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V.B.14 New Cathode Projects (LBNL) Venkat Srinivasan Lawrence Berkeley National Laboratory 1 Cyclotron Rd. MS62R0203 Berkeley, CA 94720-8168 Phone: (510) 495-2679 Fax: (510) 486-4260 E-mail: vsrinivasan@lbl.gov Start Date: January 2012 Projected End Date: December 2016 Introduction The FY 2011 Batteries for Advanced Transportation Technologies (BATT) Request for Proposals entitled “Novel Cathode Materials for High-energy Lithium Batteries” has resulted in four new projects that can help accelerate the application of such batteries in plug-in hybrid electric vehicles and electric vehicles. These projects focus on developing next-generation cathodes to increase the energy and decrease the cost of lithium-ion batteries while maintaining safety and cycle life. Approach The BATT program received 102 white papers and encouraged 28 applicants to submit full proposals. A selection committee composed of leading battery experts reviewed each proposal and recommended four for funding. In addition, some national lab researchers have been asked to submit another proposal directly to DOE for further consideration. DOE headquarters reaches funding decisions based on a peer review process, while maintaining and strengthening the national laboratory research capability. Results The awardees include three national laboratories and one university and are listed below, along with a brief description of their projects. The total requested funds are $5.81 million over four years. High Capacity Composite Cathode Materials: New Synthesis Routes and Structures, Argonne National Laboratory. Li 2 MnO 3 -stabilized composite electrode structures, such as ‘layered-layered’ xLi 2 MnO 3 (1 x)LiMO 2 (M=Mn, Ni, Co) systems are receiving attention because they can provide capacities between 200 and 250 mAh/g between 4.6 and 2.0V vs. Li. These manganeserich composite cathode structures have to be electrochemically activated above 4.4V in order to access the high capacity. Unfortunately, this process compromises the rate capability of these electrodes, which also suffer from voltage decay on cycling, thereby compromising the energy and power output of the cells and preventing their implementation in practical systems. This proposal addresses these limitations and challenges. A novel processing route using Li 2 MnO 3 as a precursor to synthesize composite electrode structures is advocated, which is based on promising results obtained over the past few months. The technique is simple, versatile and seemingly low cost; it offers the possibility of opening the door to wide exploitation and, in particular, of synthesizing and tailoring composite electrode structures, including new systems, thereby enhancing the electrochemical properties of Li-ion cells to meet the performance targets of PHEVs. In situ Solvothermal Synthesis of Novel High Capacity Cathodes, Brookhaven National Laboratory. The development of high energy density, low cost Li ion electrodes will require improved understanding of the electrode preparation reactions in order to achieve control over material properties. In this effort we will develop and utilize in situ reactors designed to investigate solvothermal synthesis reactions in real-time using synchrotron techniques. This capability will allow us to identify intermediate or transient phases and better control phase nucleation, reaction rates and material properties. The following classes of high-energy materials will be investigated: (1) Li metal borates (LiMBO 3 , M = Mn and Fe); (2) copper fluorides (CuF 2 ); (3) copper-vanadium oxides (CuV 3 O 8 ); and (4) carbonophosphates and carbonofluorosulphates (Li 3 M(CO 3 )PO 4 , Li 3 M(CO 3 )SO 4 F where M = Mn and Fe). Progress will be evaluated at the end of the second year with an up- or down-selection to continue research on those systems showing potential for achieving targets. The project deliverable is a reversible cathode with an energy density ≥700 Wh/kg, although these materials have the potential for much greater energy densities (e.g., 1400 Wh/kg). Lithium-bearing mixed polyanion (LBMP) glasses as cathode materials, Oak Ridge National Laboratory. Li-bearing mixed polyanion (LBMP) glasses will be developed as cathode materials for Li ion batteries for use in EV applications. The composition of LBMP glasses can be tailored to provide higher electrical conductivities, higher redox potentials, and higher specific energies than similar crystalline polyanion materials. The disordered covalently bonded structures of LBMP glasses could provide excellent cycleability and safety. In addition, LBMP glass compositions may enable cycleable multivalent changes in the transition metal cations, providing FY 2011 Annual Progress Report 533 Energy Storage R&D
V.B.14 New Cathode Projects (LBNL) Srinivasan – LBNL the potential to provide specific energies of 1000Wh/kg. The experimental approach combines: (1) structure and property modeling, (2) glass processing, (3) glass characterization, (4) conventional cathode production, and (5) electrical and electrochemical testing. Computer modeling will be used to suggest the most promising LBMP glass compositions in terms of electrochemical performance and glass processing capability. Classical heat-quench glass forming and sol gel processing will be used to make the LBMP glasses. Electrical conductivity and glass uniformity are key properties that will be measured. Conventional cathodes will be made and electrochemical performance will be demonstrated in coin cells with LBMP glass cathodes. High-capacity, High-voltage Cathode Materials for Lithium-ion Batteries, University of Texas at Austin. This project will design and develop materials based on polyanions that may cycle more than one Li ion per transition metal ion and/or operate above 4.3 V. Specifically, the high-capacity systems to be investigated are Li 2 MSiO 4 (M = Mn, Fe, Co, Ni, and VO) with a theoretical capacity of ~ 330mAh/g and Li 2 MP 2 O 7 (M = Mn, Fe, Co, Ni, and VO) with a theoretical capacity of ~ 220mAh/g. The high-voltage systems to be studied are LiMPO 4 with M = Co and Ni, which operate at 4.8 and 5.1V, respectively, with capacities of ~ 170 mAh/g. Additionally, Li 3 V 2 (PO 4 ) 3 with a theoretical capacity of ~ 200mAh/g and an operating voltage between 3.6 and 4.6V and Li 9 V 3 (P 2 O 7 ) 3(PO 4 ) 2 with a capacity of ~ 260mAh/g and an operating voltage between 3.6 and 4.8 V will be explored. However, synthesis and processing conditions play a critical role in realizing the full capacities of these polyanion cathodes. For example, we have shown that more than one Li ion could be reversibly extracted from carbon-coated nanostructured Li 2 MSiO 4 (M = Fe and Mn) synthesized by a microwave-solvothermal (MWST) approach. We plan to extend this approach to other systems. The major issue with the high-voltage (> 4.5 V) cathodes is the chemical instability of the cathode electrolyte interface. We have shown that the 4.8 V spinel LiMn 1.5 Ni 0.42 M 0.08 O 4 (M = Fe and Ga) exhibits good cyclability even with conventional electrolytes due to a self-segregation of Fe and Ga ions to the surface during synthesis, providing a robust cathode-electrolyte interface. We plan to adopt a similar surface-segregation strategy to improve the cyclability of the high-voltage polyanion cathodes. Energy Storage R &D 534 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.3 Olivines and Substituted Laye
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Page 19 and 20: V.B.4 Stabilized Spinels and Nano O
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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
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Page 49 and 50: V.B.10 Development of High Energy C
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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
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Page 71 and 72: V.C.1 Nanoscale Composite Hetero-st
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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
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Page 87 and 88: V.C.5 Development of High Capacity
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Page 91 and 92: V.C.6 Advanced Binder for Electrode
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Page 107 and 108: V.C.10 Atomic Layer Deposition for
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Page 117 and 118: 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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