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Whittingham – Binghamton U. V.B.5 Synthesis and Characterization of Substituted Olivines and Mn Oxides (Binghamton U.) 2. Hui Zhou, Shailesh Upreti, Natasha A. Chernova, Geoffroy Hautier, Gerbrand Ceder, and M. Stanley Whittingham “Iron and Manganese Pyrophosphates as Cathodes for Lithium Ion Batteries”, Chemistry of Materials, 2011, 23: 293-300. 3. Chunmei Ban, Zheng Li, Zhuangchun Wu, Melanie J. Kirkham, Le Chen, Yoon Seok Jung, E. Andrew Payzant, Yanfa Yan, M. Stanley Whittingham, and Anne C. Dillon “Extremely Durable High-Rate Capability of a LiNi 0.4 Mn 0.4 Co 0.2 O 2 Cathode Enabled by Single–Wall Carbon Nanotubes”, Advanced Energy Materials, 2011, 1: 58-62. 4. Zheng Li, Natasha A. Chernova, Megan Roppolo, Shailesh Upreti, Cole Petersburg, Faisal M. Alamgir, and M. Stanley Whittingham, “Comparative study of the capacity and rate capability of LiNi y Mn y Co 1-2y O 2 (y=0.5, 0.45, 0.4, 0.33)”, J. Electrochem. Soc., 2011, 158: A516-A522. 5. Shailesh Upreti, Olga V. Yakubovich, Natasha A. Chernova and M. Stanley Whittingham, “A novel lithium copper iron phosphate with idealized formulaLi 5 Cu 2+ 2 Fe 3+ (PO 4 ) 4 : crystal structure and distribution of defects”, Acta Cryst., 2011, E67: i29. 6. Hui Zhou, Shailesh Upreti, Natasha A. Chernova and M. Stanley Whittingham, “Lithium cobalt(II) pyrophosphate, Li 1.86 CoP 2 O 7 , from synchrotron X-ray powder data”, Acta Cryst. 2011, E67: i58–i59. 7. Many invited presentations, incl.: o Electrochemical Society, Materials Research Society, Pacific Power Sources Conf., IBA o U. C. San Diego, Stony Brook U., Wake Forest U., Michigan State U. o ORNL, Haldor Topsoe-Copenhagen o Local outreach FY 2011 Annual Progress Report 491 Energy Storage R&D
V.B.6 Cell Analysis-Interfacial Processes: SEI Formation and Stability on Cycling (HQ) Karim Zaghib Hydro-Quebec IREQ 1800 Lionel Boulet Varennes, QC, Canada J3X 1S1 Phone: (450) 652 8019; Fax: (450) 652 8424 E-mail: Zaghib.Karim@ireq.ca mailto:cashtiani@ENERDEL.com Subcontractor: Lawrence Berkeley National Laboratory, Berkeley, CA Start Date: March 2010 Projected End Date: September 2011 Objectives · Synthesis and evaluation of high-voltage cathode (spinel Mn-Ni) with improved electrochemical stability. · Reduce the oxidation of the cathode composition, electrolyte, and separator. Find the appropriate alternative anode composition that meets the requirement for low cost and high energy. · Continue development of ex situ and in situ SEM to increase our understanding of the failure mode of the cathode and anode materials. Technical Barriers Low energy density and poor cycle/calendar life Technical Targets · Identify a suitable technique to stabilize the interface reaction of the high-voltage oxide (Mn-Ni based, e.g., LiMn 1.5 Ni 0.5 O 4 ) cathode by surface coating with a more stable material such as an olivine. The emphasis is to improve electrochemical performance at high voltage · Investigate the effect of the type of binder, electrolyte composition, and separator on performance at high voltage · Develop high-capacity anodes based on Si composition. Accomplishments · Demonstration of the benefit of surface coating of high-voltage LiMn 1.5 Ni 0.5 O 4 cathode with LiFePO 4 olivine material · Optimize a silicon-based composition as highcapacity anode material. · Develop ex situ and in situ SEM tools for understanding the SEI layer and the failure mode in Si-based anode. Introduction BATT is searching for the next-generation systems for high energy. In 2011, BATT program management recommended working with; (i) spinel high-voltage cathode based on Mn-Ni, (ii) Si-based alloy anode and (iii) studies on SEI layers on alloy anode and cathode. Following the strategy to develop high-energy batteries, high-voltage cathodes based on Mn-Ni spinel will be studied. In the first part of the project, HQ plans to protect the surface of the cathode by a thin layer of olivine LiFePO 4 . By this process, we expect to reduce the oxidation of the electrolyte and enhance the safety of the high-voltage cathode. Dry or wet processes will be explored to modify the surface of the cathode. The HQ strategy related to the anode material is based on mixing particles of carbon-coated SiO x with graphite powder to reduce the volume expansion and increase the first-cycle coulombic efficiency. To improve the capacity of the anode; we evaluated nano-Si particles mixed with graphite as one configuration and ternary compounds nano-Si-SiOx-graphite as a second configuration. Varying Si-nano:graphite:SiOx compositions will be investigated to determine the minimum content of graphite required in the anode. Due to the major effect of the binder on the performance of the anode, various types of binder were investigated To further improve our comprehension on the SEI layer with the Si-based anodes and Mn-Ni cathodes, two analysis methods are adopted; ex situ SEM on cycled electrodes with liquid electrolyte and in situ SEM during anode cycling where the dry polymer was used as binder in the anode to avoid electrolyte evaporation. Energy Storage R&D 492 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: V.B.5 Synthesis & Characterization
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 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
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V.C.2 Interfacial Processes - Diagn
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V.C.2 Interfacial Processes - Diagn
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V.C.3 Search for New Anode Material
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V.C.4 Nano-structured Materials as
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V.C.4 Nano-structured Materials as
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V.C.5 Development of High Capacity
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V.C.5 Development of High Capacity
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V.C.6 Advanced Binder for Electrode
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V.C.6 Advanced Binder for Electrode
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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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