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Thackeray – ANL V.B.9 Layered Cathode Materials (ANL) (a) (b) Figure V - 50: (a) Surface coordination numbers; (b) Mn oxidation states of LiMn2O4 Conclusions and Future Directions Conclusions · All milestones set for this project in FY2011 were met. · The voltage-fade phenomenon in high-capacity xLi 2 MnO 3 (1-x)LiMO 2 (M=Mn, Ni, Co) electrodes was evaluated. · A new approach to synthesize composite electrode structures from a Li 2 MnO 3 precursor was identified with promising results; this project will form the basis of a new cathode project in FY2012. · Progress was made in stabilizing the surface, and improving the rate capability, of xLi 2 MnO 3 (1 x)LiMO 2 electrodes using sonochemical reactions. · Simulation of the surface structure of LiMn 2 O 4 shows that near-surface manganese ions strongly prefer the trivalent state, which provided further insight into dissolution phenomena associated, for example, with Ni-substituted LiMn 2 O 4 electrodes. Future Work (See New Cathode Project V.B.14.) · Exploit novel processing methods using Li 2 MnO 3 as a precursor to synthesize and optimize various composite electrode structures (composition and performance) with the goal of reaching/exceeding the energy and power goals required for 40-mile PHEVs and EVs. In particular, focus on ‘layered-layered’ ,‘layered-layered-spinel’- and new ‘layered-rocksalt’ xLi 2 MnO 3 (1-x)MO systems. · Focus on the stabilization of both surface and bulk structures. Use complementary experimental and theoretical approaches to improve the surface stability, rate capability and cycle life of high capacity Mn-rich oxide electrodes at high potentials. · Further explore sonication to fabricate and evaluate stable surface architectures. · Continue EFRC-related work and interact with DOE’s energy storage centers. FY 2011 Publications/Patents/Presentations Publications 1. K. A. Walz, C. S. Johnson, J. Genthe, L. C. Stoiber, W. A. Zeltner, M. A. Anderson and M. M. Thackeray, Elevated Temperature Cycling Stability and Electrochemical Impedance of LiMn 2 O 4 Cathodes with Nanoporous ZrO 2 and TiO 2 Coatings, J. Power Sources, 195, 4943 (2010). 2. A. Rockett, Y. W. Chung, H. Blaichek, S. Butterfield, R. R. Chance, C. Ferekides, M. Robinson, S. W. Snyder and M. M. Thackeray, Transformative Research Issues and Opportunities in Alternative Energy Generation and Storage, Current Opinion in Solid State & Materials Science, 15, 8-15 (2011). 3. R. Benedek and M. M. Thackeray. Simulation of the Surface Structure of Lithium Manganese Oxide Spinel, Phys. Rev. B, 83 (19): Art. No. 195439 (May 31 2011). 4. J. R. Croy, S.-H. Kang, M. Balasubramanian and M. M. Thackeray, A New Approach to Fabricating Li 2 MnO 3 -based Composite Cathode Structures for Lithium Batteries, Electrochem. Comm., 13, 1063 1066 (2011). Patents 1. M. M. Thackeray, S.-H. Kang, M. Balasubramaian and J. R. Croy, Electrode Structures and Surfaces for Li Batteries, US Patent Application, Serial No. 13/044038 (9 March 2011). FY 2011 Annual Progress Report 511 Energy Storage R&D
V.B.9 Layered Cathode Materials (ANL) Thackeray – ANL Presentations 1. K. G. Gallagher, D. Kim and S.-H. Kang, Capacity and Power Fade of Graphite/xLi 2 MnO 3 •(1-x)LiMO 2 (M=Ni, Co, Mn) Li-ion Cells, 218 th Electrochem. Soc. Meeting, Las Vegas, 10-15 October, 2010. 2. L. A. Riley, S.-H. Kang, A. S. Cavanagh, M.M. Thackeray, S. M. George, S.-H. Lee, A. C. Dillon, Li 2 MnO 3 -Stabilized LiMO 2 Cathode and ALD Coated MoO 3 Anode as a High Energy-Density Lithium-Ion Battery, 218 th Electrochemical Society (ECS) Meeting, Las-Vegas, 10-15 October (2010). 3. M. M. Thackeray, Lithium Batteries: Challenges and Opportunities in an Evolving Lithium Economy, Brown University, RI, 3 December (2010). 4. M. M. Thackeray, Electrochemical Energy Storage for Transportation: Challenges and Opportunities in an Evolving Lithium Economy, Fermilab Lecture Series, 4 February 2011. 5. M. M. Thackeray, Electrochemical Energy Storage for Transportation: Materials Challenges and Opportunities in an Evolving Lithium Battery Economy, The Future of Materials Science and Engineering in the 21st Century Workshop, Georgia Tech, Atlanta, GA, 24 February 2011. 6. M. M. Thackeray, Electrochemical Energy Storage for Transportation: Materials Challenges and Opportunities, Departmental Seminar, Northwestern University, 22 February (2011). 7. S.-H. Kang, K. G. Gallagher, D. Kim, W. Ryu, and M. M. Thackeray, Enhanced Electrochemical Behavior of xLi 2 MnO 3 (1-x)LiMO 2 (M=Mn, Ni, Co) Electrodes, International Battery Association Meeting, Cape Town, South Africa, 12-15 April (2011). 8. M. M. Thackeray, Design and Evaluation of Novel High Capacity Cathode Materials, DOE Annual Merit Review, Washington DC, 9-13 May (2011). 9. J. R. Croy, S.-H. Kang, M. Balasubramanian and M. M. Thackeray, Advances in Li 2 MnO 3 -based Electrodes for Lithium Batteries, 5th International Conference on Polymer Batteries and Fuel Cells, (PBFC-5), Argonne National Laboratory, Illinois, 1-5 August (2011). 10. M. M. Thackeray, Electrochemical Energy Storage for Transportation: Materials Challenges and Opportunities, “Design - 2 - Devices: Advanced Materials for Energy Applications”, Annual EFRC Energy Materials Symposium, Cornell University, Ithaca, NY, 12 August 2011. Energy Storage R &D 512 FY 2011 Annual Progress Report
Page 1 and 2: V. FOCUSED FUNDAMENTAL RESEARCH Int
Page 3 and 4: V.A Introduction Duong - DOE, Srini
Page 5 and 6: V.B Cathode Development V.B.1 First
Page 7 and 8: V.B.1 First Principles Calculations
Page 9 and 10: V.B.1 First Principles Calculations
Page 11 and 12: V.B.2 Cell Analysis, High-energy De
Page 13 and 14: V.B.3 Olivines and Substituted Laye
Page 19 and 20: V.B.4 Stabilized Spinels and Nano O
Page 21 and 22: V.B.4 Stabilized Spinels and Nano O
Page 23 and 24: V.B.5 The Synthesis and Characteriz
Page 25 and 26: V.B.5 Synthesis & Characterization
Page 27 and 28: V.B.6 Cell Analysis-Interfacial Pro
Page 29 and 30: V.B.6 Cell Analysis-Interfacial Pro
Page 31 and 32: V.B.7 Role of Surface Chemistry on
Page 39 and 40: V.B.8 Characterization of New Catho
Page 41 and 42: V.B.8 Characterization of New Catho
Page 43 and 44: V.B.9 Layered Cathode Materials (AN
Page 45: V.B.9 Layered Cathode Materials (AN
Page 49 and 50: V.B.10 Development of High Energy C
Page 51 and 52: V.B.10 Development of High Energy C
Page 53 and 54: V.B.11 Crystal Studies on High-ener
Page 59 and 60: V.B.12 Developing Materials for Lit
Page 65 and 66: V.B.13 Studies on the Local SOC and
Page 67 and 68: V.B.13 Studies on the Local SOC and
Page 69 and 70: V.B.14 New Cathode Projects (LBNL)
Page 71 and 72: V.C.1 Nanoscale Composite Hetero-st
Page 73 and 74: V.C.1 Nanoscale Composite Hetero-st
Page 75 and 76: V.C.2 Interfacial Processes - Diagn
Page 81 and 82: V.C.3 Search for New Anode Material
Page 83 and 84: V.C.4 Nano-structured Materials as
Page 85 and 86: V.C.4 Nano-structured Materials as
Page 87 and 88: V.C.5 Development of High Capacity
Page 89 and 90: V.C.5 Development of High Capacity
Page 91 and 92: V.C.6 Advanced Binder for Electrode
Page 93 and 94: V.C.6 Advanced Binder for Electrode
Page 95 and 96: V.C.7 Three-Dimensional Anode Archi
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ARGONNE2_CDJ403T me Pro ile V.C.7 T
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V.C.8 Metal-Based High-Capacity Li-
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V.C.8 Metal-Based High-Capacity Li-
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V.C.9 New Layered Nanolaminates for
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V.C.9 New Layered Nanolaminates for
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V.C.10 Atomic Layer Deposition for
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V.C.10 Atomic Layer Deposition for
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V.C.11 Synthesis and Characterizati
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V.C.11 Polymer-Coated Layered SiOx-
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V.C.12 Synthesis and Characterizati
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V.C.12 Silicon Clathrates for Anode
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V.C.12 Silicon Clathrates for Anode
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V.C.13 Wiring Up Silicon Nanopartic
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V.C.13 Wiring Up Silicon Nanopartic
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V.C.14 Hard Carbon Materials for Hi
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V.C.14 Hard Carbon Materials for Hi
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V.D.1 Polymer Electrolytes for Adva
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V.D.1 Polymer Electrolytes for Adva
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V.D.2 Interfacial Behavior of Elect
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V.D.2 Interfacial Behavior of Elect
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V.D.3 Molecular Dynamics Simulation
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V.D.3 Molecular Dynamics Simulation
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V.D.4 Bi-functional Electrolytes fo
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V.D.4 Bi-functional Electrolytes fo
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V.D.5 Advanced Electrolyte and Elec
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V.D.6 Inexpensive, Nonfluorinated (
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V.D.6 Nonfluorinated (or Partially
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V.D.7 Development of Electrolytes f
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V.D.8 Sulfones with Additives as El
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V.D.8 Sulfones with Additives as El
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V.D.9 Long-lived Polymer Electrolyt
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V.E Cell Analysis, Modeling, and Fa
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V.E.1 Electrode Fabrication and Fai
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V.E.2 Modeling-Thermo-electrochemis
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V.E.2 Thermo-electrochemistry, Capa
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V.E.3 Intercalation Kinetics and Io
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V.E.4 Mathematical Modeling of Next
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V.E.5 Analysis and Simulation of El
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V.E.5 Analysis and Simulation of El
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V.E.6 Investigation of Critical Par
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V.E.6 Investigation of Critical Par
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V.E.7 Predicting/Understanding New
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V.E.8 New Electrode Designs for Ult
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V.E.8 New Electrode Designs for Ult
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V.E.9 In Situ Electron Spectroscopy
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V.E.9 In situ Electron Spectroscopy
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V.F.1 Energy Frontier Research Cent
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V.F.1 Energy Frontier Research Cent
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V.F.2 Novel In Situ Diagnostics Too
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V.F.2 Novel In Situ Diagnostics Too
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V.G Integrated Lab-Industry Researc
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