• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    Talcum-doped composite separator with superior wettability and heatproof properties for high-rate lithium metal batteries

    2023-03-14 06:52:04MengqiuYngYunpengJiYunfDongBotoYunLiweiDongYunpengLiuSueHoChunhuiYngXioqingWuQingqunKongJieciHnWeiongHe
    Chinese Chemical Letters 2023年1期

    Mengqiu Yng,Yunpeng Ji,Yunf Dong,Boto Yun,Liwei Dong,Yunpeng Liu,Sue Ho,c,Chunhui Yng,c,Xioqing Wu,Qingqun Kong,Jieci Hn,Weiong He,,e,*

    a MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage,School of Chemistry and Chemical Engineering,Harbin Institute of Technology,Harbin 150080,China

    b National Key Laboratory of Science and Technology on Advanced Composites in Special Environments,and Center for Composite Materials and Structures,Harbin Institute of Technology,Harbin 150080,China

    c State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology,Harbin 150080,China

    d School of Mechanical Engineering,Chengdu University,Chengdu 610106,China

    e Chongqing Research Institute,Harbin Institute of Technology,Chongqing 401151,China

    Keywords:Lithium metal batteries Composite separator PVDF Talcum Wettability Thermal stability

    ABSTRACT Separator is supposed to own outstanding thermal stability,superior wettability and electrolyte uptake,which is essential for developing high-rate and safe lithium metal batteries (LMBs).However,commercial polyolefin separators possess poor wettability and limited electrolyte uptake.For addressing this issue,we put forward a composite separator to implement above functions by doping layered-silicate (talcum) into polyvinylidene fluoride (PVDF).With significant improvement of electrolyte absorption benefiting from the strong adsorption energy values (-1.64 ~-1.70 eV) between talcum and the electrolyte in lithium metal batteries,PVDF/Talcum (PVDF/TM) composite separator owns a small contact angle and superior electrolyte uptake.PVDF/TM composite separator with 10 wt% talcum (T-10) owns a tiny contact angle of 8°,while those of polypropylene (PP) and PVDF are 48° and 20° with commercial electrolyte.Moreover,the addition of thermotolerant talcum endows the T-10 composite separator with great thermostability,whose thermal shrinkage is only 5.39% at 150°C for 0.5 h.The cell with LiFeO4 cathode and the T-10 composite separator reaches 91.7 mAh/g in discharge capacity at 4.8 mA/cm2 (10 C),far superior to that with pure PVDF separator (56.3 mAh/g) and PP (51.4 mAh/g).

    Much effort has been made on the rechargeable lithium metal batteries (LMBs) for ever-increasing demands of novel portable electronics,long-range electric vehicles and solar/wind energy storage,owing to their high operating voltage,zero memory effect and long working lifetime [1–7].However,the increasing demand for higher energy requires continuous optimization of key components in LMBs (cathode,anode,electrolyte and separator) [8,9].As an inactive component,placed between cathode and anode,separator plays a vital role in capacity,cost-effectiveness,lifespan and safety of LMBs [10–18].

    Polyolefin-based materials,for instance,polyethylene (PE) and polypropylene (PP),are used for commercial separators in LMBs due to their high mechanical strength and low cost [19–21].However,the unsatisfactory thermal stability and wettability limit their extensive application [22–24].Massive research on polyvinylidene fluoride (PVDF) or its copolymer as separator is ongoing to address aforementioned issues,owing to its superior thermal stability and favorable wettability attributed to the strong electronabsorbing functional groups and low degree of crystallinity [22,25-28].Nonetheless,their further development is limited in two aspects: (1) short circuit caused by the low mechanical strength of PVDF-based separator associated with Li dendrites and robust electrode; and (2) rapid decay of the discharge capacity resulted from the high activity of Li anode [29,30].The stable operation of LMBs is still challenged with the unsatisfactory rate performance and heatproof [31–33],low mechanical strength of PVDFbased separators in LMBs [28,34].To break through these bottlenecks,massive strategies have been used to enhance the overall performances of PVDF-based separators [35].Recently,it has been demonstrated that polymeric separators incorporated with inorganic particles (ZrO2[36],SiO2[37],Al2O3[38] and TiO2[39]) or modified with inorganic particlesviawet method exhibit enhanced electrolyte uptake,mechanical strength and thermal stability.However,the electrolyte shows poor compatibility with the doped inorganic molecules and cells assembled with these composite separators exhibit poor rate performance,severe safety problems and low discharge specific capacity [10,28].Talcum is a type of layered silicate which is used as reinforcement material for plenty of plastics,owing to its heat-resistance,acid-resistance and insulation.Polymer incorporated with talcum shows excellent rigidity,creep-resistance and stability even at high temperature compared with those incorporated with calcium carbonate or magnesium hydrate [40–42].On one hand,layered silicate has been demonstrated owning strong interaction and showing superior compatibility with the electrolyte [8,22].Therefore,compared with inorganic particles (ZrO2,SiO2,Al2O3,and TiO2),talcum doped composite separator can improve mechanical properties without sacrificing its rate performance and safety.On the other hand,the layered structure of talcum leads to the parallel ion channels that unify the direction of Li+flows.Thus,talcum doped composite separator could improve the discharge specific capacity compared with separators doped with other inorganic particles.Talcum is widely used in composite polymers to reinforce the thermal stability and mechanical strength,reducing the cost at the same time [43].

    In our work,a high-rate,safe and low-cost half-cell is designed with the LiFePO4cathode and the composite separator fabricated by doping talcum into PVDF matrixvialiquid phase method.As compared with PVDF,PVDF/talcum (PVDF/TM) composite separator with 10 wt% talcum (T-10) owns tiny contact angle of 8° with commercial electrolyte while that of the PVDF is 20°.T-10 achieves the mechanical strength of 33 MPa while the PVDF is 15 MPa,and T-10 attains strain of 253% while that of PVDF is 107%.The cell with LiFePO4cathode and T-10 can reach 91.7 mAh/g in discharge capacity,higher than cell with PVDF separator (56.3 mAh/g) and cell with the PP separator (51.4 mAh/g) at 10 C.

    Talcum is a kind of layered silicate ore consisting of SiO2and MgO with the ratio of 2:1,which is stable with the electrolyte and the lithium when being doped with PVDF to form the composite separator [37].The crystal structure and the atomic configuration of talcum are demonstrated in Figs.S1 and S2 (Supporting information).The structural unit layer of talcum powder consists of a magnesium oxygen octahedron sandwiched by two silicon oxygen tetrahedra.After being incorporated into PVDF to form the PVDF/TM composite separator,the parallel interlayers in talcum provide active sites and uniform channels to transfer Li+[22],accelerating the transport of lithium ions as demonstrated in Fig.1a.The T-10 composite separator exhibits a more porous and uniform structure as compared with PVDF as demonstrated in Figs.1b and f.The SEM images in Fig.1c typically display the nanosheet structure of talcum,which is clearly observed in the SEM of T-10 composite separator as depictured in Figs.1f and g.The energy dispersive spectral (EDS) mapping images of Mg and Si in the T-10 composite separator show the uniform distribution of talcum particles as illustrated in Figs.1d and h.Moreover,the conclusion is further confirmed with the EDS mapping image of O in T-10 composite separator as depictured in Fig.S3 (Supporting information).The original electron image of EDS is depictured in Fig.S4(Supporting information).The crystallinities of the talcum particles,PVDF and T-10 separators are analyzedviaXRD as depictured in Fig.1e.The characteristic peaks at 9.46° and 19.49° come from the(001) and (101) planes of talcum,respectively.The peak at 28.62°is attributed to quartz,which is commonly found in clays [22].The original peak at 20.42° of PVDF becomes wide and weak after the addition of talcum,demonstrating that the addition of talcum decreases the crystallinity of the PVDF matrix slightly [44,45].The FTIR spectra of T-10 composite separator and PVDF separator are shown in Fig.1i,where the peaks at 614 cm-1and 1402 cm-1come from theαphase of PVDF [46,47].The peaks that are relevant to the stretching vibration of CF2groups appear at 485 cm-1and 1181 cm-1[22,28].The peaks at 3676 cm-1and 670 cm-1of T-10 composite separator are attributed to the presence of talcum particles.

    The thermal distribution is determined with forward looking infrared radiometer (FLIR) as demonstrated in Figs.2a-c.The T-10 and PVDF separators own the structural integrity,demonstrating the expeditious heat transfer during the whole heating process as shown in Figs.2b and c,showing a higher thermal stability than PP separators (Fig.2a).Fig.S5 (Supporting information) shows that PVDF/TM composite separators maintain the most structural integrity even after 30 min at 150°C,while PP experiences severe shrinkage with the temperature increasing.Fig.S6 (Supporting information) demonstrates that after annealing samples at different temperature,the thermal shrinkage of T-10 composite separator is 1.29% at 120°C and 5.39% at 150°C,respectively,far superior to those of PVDF and PP separators.Separators with superior mechanical strength can prevent the cell from short circuit,which is vital for the safe operation of LMBs [1,7,48,49].The mechanical behavior was investigated with strain-stress analysis as demonstrated in Fig.2d.As the ratio of talcum in PVDF/TM increases,the mechanical strength of PVDF/TM separators upgrades gently but all much higher than PVDF separator.As for the toughness of these separators,PVDF/talcum (PVDF/TM) composite separator with 5 wt%talcum (T-5) owns nearly 400% elongation,four times than that of PVDF,but sharply decreases with the continued addition of talcum.Given comprehensive comparison on mechanical strength and toughness of these composite separators,T-10 composite separator is chosen to be the ideal separator to carry on further investigation and comparison with PVDF and PP separators.Effi-cient electrolyte absorption is of great significance for transporting Li+[10,50-52].Electrolyte uptake percentages are measured by immersing the three separators in the commercial electrolyte for one hour,respectively.PVDF-based separator demonstrates a much higher electrolyte uptake percentage than PP,and T-10 composite separator owns the highest uptake percentage of 200% while PVDF of 150% and PP of 120% as demonstrated in Fig.2e.

    Thermogravimetric analysis (TGA) was conducted to further explore the heat endurance of T-10,PVDF and PP separators.The above three separators are heated ranging from 25°C to 800°C with the rate of 10°C/min.The TGA curves demonstrate that T-10 composite separator starts to lose weight at 458°C,while PVDF at 427°C and PP at 289°C,respectively (Fig.2f).Contact angle measurements are conducted on above three separators to investigate the wettability of the separators.The commercial separator PP owns the contact angle of 48° ± 1.05° due to its intrinsic hydrophobicity while PVDF with 20° ± 1.02° as depictured in Figs.2g and h [53].The T-10 composite separator owns the smallest contact angle of 8° ± 1.01° due to the intrinsic hydrophilia of PVDF and the strong compatibility of talcum with electrolyte (Fig.2i)[28].Column diagram is used to make a striking contrast among the three separators about contact angle (Fig.S7 in Supporting information).

    Rate performance of half-cell with LiFeO4cathode and PP,PVDF and PVDF/TM separators was investigated.The half-cell with LiFeO4cathode and Li anode (LFP/Li) with T-10,PVDF/talcum composite separator with 20 wt% talcum (T-20),PVDF/talcum(PVDF/TM) composite separator with 30 wt% talcum (T-30),PVDF and PP separators at 0.2 C,0.5 C,1 C,2 C,5 C and 10 C are demonstrated respectively in Fig.S8 (Supporting information).The cell with T-10 composite separator reaches 91.78 mAh/g at 10 C with the highest discharge specific capacity,far higher than those with T-20,T-30,PP and PVDF separators.To further investigate the optimal proportion of talcum in PVDF,rate performance of the cell with T-5 and PVDF/talcum composite separator with 15 wt% talcum (T-15) composite separators are selected to compare with the cells assembled with T-10 composite separator.As illustrated in Fig.S9 (Supporting information),the cell with T-10 exhibits a discharge specific capacity higher than those with T-5 and T-15 composite separators.The rate properties of the cell assembled with PP,PVDF and T-10 composite separators are selected to make a clear and strong contrast in Fig.3a.The cell with T-10 reaches discharge capacities of 154.4,152.3,149.5,141.7,117.7 and 89.8 mAh/g at 0.2 C,0.5 C,1 C,2 C,5 C and 10 C,respectively.In addition,the discharge specific capacity of the cell with the T-10 recovers to 153.7 mAh/g as 10 C rate returns to 0.2 C,which demonstrates especially stable operation of LFP/Li with T-10 composite separator.On the contrary,cell with both PVDF and PP delivers lower discharge capacity at all rates.The upgraded discharge capacity of the cell assembled with T-10 is attributed to the increased Li+channels by adding talcum which is in good agreement with Fig.1a.However,the rapid deterioration of discharge capacity happens with excessive talcum particles as a consequence of the long Li+transfer path,giving rise to the increased charge transfer resistance as demonstrated in Fig.S10 (Supporting information) [22].Given this,high-rate cycle-test is conducted on T-10 and PP separators,and discharge capacity of the battery with T-10 composite separator reaches 71.8 mAh/g while that with PP separator reaches 59.5 mAh/g in the first cycle as demonstrated in Fig.3b.LFP/Li with PVDF/TM separators are put on the working station using the cyclic voltammetry pattern to confirm the electrochemical reactivity,and the peaks at 3.3 V correspond to the reduction and 3.6 V correspond to the oxidation as demonstrated in Fig.3c,respectively.The solid electrolyte interphase (SEI) is formed during the first cycle of reduction at 3.3 V,and the other two peaks at 3.3 V are attributed to the reduction reactions of the battery.On the contrary,the three sharp peaks at 3.6 V are associated with the oxidization reactions,respectively.The cell with T-10 composite separator shows no obvious fluctuations,demonstrating the especial electrochemical stable of T-10 in half-cell which also can be confirmed in long-cycle property in Fig.3j.In addition,the CV profiles of cells with PP,PVDF,T-5,T-15,T-20 and T-30 are depictured subsequently in Fig.S11 (Supporting information).The CV curves about the first cycle of PP,PVDF and T-10 are investigated in Fig.3d,three CV curves show no difference,implying the addition of talcum in PVDF polymeric has no effect on the redox reaction of the cell.

    Fig.1.Fabrication and morphological characteristics of PVDF and T-10 separators.(a) Schematic of PVDF separator,PVDF/TM composite separator and talcum.(b,c) SEM images of PVDF and talcum particle,respectively.(d) Elemental mapping image of Mg-K in a specific acreage of T-10 composite separator.(e) XRD spectra of talcum,PVDF and T-10 separators.(f,g) SEM images of T-10 composite separator at different magnification.(h) Elemental mapping image of Si-K in a specific acreage of T-10 composite separator.(i) FT-IR spectra of T-10 and PVDF separators.

    Fig.2.Heatproof/wettability and other physical performances of PP,PVDF and T-10 separators.(a-c) FLIR pictures of PP,PVDF and the T-10 separators.(d) Tensile curves of PVDF,T-5,T-10,T-15,T-20,T-25 and T-30 separators.(e) Uptake percentage of the PP,PVDF and T-10 separators with commercial electrolyte for 1 h.(f) TG curves of PP,PVDF and T-10 separators.(g-i) Contact angles of PP,PVDF and T-10 separators.

    Fig.3.Electrochemical properties of battery with PP,PVDF and T-10 separators at room temperature.(a) Rate properties of the battery with PP,PVDF and T-10.(b) Cycling properties of the battery with PP and T-10 at 10 C.(c) CV profiles of T-10,recorded with 0.2 mV/s.(d) CV profiles of PP,PVDF and T-10,recorded with 0.2 mV/s.(e)Electrochemical impedance spectroscopy (EIS) curves of the battery with PP,PVDF,T-10,PVDF (16 μm) and T-10 (16 μm) separators.(f) Charging/discharging plots of the cell with PP,PVDF and T-10.(g-i) Charging/discharging plots of the cell with PP,PVDF and T-10,respectively.(j) Cycling properties and Coulombic efficiency of the battery assembled with PP,PVDF,T-10,PVDF (16 μm) and T-10 (16 μm) separators at 0.5 C,respectively.

    Fig.4.Electrochemical properties of cell with PP,PVDF and T-10 separators at elevated temperature.(a) EIS curves of the battery assembled with PP,PVDF and T-10 at 80 °C.(b) Cycling properties of cell with PP,PVDF and T-10 at 1 C under 80 °C.(c-e) Charging/discharging plots of cell with PP,PVDF and T-10 at 80 °C.(f) Cycling performance of cell with PP and T-10 at 1 C at 100 °C.(g) Coulombic Efficiency of cell with PP,PVDF and T-10 at 1 C under 80 °C.

    Thickness is a nonnegligible factor of the separator in lithiumbased batteries in terms of electrochemical performance and cost[12].Currently,the thickness of the academic separators is limited to about 25 μm in line with the commercial polyolefin separators.The pursue of thinner separator is becoming urgent for achieving higher energy-density and safer lithium-based batteries [54].Herein,16 μm PVDF and 16 μm T-10 separators are fabricated and assembled in the LMBs to investigate the internal resistance and cycle stability as depictured in Figs.3e and j.To acquire more direct information on the interfacial impendence,the cells with PP,PVDF,T-10,PVDF (16 μm) and T-10 (16 μm) separators are placed on the work station to explore more interface impedance information at open circuit voltage.For cells assembled with PP,PVDF and T-10 separators,minimum semicircle distance is observed in the cell with T-10 composite separator among the three Nyquist curves,demonstrating the lowest transfer impedance,as depictured in Fig.3e.What is more,cells with 16 μm PVDF and 16 μm T-10 separators show a slight decrease compared with those with 25 μm PVDF and 25 μm T-10 separators as demonstrated in Fig.3e,respectively.Results show that thin separator can reduce the internal resistance.The cells with separators sandwiched with stainless steel are fabricated to measure the ionic conductivity.The ion conductivity of T-10,PVDF and PP is calculated according to Fig.S12 and Eq.S4 (Supporting information).The ion conductivity of T-10 is 0.509 mS/cm.The symmetrical Li/Li cells with various separators are assembled and tested with 0.5 mA/cm2current density to assess the capability of the separator in suppressing the growth of Li dendrites.As demonstrated in Fig.S13 (Supporting information),the cell with T-10 composite separator shows a stable voltage profile over 480 h.In contrast,short circuit occurs on the cells assembled with PP with dramatical voltage fluctuation after 300 h.The lithium-ion transference numbers of various separators are illustrated in Fig.S14 (Supporting information).The Li+transference number is 0.534 for T-10 separator,which is slightly larger than that of PP (0.509) separators.Fig.3f illustrates the charge/discharge plots of cell with PP,PVDF and T-10 separators during the same first cycle at 0.5 C,respectively.Results show that the cell with T-10 composite separator owns a discharge specific capacity of 159.78 mAh/g,while PP of 154.67 mAh/g and PVDF of 153.69 mAh/g.The galvanostatic charging/discharging plots of the cell assembled with PP,PVDF and T-10 separators at 0.5 C are depictured in Figs.3g–i.Cycle stability plays a vital role on the stable operation of the batteries.Cyclic analysis on the cell with PP,PVDF,T-10,PVDF (16 μm) and T-10 (16 μm) separators is conducted at 0.24 mA/cm2and the active material loading is 2.83 mg/cm2,as depictured in Fig.3j.The battery with T-10 composite separator releases a higher discharge capacity of 122.6 mAh/g,which is maintained at 84% after 400 cycles,while those of the battery with PVDF and PP separators are 73% and 76%,respectively.The cells assembled with PVDF (16 μm) and T-10 (16 μm) separators deliver a slightly higher discharge specific capacity compared with cells with PVDF (25 μm) and T-10 (25 μm) separators.Especially,the cell with T-10 (16 μm) exhibits a capacity that is maintained at 96% after 400 cycles while the cell with PVDF (16 μm) overcharges after 300 cycles,which is depictured in Fig.3j.LFP/Li half-cells with the T-20 and the T-30 composite separators are also assembled to investigate the cycle stability,which is depictured in Fig.S15 (Supporting information).The linear sweep voltammetry (LSV) is conducted on symmetric Li cells with the T-10 and the PVDF separators.As shown in Fig.S16 (Supporting information),the cell with T-10 and PVDF demonstrated nearly the same voltage sweep up to 4.5 V.In conclusion,the existence of talcum in PVDF has no effect on the electrochemical window.

    Aiming to investigate the electrochemical performance of the cell assembled with these separators at high temperature,batteries with LiFPO4cathode and PP,PVDF and T-10 separators are placed on the work station to explore more interface impedance information with open circuit voltage at 80 °C.The minimum semicircle distance is observed in the cell with T-10 composite separator among the three Nyquist curves,demonstrating the lowest transfer impedance as depictured in Fig.4a.The semicircle diameters of PP,PVDF and T-10 under 80 °C in Fig.4a are all smaller than those at room temperature as depictured in Fig.3e,demonstrating that the rising in temperature can speed up the transfer of lithium ions [55].The cycle property is conducted on LFP/Li batteries with PP,PVDF and T-10 separators at 80 °C.In Fig.4b,LFP/Li battery with T-10 separator works extremely stable at 80 °C over 300 cycles,delivering 112.8 mAh/g discharge capacity with 68% retention after 300 cycles.In contrast,LFP/Li battery with PVDF and PP exhibits a sharp decrease in discharge capacity after only 120 cycles.The stable performance of LFP/Li battery with T-10 at elevated temperature is attributed to the excellent thermal stability of talcum,which is confirmed in Fig.2c and Fig.S5.The coulombic efficiency of the cell with PP,PVDF and T-10 separators is depictured in Fig.4g,demonstrating that battery with T-10 shows a more stable and higher coulombic efficiency than those with PP and PVDF separators.The galvanostatic charging/discharging plots of the cell with PP,PVDF and T-10 separators at 1 C under 80 °C is verified in Figs.4c-e.For the initial cycle,the cell with the T-10 separator performs the discharge capacity of 165.92 mAh/g at 1 C under 80 °C,while 161.67 mAh/g and 163.69 mAh/g for PVDF and PP separator as demonstrated in Figs.4c-e,respectively.The 200th cycle galvanostatic charging/discharging plots of the cell with PP,PVDF and T-10 separators are depictured in Fig.S17 (Supporting information).The temperature is raised to 100 °C to investigate the cycle stability of battery with the T-10 at higher temperature as depictured in Fig.4f.The battery with T-10 composite separator retains 40 mAh/g after 150 cycles at 100 °C while half-cell with PP shows no discharge capacity after 80 cycles.

    The enhanced electrolyte uptake featured with sharply decreased contact angle as confirmed in Figs.2e and i is associated with the strong interaction between the talcum and the electrolyte.The strong interaction between the talcum and the electrolyte is verified with the DFT simulations as demonstrated in Fig.S18 (Supporting information).The commercial electrolyte is represented by ethylene carbonate (EC),dimethyl ethylene carbonate (DEC) and ethyl methyl carbonate (EMC).The results show that the adsorption energy values between the talcum and the electrolyte are -1.65 eV for talcum-EMC,-1.70 eV for talcum-EC and -1.64 eV for talcum-DEC,which are much larger than PVDF monomer/electrolyte (-0.02 ~-0.08 eV) as demonstrated in Fig.S19 (Supporting information).Owing to the strong affinity to EMC,EC and DEC,the separator doped with talcum shows much more superior electrolyte uptake and wettability when compared with the PP and the PVDF separators.The adsorption energy value of talcum-PVDF monomer (-1.65 eV) as demonstrated in Fig.S20 (Supporting information) is analogous with hydrogen bond strength (-0.01 ~-1.68 eV),and much larger than van der Waals forces (-0.004 ~-0.04 eV) [56],demonstrating the powerful interaction between the talcum and the PVDF.The optimized model structure of electrolyte through PVDF and T-10 separators are illustrated in Fig.S21 (Supporting information),respectively.The strong interaction between the talcum and the electrolyte contributes to the large amount of electrolyte absorption on the T-10 composite separator.In contrast,only few electrolyte molecule adsorption on the PVDF as depictured in Fig.S21.

    In summary,a polymer-based composite separator with high wettability and heat resistance is fabricated by doping the lamellated-clay (talcum) into PVDF.Owing to the strong adsorption energy between the talcum and the electrolyte,the PVDF/TM composite separator owns remarkable electrolyte wettability.The enhanced mechanical strength and toughness of PVDF/TM composite separator are associated with the strong adsorption energy between the talcum and the PVDF monomer and the superior thermal stability of the composite separator is attributed to the heatproof of talcum.The existence of talcum in PVDF/TM composite separator leads to the parallel ion channels that unify the direction of Li+flows,thus improving the discharge specific capacity.Especially,the cell with the T-10 composite separator reaches a remarkable discharge capacity of 91.7 mAh/g while PVDF of 56.3 mAh/g and PP of 51.4 mAh/g at 10 C,owns extremely small contact angle of 8° with commercial electrolyte while PVDF of 20°,achieves the mechanical strength of 33 MPa while PVDF of 15 MPa,and attains strain of 253% while PVDF of 107%,respectively.This work puts forward a novel material to open up the world of the high-rate and safer lithium metal batteries.

    Declaration of competing interest

    The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

    Acknowledgments

    This research is supported by the Science Foundation of National Key Laboratory of Science and Technology on Advanced Composites in Special Environments,and the National Natural Science Foundation of China (No.12002109).

    Supplementary materials

    Supplementary material associated with this article can be found,in the online version,at doi:10.1016/j.cclet.2021.12.079.

    最新的欧美精品一区二区| 男人和女人高潮做爰伦理| 日韩一区二区三区影片| 日韩欧美一区视频在线观看 | 国产高清有码在线观看视频| 亚洲欧美一区二区三区国产| 亚洲国产毛片av蜜桃av| 国产男女超爽视频在线观看| 最黄视频免费看| 精品久久国产蜜桃| 精品久久久精品久久久| 久久久久久久国产电影| 九草在线视频观看| 国产精品国产三级专区第一集| 精品午夜福利在线看| 男男h啪啪无遮挡| 久久精品久久久久久久性| 一级爰片在线观看| 免费观看av网站的网址| 菩萨蛮人人尽说江南好唐韦庄| 在线观看美女被高潮喷水网站| 国产成人aa在线观看| 少妇精品久久久久久久| 亚洲第一区二区三区不卡| 成人国产麻豆网| 国产精品三级大全| av国产精品久久久久影院| 午夜久久久在线观看| 免费看光身美女| 午夜免费男女啪啪视频观看| 人妻 亚洲 视频| 黄色欧美视频在线观看| 我的女老师完整版在线观看| 国产一区二区在线观看日韩| 一区二区av电影网| 18禁裸乳无遮挡动漫免费视频| 各种免费的搞黄视频| 日韩av免费高清视频| 我要看日韩黄色一级片| 久久99热这里只频精品6学生| videossex国产| 午夜久久久在线观看| 草草在线视频免费看| av免费观看日本| 多毛熟女@视频| 日本欧美国产在线视频| 男人添女人高潮全过程视频| 亚洲精品视频女| 国产精品无大码| 日韩欧美 国产精品| 日本黄色片子视频| 99久久综合免费| 一区二区三区免费毛片| 女性被躁到高潮视频| 人妻系列 视频| 午夜精品国产一区二区电影| 久久久久久久久久久丰满| 一级毛片aaaaaa免费看小| 欧美人与善性xxx| 成人免费观看视频高清| 欧美三级亚洲精品| 汤姆久久久久久久影院中文字幕| 少妇丰满av| 大码成人一级视频| 国产精品熟女久久久久浪| 一个人免费看片子| av网站免费在线观看视频| 亚洲av福利一区| 免费观看的影片在线观看| 97在线人人人人妻| 欧美区成人在线视频| 极品人妻少妇av视频| 六月丁香七月| 丝袜喷水一区| 男女啪啪激烈高潮av片| 欧美少妇被猛烈插入视频| 久久久久精品性色| 赤兔流量卡办理| 久久热精品热| av天堂久久9| 少妇 在线观看| 久热这里只有精品99| 边亲边吃奶的免费视频| 亚洲国产精品一区三区| 亚洲国产成人一精品久久久| 人体艺术视频欧美日本| 一边亲一边摸免费视频| 秋霞在线观看毛片| 免费大片黄手机在线观看| 成人黄色视频免费在线看| 天堂8中文在线网| 天堂俺去俺来也www色官网| 18+在线观看网站| 这个男人来自地球电影免费观看 | 一级毛片久久久久久久久女| 国产精品久久久久久精品古装| 国产毛片在线视频| 久久久久精品久久久久真实原创| 午夜老司机福利剧场| 精品亚洲乱码少妇综合久久| 黄色日韩在线| 自拍欧美九色日韩亚洲蝌蚪91 | 一区二区三区精品91| 国产高清国产精品国产三级| 晚上一个人看的免费电影| 国产在线免费精品| 人人妻人人澡人人看| 美女福利国产在线| 久久精品国产亚洲av天美| 国产一区二区三区综合在线观看 | 亚洲精品视频女| 成人影院久久| 国产欧美日韩一区二区三区在线 | 精品国产一区二区久久| 99久久精品国产国产毛片| 国产一区有黄有色的免费视频| 免费观看av网站的网址| 亚洲精品国产成人久久av| 一级黄片播放器| 国产伦理片在线播放av一区| 国产精品秋霞免费鲁丝片| 精品少妇内射三级| 国产高清三级在线| 午夜日本视频在线| 啦啦啦视频在线资源免费观看| 九九爱精品视频在线观看| 国产高清不卡午夜福利| 久久久久视频综合| 亚洲精品第二区| 伦精品一区二区三区| 国产熟女午夜一区二区三区 | 精品99又大又爽又粗少妇毛片| 免费av不卡在线播放| 七月丁香在线播放| 一级黄片播放器| 免费看光身美女| 亚洲国产av新网站| 国内精品宾馆在线| 人人妻人人爽人人添夜夜欢视频 | 亚洲欧美日韩另类电影网站| 岛国毛片在线播放| 一级片'在线观看视频| 国产黄色视频一区二区在线观看| 中文资源天堂在线| 亚洲av成人精品一二三区| 18禁在线无遮挡免费观看视频| 久久久久久久亚洲中文字幕| 一区二区三区精品91| av国产精品久久久久影院| 亚洲精品一区蜜桃| 一级,二级,三级黄色视频| 青青草视频在线视频观看| 18禁动态无遮挡网站| 亚洲成色77777| 十分钟在线观看高清视频www | 色视频www国产| 国产在线视频一区二区| 成人国产av品久久久| 免费看av在线观看网站| 人体艺术视频欧美日本| 丰满迷人的少妇在线观看| 久久久久久久大尺度免费视频| 久久久国产精品麻豆| 99久久中文字幕三级久久日本| 简卡轻食公司| 精品酒店卫生间| 免费不卡的大黄色大毛片视频在线观看| 成年人午夜在线观看视频| kizo精华| 桃花免费在线播放| 男人和女人高潮做爰伦理| 午夜精品国产一区二区电影| 亚洲丝袜综合中文字幕| 女人久久www免费人成看片| 成人毛片60女人毛片免费| 亚洲av男天堂| 亚洲精品第二区| 久久久久国产网址| 一边亲一边摸免费视频| 自线自在国产av| 亚洲国产精品一区二区三区在线| 嫩草影院新地址| 三上悠亚av全集在线观看 | 乱系列少妇在线播放| 人妻一区二区av| 亚洲欧美成人综合另类久久久| 一本大道久久a久久精品| 日韩欧美一区视频在线观看 | 乱码一卡2卡4卡精品| a级毛片在线看网站| 免费观看性生交大片5| 亚洲不卡免费看| 亚洲精品aⅴ在线观看| 狂野欧美激情性xxxx在线观看| 男人狂女人下面高潮的视频| 男的添女的下面高潮视频| 在线观看美女被高潮喷水网站| 国产乱人偷精品视频| 两个人的视频大全免费| 亚洲国产精品一区三区| 免费少妇av软件| 日产精品乱码卡一卡2卡三| 久久韩国三级中文字幕| a级一级毛片免费在线观看| 69精品国产乱码久久久| 成年人午夜在线观看视频| 久久久久久久久久成人| 亚洲av.av天堂| 久久精品夜色国产| av.在线天堂| 99九九线精品视频在线观看视频| 日韩视频在线欧美| 亚洲av成人精品一二三区| 欧美日韩av久久| 黄色配什么色好看| 欧美少妇被猛烈插入视频| 久久久久久久国产电影| 国产黄色免费在线视频| 能在线免费看毛片的网站| 久久毛片免费看一区二区三区| 国产极品粉嫩免费观看在线 | 啦啦啦啦在线视频资源| 午夜福利在线观看免费完整高清在| 成人影院久久| 中文字幕久久专区| 国产成人91sexporn| 亚洲欧美一区二区三区国产| 免费观看av网站的网址| 亚洲情色 制服丝袜| 国产乱人偷精品视频| 亚洲激情五月婷婷啪啪| 大香蕉97超碰在线| 亚洲欧美日韩东京热| 大片电影免费在线观看免费| 亚洲av在线观看美女高潮| 国内少妇人妻偷人精品xxx网站| 国产成人免费无遮挡视频| 日韩一区二区视频免费看| 少妇被粗大猛烈的视频| 秋霞在线观看毛片| 国产精品一区二区性色av| 国产综合精华液| 丝袜喷水一区| 日本色播在线视频| 99热6这里只有精品| 久久女婷五月综合色啪小说| 国产亚洲最大av| 国产深夜福利视频在线观看| 亚洲熟女精品中文字幕| 亚洲人与动物交配视频| 高清午夜精品一区二区三区| 少妇裸体淫交视频免费看高清| 国产精品麻豆人妻色哟哟久久| 少妇人妻一区二区三区视频| 秋霞在线观看毛片| 亚洲精品aⅴ在线观看| 在线观看免费高清a一片| 久久久精品免费免费高清| 视频区图区小说| 最近2019中文字幕mv第一页| 日韩熟女老妇一区二区性免费视频| 成人特级av手机在线观看| 又爽又黄a免费视频| 免费高清在线观看视频在线观看| 色婷婷久久久亚洲欧美| 精品国产露脸久久av麻豆| 99九九线精品视频在线观看视频| 久热这里只有精品99| 国产成人91sexporn| 久久精品久久久久久久性| 亚洲欧美精品自产自拍| 一级毛片我不卡| 久久av网站| 国产欧美另类精品又又久久亚洲欧美| 天堂俺去俺来也www色官网| 日韩成人伦理影院| 亚洲av福利一区| 欧美 日韩 精品 国产| 亚洲精品aⅴ在线观看| 免费大片18禁| 纯流量卡能插随身wifi吗| 三级国产精品欧美在线观看| 在线观看国产h片| 少妇 在线观看| 国产精品久久久久久久电影| 嫩草影院入口| 免费大片黄手机在线观看| av一本久久久久| 一个人免费看片子| 色婷婷av一区二区三区视频| 在线亚洲精品国产二区图片欧美 | 亚洲精品国产成人久久av| 成年av动漫网址| 欧美区成人在线视频| 亚洲人与动物交配视频| av在线老鸭窝| 精品国产一区二区三区久久久樱花| 久久久久精品久久久久真实原创| 久久人人爽av亚洲精品天堂| 极品教师在线视频| 欧美+日韩+精品| 免费观看的影片在线观看| 国产欧美日韩精品一区二区| 亚洲精品自拍成人| 综合色丁香网| 老熟女久久久| 国产av码专区亚洲av| 国产男女内射视频| 麻豆精品久久久久久蜜桃| 伊人久久精品亚洲午夜| 亚洲美女视频黄频| 2021少妇久久久久久久久久久| 国产伦精品一区二区三区四那| 国产亚洲5aaaaa淫片| 高清不卡的av网站| 伊人久久精品亚洲午夜| 色视频在线一区二区三区| h视频一区二区三区| av免费在线看不卡| 又爽又黄a免费视频| 久久精品国产自在天天线| 国产淫片久久久久久久久| 人人妻人人爽人人添夜夜欢视频 | 亚洲av成人精品一区久久| 人妻制服诱惑在线中文字幕| 最黄视频免费看| 久久久久网色| 肉色欧美久久久久久久蜜桃| 精品久久久精品久久久| 国产av精品麻豆| 久久97久久精品| 尾随美女入室| 国产高清国产精品国产三级| 午夜视频国产福利| 精品久久国产蜜桃| 国产伦精品一区二区三区四那| 亚洲精品色激情综合| 亚洲精品一区蜜桃| 国产成人91sexporn| 精品99又大又爽又粗少妇毛片| 国产精品无大码| 99热全是精品| 免费人妻精品一区二区三区视频| 建设人人有责人人尽责人人享有的| 女人久久www免费人成看片| 99久久精品热视频| 一级黄片播放器| 少妇高潮的动态图| 一级a做视频免费观看| 另类精品久久| 免费观看av网站的网址| 日韩成人av中文字幕在线观看| 黑人巨大精品欧美一区二区蜜桃 | 五月玫瑰六月丁香| 国产精品女同一区二区软件| 亚洲国产欧美日韩在线播放 | 噜噜噜噜噜久久久久久91| 美女国产视频在线观看| 久久久久国产精品人妻一区二区| 精品99又大又爽又粗少妇毛片| 国产高清不卡午夜福利| 国产视频首页在线观看| 建设人人有责人人尽责人人享有的| 十八禁网站网址无遮挡 | 亚洲高清免费不卡视频| videos熟女内射| 久久99精品国语久久久| 亚洲成人手机| 少妇的逼水好多| 日韩不卡一区二区三区视频在线| 大片免费播放器 马上看| 欧美变态另类bdsm刘玥| 美女主播在线视频| 国产精品99久久99久久久不卡 | 高清毛片免费看| 欧美xxⅹ黑人| av卡一久久| 五月天丁香电影| 国模一区二区三区四区视频| 少妇被粗大的猛进出69影院 | 国产精品熟女久久久久浪| 久久毛片免费看一区二区三区| 色婷婷av一区二区三区视频| 丝袜在线中文字幕| 一级,二级,三级黄色视频| videossex国产| 成年人免费黄色播放视频 | 丰满饥渴人妻一区二区三| 乱人伦中国视频| 精品国产一区二区三区久久久樱花| 精品少妇久久久久久888优播| 国产精品国产三级国产专区5o| 午夜免费观看性视频| 国产极品天堂在线| 97在线视频观看| 日韩 亚洲 欧美在线| 午夜免费男女啪啪视频观看| 成人美女网站在线观看视频| 日韩 亚洲 欧美在线| 日韩欧美一区视频在线观看 | 99热国产这里只有精品6| 免费av中文字幕在线| 国模一区二区三区四区视频| 如何舔出高潮| 国产在线男女| 国产精品成人在线| 久久99热这里只频精品6学生| 国产乱来视频区| 日韩在线高清观看一区二区三区| 如日韩欧美国产精品一区二区三区 | 亚洲av.av天堂| 午夜91福利影院| 麻豆成人av视频| √禁漫天堂资源中文www| 中文字幕人妻熟人妻熟丝袜美| 亚洲欧美精品专区久久| 久久国产精品大桥未久av | a级毛色黄片| 久久久久久久久久久免费av| 国产精品人妻久久久影院| 99热全是精品| 亚洲,欧美,日韩| 最近最新中文字幕免费大全7| 六月丁香七月| 亚洲国产色片| 久久国内精品自在自线图片| 在线观看免费视频网站a站| 婷婷色综合大香蕉| av不卡在线播放| 欧美+日韩+精品| 97在线视频观看| 久久精品熟女亚洲av麻豆精品| 又大又黄又爽视频免费| 欧美 亚洲 国产 日韩一| 国产午夜精品一二区理论片| 日韩制服骚丝袜av| 日韩一区二区三区影片| 欧美日韩综合久久久久久| 观看美女的网站| 久久久精品免费免费高清| 色吧在线观看| 男人狂女人下面高潮的视频| 日韩av不卡免费在线播放| 亚洲精品国产av成人精品| 欧美人与善性xxx| 黑人猛操日本美女一级片| videos熟女内射| 最新中文字幕久久久久| 国产日韩欧美视频二区| 精品熟女少妇av免费看| 美女福利国产在线| 99国产精品免费福利视频| 有码 亚洲区| av在线app专区| 26uuu在线亚洲综合色| 日韩一区二区三区影片| 人妻夜夜爽99麻豆av| 大片免费播放器 马上看| 在线天堂最新版资源| av女优亚洲男人天堂| 亚洲精品乱码久久久久久按摩| 亚洲精品乱码久久久v下载方式| 男女啪啪激烈高潮av片| 视频区图区小说| 欧美日韩视频高清一区二区三区二| 亚洲三级黄色毛片| 最黄视频免费看| 麻豆乱淫一区二区| 成人毛片60女人毛片免费| 午夜福利影视在线免费观看| 岛国毛片在线播放| 久久99热这里只频精品6学生| 日韩在线高清观看一区二区三区| 午夜久久久在线观看| 涩涩av久久男人的天堂| 免费播放大片免费观看视频在线观看| 少妇熟女欧美另类| 成人毛片60女人毛片免费| 午夜老司机福利剧场| 岛国毛片在线播放| 亚洲欧洲精品一区二区精品久久久 | 男女无遮挡免费网站观看| 菩萨蛮人人尽说江南好唐韦庄| 免费看av在线观看网站| 男女啪啪激烈高潮av片| 老司机影院成人| 插逼视频在线观看| 国产av国产精品国产| a级片在线免费高清观看视频| 国产精品人妻久久久影院| 又爽又黄a免费视频| 亚洲综合色惰| 国产伦精品一区二区三区四那| 在线观看美女被高潮喷水网站| 波野结衣二区三区在线| 精品人妻熟女av久视频| 亚洲熟女精品中文字幕| av在线老鸭窝| 欧美性感艳星| 99视频精品全部免费 在线| 日韩 亚洲 欧美在线| 777米奇影视久久| 国产精品不卡视频一区二区| 六月丁香七月| 久久热精品热| 国产精品蜜桃在线观看| 亚洲精品色激情综合| 欧美老熟妇乱子伦牲交| 国产免费一区二区三区四区乱码| 22中文网久久字幕| 久热久热在线精品观看| 色婷婷av一区二区三区视频| 另类亚洲欧美激情| 啦啦啦视频在线资源免费观看| 永久网站在线| 国产精品久久久久久精品古装| 亚洲av男天堂| 国产精品不卡视频一区二区| 99九九在线精品视频 | 嘟嘟电影网在线观看| 丰满人妻一区二区三区视频av| 日韩欧美一区视频在线观看 | 国产成人一区二区在线| 国产成人a∨麻豆精品| 永久免费av网站大全| 在线观看www视频免费| 99久久精品热视频| av视频免费观看在线观看| 久久国产亚洲av麻豆专区| 我的老师免费观看完整版| 免费看日本二区| 亚州av有码| 国产成人一区二区在线| 美女cb高潮喷水在线观看| 国产成人精品久久久久久| 青春草国产在线视频| 亚洲av成人精品一二三区| 午夜免费观看性视频| 高清不卡的av网站| 成人毛片a级毛片在线播放| 国产亚洲一区二区精品| 精品国产一区二区久久| 久久久精品免费免费高清| 午夜福利视频精品| 日韩av不卡免费在线播放| 蜜桃久久精品国产亚洲av| 国产亚洲午夜精品一区二区久久| 伦理电影大哥的女人| 欧美日韩av久久| 欧美日韩视频精品一区| 免费少妇av软件| 黄色怎么调成土黄色| 日本免费在线观看一区| 国产亚洲一区二区精品| 18禁裸乳无遮挡动漫免费视频| 久久av网站| 我要看黄色一级片免费的| 久久99精品国语久久久| 国产色爽女视频免费观看| 天堂8中文在线网| 全区人妻精品视频| 国产无遮挡羞羞视频在线观看| 十分钟在线观看高清视频www | 日韩av免费高清视频| 大香蕉久久网| 水蜜桃什么品种好| 一区二区av电影网| 蜜桃在线观看..| 能在线免费看毛片的网站| 亚洲精品日韩在线中文字幕| 久久精品国产a三级三级三级| 免费av中文字幕在线| av天堂中文字幕网| 一级黄片播放器| 色吧在线观看| 精品人妻熟女毛片av久久网站| 2021少妇久久久久久久久久久| 亚洲天堂av无毛| 成年女人在线观看亚洲视频| 国产精品久久久久久av不卡| 久久久亚洲精品成人影院| 亚洲国产精品国产精品| av天堂久久9| 欧美三级亚洲精品| 欧美日韩亚洲高清精品| 高清av免费在线| 精品酒店卫生间| 在线免费观看不下载黄p国产| 色婷婷av一区二区三区视频| 色5月婷婷丁香| 色婷婷久久久亚洲欧美| 五月伊人婷婷丁香| 日韩精品免费视频一区二区三区 | 美女脱内裤让男人舔精品视频| 日韩一区二区三区影片| av免费在线看不卡| 伦精品一区二区三区| 亚洲四区av| 成人黄色视频免费在线看| 欧美97在线视频| 中文字幕av电影在线播放| 日韩一本色道免费dvd| 成年av动漫网址| 成人特级av手机在线观看| 夫妻性生交免费视频一级片| 国产中年淑女户外野战色| 欧美日韩精品成人综合77777| 夜夜爽夜夜爽视频| 91在线精品国自产拍蜜月| 全区人妻精品视频| 人妻少妇偷人精品九色| 男女啪啪激烈高潮av片| 国产亚洲一区二区精品| 观看免费一级毛片| 亚洲美女视频黄频|