Li_(1.5)Al_(0.5)Ge_(1.5)P_3O_(12)/高分子固体电解质表界面结构与分子运动的固体NMR研究
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摘要
相对于传统锂离子电池,全固态锂电池具有安全性能高、循环寿命长、能量密度高等优点,是目前锂电池研究领域的热点之一.作为全固态锂电池的核心组成部分,固体电解质是实现全固态锂电池高性能的关键材料.本文设计了一种高分子-锂盐-陶瓷的复合物固体电解质.通过多种固体核磁共振(NMR)方法研究了该材料中高分子-陶瓷的界面层结构和界面高分子链段的分子运动.
All solid state lithium-ion batteries have the advantages of high safety, long cycle life and high energy density, as compared with the conventional lithium-ion batteries, and have been attracting more and more research interest. Solid electrolyte is a crucial component of all solid state lithium-ion batteries, which largely determine the performance of the batteries. In this work, a polymer-lithium-ceramics complex was designed and synthesized. The structure and dynamics of the polymer-ceramic interface was studied with solid-state NMR techniques.
All solid state lithium-ion batteries have the advantages of high safety, long cycle life and high energy density, as compared with the conventional lithium-ion batteries, and have been attracting more and more research interest. Solid electrolyte is a crucial component of all solid state lithium-ion batteries, which largely determine the performance of the batteries. In this work, a polymer-lithium-ceramics complex was designed and synthesized. The structure and dynamics of the polymer-ceramic interface was studied with solid-state NMR techniques.
引文
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[28]CALUCCI L,GALLESCHI L,GEPPI M,et al.Structure and dynamics of flour by solid state NMR:effects of hydration and wheat aging[J].Biomacromolecules,2004,5(4):1536-1544.
[29]BRUS J,DYBAL J,SCHMIDT P,et al.Order and mobility in polycarbonate-poly(ethylene oxide)blends studied by solid-state NMR and other techniques[J].Macromolecules,2000,33(17):6448-6459.
[2]TARASCON J M,ARMAND M.Issues and challenges facing rechargeable lithium batteries[J].Nature,2001,414(6861):359-367
[3]ROBINSON A L,JANEK J.Solid-state batteries enter EV fray[J].MRS Bulletin,2014,39(12):1046-1047.
[4]KAMAYA N,HOMMA K,YAMAKAWA Y,et al.A lithium superionic conductor[J].Nat Mater,2011,10(9):682-686.
[5]TREVEY J E,GILSDORF J R,MILLER S W,et al.Li2S-Li2O-P2S5 solid electrolyte for all-solid-state lithium batteries[J].Solid State Ionics,2012,214:25-30.
[6]SMITHA B,SRIDHAR S,KHAN A A.Solid polymer electrolyte membranes for fuel cell applications—a review[J].J Membrane Sci,2005,259(1,2):10-26.
[7]MANUEL STEPHAN A,NAHM K S.Review on composite polymer electrolytes for lithium batteries[J].Polymer,2006,47(16):5952-5964.
[8]LUNTZ A C,VOSS J,REUTER K.Interfacial challenges in solid-state Li ion batteries[J].J Phys Chem Lett,2015,6(22):4599-4604.
[9]ZHU Y Z,HE X F,MO Y F.Origin of outstanding stability in the lithium solid electrolyte materials:insights from thermodynamic analyses based on first-principles calculations[J].ACS Appl Mater Interfaces,2015,7(42):23685-23693.
[10]SAKUDA A,HAYASHI A,OHTOMO T,et al.All-solid-state lithium secondary batteries using Li Co O2 particles with pulsed laser deposition coatings of Li2S-P2S5 solid electrolytes[J].J Power Sources,2011,196(16):6735-6741.
[11]OHTA N,TAKADA K,ZHANG L Q,et al.Enhancement of the high-rate capability of solid-state lithium batteries by nanoscale interfacial modification[J].Adv Mater,2006,18(17):2226-2229.
[12]SAKUDA A,HAYASHI A,TATSUMISAGO M.Interfacial observation between Li Co O2 electrode and Li2S-P2S5 solid electrolytes of all-solid-state lithium secondary batteries using transmission electron microscopy[J].Chem Mater,2010,22(3):949-956.
[13]OHTA N,TAKADA K,SAKAGUCHI I,et al.Li Nb O3-coated Li Co O2 as cathode material for all solid-state lithium secondary batteries[J].Electrochem Commun,2007,9(7):1486-1490.
[14]DOKKO K,HOSHINA K,NAKANO H,et al.Preparation of Li Mn2O4 thin-film electrode on Li1+xAlxTi2-x(PO4)3 NASICON-type solid electrolyte[J].J Power Sources,2007,174(2):1100-1103.
[15]HOSHINA K,YOSHIMA K,KOTOBUKI M,et al.Fabrication of Li Ni0.5Mn1.5O4 thin film cathode by PVP sol-gel process and its application of all-solid-state lithium ion batteries using Li1+xAlxTi2-x(PO4)3 solid electrolyte[J].Solid State Ionics,2012,209,210(8):30-35.
[16]KOTOBUKI M,HOSHINA K,KANAMURA K.Electrochemical properties of thin Ti O2 electrode on Li1+xAlxGe2-x(PO4)3 solid electrolyte[J].Solid State Ionics,2011,198(1):22-25.
[17]ZHOU W D,WANG S F,LI Y T,et al.Plating a dendrite-free lithium anode with a polymer/ceramic/polymer sandwich electrolyte[J].J Am Chem Soc,2016,138(30):9385-9388.
[18]TIKEKAR M D,CHOUDHURY S,TU Z Y,et al.Design principles for electrolytes and interfaces for stable lithium-metal batteries[J].Nature Energy.2016,1(9):16114-16120.
[19]MAIER J.Ionic conduction in space charge regions[J].Prog Solid State Chem,1995,23(3):171-263.
[20]ONG S P,MO Y F,RICHARDS W D,et al.Phase stability,electrochemical stability and ionic conductivity of the Li10±1MP2X12(M=Ge,Si,Sn,Al or P,and X=O,S or Se)family of superionic conductors[J].Energy Environ Sci,2012,6(1):148-156.
[21]WENZEL S,WEBER D A,LEICHTWEISS T,et al.Interphase formation and degradation of charge transfer kinetics between a lithium metal anode and highly crystalline Li7P3S11,solid electrolyte[J].Solid State Ionics,2016,286:24-33.
[22]WENZEL S,RANDAU S,LEICHTWEI?T,et al.Supporting information for:direct observation of the interfacial in-stability of the fast ionic conductor Li10Ge P2S12 at the lithium metal anode[J].Chem Mater,2016,28(7):2400-2407
[23]BOTTKE P,RETTENWANDER D,SCHMIDT W,et al.Ion dynamics in solid electrolytes:NMR reveals the elementary steps of Li+hopping in the garnet Li6.5La3Zr1.75Mo0.25O12[J].Chem Mater,2015,27(19):6571-6582.
[24]MICHAN A L,LESKES M,GREY C P.Voltage dependent solid electrolyte interphase formation in silicon electrodes:Monitoring the formation of organic decomposition products[J].Chem Mater,2016,28(1):385-398.
[25]HE K,WANG Y H,ZU C K,et al.High-temperature X-ray analysis of phase evolution in lithium ion conductor Li1.5Al0.5Ge1.5(PO4)3[J].Mater Charact,2013,80:86-91.
[26]JAEGER C,HEMMANN F.EASY:A simple tool for simultaneously removing background,deadtime and acoustic ringing in quantitative NMR spectroscopy.Part II:Improved ringing suppression,application to quadrupolar nuclei,cross polarisation and 2D NMR[J].Solid State Nucl Magn Reson,2014,63-64:13-19.
[27]JAEGER C,HEMMANN F.EASY:A simple tool for simultaneously removing background,deadtime and acoustic ringing in quantitative NMR spectroscopy—Part I:Basic principle and applications[J].Solid State Nucl Magn Reson,2014,57-58:22-28.
[28]CALUCCI L,GALLESCHI L,GEPPI M,et al.Structure and dynamics of flour by solid state NMR:effects of hydration and wheat aging[J].Biomacromolecules,2004,5(4):1536-1544.
[29]BRUS J,DYBAL J,SCHMIDT P,et al.Order and mobility in polycarbonate-poly(ethylene oxide)blends studied by solid-state NMR and other techniques[J].Macromolecules,2000,33(17):6448-6459.