Special polymers. 1. Polymer electrolytes 2. Conjugated polymers and organic electronics. Jorge Morgado, IST_2012

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1 Special polymers 1. Polymer electrolytes 2. Conjugated polymers and organic electronics Jorge Morgado, IST_2012

2 Dissolving an ionic salt in water

3 Polymer electrolytes vs polyelectrolytes Polymer electrolytes = polymer (solvent) + ionic salt SolvaHng polymers: PEO (Tg - 60 o C, Tm 65 o C) PPO (amorphous) Polyphosphazenes: O P O N n O O O CH 3 n Tg=- 83 o C Upon addi2on of ionic salt: Tg and viscosity increase O O

4

5 Non solva2ng polymers: PMO PTMO (CH 2 O) n (CH 2 CH 2 CH 2 O) n Spacing and conformahonal flexibility of the monomers Solva2on interachon between the oxygen atom (Lewis acid) and the cahons (Lewis base) Ca2ons: metals and lanthanides Anions: CF 3 SO 3- and (CF 3 SO 2 ) 2 N - (suppresses crystallinity in PEO/Li + ) CaHons act as transient cross- linking agents

6 Samples (films) prepara2on: 1. Mixed soluhon followed by solvent evaporahon (solvent cashng) 2. AddiHon of the ionic salt to the polymer melt 3. Mixing of the solid at low temperature followed by pressing When using (semi)crystalline polymers, such as PEO, there may be formed crystalline phases containing the salt. Salt is distributed between crystalline and amorphous domains Ionic conduchvity due to the salt in the amorphous regions (only?).

7 The most studied system: PEO + salt

8 Structure of crystalline PEO 6 :LiAsF 6 Thin lines indicate coordinahon around the Li+ cahon. Blue spheres, lithium; white spheres, arsenic; magenta, fluorine; green, carbon; red, oxygen.

9 Ionic conduc2vity Processes: SolvaHon and ionic mobility In order to maximize ions concentra8on: Polymers with high dielectric constant Salts with low la;ce energy σ = i n i Z i In conven8onal solid electrolytes (crystalline materials) (RbAg 4 I 5 (σ RT 0.2 S/cm); Rb 4 Cu 16 I 7- x Cl 13- x (σ RT 1 S/cm) µ i σ = σ 0 e E a RT

10 Ionic conduc2vity For polymer electrolytes: Vogel, Tamman and Fulcher (VTF) equa8on A - constant, propor8onal to the ionic charge carriers concentra8on T 0 temperature at which the configura8onal entropy is zero, (in general varies from Tg- 50 to Tg- 20 o C) VTH equa8on is equivalent to the empirical WLF equa8on (good fit from Tg up to Tg+100 oc) log η η g = σ = A T 1 2 e 17.44(T Tg) (T Tg) = log σ σ g = log a T B T T 0

11 Ionic conduc2vity

12 Ionic conduc2vity

13 Ionic conduc2vity The equivalence between VTF and WLF equa8ons means that the ionic conductance is associated to structural movements of the polymer chains transient cross- links. Both VTF and WLF equa8ons rely on the concept of free volume. The VTF equa8on can be derived from the configura8onal entropy model.

14 Room temperature ionic conduc2vity Polymer electrolyte Polymer Electrolyte

15 Requirements for applica:ons in ba5eries (- 40 to 70 o C): σ in the range 10-4 to 10-3 S/cm Thermal and dimensional stabilityl Chemical compa8bility with the electrode materials Electrochemical stability window Lithium ba5eries Li(s)/Polymer electrolyte/cathode Cathode- Composite materials (V 6 O 13, TiO 2, )

16 Crystalline polymer electrolytes For 30 years it has been accepted that ionic conduchvity in polymer electrolytes occurred exclusively in the amorphous phase, above the glass transihon temperature Tg. Crystalline polymer electrolytes were considered to be insulators. But recent studies have shown that this is not the case: the 6:1 crystalline complexes PEO 6 :LiXF 6 ; X = P, As, Sb demonstrate ionic conduchvity. The Li + ions reside in tunnels formed by the polymer chains. ZLATKA GADJOUROVA, YURI G. ANDREEV, DAVID P. TUNSTALL & PETER G. BRUCE, Ionic conduchvity in crystalline polymer electrolytes, Nature 412, (02 August 2001);

17 Structure of crystalline PEO 6 :LiAsF 6 Thin lines indicate coordinahon around the Li + cahon. Blue spheres, lithium; white spheres, arsenic; magenta, fluorine; green, carbon; red, oxygen

18 Ionic conduchvity sigma (S cm - 1 ) of amorphous (open circles) and crystalline (filled circles) PEO 6 :LiSbF 6 as a funchon of temperature

19 References: Applica8ons of Electroac8ve Polymers, ed. Bruno Scrosa8, Chapman&Hall, M.A. Ratner e D.F. Shriver, Chem. Rev. 88, (1988). M.A. Ratner e A. Nitzan, Faraday Discuss. Chem. Soc. 88, (1989). B.L. Papke, M.A. Ratner e D.F. Shriver, J. Electrochem. Soc. 129, (1982).

20 Conjugated polymers Polyacetylene H H H H Trans- polyaceylene

21 Conjugated polymers Trans- polyacetylene Repeat unit

22 Conjugated polymers Uniform infinit chain of trans- polyacetylene Delocalized π orbitals

23 Conjugated polymers Real trans- polyacetylene π electronic density is not uniform Bond alternahon LocalizaHon of single and double bonds (Peierls transihon) Energy gap in the π band Metalic state (delocalized electrons) LUMO HOMO Semiconductor! - OpHcs - Electronics - Doping InsulaHng sate

24 Conjugated polymers Silicon_typical semiconductor

25 Conjugated polymers Insoluble conjugated polymers

26 Conjugated polymers Soluble conjugated polymers

27 References

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