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Binder Interactions in the Electrodes of the Lithium-Ion Batteries Gao Liu

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Binder Interactions in the Electrodes of the Lithium-Ion Batteries Gao Liu Binder Interactions in the Electrodes of the Lithium-ion Batteries Gao Liu, Honghe Zheng, Xiangyun Song, Paul Ridgeway, Suhan Kim, Andrew Minor, Yonghong Deng, and Vince Battaglia Lawrence Berkeley National Laboratory TFUG Conference, San Jose, CA February 17th, 2009 Outline • A introduction to Lithium-ion battery. •Energy vs. Power. •Cost. •Structure. •Cathode and anode performance. •Cell performance improvement. • Cathode electrode optimization. •Three components cathode – a polymer composite. •Acetylene black and polymer binder as conductive glue. •The mathematic modeling of the electrode electronic conductivity – the nano-scale interaction between PVDF and particles. •The cell performance governed by the interaction. Relative Performance of Various Electrochemical Energy-Storage Devices 1000 6 IC Engine 4 Fuel Cells EV – Electric Vehicle 100 h EV goal 2 HEV – Hybrid-Electric Li-ion Vehicle 100 PHEV goal PHEV– Plug-in Hybrid- 6 Ni-MH 4 Electric Vehicle Lead-Acid HEV goal 2 10 h 10 6 Capacitors 4 Specific Energy (Wh/kg) Specific Energy 1 h 0.1 h 36 s Range 2 3.6 s 1 0 1 2 3 4 10 10 10 10 10 Specific Power (W/kg) Acceleration Source: Product data sheets • Goals developed in cooperation with DOE and United States Advanced Battery Consortium (USABC) under the FreedomCAR partnership • USABC is a cooperative of major automotive manufactures • Li-ion batteries have higher performance compared to Nickel-metal hydrides batteries. However, research is needed to simultaneously address the life, cost, and abuse tolerance issues Cost of Consumer Electronics Batteries 1,800 $/kWh Cost Trend in Japan – Small Rechargeable 1,600 Cells Averaged Across Sizes 1,400 1,200 1,000 800 $/kWh NiMH 600 NiCd 400 Li-ion 200 0 J M S J M S J M S J M S J M S J M S J M S J M S 1999 2000 2001 2002 2003 2004 2005 2006 Source: U.S. DOE Source: TIAX, based on METI data Performance and cost drivers for Li-ion cells However, numerous problems remain before use in vehicles Modern Li-ion Battery Lithium-ion battery Electrolyte e− LiPF6 in Ethylene e− e− carbonate/diethyl Anode: Cathode: carbonate Conductive additives Separator Binder Li+ + - + - Li +e +C6→LiC6 LiCoO2→Li +e +CoO2 Innovation can occur via new material development, or by better engineering A commercial Lithium-ion Rechargeable 26650 Cell Open from the anode side Anode crimped closed Cathode side of the jelly roll Open up the jelly roll SEM Images of Cathode and Anode Surfaces Cathode Anode Cycling of a Graphite-LiCoO2 Cell Electrolyte oxidation Cobalt oxide + - 140 mAh/g LiCoO2→Li +e +CoO2 Electrolyte: LiPF6 in Ethylene carbonate/diethyl carbonate Solvent reduction- Passive film formation Voltage (V) vs. Li Voltage + - Li +e +C6→LiC6 Graphite 372 mAh/g x in Li C or y in Li CoO x 6 1-0.6y 2 Lithium deposition Energy Density Increase of Consumer Electronic Li-ion Batteries Theoretical Energy Density Source: TIAX, LLC Complete Cathode Electrodes Materials Electrode LiNi0.80Co0.15Al0.05O2 Ave. diam.: 10 μm Surface area: 0.78 m2/g Scale bar: 10 μm Acetylene black (AB) Ave. diam.: 50 nm Surface area: 60.4 m2/g Scale bar: 100 nm Scale bar: 10 μm PVDF Polymer Binder Molecular weight: 760,000 Laminates without Active Material The Electronic Conductivity of AB/PVDF films from 4-point probe measurements LiNi0.80Co0.15Al0.05O2/Graphite Cells AB:PVDF (AB+PVDF)% in the cathode electrode Most conductive 0.8:1 3.6%; 9%; 18%; 27% Least conductive 0.2:1 1.2%; 2.4%; 4.8%; 9.6%; 24% 0.4:1 2.8%; 11.2%; 21% 0.6:1 3.2%; 12.8%; 24% The Modeling Results of Active material/AB/PVDF ρ keff = Ɛ *k0(AB/PVDF) TEM Images of the Morphology of AB/PVDF Conductive Matrix AB:PVDF = 0.2:1 (w/w) 0.5:1 0.8:1 1:1 200 nm 140 nm 140 nm 200 nm Scale bar Three Different States of Polymer When in Contact with Particles Immobilized polymer* 1-100 nm Free polymer Immobilized polymer Bound polymer Bound polymer^ Micron to nano size particle Bound polymer layer and immobilized polymer layer form Fixed Layer on the surface of particles. * Dannenberg, E. M., Polymer, 14, 309 (1973) ^Westlinning, H and Butecnuth, G., Makromol. Chem., 47, 215 (1961) Cathode Material vs. Acetylene Black Particles Fixed layers Active Material Acetylene Black Fixed layer of binder on acetylene black material surface. Single AB particle size: 40 nm. Fixed layer of binder on active material surface. Free binder Active material size: 10 μm Matrix Conductivity of the Electrode Reflects the Competition for Binder between AB and Active Materials AB/PVDF e- from AB/PVDF films AB/PVDF/Active material - e k0 = f(AB/PVDF) ρ keff = Ɛ *k0(AB/PVDF’) PVDF’ =PVDF - cathode particle immobilized PVDF A Model and Experimental Comparison of the Conductivities Active Material/AB/PVDF Complete Cells LiNi0.80Co0.15Al0.05O2/Graphite Cells AB:PVDF = 0.8:1 (Most Conductive) HPPC Test EIS at 40% DOD (AB+PVDF) Decrease cell resistance 32 Hz 5012 Hz LiNi0.80Co0.15Al0.05O2/Graphite Cells AB:PVDF = 0.2:1 (Least Conductive) HPPC Test EIS at 40% DOD 170 1.2% (AB+PVDF) (AB+PVDF) c 2.4% A ) 2 4.8% •cm 130 9.6% Ω 24% 200 Hz 794 Hz 90 1259 Hz Increase cell resistance 316 Hz 1585 Hz 50 Discharge ASI ( 10 0% 20% 40% 60% 80% 100% Depth of Discharge LiNi0.80Co0.15Al0.05O2/Graphite Cells AB:PVDF = 0.4:1 HPPC Test EIS at 40% DOD 2.8% (AB+PVDF) (AB+PVDF) c 170 11.2% ) ) 2 21% •cm 130 Ω 1580 Hz Increase cell resistance 90 200 Hz 2510 Hz 50 Discharge ASI ( ASI Discharge 10 0% 20% 40% 60% 80% 100% Depth of Discharge LiNi0.80Co0.15Al0.05O2/Graphite Cells AB:PVDF = 0.6:1 HPPC Test EIS at 40% DOD (AB+PVDF) 63 Hz Stable resistance 3980 Hz The Distribution of Binder, AB, and Active Material at Different Combinations AB:PVDF = 0.8:1 AB:PVDF = 0.2:1 Active Low Material High Low High Content: Electronic Conductivity: Small Change Small Change Interfacial impedance of the electrodes: The Interfacial Impedances of All Compositions HEV region Energy density is less important. AB:PVDF P-HEV/EV region Energy density is important. Conclusions •The amount of binder plays critical role in the composite electrode beyond providing mechanical integrity. •The binder to conductive carbon ratio dictates the electronic conductivity of the laminate. The addition of active material alters the ratio through competition for the binder. •The electronic conductivity of a laminate appears to be reflected in the charge transfer capability of the laminate. •High acetylene black content, such as AB:PVDF > 0.8:1, tends to produce electrodes with lower electronic conductivity and higher charge transfer at high active material loadings. •Low acetylene black content, such as AB:PVDF < 0.4:1, tends to produce electrodes with higher electronic conductivities at high active material loadings. Acknowledgments •Assistant Secretary for Energy Efficiency and Renewable Energy, Office of FreedomCAR and Vehicle Technologies of the U.S. Department of Energy. Contract # DE-AC03-76SF00098. •Electron microscopy performed at the National Center for Electron Microscopy, Lawrence Berkeley Lab, U.S. Department of Energy. Contract # DE-AC02-05CH11231. •Toda American for the NCA Material. •Denka Japan for the acetylene black conductive additive. Thank you for your attention! End.
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