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Angell – ASU V.D.8 Sulfones with Additives as Electrolytes (ASU) impressive in view of the immediate exfoliation that occurs when EMS is used alone as solvent. We note that the fluorosulfonyl group is also implicated in the efficacy of the bis-fluorosulfonylimide anion as an SEI-forming agent (observed in Japanese laboratories). Figure V - 168: Conductivities of sulfolane-DMC mixtures Figure V - 169: Walden plot for assessing ionicities. Conversely, and keeping in mind that it enhances cell safety, it should be recognized that although sulfolane is more than an order of magnitude more viscous than EC:DMC, it only gives up a factor of two or so in conductivity. At the same time the solution gains in electrochemical stability. The gain should be even greater for the acyclic sulfone EMS, the “window” of which is the widest on record. It should be noted that sulfolane as solvent has already passed tests of stability against the LNMO high voltage cathode in the 1,000 cycle tests reported by Amine and colleagues, at ANL. To consider solutions based on EMS, data are presented in Figure V - 170. It is seen that the mixture of EMS and FMS has a very favorable temperature dependence such that at 70ºC it has a conductivity not only as high as the EMS-DMC solvent, but almost as high as that of EC:DMC in Figure V - 167. Figure V - 171 shows that the electrochemical stability is above 5.5 volts, and Figure V - 172 shows that a graphite anode half cell quickly establishes a stable SEI and then intercalates lithium reversibly. This is Figure V - 170: Conductivities with EMS and FMS co-solvents EMS with FMS co-solvent also supports cycling at the graphite anode, though the SEI does not form as rapidly and efficiently as with sulfolane. Turning to the cathode half cell, less success has been had, but the preparation of the cathode is more complex and there has been no access to proper cathode preparation facilities (spin-coaters etc). The results are shown in Figure V - 173, and it is found, in follow-up experiments, that the electrodes prepared in the ASU lab cannot be charged beyond 4.7 V before some irreversibility is encountered. In view of the success reported by the Amine lab, we will not consider the EMS-FMS solvent based electrolyte a failure until tests on more satisfactory cathodes can be carried out. Dr. Ueno, now back in Japan, has offered to use sophisticated electrode fabrication tools available in his current laboratory to prepare more reliable cathodes and thereby to establish the true efficacy of the sulfone-based electrolytes for high voltage cells of the LNMO type. Figure V - 171: Oxidative stabilities of EMS and FMS FY 2011 Annual Progress Report 623 Energy Storage R&D
V.D.8 Sulfones with Additives as Electrolytes (ASU) Angell – ASU Figure V - 172: Li deposition and stripping at a graphite anode sulfolane:MFS as solvent 2. Nanoporous nets as electrolyte supports. After months of frustrating effort trying to produce reversible H- bonded models of the open nets we had conceived for this projects’ electrolyte support, we changed course to tackle directly the covalent net versions that were expected to be irreversible. We have immediately been rewarded with success. The flexible solid film seen in Figure V - 174a is a new product for which we show XRD patterns and their conversion to real space distributions in Figure V - 174b. These establish that an open network with ~15-20Å pores has been obtained. We have successfully prepared a second version using struts 3 times as long, which are of extremely low density, and should support both solution and ionic liquid electrolytes up to 200ºC. Figure V - 174: Nanoporous film, w/ XRD analysis, showing ~20nm pores in continuous film structure Future work Nets and their liquid-filled properties will be explored. FY 2011 Publications/Presentations 1. 2011 DOE Annual Peer Review Meeting talk 2. Nature Materials (in preparation). Figure V - 173: CV for 1M LiPF6-EMS-MSF (1:1 by wt) on LNMO cathode. Scan rate 0.2mV/sec. Working electrode: LNMO composite placed on Al substrate, Li ref and counter electrode Energy Storage R &D 624 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
Page 107 and 108: V.C.10 Atomic Layer Deposition for
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Page 111 and 112: V.C.11 Synthesis and Characterizati
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Page 115 and 116: V.C.12 Synthesis and Characterizati
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
Page 127 and 128: V.C.14 Hard Carbon Materials for Hi
Page 129 and 130: V.D.1 Polymer Electrolytes for Adva
Page 131 and 132: V.D.1 Polymer Electrolytes for Adva
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
Page 139 and 140: V.D.3 Molecular Dynamics Simulation
Page 141 and 142: V.D.4 Bi-functional Electrolytes fo
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Page 145 and 146: V.D.5 Advanced Electrolyte and Elec
Page 147 and 148: V.D.6 Inexpensive, Nonfluorinated (
Page 149 and 150: V.D.6 Nonfluorinated (or Partially
Page 151 and 152: V.D.7 Development of Electrolytes f
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Page 161 and 162: V.D.9 Long-lived Polymer Electrolyt
Page 163 and 164: V.E Cell Analysis, Modeling, and Fa
Page 165 and 166: V.E.1 Electrode Fabrication and Fai
Page 167 and 168: V.E.2 Modeling-Thermo-electrochemis
Page 169 and 170: V.E.2 Thermo-electrochemistry, Capa
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 187 and 188: V.E.7 Predicting/Understanding New
Page 189 and 190: V.E.8 New Electrode Designs for Ult
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Page 193 and 194: V.E.9 In Situ Electron Spectroscopy
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Page 197 and 198: V.F.1 Energy Frontier Research Cent
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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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V.G Integrated Lab-Industry Researc
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