.2–3.2) and then decreased (pH 3.2–11.9) with increasing pH. The pH-stimulus-responsive swelling behavior of the PDMAEMA–20% CA gel was similar to that of the PDMAEMA–10% CA gel except for the unique swelling behavior exhibited in the lower pH region. The unique decrease in SR in strong acidic solutions was attributed to aggregations driven by the hydrophobic interactions between CA molecules. Phase separation of the gel in strongly acidic solutions was observed; that is, the margin of the swollen gel was transparent and elastic (cellular structure), whereas the core of it was opaque (aggregated structure) as recorded by scanning electron microscopy. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2014, 131, 39998.
Co-reporter:Xiaosheng Cai;Qilu Zhang;Shuojue Wang;Jing Peng
Journal of Materials Science 2014 Volume 49( Issue 16) pp:5667-5675
Publication Date(Web):2014 August
DOI:10.1007/s10853-014-8286-0
A series of graphene materials are prepared by intercalation of graphene oxide (GO) with different surfactants, cetyltrimethylammonium bromide (CTAB), n-octyltrimethylammonium bromide, tetramethylammonium bromide, and sodium dodecylbenzene sulfonate, subsequently by γ-ray induced reduction in N-methyl-2-pyrrolidone (NMP) at room temperature. GO can be reduced by the electrons generated from the radiolysis of NMP under γ-ray irradiation, and reduced GO is simultaneously functionalized by the radiolytic product of NMP. Cationic surfactant CTAB with longer alkyl chains can effectively promote the reduction process of GO by preventing the aggregation of graphene sheets, which has been testified by X-ray photoelectron spectroscopy, X-ray diffraction, thermogravimetric analysis, Raman spectroscopy, and Fourier transform infrared spectroscopy analyses. Furthermore, when the as-prepared graphene/polyaniline composites are used for supercapacitor electrode materials, there is a highest specific capacitance of 484 F g−1 at a current density of 0.1 A g−1 for the graphene produced in the presence of cationic surfactant CTAB.
Co-reporter:Qilu Zhang, Youwei Zhang, Zhaohui Gao, Hui-Ling Ma, Shuojue Wang, Jing Peng, Jiuqiang Li and Maolin Zhai
Journal of Materials Chemistry A 2013 vol. 1(Issue 2) pp:321-328
Publication Date(Web):16 Oct 2012
DOI:10.1039/C2TC00078D
A facile method has been developed to synthesize a high-quality platinum nanoparticle (PtNP) decorated graphene via one-step γ-ray induced reduction of graphite oxide (GO) and chloroplatinic acid at room temperature. GO and Pt(IV) precursor salt could be co-reduced by the electrons generated from the radiolysis of ethylene glycol under γ-ray irradiation. The synchronous reduction of the metal precursor and regulation of pH greatly increased the ratio of C/O in the reduced GO (RGO). PtNPs with an average diameter of 1.8 nm were uniformly dispersed on the surface of RGO sheets. The as-prepared PtNP–RGO composites as supercapacitor electrodes displayed a specific capacitance of 154 F g−1 at a current density of 0.1 A g−1 and the value retained as high as 72.3% at 20 A g−1 which was significantly enhanced compared to 16.2% capacity retention of RGO prepared by the same method. The investigation of electrochemical performances suggests that PtNPs play an important role in enhancing supercapacitor performance with high rate capability by accelerating the electron transfer and increasing the electrochemical active surface area of RGO.
Co-reporter:Shuojue Wang, Youwei Zhang, Hui-Ling Ma, Qilu Zhang, Weigao Xu, Jing Peng, Jiuqiang Li, Zhong-Zhen Yu, Maolin Zhai
Carbon 2013 Volume 55() pp:245-252
Publication Date(Web):April 2013
DOI:10.1016/j.carbon.2012.12.033
A simple and environmentally friendly approach for the preparation of graphene nanosheets decorated with silver nanoparticles (Ag NPs) has been developed by gamma irradiation at room temperature. Graphene oxide (GO) and silver ions are simultaneously reduced by the electrons generated from the radiolysis of solvent. The addition of ionic liquid plays an important role in GO reduction by scavenging oxidative radicals generated during irradiation. Besides, the ionic liquid also benefits the dispersion and size distribution of Ag NPs. Raman signals of the obtained Ag-reduced graphene oxide are significantly enhanced, exhibiting obvious surface-enhanced Raman scattering activity.
Co-reporter:Yinyong Ao, Jing Peng, Liyong Yuan, Zhenpeng Cui, Cheng Li, Jiuqiang Li and Maolin Zhai
Dalton Transactions 2013 vol. 42(Issue 12) pp:4299-4305
Publication Date(Web):20 Dec 2012
DOI:10.1039/C2DT32418K
The trace water-soluble radiolytic products of neat 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C4mim][NTf2]) were identified by analysing water-washed samples of γ-ray irradiated ionic liquids. CF3SO2OH, CF3SOOH, CF3SO2NH2, HF and H2SO3 were confirmed as main radiolytic products of [C4mim][NTf2], and the total radiation chemical yields of the water-soluble radiolytic products (0.35 μmol J−1) and that of hydrogen ions (0.46 ± 0.02 μmol J−1) were determined by using ion chromatography and neutralization titration, respectively. It was found that the water-soluble radiolytic products of [C4mim][NTf2] greatly reduced the extraction efficiency of Sr2+ from water to irradiated [C4mim][NTf2], while the water-insoluble radiolytic products of [C4mim][NTf2] had a slight influence on the Sr2+ extraction.
Co-reporter:Jun Ma, Shuojue Wang, Jing Peng, Jie Yuan, Chuhong Yu, Jiuqiang Li, Xuecheng Ju, Maolin Zhai
European Polymer Journal 2013 Volume 49(Issue 7) pp:1832-1840
Publication Date(Web):July 2013
DOI:10.1016/j.eurpolymj.2013.04.010
•Covalently functionalized Nafion membranes were prepared by gamma irradiation.•A cationic charged polymer layer was grown on the surface of Nafion membrane.•The obtained membranes largely reduced vanadium ion crossover for VRFB.Nafion membrane has been covalently functionalized with a cationic charged layer synthesized by radiation-induced graft copolymerization of N,N-dimethylaminoethylmethacrylate (DMAEMA) into Nafion substrate and subsequent protonation to reduce vanadium ion crossover for the application in vanadium redox flow battery (VRFB). The chemical composition and structure of the modified Nafion were characterized by microscopic Fourier transform infrared spectroscopy and thermogravimetric analysis. The grafting behavior was monitored by changing the experimental parameters including dose, dose rate and monomer concentration. The growth of cationic charged layer was studied by surface composition analysis of the membranes using X-ray photoelectron spectroscopy and atomic force microscope. The conductivity and permeability of vanadium ions of the obtained membranes with varying grafting yields were also measured. The functionalized Nafion membrane with a barrier layers displayed substantial resistance to permeability of vanadium ions accompanied by a relatively lower conductivity in comparison to that of the pristine Nafion membrane. The selectivity of the protonated Nafion-g-PDMAEMA membranes was higher than that of Nafion membrane, indicating the strategy is suitable for modifying Nafion membrane aiming at VRFB system. This work paves the way for the development of a new class of Nafion-based membranes for the application of VRFB.Graphical abstract
Co-reporter:Zhen Dong;Qilu Zhang;Chuhong Yu;Jing Peng;Jun Ma;Xuecheng Ju
Ionics 2013 Volume 19( Issue 11) pp:1587-1593
Publication Date(Web):2013 November
DOI:10.1007/s11581-013-0905-2
Poly(vinylidene fluoride)-based polymer electrolytes using ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsufonyl)imide as the plasticizer were prepared by solution casting method. The effects of the solvent evaporation temperature (SET) and ionic liquid content (ILC) on the properties and structures of the polymer electrolytes were investigated by characterization of scanning electron microscope (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry, as well as mechanical and ionic conductivity test. It was confirmed that both SET and ILC had significant influence on the morphology, degree of crystallinity, mechanical properties, and ionic conductivity of the prepared polymer electrolytes. With ILC of 40 %, an excellent polymer electrolyte can be obtained at SET of 60 °C, which exhibited ionic conductivity up to ca. 10−4 S/cm at room temperature, accompanied by excellent tensile strength of 22.8 MPa and elongation at break of 540 %.
Co-reporter:Youwei Zhang;Hui-Ling Ma;Jing Peng
Journal of Materials Science 2013 Volume 48( Issue 5) pp:1883-1889
Publication Date(Web):2013 March
DOI:10.1007/s10853-012-6951-8
Chemically reduced and functionalized graphene oxide (GO) was prepared by refluxing of GO with ethylenediamine (ED) using dimethyl formamide (DMF) as solvent. It was confirmed that both ED and DMF contributed to the reduction and functionalization of GO. The resulting adsorbent (ED–DMF–RGO) with amine groups was highly efficient in removing Cr(VI) from its aqueous solution and could be easily separated by filtration. The optimum pH for total Cr removal was observed at pH 2.0 and the Cr(VI) removal capacity of ED–DMF–RGO at this pH was 92.15 mg g−1, which was about 27 times higher than that of activated carbon, even nearly 4–8 times higher than that of various modified activated carbons. The presence of other ions such as Na+, K+, Ca2+, Cl−, and Br− had little effect on the removal of Cr(VI). Interestingly, Cr(VI) was reduced to low-toxic Cr(III) during the adsorption process, which followed an indirect reduction mechanism. Both the Cr(VI) adsorption and subsequent reduction of adsorbed Cr(VI) to Cr(III) contributed to the Cr(VI) removal. The obtained ED–DMF–RGO may be applicable in Cr(VI) removal if they are produced on a large scale and at low price in near future.
Co-reporter:YinYong Ao;Jing Peng;YouWei Zhang;LiYong Yuan;ChuHong Yu
Science Bulletin 2013 Volume 58( Issue 14) pp:1663-1669
Publication Date(Web):2013 May
DOI:10.1007/s11434-013-5667-8
Bis(2-propyloxy)calix[4]crown-6 (BPC6) is an effective separation agent for cesium removing from spent nuclear fuel. The study on radiolytic behavior of BPC6 itself under γ-irradiation was required for evaluating its feasibility of practical application. It was found that BPC6 exhibited excellent radiation stability at dose less than 100 kGy. However, the isopropyl groups in BPC6 underwent oxidation and dealkylation to form carbonyl groups and phenolic hydroxyl groups at dose above 300 kGy, respectively. When the dose was more than 1000 kGy, the ring opening of crown ether structure of BPC6 resulted in the formation of phenolic hydroxyl groups as well. The formation of radiolytic products containing phenolic hydroxyl groups during the irradiation of BPC was confirmed by using FeCl3 as a probe. Combining with the radiolytic behavior of two model chemicals (1-isopropoxybenzene and benzo-18-crown-6 ether), the radiolytic behavior and mechanism of BPC6 under γ-irradiation was testified further.
Co-reporter:Jie Yuan;Chuhong Yu;Jing Peng;Yu Wang;Jun Ma;Jingyi Qiu;Jiuqiang Li
Journal of Polymer Science Part A: Polymer Chemistry 2013 Volume 51( Issue 24) pp:5194-5202
Publication Date(Web):
DOI:10.1002/pola.26949
ABSTRACT
Sodium styrene sulfonate (SSS) and N,N-dimethylaminoethyl methacrylate (DMAEMA) are grafted into poly(vinylidene difluoride) (PVDF) film using γ-radiation techniques. SSS could be co-grafted successfully with DMAEMA, although it is difficult to be grafted solely into PVDF films. Through subsequent protonation process, an amphoteric ion exchange membrane (AIEM) is synthesized facilely and environmentally benignly. The degree of grafting (DOG) increases with absorbed dose and levels off at 40 kGy. Micro-FTIR and X-ray photoelectron spectroscopy analyses confirm the existence of the designed units and quaternization of DMAEMA units in the grafted films. The quaternization and grafting occurring at the same time makes it a unique way to synthesize quaternized AIEM in one step. Finally, an AIEM with a DOG of 43% is assembled in the vanadium redox flow battery (VRFB) system, and the VRFB maintains an open circuit voltage higher than 1.4 V after placed for 85 h, which is much longer than that with Nafion117 membrane. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 5194–5202
Co-reporter:Youwei Zhang, Hui-Ling Ma, Qilu Zhang, Jing Peng, Jiuqiang Li, Maolin Zhai and Zhong-Zhen Yu
Journal of Materials Chemistry A 2012 vol. 22(Issue 26) pp:13064-13069
Publication Date(Web):10 May 2012
DOI:10.1039/C2JM32231E
We demonstrate a facile and environmentally friendly approach to prepare well-dispersed graphene sheets by γ-ray induced reduction of a graphene oxide (GO) suspension in N,N-dimethyl formamide (DMF) at room temperature. GO is reduced by the electrons generated from the radiolysis of DMF under γ-ray irradiation. The reduced GO by γ-ray irradiation (G-RGO) can be re-dispersed in many organic solvents, and the resulting suspensions are stable for two weeks due to the stabilization of N(CH3)2+ groups on G-RGO. Additionally, G-RGO is efficient in improving the conductivity of polystyrene (PS). Its PS nanocomposites exhibit a sharp transition from electrically insulating to conducting with a low percolation threshold of 0.24 vol% and a high electrical conductivity of 45 S m−1 is obtained with only 2.3 vol% of G-RGO. The superior electrical conductivity is attributed to the uniform dispersion of the G-RGO sheets in the PS matrix.
Co-reporter:Hui-Ling Ma, Youwei Zhang, Qi-Hui Hu, Dong Yan, Zhong-Zhen Yu and Maolin Zhai
Journal of Materials Chemistry A 2012 vol. 22(Issue 13) pp:5914-5916
Publication Date(Web):22 Feb 2012
DOI:10.1039/C2JM00145D
Ethylenediamine-reduced graphene oxide (ED-RGO) sheets were prepared by simple refluxing of graphene oxide (GO) solution with ethylenediamine (ED), which effectively reduced toxic Cr(VI) to less toxic Cr(III) by an indirect reduction mechanism with the assistance of π electrons on the carbocyclic six-membered ring of ED-RGO.
Co-reporter:Guowen Hu, Yu Wang, Jun Ma, Jingyi Qiu, Jing Peng, Jiuqiang Li, Maolin Zhai
Journal of Membrane Science 2012 Volumes 407–408() pp:184-192
Publication Date(Web):15 July 2012
DOI:10.1016/j.memsci.2012.03.042
A novel amphoteric ion exchange membrane (AIEM) was synthesized by radiation-induced grafting α-methyl styrene (AMS) and dimethylaminoethyl methacrylate (DMAEMA) into poly(vinylidenedifluoride) (PVDF) films, followed by sulfonation and protonation processes. The monomer AMS could be co-grafted successfully with DMAEMA in the presence of AlCl3 although it was difficult for AMS to be grafted solely into PVDF films. The grafting yield (GY) increased with absorbed dose up to about 40 kGy. It was found that the ratio of DMAEMA to AMS in the poly(DMAEMA-co-AMS) grafts changed slightly with various monomer ratio of DMAEMA to AMS in the feed by elemental analysis. The Micro-FTIR and XPS analyzes testified that the AIEM had been prepared as designed. The AIEM with a GY of 40% showed similar conductivity, higher IEC and lower permeability of vanadium ions compared with Nafion117 membrane. The vanadium redox flow battery (VRFB) assembled with the AIEM of 41.1% GY maintained an open circuit voltage higher than 1.4 V after placed for 60 h, which was much longer than that with the Nafion117 membrane. Therefore, it is expected to be excellent candidate for the application of VRFB.Highlights► AMS can be co-grafted into PVDF film with DMAEMA in the presence of AlCl3. ► The AIEM had a permeability of vanadium ions 10 times lower than that of Nafion117. ► The chemical stability of the AIEM showed better when St was substituted by AMS. ► The OCV of VRFB with the AIEM showed better performance than that with Nafion117.
Co-reporter:Youwei Zhang, Ling Xu, Long Zhao, Jing Peng, Cancan Li, Jiuqiang Li, Maolin Zhai
Carbohydrate Polymers 2012 Volume 88(Issue 3) pp:931-938
Publication Date(Web):15 April 2012
DOI:10.1016/j.carbpol.2012.01.040
A novel cellulose-based adsorbent was prepared by radiation-induced grafting of styrene onto the surface of cellulose microspheres, followed by acetylation and amination processes. The grafting yield was adjusted by the total absorbed dose, dose rate and the concentration of styrene. The structure of the adsorbent was characterized by micro-FTIR, XPS and SEM. The adsorption of Cr(VI) ions has been investigated as a function of contact time, adsorbent feed, pH, Cr(VI) and NaCl concentration. It was found that adsorption equilibrium could be achieved within 30 min for initial Cr(VI) of 100 mg L−1. The adsorption kinetics was well described by the pseudo-second order model equation, and the adsorption isotherm was better fitted by the Langmuir mode. The maximum theoretical Cr(VI) uptake of the adsorbent was 123.4 mg g−1. The influence of NaCl concentration on Cr(VI) uptake and XPS analysis revealed that Cr(VI) ions were adsorbed through ion-exchange mechanism.Highlights► A novel cellulose-based adsorbent was prepared by radiation technique. ► The adsorbent possesses complex and porous surface texture in acidic solution. ► The adsorption equilibrium of Cr(VI) could be achieved within 30 min. ► Cr(VI) adsorption followed pseudo-second order mode through ion-exchange mechanism. ► The maximum theoretical Cr(VI) uptake was 123.4 mg g−1 based on Langmuir isotherm.
Co-reporter:Qilu Zhang, Maolin Zhai, Jing Peng, Yan Hao, Jiuqiang Li
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms 2012 Volume 286() pp:334-340
Publication Date(Web):1 September 2012
DOI:10.1016/j.nimb.2012.01.005
Carboxymethylated chitosan (CMCts) protected ruthenium nanoparticles (RuNPs) were synthesized by γ-radiation-induced reduction of metal ions at room temperature. The characteristics of RuNPs/CMCts composites prepared under different experimental conditions have been investigated by means of TEM, XPS and TGA. The results indicated that the average size of RuNPs increases as the concentration of precursor decreases. Narrowly distributed nanocomposites have been obtained when low molecular weight CMCts (LM-CMCts, Mn = 4400 Da) was utilized as stabilizer. The TEM images demonstrated the RuNPs prepared in a wide pH range of 4.5–12.3 can be dispersed uniformly in the alkalic CMCts solution for more than 2 months with the average particle sizes of 1.0–3.0 nm. XPS spectrum confirmed the ruthenium ions have been reduced to metal atoms by irradiation. TGA curves indicated that RuNPs/CMCts composites exhibited good thermal stability at temperature less than 200 °C and strong interactions existed between the metal nanoparticles and stabilizer molecules.Highlights► Biocompatible RuNPs were successfully produced by γ-irradiation for the first time. ► RuNPs in a pH range of 4.5–12.3 dispersed uniformly with the sizes of 1.0–3.0 nm. ► Narrowly distributed RuNPs have been obtained when LM-CMCts was used as stabilizer. ► TGA curves suggested the carboxymethyl group in CMCts can stabilize RuNPs.
Co-reporter:Jun Ma, Yu Wang, Jing Peng, Jingyi Qiu, Ling Xu, Jiuqiang Li, Maolin Zhai
Journal of Membrane Science 2012 s 419–420() pp: 1-8
Publication Date(Web):
DOI:10.1016/j.memsci.2012.04.034
Co-reporter:Cancan Li;Ling Xu;Jing Peng;Jiuqiang Li
Journal of Applied Polymer Science 2011 Volume 120( Issue 4) pp:2027-2033
Publication Date(Web):
DOI:10.1002/app.33328
Abstract
An overshooting effect was observed during the swelling procedure of poly(dimethylaminoethyl methacrylate) (PDMAEMA) gel for the first time. The effects of the temperature, ionic strength, and pH on the overshooting effect of the PDMAEMA gel were investigated. We found that the overshooting effect of the gel could not be eliminated by changing the temperature; however, the overshooting effect was indiscernible in high-concentration NaCl solutions (>0.2 mol/L) and basic (pH 11.9) and acidic solutions (pH = 2.1). The overshooting effect of the PDMAEMA gel was attributed to the dynamic conformational changes of the side chains of dimethylaminoethyl methacrylate (DMAEMA) units during the swelling of the gels. In the presence of NaCl or NaOH, the stretching of the macromolecular chains of the gels was disrupted. While in acidic solution, the protonation of tertiary amino groups in the DMAEMA units made the side chains of the DMAEMA units change from the cyclic conformation to the stretched one; this was analyzed with the aid of Fourier transform infrared spectroscopy. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011
Co-reporter:Yu Wang, Jingyi Qiu, Jing Peng, Ling Xu, Jiuqiang Li, Maolin Zhai
Journal of Membrane Science 2011 376(1–2) pp: 70-77
Publication Date(Web):
DOI:10.1016/j.memsci.2011.04.002
Co-reporter:Chao Xu, Liyong Yuan, Xinghai Shen and Maolin Zhai
Dalton Transactions 2010 vol. 39(Issue 16) pp:3897-3902
Publication Date(Web):17 Mar 2010
DOI:10.1039/B925594J
The removal of radioactive 137Cs from nuclear waste is of great importance for both the environment and energy saving. Herein, we report a study on the removal of Cs+ using a calix crown ether bis(2-propyloxy)calix[4]crown-6 (BPC6) in ionic liquids [Cnmim][NTf2], where [Cnmim]+ is 1-alkyl-3-methylimidazolium and [NTf2]− is bis(trifluoromethylsulfonyl)imide. The BPC6/[Cnmim][NTf2] system is highly efficient in removing Cs+ from aqueous solution, even at a low concentration of BPC6. HNO3 and metal ions such as Na+, Al3+ in the aqueous phase interfered with the extraction of Cs+ by competitive interaction with BPC6 and/or salting-out effect. UV analysis confirmed that the extraction of Cs+ by the BPC6/[Cnmim][NTf2] system involves a dual extraction mechanism, i.e., via exchange of BPC6·Cs+ complex or Cs+ by [Cnmim]+. Irradiation of [C4mim][NTf2] dramatically decreases Cs+ partitioning in the ionic liquid phase by the competitive interaction of radiation-generated H+ with BPC6, while irradiation of BPC6/[C4mim][NTf2] decreases Cs+ partitioning more markedly due to the radiolysis of BPC6.
Co-reporter:Min Wang, Ling Xu, Cancan Li, Zhiying Yue, Maolin Zhai, Jiuqiang Li
Colloids and Surfaces A: Physicochemical and Engineering Aspects 2010 Volume 356(1–3) pp:89-96
Publication Date(Web):5 March 2010
DOI:10.1016/j.colsurfa.2009.12.033
Hydroxypropyl methylcellulose phthalate (HPMCP) gel was synthesized from the sodium form of HPMCP by radiation-induced crosslinking, followed by converting the phthalate groups on HPMCP to non-ionic forms via ion exchange. The non-ionic H-type gels showed different phase transition behaviors from Na-type gels. Significant antipolyelectrolyte swelling behavior of this amphiphilic gel was observed in various aqueous salt solutions, comparing with the polyelectrolyte swelling behavior of ionic HPMCP gels. After immersed in aqueous salt solution, the morphology of H-type HPMCP gels changed from heterogeneous structure to homogeneous structure. The swelling behavior of the gels in several circumstances with potential applications, for instance, solutions with different temperature and pH, surfactants, and typical drug models, were investigated. H-type HPMCP gels showed similar temperature and pH-stimuli responses to that of Na-type HPMCP gels. Furthermore, H-type HPMCP gels showed different swelling behaviors in cationic surfactant (C12TAB) and anionic surfactant (SDS) solutions. The investigations regarding drug embedment and release of this amphiphilic gel in inorganic salt and BSA solutions revealed that the embedment amount and release ratio were both high due to the improved swelling ability in saline condition of H-type HPMCP gels.
Co-reporter:Jingyi Qiu, Junzhi Zhang, Jinhua Chen, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li, Genshuan Wei
Journal of Membrane Science 2009 Volume 334(1–2) pp:9-15
Publication Date(Web):15 May 2009
DOI:10.1016/j.memsci.2009.02.009
Poly(vinylidene difluoride) (PVDF) film was grafted with styrene (St) and dimethylaminoethyl methacrylate (DMAEMA) using γ-irradiation techniques. Through subsequent sulfonation and protonation processes, a new kind of amphoteric ion exchange membrane (AIEM) was synthesized. The grafting yield (GY) increased with absorbed dose and leveled off at about 60 kGy. The composition of poly(St-co-DMAEMA) grafts was correlated to the ratio of St to DMAEMA monomer in the feed. Micro-FTIR and XPS analyses testified that the grafting and sulfonation of St unit in poly(St-co-DMAEMA) grafts had been carried out as designed. Further characterizations showed that the properties of the AIEM strongly depended on the composition and GY of the film, i.e. higher content of DMAEMA brought lower permeability of vanadium ions and conductivity, while higher GY led to higher water uptake, ion exchange capacity (IEC) and conductivity. Finally, an AIEM with a GY of 26.1% was assembled and tested in the vanadium redox flow battery (VRFB) system. It was found that the VRFB assembled with the AIEM maintained an open circuit voltage (OCV) higher than 1.2 V after placed for 68 h, which was much longer than that with the Nafion117 membrane. Therefore, this work provides a novel method to develop potential substitute of Nafion membranes to be applied in VRFB system.
Co-reporter:Jingyi Qiu, Maolin Zhai, Jinhua Chen, Yu Wang, Jing Peng, Ling Xu, Jiuqiang Li, Genshuan Wei
Journal of Membrane Science 2009 Volume 342(1–2) pp:215-220
Publication Date(Web):15 October 2009
DOI:10.1016/j.memsci.2009.06.043
A novel ETFE-based amphoteric ion exchange membrane (AIEM) was prepared through a two-step radiation-induced grafting technique. ETFE film was first grafted with styrene (St) (denoted as ETFE-g-PS), followed with a sulfonation treatment to obtain a cation exchange membrane (ETFE-g-PSSA). The ETFE-g-PSSA membrane was subsequently grafted with dimethylaminoethyl methacrylate (DMAEMA) and then protonated, resulting in an AIEM with both anionic and cationic groups. The grafting yields (GY) in the above two steps increased with absorbed dose and leveled off at about 30 kGy and 20 kGy, respectively. Micro-FTIR and XPS analyses testified that the AIEM had been prepared as designed. The obtained AIEM exhibited high ion exchange capacity (IEC) and conductivity, as well as significantly reduced permeability of vanadium ions. Vanadium redox flow battery (VRFB) assembled with the AIEM maintained an open circuit voltage (OCV) higher than 1.3 V after placed for 300 h, and exhibited higher columbic efficiency and energy efficiency than that with Nafion 117 membrane.
Co-reporter:Yan Hao, Jing Peng, Jiuqiang Li, Maolin Zhai, Genshuan Wei
Carbohydrate Polymers 2009 Volume 77(Issue 4) pp:779-784
Publication Date(Web):19 July 2009
DOI:10.1016/j.carbpol.2009.02.025
This paper reports a homogeneous modification of microcrystalline cellulose (MCC) in ionic liquids via radiation-induced grafting. Thermosensitive poly (N-isopropylacrylamide) (PNIPAAm) was successfully grafted onto MCC in 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) ionic liquid using γ-ray irradiation technique at room temperature. The grafting yield (GY) increased with dose up to 40 kGy, while decreased slightly with dose rate from 22 to 102 Gy/min. The results of TGA indicated that cellulose grafted PNIPAAm (cellulose-g-PNIPAAm) had higher thermal stability than that of ungrafted regenerated cellulose (reg-cellulose). The crystalline structure of original MCC was largely destroyed during the dissolution process according to the XRD profiles, and grafting PNIPAAm onto cellulose further decreased the intensity of crystallinity. SEM showed that reg-cellulose and cellulose-g-PNIPAAm films displayed dense and homogeneous morphology. Moreover, the resulting cellulose-g-PNIPAAm exhibited obvious thermal sensitivity with a lower critical solution temperature around 35 °C, which was observed from the swelling behavior in water at different temperatures.
Co-reporter:Liyong Yuan, Chao Xu, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li, Genshuan Wei and Xinghai Shen
Dalton Transactions 2009 (Issue 38) pp:7873-7875
Publication Date(Web):04 Aug 2009
DOI:10.1039/B911026G
SO32− is identified as one of the radiolytic products of the ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C4mim][NTf2]) during the removal of strontium ions (Sr2+) from aqueous solution.
Co-reporter:Maolin Zhai, Jinhua Chen, Shin Hasegawa, Dengrong Li, Hiroyuki Oku, Yasunari Maekawa
European Polymer Journal 2009 Volume 45(Issue 6) pp:1668-1673
Publication Date(Web):June 2009
DOI:10.1016/j.eurpolymj.2009.03.008
A perfluorinated vinyl ether monomer, 2-bromotetrafluoroethyl trifluorovinyl ether (BrTFF) was grafted into crosslinked poly(tetrafluoroethylene) (cPTFE) films by γ-rays irradiation under different conditions. The irradiation with absorbed doses more than 550 kGy gave the poly(BrTFF) grafted cPTFE membranes with grafting yields of more than 20%. FTIR spectra and SEM–EDS testified that BrTFF was successfully grafted into cPTFE films homogeneously in the film perpendicular direction. TGA analysis of the grafted films indicated that the perfluorinated poly(BrTFF) grafts were phase-separated from the PTFE region due to the crosslinked structure of the cPTFE based film, but the grafted films still had high thermal stability (above 300 °C). DSC measurements showed the decrease of melting temperature, but the increase of both heat of fusion and degree of crystallinity in cPTFE film after grafting. The grafted film, a new kind of perfluorinated polymer with bromine active groups and good mechanical properties, is expected to be modified for new applications.
Co-reporter:Ling Xu, Xin Li, Liyong Yuan, Maolin Zhai, Jing Peng, Jiuqiang Li
Journal of Fluorine Chemistry 2009 Volume 130(Issue 10) pp:959-965
Publication Date(Web):October 2009
DOI:10.1016/j.jfluchem.2009.07.014
Most of the hydrogels deswell more remarkably in F− containing solutions than in other monovalent anion containing solutions. However, significant deswelling followed by abnormal reswelling of polymer gel in KF solutions with increasing F− concentration was observed in a series of polymer gels consisted of phenyl rings, for instance, poly(styrene sulfonic acid) (PSSA), hydroxypropyl methylcellulose phthalate (HPMCP) and poly(4-vinyl phenol) (P4VPh) gel. Driving force of this phenomenon was studied to reveal the specific interactions involved in the aqueous systems of aromatic polymers. Elemental analysis and XPS results suggest that F− is embedded to the gel by the physical adsorption of KF, as well as the interactions between phenyl ring and F−. Further theoretical calculations revealed that the interaction may be (phenyl)CH⋯F−(H2O)n interaction, which is stronger than (phenyl)CH⋯(H2O)n hydrogen bond. This kind of interaction decreases with the increasing water number and it is invalid when the surrounding water number is more than 5 for the phenol–F−(H2O)n system. Therefore, we conclude that F− could bind to phenyl ring via such (phenyl)CH⋯F−(H2O)n interaction in solutions with low hydrophilicity. The strong polarization effect of F− and (phenyl)CH⋯F−(H2O)n interaction are two important driving forces for the reswelling of gels.The mechanism for the abnormal reswelling of some aromatic polymer gels in concentrated KF solutions was elucidated by swelling study, elemental analysis, XPS and computational methods. The strong polarization effect of F− and (phenyl)CH⋯F−(H2O)n interaction are two important ingredients for the reswelling of gels.
Co-reporter:Liyong Yuan, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li and Genshuan Wei
The Journal of Physical Chemistry B 2009 Volume 113(Issue 26) pp:8948-8952
Publication Date(Web):June 1, 2009
DOI:10.1021/jp9016079
The applications of room-temperature ionic liquids (RTILs) in separation of high level radioactive nuclides demand a comprehensive knowledge of the stability and metal ion extraction of RTILs under radiation. Herein, we assessed the influence of γ-irradiation on the [C4mim][NTf2]-based extraction system, where [C4mim]+ is 1-butyl-3-methylimidazolium and [NTf2]− is bis(trifluoromethylsulfonyl)imide, by solvent extraction of Sr2+ using irradiated [C4mim][NTf2] in combination with dicyclohexyl-18-crown-6 (DCH18C6). It was found that the degree of extraction for Sr2+ from water to irradiated [C4mim][NTf2] decreased compared with that to unirradiated [C4mim][NTf2], and the decrement enhanced obviously with increasing dose. NMR spectroscopic probe analysis revealed the formation of acids during irradiation of [C4mim][NTf2]. The decrease of Sr2+ partitioning in irradiated [C4mim][NTf2] is attributed to the competition between H+ with Sr2+ to interact with DCH18C6. Accordingly, washing irradiated [C4mim][NTf2] with water gives a simple way of ionic liquid recycling. Furthermore, the degree of extraction for Sr2+ from 3 mol·L−1 nitric acid solution to [C4mim][NTf2] is independent of the irradiation of [C4mim][NTf2] since the amount of the radiation-generated H+ is negligible in such a high acidic solution.
Co-reporter:Maolin Zhai, Jinhua Chen, Shin Hasegawa, Yasunari Maekawa
Polymer 2009 50(5) pp: 1159-1165
Publication Date(Web):
DOI:10.1016/j.polymer.2009.01.014
Co-reporter:Cancan Li, Ling Xu, Maolin Zhai, Jing Peng, Chao Yang, Jiuqiang Li, Genshuan Wei
Polymer 2009 50(20) pp: 4888-4894
Publication Date(Web):
DOI:10.1016/j.polymer.2009.08.018
Co-reporter:Jingyi Qiu, Long Zhao, Maolin Zhai, Jiangfeng Ni, Henghui Zhou, Jing Peng, Jiuqiang Li, Genshuan Wei
Journal of Power Sources 2008 Volume 177(Issue 2) pp:617-623
Publication Date(Web):1 March 2008
DOI:10.1016/j.jpowsour.2007.11.089
A poly(vinylidene difluoride) (PVDF) membrane was grafted with styrene (St) and maleic anhydride (MAn) using an electron-beam-induced pre-irradiation grafting technique. The grafted membrane (PVDF-g-PS-co-PMAn) was then sulfonated and hydrolyzed to give an ion exchange membrane (denoted as PVDF-g-PSSA-co-PMAc) for vanadium redox flow batteries (VRB) use. Micro-FTIR analysis indicated that PVDF was successfully grafted and sulfonated at the above condition, and the membrane with a high grafting yield (GY) can be easily prepared in a St/MAn binary system at low dose due to a synergistic effect. The water uptake and ion exchange capacity (IEC) of the PVDF-g-PSSA-co-PMAc membrane increased with GY, so too did the conductivity. At a GY of 33.6%, the resulting PVDF-g-PSSA-co-PMAc membrane showed a much higher IEC and conductivity than a conventional Nafion117 membrane, and a much lower permeability of vanadium ions: ca. 1/11 to 1/16 of that through Nafion117. Open circuit voltage measurements showed that the VRB assembled with the PVDF-g-PSSA-co-PMAc membrane maintained values above 1.3 V after a period of 33 h, which was much longer than that with the Nafion117 membrane. It is expected that this work provides a new approach for the fabrication of ion exchange membranes for VRB.
Co-reporter:Min Wang, Ling Xu, Maolin Zhai, Jing Peng, Jiuqiang Li, Genshuan Wei
Carbohydrate Polymers 2008 Volume 74(Issue 3) pp:498-503
Publication Date(Web):4 November 2008
DOI:10.1016/j.carbpol.2008.04.008
The carboxymethylated chitosan (CMCts) hydrogels were synthesized by γ-ray radiation-induced crosslinking at paste-like state with the concentration of CMCts from 12% to 22%. The gel fraction firstly increased with adsorbed dose and leveled off at ca. 20 kGy. The diffusion behavior of water in CMCts gels was Fickian diffusion, and the swelling of CMCts gels was affected by pH and ionic strength. Preliminary crosslinking mechanism of CMCts with γ-ray irradiation was discussed based on the FTIR and sol-gel analysis. The adsorption kinetics study showed that the adsorption of Fe(III) ions onto CMCts gels was very fast (ca. 20 min) due to the coordination of Fe(III) ions with amino, hydroxyl and carboxyl groups of CMCts molecules. pH 4.7 was the optimum for the adsorption of Fe(III) ions onto CMCts gels. The maximum uptake of Fe(III) ions, based on Langmuir equation, was determined to be 18.5 mg/g gel.
Co-reporter:Liyong Yuan, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li and Genshuan Wei
Dalton Transactions 2008 (Issue 45) pp:6358-6360
Publication Date(Web):24 Sep 2008
DOI:10.1039/B811413G
The preliminary results presented here show that γ-irradiation of ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate ([C4mim][PF6]) markedly decreases Sr2+ partitioning in the crown ether/[C4mim][PF6] extraction phase due to the competition between radation-generated H+ and Sr2+ to interact with the crown ether, however, washing irradiated [C4mim][PF6] with water gives a simple way of recycling the ionic liquid.
Co-reporter:Min Wang, Ling Xu, Xuecheng Ju, Jing Peng, Maolin Zhai, Jiuqiang Li, Genshuan Wei
Polymer Degradation and Stability 2008 Volume 93(Issue 10) pp:1807-1813
Publication Date(Web):October 2008
DOI:10.1016/j.polymdegradstab.2008.07.013
Carboxymethylated chitosan (CMCt) hydrogels were synthesized by γ-ray radiation-induced crosslinking in the presence of acids or polyfunctional monomers. Compared with that of CMCt hydrogels synthesized without additives, the gel fraction was improved and the gelation dose was decreased obviously after incorporating acids or polyfunctional monomers into CMCt hydrogels. The diffusion behavior of water in the CMCt gels prepared at different conditions was Fickian diffusion, and the swelling of the CMCt gels displayed characteristic pH sensitivity, which was analyzed by fluorescence molecular probes. Preliminary mechanism of radiation-induced crosslinking of CMCt in the presence of acids or polyfunctional monomers was discussed based on the FTIR and sol–gel analysis. Furthermore, it was found that CMCt hydrogels were hydrodegradable with high temperature (>60 °C), and incorporating polyfunctional monomers into the CMCt hydrogels also could improve the thermal stability of the CMCt hydrogels obviously.
Co-reporter:Ling Xu;Ling Huang;Jing Peng;Jiuqiang Li ;Genshuan Wei
Journal of Polymer Science Part A: Polymer Chemistry 2008 Volume 46( Issue 2) pp:473-480
Publication Date(Web):
DOI:10.1002/pola.22398
Abstract
An amphiphilic electrolyte, methacryloxyethyl dimethyloctane ammonium bromide (MODAB), was synthesized by quaternization of dimethylaminoethyl methacrylate (DMAEMA) with 1-bromooctane. Then amphiphilic PMODAB gel was synthesized by radiation cross-linking with ethyleneglycol dimethacrylate as cross-linker. PMODAB gels possess distinguished different swelling behaviors with those of DMAEMA hydrogels: (1) Antipolyelectrolyte phenomenon was observed in NaCl solution, that is, a remarkable increment of equilibrium degree of swelling (EDS) in the low NaCl concentration region (10−4 to 10−3 mol L−1), followed by a significant decrease (10−3 to 0.2 mol L−1), and a collapsed state (>0.2 mol L−1); (2) Compared with PDMAEMA, PMODAB was a temperature-sensitive polymer which showed an upper critical solution temperature (UCST) behavior. The EDS of PMODAB gel dramatically increased at the UCST; (3) In the 0.2 mol L−1 NaCl solutions, PMODAB gel swelled more significantly in a basic condition (pH > 10) than that in an acidic condition. The special volume phase transition behavior of PMODAB gel is ascribed to the hydrophobic interaction between octyl groups and the formation of ion-cluster between tetra-alkyl ammonium cation and Br−, which lead to the aggregation of gel structure and could be affected by the composition and temperature of the surrounding solution. © 2007 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 473–480, 2008
Co-reporter:Ling Huang;Maolin L. Zhai;Dewu W. Long;Jing Peng
Journal of Nanoparticle Research 2008 Volume 10( Issue 7) pp:1193-1202
Publication Date(Web):2008 October
DOI:10.1007/s11051-007-9353-0
The silver nanoparticles (AgNPs) were synthesized in an alkalic aqueous solution of silver nitrate (AgNO3)/carboxymethylated chitosan (CMCTS) with ultraviolet (UV) light irradiation. CMCTS, a water-soluble and biocompatible chitosan derivative, served simultaneously as a reducing agent for silver cation and a stabilizing agent for AgNPs in this method. UV–vis spectra and transmission electron microscopy (TEM) images analyses showed that the pH of AgNO3/CMCTS aqueous solutions, the concentrations of AgNO3 and CMCTS can affect on the size, amount of synthesized AgNPs. Further by polarized optical microscopy it was found that the CMCTS with a high molecular weight leads to a branch-like AgNPs/CMCTS composite morphology. The diameter range of the AgNPs was 2–8 nm and they can be dispersed stably in the alkalic CMCTS solution for more than 6 months. XRD pattern indicated that the AgNPs has cubic crystal structure. The spectra of laser photolysis of AgNO3/CMCTS aqueous solutions identified the early reduction processes of silver cations (Ag+) by hydrated electron \((\hbox{e}_{\rm aq}^{-})\) formed by photoionization of CMCTS. The rate constant of corresponding reduction reaction was 5.0 × 109 M−1 s−1.
Co-reporter:Jingyi Qiu, Ling Xu, Jing Peng, Maolin Zhai, Long Zhao, Jiuqiang Li, Genshuan Wei
Carbohydrate Polymers 2007 Volume 70(Issue 2) pp:236-242
Publication Date(Web):20 September 2007
DOI:10.1016/j.carbpol.2007.04.001
Activated carbon (AC) was incorporated into carboxymethylcellulose (CMC) to form CMC/AC hybrid hydrogels with excellent elasticity and flexibility by radiation crosslinking. The effect of AC on the formation, properties and structure of CMC/AC hybrid hydrogels was discussed in terms of gel fraction, gel strength, gel swelling, TGA, FTIR spectra and SEM image. Compared with pure CMC hydrogel, the gel fraction, gel strength and thermal stability were improved obviously after incorporating AC into CMC hydrogels, and similar swelling ability were maintained up to the hybrid of 5%AC. FTIR and TGA spectra of the prepared gels after extracting sol revealed two findings: (1) radiation crosslinking reaction of CMC occurs in side chain of CMC molecules due to the presence of –OH and –CH2 groups; (2) AC enhanced the radiation crosslinking of CMC because AC was binding to CMC through physical adsorption and hydrogen bond as well as other interactions. From SEM images, it was found that AC particles were embedded in the network of CMC gels to form a uniform structure.
Co-reporter:Yalong Zhang, Ling Xu, Min Yi, Maolin Zhai, Jianrui Wang, Hongfei Ha
European Polymer Journal 2006 Volume 42(Issue 11) pp:2959-2967
Publication Date(Web):November 2006
DOI:10.1016/j.eurpolymj.2006.08.008
Novel pH/temperature sensitive hydrogel was synthesized by radiation induced copolymerization and cross-linking of dimethylaminoethyl methacrylate (DMAEMA) and diallyldimethyl ammonium chloride (DADMAC). Reactivity ratio of DADMAC (r1) and DMAEMA (r2) was determined as 1.02 and 0.98, which means that poly(DMAEMA-co-DADMAC) is an azeotropic copolymer. Content of DADMAC, i.e., charge density of the hydrogel was found to influence their properties significantly. Compared with polyDMAEMA hydrogel, poly(DMAEMA-co-DADMAC) showed enhanced equilibrium degree of swelling (EDS). Low critical solution temperature (LCST) of the hydrogel increased with the charged density. Content of DADMAC had no effect on the pH dependence of the final gel. Aiming at its application as a carrier for Chinese herb extract delivery system, the embedment and pH/temperature dependence of controlled release were investigated using notoginsenoside as a model drug. The maximum embedment amount of notoginsenoside was obtained in a gel containing 3 mol.% DADMAC. The temperature dependence and pH dependence of notoginsenoside release followed the same trend as that of EDS, for instance, higher ratio of notoginsenoside release occurred at 25 °C and pH 1.7, at which higher EDS was obtained. By these means, the release of notoginsenoside can be controlled by adjusting the pH, ionic strength, temperature of solution as well as the composition and structure of the gel.
Co-reporter:Maolin Zhai, Yanqun Zhang, Jing Ren, Min Yi, Hongfei Ha, John F. Kennedy
Carbohydrate Polymers 2004 Volume 58(Issue 1) pp:35-39
Publication Date(Web):1 October 2004
DOI:10.1016/j.carbpol.2004.06.010
A series of blended hydrogels composed of poly-N-isopropylacrylamide (polyNIPAAm) and Kappa carrageenan have been prepared by γ-irradiation. The hydrogels obtained by this method were transparent and elastic and the gel strength was improved greatly. Measurements showed that the polyNIPAAm/Kappa carrageenan blends were hydrogels, which not only had pH and temperature sensitivities, but also exhibited a chloride ion-induced phase transition.
Co-reporter:Chuhong Yu, Jing Peng, Jiuqiang Li, Maolin Zhai
Radiation Physics and Chemistry (November 2012) Volume 81(Issue 11) pp:1736-1740
Publication Date(Web):1 November 2012
DOI:10.1016/j.radphyschem.2012.06.005
Dicyclohexano-18-crown-6 (DCH18C6) aqueous solution was irradiated using 60Co source and precipitates containing yellow transparent blocks (PA) and powders (PB) were obtained. TGA analysis confirms that both PA and PB have higher thermal stability than DCH18C6. Both DSC and GPC results suggest that PA might be oligomer and PB were ultrahigh molecular weight polymers. The FTIR spectra indicate that both PA and PB have similar chemical structures containing carboxyl and hydroxyl groups. By using scavengers, it was found that the formation of PA and PB is attributed to the radiation-induced radical polymerization of DCH18C6, and ·OH radical produced by water radiolysis might be a critical species for the formation of PA and PB. These studies help to understand the radiation chemistry behavior of DCH18C6 in the reprocessing of nuclear fuel.Highlight► Dicyclohexano-18-crown-6 (DCH18C6) aqueous solution was irradiated by 60Co source. ► Transparent yellow blocks (PA) and powders (PB) precipitates were obtained. ► PA and PB are determined as oligomers and ultra-high molecular weight polymers, respectively. ► The formation mechanism of precipitates is the radiation-induced radical polymerization. ►·OH radical from water radiolysis is a critical species for the formation of precipitates.
Co-reporter:Hui-Ling Ma, Long Zhang, Youwei Zhang, Shuojue Wang, Chao Sun, Hongyan Yu, Xinmiao Zeng, Maolin Zhai
Radiation Physics and Chemistry (January 2016) Volume 118() pp:21-26
Publication Date(Web):1 January 2016
DOI:10.1016/j.radphyschem.2015.03.028
•Graphene/canbon nanotubes hybrids were synthesized by γ-ray irradiation.•The hybrids exhibited a three-dimensional (3D) interconnected network structure.•The hybirds could effectively improve mechanical properities of PVA matrix.Graphene/carbon nanotubes (G/CNTs) hybrid fillers were synthesized by γ-ray radiation reduction of graphene oxide (GO) in presence of CNTs. The obtained hybrid fillers with three-dimensional (3D) interconnected network structure were characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). Poly(vinyl alcohol) (PVA) composite films with enhanced mechanical properties and thermal stability were subsequently prepared by solution blending of G/CNTs with PVA matrix. The tensile strength and Young's modulus of PVA composite films containing 1 wt% G/CNTs were measured to be 81.9 MPa and 3.9 GPa respectively, which were 56% and 33.6% higher than those of pure PVA. These substantial improvements could be attributed to the interconnected 3D structure of G/CNTs, homogeneous dispersion as well as the strong hydrogen-bonding interaction between G/CNTs and PVA macromolecular chains.
Co-reporter:Cancan Li, Youwei Zhang, Jing Peng, Hao Wu, Jiuqiang Li, Maolin Zhai
Radiation Physics and Chemistry (August 2012) Volume 81(Issue 8) pp:967-970
Publication Date(Web):1 August 2012
DOI:10.1016/j.radphyschem.2011.11.003
Cellulose microsphere (CMS) adsorbent was prepared by radiation-induced grafting of dimethylaminoethyl methacrylate (DMAEMA) onto CMS followed by a protonation process. The FTIR spectra analysis proved that PDMAEMA was grafted successfully onto CMS. The adsorption of Cr(VI) onto the resulting adsorbent was very fast, the equilibrium adsorption could be achieved within 15 min. The adsorption capacity strongly depended on the pH of the solution, which was attributed to the change of both the existed forms of Cr(VI) and the tertiary-ammonium group of PDMAEMA grafted CMS with the pH. A maximum Cr(VI) uptake (ca. 78 mg g−1) was obtained as the pH was in the range of 3.0–6.0. However, even in strong acid media (pH 1.3), the adsorbents still showed a Cr(VI) uptake of 30 mg g−1. The adsorption behavior of the resultant absorbent could be described with the Langmuir mode. This adsorbent has potential application for removing heavy metal ion pollutants (e.g. Cr(VI)) from wastewater.Highlights► A cellulosic adsorbent was successfully prepared by radiation grafting PDMAEMA onto CMS followed by protonation process. The max. grafting yield (GY) under the optimal condition was 33.3%. ► The resulting adsorbent possessed good adsorption capacity of Cr(VI). The equilibrium adsorption could be achieved within 15 min, which is very fast compared with other adsorbents (at least 2 h). ► The adsorption capacity strongly depended on the pH of the solution, a maximum Cr(VI) uptake (ca. 78 mg g−1) was obtained as the pH was in the range of 3.0–6.0. Even in strong acid media (pH1.3), the adsorbents still showed a Cr(VI) uptake of 30 mg g−1. ► The adsorption behavior of the resultant absorbent could be described with the Langmuir mode.
Co-reporter:Pengfei Cao, Jing Peng, Jiuqiang Li, Maolin Zhai
Journal of Power Sources (15 April 2017) Volume 347() pp:210-219
Publication Date(Web):15 April 2017
DOI:10.1016/j.jpowsour.2017.02.056
Co-reporter:Shuojue Wang, Junzi Liu, Liyong Yuan, Zhenpeng Cui, Jing Peng, Jiuqiang Li, Maolin Zhai and Wenjian Liu
Physical Chemistry Chemical Physics 2014 - vol. 16(Issue 35) pp:NaN18735-18735
Publication Date(Web):2014/07/24
DOI:10.1039/C4CP01905A
The application of room-temperature ionic liquids (RTILs) in nuclear spent fuel recycling requires a comprehensive knowledge of radiation effects on RTILs. Although preliminary studies indicate a relatively high radiation stability of RTILs, little attention is paid to the color change of RTILs, an obvious phenomenon of RTILs during irradiation. In this paper, we have investigated radiation-induced darkening and decoloration of 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BMIm][NTf2]), an ionic liquid representing the most popular class of RTILs, by means of UV-Vis analysis and time-dependent density functional theory calculations. Based on the experimental and computational results, it is proposed that the color change of [BMIm][NTf2] upon irradiation originates from the formation of double bonds in the aliphatic chains of pristine organic cations (or radiolytic products of RTILs) and various associated species containing these “double-bond products”. This work sheds light on the understanding of the radiation-induced color change of RTILs.
Co-reporter:Youwei Zhang, Hui-Ling Ma, Qilu Zhang, Jing Peng, Jiuqiang Li, Maolin Zhai and Zhong-Zhen Yu
Journal of Materials Chemistry A 2012 - vol. 22(Issue 26) pp:NaN13069-13069
Publication Date(Web):2012/05/10
DOI:10.1039/C2JM32231E
We demonstrate a facile and environmentally friendly approach to prepare well-dispersed graphene sheets by γ-ray induced reduction of a graphene oxide (GO) suspension in N,N-dimethyl formamide (DMF) at room temperature. GO is reduced by the electrons generated from the radiolysis of DMF under γ-ray irradiation. The reduced GO by γ-ray irradiation (G-RGO) can be re-dispersed in many organic solvents, and the resulting suspensions are stable for two weeks due to the stabilization of N(CH3)2+ groups on G-RGO. Additionally, G-RGO is efficient in improving the conductivity of polystyrene (PS). Its PS nanocomposites exhibit a sharp transition from electrically insulating to conducting with a low percolation threshold of 0.24 vol% and a high electrical conductivity of 45 S m−1 is obtained with only 2.3 vol% of G-RGO. The superior electrical conductivity is attributed to the uniform dispersion of the G-RGO sheets in the PS matrix.
Co-reporter:Yinyong Ao, Hanyang Zhou, Weijin Yuan, Shuojue Wang, Jing Peng, Maolin Zhai, Jianyong Wang, Ziqiang Zhao, Long Zhao and Yuezhou Wei
Dalton Transactions 2014 - vol. 43(Issue 14) pp:NaN5585-5585
Publication Date(Web):2014/01/13
DOI:10.1039/C3DT53297F
Helium ion (He+) beam produced by a heavy ion linear accelerator was used to simulate α-rays for studying the radiation effect on 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ionic liquid ([C4mim][NTf2]). The water-soluble radiolytic products of [C4mim][NTf2] under He+ beam irradiation were analysed, and it was found that they were similar to those by γ-ray irradiation, but their amount was much less than that by γ-ray irradiation, which was attributed to the recombination of [C4mim][NTf2] radical cations in track by high linear energy transfer (LET) radiations of the He+ beam. The extracting behaviour of Dy3+ using irradiated [C4mim][NTf2] in combination with alkylated bis-triazinyl-pyridine (CA-BTP) was assessed, and found that the influence of He+ beam on the extraction was less than that of γ-ray irradiation. In addition, radiolytic products have a different influence on Dy3+ extraction at different doses; Dy3+ partitioning decreases at 50 kGy due to the protonation of CA-BTP and the inhibition of cation exchange mechanism by radiation-formed hydrogen ions. The abnormal increase of Dy3+ partitioning at 100 kGy is mainly attributed to the precipitation formed between Dy3+ and radiolytic products (F− and SO32−).
Co-reporter:Yimeng Wang, Jingyi Qiu, Jing Peng, Jiuqiang Li and Maolin Zhai
Journal of Materials Chemistry A 2017 - vol. 5(Issue 24) pp:NaN12399-12399
Publication Date(Web):2017/05/16
DOI:10.1039/C7TA02291C
We demonstrated a one-step synthesis method for a novel gel polymer electrolyte (named PDMP-Li GPE) based on 3-(dimethylamino) propyl methacrylate, poly(ethylene glycol) diacrylate and 1 M LiPF6 liquid electrolyte solution by a γ-radiation technique for lithium-ion batteries. The resultant PDMP-Li GPE exhibited good thermal stability, excellent mechanical strength and high ionic conductivity, and the highest ionic conductivity reached 8.88 × 10−3 S cm−1 at 25 °C. The LiFePO4/PDMP-Li GPE/graphite pouch-type cell exhibited more than 97% columbic efficiency and the capacity retention was about 86% after 50 cycles at 0.1C. With these outstanding characteristics, it is expected to be a promising candidate for the application in polymer lithium-ion batteries.
Co-reporter:Shuojue Wang, Hui-Ling Ma, Jing Peng, Youwei Zhang, Jian Chen, Liangliang Wang, Ling Xu, Jiuqiang Li and Maolin Zhai
Dalton Transactions 2015 - vol. 44(Issue 16) pp:NaN7625-7625
Publication Date(Web):2015/03/17
DOI:10.1039/C5DT00101C
A novel polymeric ionic liquid gel (PIL gel) was simply synthesized by γ-radiation-induced polymerization of ionic liquid monomer 1-allyl-3-vinylimidazolium chloride and crosslinking at ambient temperature without any additives. By changing the radiation dose, the properties of the resulting gel including the gel fraction, crosslinking density and equilibrium degree of swelling were optimized. The resulting PIL gel exhibited a superior adsorption ability toward Cr(VI) in aqueous solutions with a broad pH range (1–7) through anion exchange. It was found that the adsorption kinetics followed the pseudo-second-order model. The adsorption of Cr(VI) by the PIL gel obeyed the Langmuir isotherm equation with a theoretical maximum adsorption capacity of 283 mg g−1, twice the highest value for ionic liquid-based adsorbents that have been reported. In addition, the PIL gel could be recovered using a NaCl solution or a NaOH solution without much decreasing the adsorption capacity. This work paves the way for the scale-up production of PIL gels using the radiation technique for potential application in heavy metal removal.
Co-reporter:Yinyong Ao, Jing Peng, Liyong Yuan, Zhenpeng Cui, Cheng Li, Jiuqiang Li and Maolin Zhai
Dalton Transactions 2013 - vol. 42(Issue 12) pp:NaN4305-4305
Publication Date(Web):2012/12/20
DOI:10.1039/C2DT32418K
The trace water-soluble radiolytic products of neat 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C4mim][NTf2]) were identified by analysing water-washed samples of γ-ray irradiated ionic liquids. CF3SO2OH, CF3SOOH, CF3SO2NH2, HF and H2SO3 were confirmed as main radiolytic products of [C4mim][NTf2], and the total radiation chemical yields of the water-soluble radiolytic products (0.35 μmol J−1) and that of hydrogen ions (0.46 ± 0.02 μmol J−1) were determined by using ion chromatography and neutralization titration, respectively. It was found that the water-soluble radiolytic products of [C4mim][NTf2] greatly reduced the extraction efficiency of Sr2+ from water to irradiated [C4mim][NTf2], while the water-insoluble radiolytic products of [C4mim][NTf2] had a slight influence on the Sr2+ extraction.
Co-reporter:Chao Xu, Liyong Yuan, Xinghai Shen and Maolin Zhai
Dalton Transactions 2010 - vol. 39(Issue 16) pp:NaN3902-3902
Publication Date(Web):2010/03/17
DOI:10.1039/B925594J
The removal of radioactive 137Cs from nuclear waste is of great importance for both the environment and energy saving. Herein, we report a study on the removal of Cs+ using a calix crown ether bis(2-propyloxy)calix[4]crown-6 (BPC6) in ionic liquids [Cnmim][NTf2], where [Cnmim]+ is 1-alkyl-3-methylimidazolium and [NTf2]− is bis(trifluoromethylsulfonyl)imide. The BPC6/[Cnmim][NTf2] system is highly efficient in removing Cs+ from aqueous solution, even at a low concentration of BPC6. HNO3 and metal ions such as Na+, Al3+ in the aqueous phase interfered with the extraction of Cs+ by competitive interaction with BPC6 and/or salting-out effect. UV analysis confirmed that the extraction of Cs+ by the BPC6/[Cnmim][NTf2] system involves a dual extraction mechanism, i.e., via exchange of BPC6·Cs+ complex or Cs+ by [Cnmim]+. Irradiation of [C4mim][NTf2] dramatically decreases Cs+ partitioning in the ionic liquid phase by the competitive interaction of radiation-generated H+ with BPC6, while irradiation of BPC6/[C4mim][NTf2] decreases Cs+ partitioning more markedly due to the radiolysis of BPC6.
Co-reporter:Liyong Yuan, Chao Xu, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li, Genshuan Wei and Xinghai Shen
Dalton Transactions 2009(Issue 38) pp:NaN7875-7875
Publication Date(Web):2009/08/04
DOI:10.1039/B911026G
SO32− is identified as one of the radiolytic products of the ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C4mim][NTf2]) during the removal of strontium ions (Sr2+) from aqueous solution.
Co-reporter:Liyong Yuan, Jing Peng, Ling Xu, Maolin Zhai, Jiuqiang Li and Genshuan Wei
Dalton Transactions 2008(Issue 45) pp:NaN6360-6360
Publication Date(Web):2008/09/24
DOI:10.1039/B811413G
The preliminary results presented here show that γ-irradiation of ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate ([C4mim][PF6]) markedly decreases Sr2+ partitioning in the crown ether/[C4mim][PF6] extraction phase due to the competition between radation-generated H+ and Sr2+ to interact with the crown ether, however, washing irradiated [C4mim][PF6] with water gives a simple way of recycling the ionic liquid.
Co-reporter:Hui-Ling Ma, Youwei Zhang, Qi-Hui Hu, Dong Yan, Zhong-Zhen Yu and Maolin Zhai
Journal of Materials Chemistry A 2012 - vol. 22(Issue 13) pp:NaN5916-5916
Publication Date(Web):2012/02/22
DOI:10.1039/C2JM00145D
Ethylenediamine-reduced graphene oxide (ED-RGO) sheets were prepared by simple refluxing of graphene oxide (GO) solution with ethylenediamine (ED), which effectively reduced toxic Cr(VI) to less toxic Cr(III) by an indirect reduction mechanism with the assistance of π electrons on the carbocyclic six-membered ring of ED-RGO.
Co-reporter:Qilu Zhang, Youwei Zhang, Zhaohui Gao, Hui-Ling Ma, Shuojue Wang, Jing Peng, Jiuqiang Li and Maolin Zhai
Journal of Materials Chemistry A 2013 - vol. 1(Issue 2) pp:NaN328-328
Publication Date(Web):2012/10/16
DOI:10.1039/C2TC00078D
A facile method has been developed to synthesize a high-quality platinum nanoparticle (PtNP) decorated graphene via one-step γ-ray induced reduction of graphite oxide (GO) and chloroplatinic acid at room temperature. GO and Pt(IV) precursor salt could be co-reduced by the electrons generated from the radiolysis of ethylene glycol under γ-ray irradiation. The synchronous reduction of the metal precursor and regulation of pH greatly increased the ratio of C/O in the reduced GO (RGO). PtNPs with an average diameter of 1.8 nm were uniformly dispersed on the surface of RGO sheets. The as-prepared PtNP–RGO composites as supercapacitor electrodes displayed a specific capacitance of 154 F g−1 at a current density of 0.1 A g−1 and the value retained as high as 72.3% at 20 A g−1 which was significantly enhanced compared to 16.2% capacity retention of RGO prepared by the same method. The investigation of electrochemical performances suggests that PtNPs play an important role in enhancing supercapacitor performance with high rate capability by accelerating the electron transfer and increasing the electrochemical active surface area of RGO.
Co-reporter:Yinyong Ao, Weijin Yuan, Tianlin Yu, Jing Peng, Jiuqiang Li, Maolin Zhai and Long Zhao
Physical Chemistry Chemical Physics 2015 - vol. 17(Issue 5) pp:NaN3462-3462
Publication Date(Web):2014/12/11
DOI:10.1039/C4CP04294H
The quantitative analysis and identification of the radiolytic products of dicyclohexano-18-crown-6 (DCH18C6), 4′,4′′(5′′)-di-tert-butyldicyclohexano-18-crown-6 (DtBuCH18C6) and benzo-18-crown-6 (B18C6) in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([C4mim][NTf2]) ionic liquid after irradiation were performed for the first time. It was found that the yield for radiolytic destruction of DCH18C6 and DtBuCH18C6 was less than that for B18C6. The main radiolytic products were identified as substituted crown ethers formed between crown ether and active radicals such as methyl, trifluoromethyl, butyl, and [C4mim]˙ radicals generated during the irradiation of the crown ether–[C4mim][NTf2] system. The radiation effect on the Sr2+ partitioning of the crown ether–[C4mim][NTf2] system shows further that DCH18C6–[C4mim][NTf2] and DtBuCH18C6–[C4mim][NTf2] still have good extractability for Sr2+ after irradiation. The extraction ability of DCH18C6–[C4mim][NTf2] and DtBuCH18C6–[C4mim][NTf2] system for Sr2+ decreased by 14.4% and 18.2% even at 500 kGy, respectively.