Modeling the next battery generation: Lithium-sulfur and lithium-air cells
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1 Modeling the next battery generation: Lithium-sulfur and lithium-air cells D. N. Fronczek, T. Danner, B. Horstmann, Wolfgang G. Bessler German Aerospace Center (DLR) University Stuttgart (ITW) Helmholtz Institute Ulm for Electrochemical Energy Storage (HIU)
2 Research profile: Computational battery technology Lithium-ion technology Post-lithium-ion cells LiFePO 4 batteries: Electrochemistry and impedance e Li + Lithium-sulfur cells: Redox chemistry and transport Understanding and optimization of physicochemical behavior Analysis of cycling properties and chemical reversibility Thermal management and runaway risk Understanding and optimization of thermal and safety behavior Lithium-air cells: Multi-phase chemistry and reversibility Improvement of porous air electrode Multi-scale and multi-physics modeling and numerical simulation Sliede 2
3 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 3
4 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 4
5 Li-S and Li-O: Challenges Complex multi-phase management Li-S: Solid reactant S 8 and product Li 2 S, solid precipitates Li-O: Solid, liquid and gas phase involved Complex chemistry Li-S: Polysulfide ion intermediates Li-O: Oxygen reduction as traditional problem of electrochemistry Low cycleability, low efficiency Computational modeling for understanding and optimization Sliede 5
6 1D/2D generic modeling framework Electrochemical cell of up to seven layers Each layer consists of arbitrary number of solid, liquid and/or gaseous bulk phases Each layer can contain an arbitrary number of interfaces (phase boundaries) Each bulk phase consists of arbitrary number of chemical species Chemistry takes place at interfaces Transport mechanisms (liquid, solid, gas) Continuum (homogenization) approach J. P. Neidhardt, D. N. Fronczek, T. Jahnke, T. Danner, B. Horstmann and W. G. Bessler, J. Electrochem. Soc., submitted (2012). Sliede 6
7 Chemical reactions at interfaces Mass-action kinetics describes chemical source terms ν stoichiometric coefficient k reaction rate constant c concentration of reactants Rate constants described by modified Arrhenius expression. Reverse rate follows from thermodynamic consistency. Preexponential factor Temperature dependence (Activation energy E act ) Potential dependence (Half-cell potential φ) Sliede 7
8 Multi-phase management The volume fraction ε i of each phase i depends on time ε volume fraction ρ density R chemical formation rate M molar mass Volume fractions sum up to one. Def. of compressible phase necessary. Microstructural effects enter via interfacial area and transport coefficients A V volume-specific surface area / m 2 /m 3 D diffusion coefficient σ Conductivity Sliede 8
9 Mass and charge transport in liquid electrolyte Species conservation (Nernst-Planck equation) Charge neutrality Diluted solution theory (Li-S) Concentrated solution theory (Li-O) Sliede 9
10 m Multi-scale simulation framework DENIS: Detailed Electrochemistry and Numerical Impedance Simulation In-house C/C++ software Workhorse of the DENIS group Electrode Cell System Stack MATLAB Coupling DENIS- SIMULINK ANSYS/COMSOL Coupling DENIS- ANSYS/COMSOL for CFD simulations nm Interfaces CANTERA LIMEX Implicit DAE solver (Deuflhard, Berlin) Coupling with CANTERA (Goodwin, Caltech) for chemistry source terms and transport coefficients Sliede 10
11 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 11
12 Li-S battery modeling domain Cathode properties: Thickness: 41 µm Phases (charged state): Sulfur ε = 0.16 Carbon ε = 0.06 Electrolyte ε = 0.78 Li 2 S ε = 10 7 Interfaces: Sulfur-Electrolyte Carbon-Electrolyte Li 2 S-Electrolyte Anode: Lithium metal Sliede 12
13 Li-S battery model: Thermodynamics and transport Species Molar Gibbs energy / kj mol 1 Density / Initial concentration Diffusion coefficient / 1 m 2 s Li kg m -3 C kg m -3 (solid) S kg m -3 Li 2 S C 4 H 6 O mol m 3 Li mol m PF mol m S mol m S mol m S mol m S mol m S mol m (liquid) S mol m Parameters converted from Kumaresan et al., J. Electrochem. Soc. 155, A576 (2008) Sliede 13
14 Li-S battery model: Reactions and kinetics Reaction Preexponential factor, Preexponential factor, forward reaction reverse reaction Li Li + + e m 5 mol 2 s 1 1 m 2 mol s 1 S 8 (solid) S 8 (liquid) m 0.5 mol 0.5 s 1 1 s S 8 (solid) + e 1 2 S m 0.5 mol 0.5 s m 0.5 mol 0.5 s S e 2 S m mol 0.5 s m 4 mol 1 s 1 S e 3 2 S s m mol 0.5 s S e S m 0.5 mol 0.5 s s S e S m 0.5 mol 0.5 s s 1 2 Li + + S 2 Li 2 S (solid) m 6 mol 2 s s 1 Parameters converted from Kumaresan et al., J. Electrochem. Soc. 155, A576 (2008) Sliede 14
15 Li-S: Simulated discharge curve and phase change Discharge shows typical two-stage behavior Solid S 8 is fully consumed before solid Li 2 S is formed Cell voltage / V Time / h S 8 Li 2 S Volume fraction / % Discharge capacity / mah/g sulfur Sliede 15
16 Li-S: Simulated ionic species concentrations First stage: Sulfur polyanions are formed Second stage: Sulfur polyanions are reduced End of discharge: No more sulfur polyanions Concentration / mol/m Time / h Li + S 2- S 2-8 PF - 6 S 8(l) S 2-6 S 2-2 S Discharge capacity / Ah/g sulfur Sliede 16
17 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 17
18 Li-O battery modeling domain Cathode properties: Thickness: 750 µm Phases: Carbon ε = 0.25 Electrolyte ε = 0.75 Li 2 O 2 ε = 10 7 Interfaces: Carbon- Electrolyte- Li 2 O 2 Electrolyte: LiPF 6 / Stable organic solvent Anode: Metallic lithium Sliede 18
19 Li-O battery model: Thermodynamics and kinetics Species Molar Gibbs energy / kj mol 1 Density / Initial concentration Li kg m 3 Li mol m 3 - PF mol m 3 (gas) O % (dissolved) O mol m 3 Li 2 O kg m 3 EC-EMC mol m 3 Reaction Preexponential factor, Activation forward reaction energy Li Li + + e m s 1 0 O 2 (gas) O 2 (dissolved) Assumed in equilibrium 2 Li + + O 2 (dissolved) + 2 e Li 2 O m 7 mol -2 s 1 0 Parameters converted from: P. Andrei, J. P. Zheng, M. Hendrickson and E. J. Plichta, J. Electrochem. Soc., 157, A1287 (2010); A. Nyman, M. Behm and G. Lindbergh, Electrochim. Acta, 53, 6356 (2008); R. C. Weast, Handbook of chemistry and physics, CRC Press (1982). Sliede 19
20 Li-O: Simulated discharge behavior Discharge curves simulated for different current densities Polarization losses increase with increasing current density Capacity strongly depends on current density Voltage (V) A/m A/m 2 1 A/m A/m Specific capacity (mah / g c ) Sliede 20
21 Li-O: Spatial distribution O 2 Strong gradients of dissolved O 2 in organic electrolyte At high currents, reactions are confined to regions close to channel Rate-limiting O 2 diffusion is origin of polarization losses c(o 2 ) [mol / m 3 ] i=0.01 A/m 2 i=0.1 A/m 2 i=0.5 A/m 2 i=1 A/m 2 SOC = 50% i=10 A/m 2 i Faraday /<i Faraday > SOC = 50% i=0.01 A/m 2 i=0.1 A/m 2 i=0.5 A/m 2 i=1 A/m 2 i=10 A/m Distance [mm] 2 Sliede 21
22 Li-O: Pore clogging O 2 Free porosity decreases upon discharge Pore clogging by product Li 2 O 2 Clogging stronger close to channel Strong gradients for high currents Pore clogging is origin of current-dependent capacity loss ε [m 3 / m 3 ] ε [m 3 / m 3 ] i=10 A/m 2 i = 0.5 A/m 2 SOC 100% SOC 75% SOC 50% SOC 25% SOC 0% i=1 A/m 2 i=0.5 A/m 2 i=0.1 A/m 2 i=0.01 A/m 2 SOC = 50% Distance [mm] Sliede 22
23 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 23
24 Aqueous Li-O: LiOH as soluble intermediate Oxygen reduction: O e + 2 H 2 O 4 OH (aq) Precipitation: Li + + OH + H 2 O LiOH H 2 O(s) Sliede 24
25 Aqueous Li-O modeling domain Cathode properties: Thickness: 500 µm Phases (start composition): Carbon ε = 0.25 Water ε = 0.75 LiOH H 2 O ε = 10 7 Interfaces: Carbon-Electrolyte-LiOH H 2 O Separator properties: Porous thickness: 100 µm Ideal separation from anode assumed (e.g., Li + -conducting glass) Sliede 26
26 Results: Aqueous Li-O battery Two-stage discharge I: Dissolved LiOH Small voltage variation II: Precipitation of LiOH H 2 O Constant voltage End of discharge: Capacity limited by LiOH precipitation Cell Voltage / V I II Li + (aq), OH - (aq) U LiOH H 2 O(s) 0 1x10 5 2x10 5 3x10 5 4x10 5 5x Time / s Mean Molality Li + / mol Li +/ kg H2O Mean Volume Fraction LiOH / - Sliede 27
27 Concentration distribution A Li + /OH concentration gradient, peak at anode B Increasing Li + /OH concentration C Beginning LiOH precipitation within separator close to anode D LiOH precipitation at oxygen inlet and anode surface End of discharge due to LiOH film on anode surface Volume fraction LiOH H 2 O / - Volume fraction LiOH H 2 O / A Cathode Separator Time / s C Cell Voltage / V Cathode A B C D 0 1x10 5 2x10 5 3x10 5 4x10 5 5x Separator Distance from channel / µm B Mean Molality Li + / molli +/ kg H2O Mean Volume Fraction LiOH / - Cathode Separator D Distance from channel / µm Cathode Sep. Sliede 28 Molality Li + / mol Li +/ kg H2O Molality Li + / mol Li +/ kg H2O
28 Motivation and approach Lithium-sulfur Lithium-air (organic) Lithium-air (aqueous) Conclusions Sliede 29
29 Summary: Next-generation battery modeling Li-S and Li-O batteries: High energy density, low cycleability Challenges: Complex chemistry and complex multi-phase behavior Chemistry, phases and transport included into modeling framework Li-S: Two-stage behavior: Dissolution, charge transfer, precipitation mechanism Li-O organic: Low oxygen diffusivity and pore clogging at channel Li-O aqueous: Low oxygen diffusivity and pore clogging at anode Thank you for your attention! Sliede 30
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