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Janke – ORNL V.D.9 Long-lived Polymer Electrolytes (ORNL) Log s / Scm -1 -3.0 -3.5 -4.0 -4.5 -5.0 -5.5 -6.0 -6.5 -7.0 A 1Mev Ref 1 x 10 13 ion/cm 2 1 x 10 14 ion/cm 2 2 x 10 14 ion/cm 2 3 x 10 14 ion/cm 2 A -7.5 -8.0 2.6 2.8 3.0 3.2 3.4 3.6 1000 / T (K -1 ) Log s / Scm -1 -3.0 -3.5 -4.0 -4.5 -5.0 -5.5 -6.0 -6.5 -7.0 B 5 x 10 13 ion /cm 2 Ref 0.5 M ev 1.0 M ev 2.5 M ev 3.7 M ev B -7.5 -8.0 2.6 2.8 3.0 3.2 3.4 3.6 1000 / T (K -1 ) Figure V - 178: The temperature dependence of the ionic conductivities of the membranes after irradiation at a fixed ion beam energy of 1 MeV and at different doses (A); and under different ion beam energies at a fixed ion beam dose of 5x10 13 ion/cm 2 (B). Conclusions and Future Directions As shown in the results, it is difficult to evaluate the effect of the surface treatment on the prevention of dendrite formation at room temperature using linear PEO. However, if evaluated at higher temperature, the surface effect will be disturbed due to the linear structure of PEO. In the future, we would like to make a series of crosslinked membranes with short PEO side chains, such as those based on polyethylene glycol dimethacrylate. Once cross-linked these membranes cannot flow at higher temperature so that they can be further surface treated using the same ion beam irradiation technique, followed by cycling evaluation at medium temperatures under high current to check the dendrite prevention effect. Figure V - 179: The typical cycling profile of (A) reference and (B) the sample irradiated at the beam energy of 1Mev and dose of 1x10 13 ion/cm 2 under the cycling sequence of 2 hour charge, 1 hour rest, 2 hour discharge and 1 hour rest. Acknowledgment Ion beam irradiations were conducted at UES, Inc. in Dayton, OH. References 1. Patil et al., Mater. Res. Bull. 2008, 43, 1913. 2. D. Howell, VT Program, Office of EERE, U.S. DOE, Washington, DC, 2008. 3. M. Rosso et. al., Electrochimica Acta 2006, 51, 5334. 4. C.W. Monroe and J. Newman, Journal of the Electrochemical Society 2005, 152:2, A396. FY 2011 Annual Progress Report 627 Energy Storage R&D
V.E Cell Analysis, Modeling, and Fabrication (DOE) Duong – DOE V.E Cell Analysis, Modeling, and Fabrication V.E.1 Electrode Fabrication and Failure Analysis (LBNL) Vincent Battaglia (Principal Investigator) Lawrence Berkeley Nationl Laboratory 1 Cyclotron Road M.S.70R0108B Berkeley, CA 94720 Phone: (510) 486-7172; Fax: (510) 486-4260 E-mail: vsbattaglia@lbl.gov Start Date: October 1, 2009 Projected End Date: September 31, 2013 Objectives · Develop fundamental understanding of the effect of electrode fabrication procedures on cell performance. · Develop techniques for evaluating cell failure. · Provide full- and half-cell evaluations of materials with the potential to improve energy density or life over the baseline. Technical Barriers Electrode performance as a function of electrode fabrication is poorly understood. Measuring the cycle life of a new material can be confounded with poor electrode fabrication. All Li-ion cells fail with time. Much of the failure is a result of side reactions in the anode and/or the cathode; although, the rate of cell failure is only a fraction of the rate of the side reactions. Understanding the underlying source of cell failure is critical to solving the problem. For FY2011, the BATT Program decided to put more emphasis on higher voltage systems as this is a path to higher energy density cells. The Program selected the high-voltage LiNi 1/2 Mn 3/2 O 4 spinel material as a baseline for the studies. Understanding how this material fails against different counter electrodes may provide clues to its failure mechanism/s. Technical Targets · Develop electrode fabrication capabilities that allow for the cycling of materials to > 1000 cycles. · Assess the rate of capacity fade of LiNi 1/2 Mn 3/2 O 4 against the PHEV and EV life targets. Accomplishments · Measured the rate of side reactions on graphite and NCM when each is cycled against Li and when cycled against each other. · Determined the upper cut-off voltage limit when cycling LiNi 1/2 Mn 3/2 O 4 against Li and against graphite. · Measured the rate of capacity fade of the LiNi 1/2 Mn 3/2 O 4 cell and showed that the side reactions are 4 times greater than the rate of capacity fade. · Measured the amount of dissolution of fresh electrodes of LiNi 1/2 Mn 3/2 O 4 in electrolyte. Introduction Cell manufacturing in the US is improving. Cells are now seen to last 1000 cycles, but not 5000 cycles as is required for PHEVs. This group’s cell manufacturing capabilities have kept pace. Our goal is to test good materials in cells and identify main sources of fade, in the face of limited capcity fade. Since most cells appear to die as a result of deleterious side reactions, we will pay special attention to the rate of these reactions and attempt to identify those that are benign and those that contribute to failure. We will develop new electrochemical methods where necessary. If the challenging energy density targets of EVs and PHEVs are to be realized, materials capable of cycling larger quatities of lithium and at higher voltages are required. To begin developing high-voltage electrolytes, high-voltage cathodes are required. LiNi 1/2 Mn 3/2 O 4 intercalates lithium with a flat potential at 4.7 V. This material will be evaluated for its performance and cycleability against different counter electrodes. Approach The BATT Program has identified the high-voltage Ni-spinel material as part of a system of interest. Our role is to identify a baseline cell chemistry. This chemistry must have reasonably good cycleability. Once established, our role is to quatify the sources of fade, whether it is power or energy. We accomplish this through particle analysis, electrode analysis, half-cell analysis, and full cell Energy Storage R &D 628 FY 2011 Annual Progress Report
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V. FOCUSED FUNDAMENTAL RESEARCH Int
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V.A Introduction Duong - DOE, Srini
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V.B Cathode Development V.B.1 First
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V.B.1 First Principles Calculations
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V.B.1 First Principles Calculations
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V.B.2 Cell Analysis, High-energy De
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V.B.3 Olivines and Substituted Laye
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V.B.4 Stabilized Spinels and Nano O
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V.B.4 Stabilized Spinels and Nano O
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V.B.5 The Synthesis and Characteriz
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V.B.5 Synthesis & Characterization
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V.B.6 Cell Analysis-Interfacial Pro
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V.B.6 Cell Analysis-Interfacial Pro
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V.B.7 Role of Surface Chemistry on
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V.B.8 Characterization of New Catho
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V.B.8 Characterization of New Catho
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V.B.9 Layered Cathode Materials (AN
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V.B.10 Development of High Energy C
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V.B.10 Development of High Energy C
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V.B.11 Crystal Studies on High-ener
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V.B.12 Developing Materials for Lit
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V.B.13 Studies on the Local SOC and
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V.B.13 Studies on the Local SOC and
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V.B.14 New Cathode Projects (LBNL)
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V.C.1 Nanoscale Composite Hetero-st
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V.C.1 Nanoscale Composite Hetero-st
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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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Page 117 and 118: V.C.12 Silicon Clathrates for Anode
Page 119 and 120: V.C.12 Silicon Clathrates for Anode
Page 121 and 122: V.C.13 Wiring Up Silicon Nanopartic
Page 123 and 124: V.C.13 Wiring Up Silicon Nanopartic
Page 125 and 126: V.C.14 Hard Carbon Materials for Hi
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Page 129 and 130: V.D.1 Polymer Electrolytes for Adva
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Page 133 and 134: V.D.2 Interfacial Behavior of Elect
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Page 137 and 138: V.D.3 Molecular Dynamics Simulation
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Page 141 and 142: V.D.4 Bi-functional Electrolytes fo
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Page 171 and 172: V.E.3 Intercalation Kinetics and Io
Page 177 and 178: V.E.4 Mathematical Modeling of Next
Page 179 and 180: V.E.5 Analysis and Simulation of El
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Page 183 and 184: V.E.6 Investigation of Critical Par
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Page 193 and 194: V.E.9 In Situ Electron Spectroscopy
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Page 201 and 202: V.F.2 Novel In Situ Diagnostics Too
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Page 205 and 206: V.G Integrated Lab-Industry Researc
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