ࡱ> _a^lfhSbjbj 4d,+8 aS!(!""""""tRvRvRvRvRvRvR$UXR"""""R""S000"""tR0"tR006JL"0lF)K`R1S0aSK Z,& Z8LL8 ZL""0"""""RR."""aS"""" Z""""""""" : SAXS Studies of TiO2 Nanoparticles in Polymer Electrolytes A. Turkovi Ruer Boakovi Institute, POBox 180, HR-10002 Zagreb, Croatia Electrolytes as nanostructured materials are very attractive for batteries or othertypes of electronic devices. (PEO)8ZnCl2 polymer electrolytes and nanocomposites (PEO)8ZnCl2/TiO2 were prepared from PEO and ZnCl2 and with addition of TiO2 nanograins.The influence of TiO2 nanograins was studied by small-angle X-ray scattering (SAXS) simultaneously recorded with wide-angle X-ray scattering (WAXD) and differential scanningcalorimetry (DSC) at the synchrotron ELETTRA. It was shown by previous impedance spectroscopy (IS) that the room temperature conductivity of nanocomposite polymer electrolyte increased more than two times above 65C, relative to pure composites of PEO and salts. The SAXS/DSC measurements yielded insight into the temperature-dependent changes of the grains of the electrolyte as well as to differences due to different heating and cooling rates. The crystal structure and temperatures of melting and crystallization of the nanosize grains was revealed bythe simultaneous WAXD measurements. Introduction Electromagnetic radiation can be used to obtain information about materials whose dimensions are on the same order of magnitude as the radiation wavelength. Since the larger the diffraction angle the smaller the length scale probed, wide angle X-ray diffraction (WAXD) is used to determine the crystal structure on the atomic length scale while small-angle X-ray scattering (SAXS) is used to explore the microstructure on the nanometer scale. SAXS experiments are suitable to determine the structure of nanocomposite polymer electrolyte. Polymeric complexes of (PEO)n with ZnCl2 have been used, due to their stability and very high conductivity (1,2). Our research was aimed at optimizations of electrolyte properties (3) as these materials are attractive as electrolytes for second generation of polymer-based rechargeable batteries (4). The aim of the present investigation was to study the temperature behavior of the nanocomposite (PEO)8ZnCl2 electrolyte by simultaneous SAXS/WAXD/DSC measurements. This structural investigation will provide answer to the question about the behavior of nanosizes through the superionic phase transition, which occurs at ~65 C. Experimental The polymer-salt complex was prepared by dissolving ZnCl2 (p.a. Merck) and poly(ethylene oxide) (laboratory reagent, BDH Chemicals, Ltd., Poole, England, Polyox WSR-301, MW=4x106, Prod 29740) in 50 % ethanol-water solution in stoichiometric proportions [3]. Simultaneous SAXS/WAXD/DSC measurements were performed at the Austrian SAXS beamline at the synchrotron ELETTRA, Trieste (5). Photon energy of 8 keV was used, and the size of the incident photon beam on the sample was 0.1 x 5 mm2 (h x w). For each sample, SAXS and WAXD patterns were measured simultaneously in transmission setup using two 1D single photon counting gas detectors. The in-line micro-calorimeter built by the group of Michel Ollivon (CNRS, Paris, France) (6) was used to measure simultaneously SAXS/WAXD and high sensitivity DSC from the same sample. DSC phase transition temperature was determined at the intersection of tangent to the peak and the baseline. SAXS is observed when electron density inhomogeneities of nanosized objects exist in the sample. If identical grains of constant electron density  are imbedded in a medium of constant 0, only the difference =(-0) will be relevant for scattering. The amplitude is proportional to  as only the contrast to the surrounding medium is effective. For the central part of the scattering curve, the universal Guinier approximation for all types of scattering objects/grains is valid (7-11): EMBED Equation.3 [1] where R is the gyration radius which is the average square distance from the centre of masses within the particles. For WAXD the diameter of the nanocrystalline grains is obtained by the Debye-Scherer equation: EMBED Equation.3 [2] where  is wavelength of the incident X-ray beam, and  is full width at half maximum (FWHM) of the WAXD line. Results Figure 1 shows the results from the DSC, SAXS and WAXD measurements on polymer electrolyte (PEO)8ZnCl2/TiO2 nanocomposite which were performed simultaneously at the SAXS-beamline of ELETTRA. The evolution of the average radii of grain sizes obtained by applying equation (1)  Figure 1. DSC, WAXD and SAXS results for nanocomposite polyelectrolyte (PEO)8ZnCl2 in the temperature range from 20C to 100C at rate of A) 1C/min, B) 1C/min, C) 3C/min and D) 5C/min a) showing the DSC heating and cooling cycle (denoted with DSC), b) showing evolution of the intensity of the strong WAXD line at 2( =19.21, c) showing radius of gyration (RG) in the cooling cycle of SAXS (denoted with TC) and d) presenting RG in the heating cycle of SAXS (denoted with TH). is compared to the corresponding DSC and WAXD spectra behaviour. In the heating cycle the superionic phase transition can be seen as the sudden drop of the nanograin sizes at the phase transition temperature. In the cooling part a hysteresis can be seen as the phase transition occurs at lower temperature. The endothermic and exothermic peaks found in DSC during the same temperature cycle follow the sudden changes in the average nanograin sizes as obtained from the SAXS measurements and drops of the intensity in the WAXD spectra. In the heating cycle with rate of 1C/min in the SAXS data there are two trends, first an increasing of the grain size up to 74C and then a sudden drop at this phase transition temperature. The DSC spectrum for the rate of 1C/min shows that the phase transition temperature is 67C, which is determined at the beginning of the peak in the heating cycle. Both, the SAXS and DSC data show a hysteresis, i.e. much lower phase transition temperatures than 65C in the cooling cycle. This temperature is the melting temperature of the PEO crystallites i.e. spherulites [12]. In the case of the nanocomposite polymer electrolyte, combined forms of PEO and ZnCl2, ZnCl2 influence the melting temperature. TABLE I. Changes of average grain radius / nm calculated by (1), R=D/2 as determined from (2) and phase transition temperatures T (in C) in (PEO)8ZnCl2 polyelectrolyte during heating and cooling as determined by SAXS/WAXD/DSC measurements.(PEO)8ZnCl2heatingSAXSWAXDDSCHeating rate (C/min)t (C)R (nm)t (C)R (nm)t (C)1746.0-6.4 5.9-6.07127-43671635.8-6.3 6.1-6.06131-42 623656.3-6.2 6.0-6.25635-28615506.2-6.3 6.1-6.05236-3660(PEO)8ZnCl2 coolingSAXSWAXDDSCCooling rate(C/min)t (C)R (nm)t (C)R (nm)t (C)1536.1-6.0 6.0-6.05323-37551576.0-6.3 6.1-6.24633-36553506.2-6.2 6.2-6.13831-43525 496.3-6.1 6.2-6.23536-3748 The WAXD recordings were done simultaneously with the SAXS and DSC measurements. Above the phase transition temperature the WAXD spectra are registering the amorphous phase of the polymer electrolyte. The WAXD data are giving the information of the side chain order. During the heating and cooling cycles the side chain ordering is giving us information of the lateral domain sizes or spherulites. The WAXD results for all heating and cooling rates are, together with SAXS and DSC data, presented in the Table 1. The combination of the three methods reveals the nature of the physical transformation of the polymer electrolyte into a super ionic conductor. The nanocomposite crystalline and amorphous polymer matrix is turning into an amorphous highly conductive phase. In contrast to WAXD, which exhibits lines and crystalline grains only in the low temperatures crystalline phases, SAXS is showing the existence of nanograins in both the low and high temperature phase. At the phase transition temperature the grain size changes, it is becoming smaller at higher temperatures. The nature of the nanograins as seen by SAXS is not just the pure crystalline, but also the partly amorphous form, while WAXD records only pure crystalline nanograins. Thus the picture of the highly conductive phase consists of a completely amorphous polymer matrix, which is known to be suitable for ionconduction by elastic movement of PEO chains, and of nanograins of combined PEO/ZnCl2 and ZnCl2 structures, which could also contribute to Zn2+-ion conduction by a hopping mechanism. Under proper circumstances, the presence of ion-transport pathways can be as important as polymer segmental motion [13,14]. The nanopolymer (PEO)8ZnCl2 /TiO2 electrolyte, has phase transition temperature of 74C [16], which is somewhat higher than 65C for melting of spherulites in pure PEO. Conclusion The combined SAXS/WAXD/DSC measurements have shown that the nanostructure of the nanopolymer electrolyte (PEO)8ZnCl2 is changing during the crystalline-amorphous phase transition to a highly conductive superionic phase. The conductivity is higher and the phase transition temperature lower than for the (PEO)8ZnCl2, which are desirable properties for application in batteries. The significant role that the nanodimensions of the electrolyte material play in the Zn2+-ion mobility was discussed. The combined SAXS/WAXD information about the evolution of the average grain sizes during the phase transition gave insight into the nanomorphology, which influences the ionic transport in a nanocomposite polymer electrolyte. Further optimizations of the electrolyte properties are in progress since these nanostructured materials are very attractive for batteries or other types of electronic devices Acknowledgments The Ministry of Education, Science and Sport of the Republic of Croatia is thanked for support of this work. Experimental assistance at SAXS - beamline at ELETTRA is acknowledged for P. Dub ek and S. Bernstorff. References T.M.A. Abrantes, LJ.Alcacer and C.A.C. Sequeira, Solid State Ionics 18/19 (1986) 315. M.J.C. Plancha, C.M. Rangel and C.A.C. Sequeira, Solid State Ionics 116 1999) 293. A. Turkovi, M. Pavlovi, P. Dub ek, M. Lu i-Lav evi, B. Etlinger and S. Bernstorff, J. Electrochem. Soc.154/6 (2007) A554. a) S.J. Visco, M. Liu, L.C. Dejonge, Cell for making secondary batteries, Patent number 5162175, Nov.10, (1992); b) F. Brochu, M. 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