CH5715 Energy Conversion and Storage. Electrolytes. For lecture notes: energy-conversion-and-storage/
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1 CH5715 Energy Conversion and Storage Electrolytes For lecture notes: energy-conversion-and-storage/ Textbook Solid State Electrochemistry Cambridge - P. G. Bruce
2 Electrolytes Solution Polymer Ceramic Solid electrolyte Physical aspects of solid electrolytes
3 salt + solvent solution -ve DG DG = DH TDS DS of salt increases Solution Electrolytes DS of solvent decreases Overall DS positive but still small Dissolution depends on enthalpy changes NaCl does not dissolve in hexane
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5 Aprotic
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7 Anions less strongly solvated; barely solvated in non-aqueous solvents. First: ions interact with the solvent molecules immediately surrounding them ion-solvent interactions Second: ions interact with each other. Around any ion there will be an atmosphere of oppositely charged ions. Net negative charge around each cation will interact electrostatically with it lower energy. This is termed Debye-Hückel ion atmosphere ion-ion interactions
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9 Electrolytes Polymer electrolytes are particularly promising-safety However, liquids now widely commercialised in solid state batteries. Organic electrolyte encapsulated in polymer mesh
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12 J.B. Goodenough and Y.S. Kim Chem. Mater., 22, (2010)
13 Electrolyte characteristics for Batteries 1) Large electrolyte potential window Eg so does not decompose across potential range: 2) Retention of the electrode/electrolyte interface during cycling when the electrode particles are changing their volume. 3) A Li -ion conductivity s Li >10-4 S/cm over the temperature range of battery operation. 4) An electronic conductivity s e <10-10 S/cm. 5) A transference number s Li /s total ~1 6) Chemical stability over ambient temperature ranges and temperatures in the battery under high power. 7) Chemical stability with respect to the electrodes, including the ability to form rapidly a passivating solid/electrolyte-interface (SEI) layer. 8) Safe materials, i.e., preferably nonflammable and nonexplosive if short-circuited. 9) Low toxicity and low cost.
14 Polymer Electrolytes Schematic representations of polymer electrolyte networks. a, Pure (dry) polymer consisting of entangled chains, through which the Li ions (red points) move assisted by the motion of polymer chains. b, A hybrid (gel) network consisting of a semicrystalline polymer, whose amorphous regions are swollen in a liquid electrolyte, while the crystalline regions enhance the mechanical stability. c, A poly-olefin membrane (Celgard for instance) in which the liquid electrolyte is held by capillaries.
15 1 PEO-LiCF 3 SO 3 ; 2 new solutes with high-dissociation PEO-Li [(CF 3 SO 2 ) 2 N] bis(trifluoromethanesulfone)imide (TFSI) 3 low-tg combination polymer; 4 plasticized polymer electrolyte PEO-Li[(CF 3 SO 2 ) 2 N] +25% w/w PEG-dimethylether (mol wt, 250) 5,6 liquid crystalline polymer electrolytes 7 gel-type polymer (X-linked PEO-dimethacrylate- Li [(CF 3 SO 2 ) 2 N]-PC 70%); 8 liquid electrolyte PC/DME LiCF 3 SO 3 ; trifluoromethanesulfonate 9 liquid electrolyte EC/DMC-LiPF 6 at low temperature ; 10 gel electrolyte P(VDF-HFP)/EC/DMC-LiPF 6.
16 Local Coordination
17 Crab-like motion assisted by chains Solid State Electrochemistry Bruce
18 Crystalline vs Amorphous Polymer Electrolytes
19 Polymer Electrolytes do form Crystalline Phases with salts
20 Crystal Structure
21 Crystalline polymer electrolytes PEO6:LiAsF6 P. G. Bruce et al. Nature 398, 72 (1999) P. G. Bruce et al. Nature 412, 520 (2001); P. G. Bruce et al. Nature 433, 50 (2005).
22 Note MWt 1000 Xlline vs 100,000 Amorphous Zlatka Gadjourova, Yuri G. Andreev, David P. Tunstall* & Peter G. Bruce
23 Putting together a lithium battery
24 CH5715 Energy Conversion and Storage Ionic Conduction 2 John T.S. Irvine Room 216 jtsi@st-and.ac.uk
25 Electrolytes Polymer electrolytes are particularly promising-safety However, liquids now widely commercialised in solid state batteries. Organic electrolyte encapsulated in polymer mesh Solid electrolytes not widely used now Considerable interest in incorporating batteries into printed circuit boards - crystalline electrolytes LiI formed in situ has been used, similar to AgI
26 Ion-Conducting Membranes Ionic Conductivity (Scm-1) Ionic crystals < Solid Electrolytes ceramic membranes Ion-conducting polymers Strong liquid electrolytes ne = f(t) Nernst Einstein relation m= qd/kt.
27 SOLID ELECTROLYTES
28 Ionic Radii
29 (S/cm) T ( C) E-3 1E-4 1E E-3 BaH2 8-YSZ 10-YSZ 10-ScSZ CGO20 CGO10 Nd doped BaCeO E-4 1E /T (1/K) Verbraeken Nature Materials
30 CRYSTALLINE IONIC CONDUCTORS Defects in solids Ionic migration in solids Fast ion conductors Examples of Solid Electrolytes
31
32 Schottky Vacancies
33 Point defects and cation migration
34 Intrinsic Conductivity [VNa ][VCl ] N V2 K 2 [ Na ][Cl ] N E f = Energy of formation for VNa and VCl K = C exp( E f / kt ) N V N C exp( E f / kt ) C exp( E f / 2 kt )
35 Extrinsic conductivity Aliovalent doping eg NaCl 2 Na+ Cd2+ + VNaZrO2 2 Zr4+ 2 Y3+ + VO2+ CaF2 Ca2+ Y3+ + FI-
36 Na Cl Cl Em+ ½ Ef Na Log(sT) Em Cl Na Cl 1/T Jump mechanism in 3d space Influence of dopants on conductivity behaviour in NaCl
37 Vacancy and Interstitial Conduction Mechanisms Interstitialcy mechanism
38 Ionic Migration/Ionic Conductivity Ionic Conductivity (Scm-1) Ionic crystals < Solid Electrolytes Strong liquid electrolytes ne = f(t) Nernst Einstein relation m= qd/kt.
39
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41 m m m m m m
42 Ionic hopping model Ea d------arrhenius equation T A exp( Ea / kt ) A - relates to number of carriers per unit volume, a02, jump frequency Ea = Activation Energy
43 Ionic Conductivity q H m 2 N VO (1 VO )a0 0 exp S S kt kt 2 Equation for conductivity contains number of vacancies plus a term which indicates how easily they move through the crystal lattice. DHm is migration enthalpy Energy DHm Position Ions jump from site to site Requires a vacant site to jump into Jumps biased by electric field Jumps require thermal energy to get over energy barrier. Need low DHm for high ionic conductivity
44 Electrolytic domain Log [defect] VO e h Log PO2 Log [conductivity] Electrons and holes have higher mobilities than ions Variable valence metal ions (e.g. transition metals) are bad for solid oxide electrolytes n p ionic domain Log PO2
45 LaGaO3 Oxide ion electrolyte La0.8Sr0.2Ga0.9Mg0.1O? VO oxide ion conduction 2VO +1/2O2 OOX + 2h+ Below 300oC in air electronic
46 Ionic transference number tion ion ion el For a SOFC electrolyte working over a range of PO2 cathode tion t d ln PO 2 ion anode cathode O2 ln P ln P anode O2 Need <tion> to be close to 1 e.g.>0.99
47 In proton conductors there is a temperature gap where proton conduction is too low The Norby Gap T. Norby, Solid State Ionics 125 (1999) 1
48 SOLID ELECTROLYTES
49 Structure of Beta-Alumina b b
50 b-alumina M2O.nX2O3 - M - Alkali, Cu, Ag, H3O, X - Al, Ga, Fe NaAl11O17 ideal Na - b (8-11), b"(5-7) Structure consists of spinel blocks separated by less dense layers - conduction planes. 2 dimensional Na conductor Ea ~ 0.16 ev
51 Beta battery Na/S operates at oC
52 P
53 Zebra battery
54 Li ion Conductors Best are 1-2 orders of magnitude less conductive than Na - alumina, ie Scm-1 Li3N - layered structure Li, LiN2 Li alumina Li0.5La0.5TiO3 Various Li silicate frameworks LISICON Li polymer electrolytes are good alternative.
55 ANION CONDUCTORS Fluorite anion conductors PbF2, SnPbF Scm-1 at room temperature LaxSr1-xF2 ZrO2 based ion conductors, Y2O3 and CaO doping Conductivities 10-2 Scm-1 at 1000oC
56 Question The ionic resistance of 1%CdCl2 doped NaCl decreases with temperature according to Arrhenius behaviour, with an increase in activation energy for conduction from 0.7eV to 1.3 ev at 500oC as temperature increases. Sketch this on a schematic Arrhenius type plot and suggest why this change occurs. Also add to this diagram a plot showing how the traces for 2% and 3% doping of NaCl with CdCl2 would appear.
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