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George, Lee – Colorado U., Dillon – NREL V.C.10 Atomic Layer Deposition for Amorphous Silicon Anodes (Colorado U.) Figure V - 111: Cycling performance of NG and LiCoO2 full cells where various electrodes are coated with Al2O3. Noteworthy First-Year Collaborations: NREL worked with Stan Whittingham’s group at SUNY Binghamton to show that LiNi y Mn y Co 1-2y O 2 can cycle stably for 500 cycles at both 5C and 10C with capacities of approximately 130 and 110 mAh/g, respectively. (See report V.B.5.). The cathode was enabled by using carbon single-walled nanotubes as both the conductive additive and binder with an active material loading of 95 wt.%. Anodes containing Si and a conductive binder developed by Gao Lui at LBNL were also coated with Al 2 O 3 , and preliminary results indicate that the performance of thicker electrodes is improved. Conclusions and Future Directions It has been demonstrated that ALD coatings of Al 2 O 3 improve the durable cycling of thick Si-electrodes containing various forms of Si. A Coatings Group to better understand the mechanism of various coatings on new electrodes has been formed. In future work, the mechanism of the Al 2 O 3 and other coatings will also be explored. In FY12 exploration of the mechanism as well as enabling durable high rate capability for thick Si electrodes will be emphasized. Enabled with Single-Wall Carbon Nanotubes” Advanced Energy Materials 1, 58 (2011). 5. Riley, L.A. et. al. "Improved mechanical integrity of ALD-coated composite electrodes for Li-ion Batteries", Electrochemical and Solid State Letters 14, A29 (2011). 6. Riley, L.A. et. al. "Electrochemical Effects of ALD Surface Modification on Combustion Synthesized LiNi 1/3 Mn 1/3 Co 1/3 O 2 as a Layered-Cathode Material," 196, 3317 (2011). 7. Scott, I.D. et al. “Ultrathin Coatings on Nano LiCoO 2 for Li-Ion Vehicular Applications” Nano Lett. 11, 414 (2011). 8. Dillon, A.C. “Carbon Nanotubes for Photoconversion and Electrical Energy Storage.” Chem. Rev. 110, 6856 (2010). Invited Presentations (contributed not listed) 1. Dillon, A.C. ALD of Al 2 O 3 for Highly Improved Performance in Li-ion Battery Electrodes invited, ALD2011, Boston, MA, July 2011. 2. Ban, C., invited “Binder-free High Rate Capability Li-ion Electrodes” Materials Research Society Spring Meeting, San Francisco, CA, April 2011. 3. Dillon, A.C. invited International Battery Association Meeting, Cape Town, South Africa, April, 2011. (Presented by M.S. Whittingham.) 4. Dillon, A.C. “Methods to Achieve Durable High Rate with High Capacity for Li-ion Batteries” key note Special ACS Symposium in Honor of Debra R. Rolison, Anaheim, CA March 2011. 5. Dillon, A.C., “High Rate and High Capacity Metal Oxide Anodes” invited American Vacuum Society Fall Meeting, Albuquerque, NM, Oct. 2010. FY 2011 Publications/Presentations 1. Jung, Y.S., et al., “Unraveling the Unexpected Improved Performance of ALD Coated LiCoO 2 /Graphite Li-ion Batteries” JACS (Submitted). 2. E. Kang, et al., “Magnetite Nanoparticles Confined in Mesocellular Carbon Foam for High Performance Anode Materials of Lithium-Ion Batteries,” Adv. Funct. Mater., 21, 2430 (2011). 3. Dillon, A.C., et al., “HWCVD MoO 3 Nanoparticles and a-Si for Next Generation Li-Ion Anodes” Thin Solid Films 519, 4495 (2011). 4. Ban, C. et al. “Extremely Durable High-Rate Capability of an LiNi 0 . 4 Mn 0 . 4 Co 0 . 2 O 2 Cathode FY 2011 Annual Progress Report 575 Energy Storage R&D
V.C.11 Synthesis and Characterization of Si/SiO x -Graphene Nanocomposite Anodes and Polymer Binders (PSU) Donghai Wang and Michael A. Hickner (PI) The Pennsylvania State University Department of Mechanical and Nuclear Engineering Department of Materials Science and Engineering 328 Reber Building University Park, PA 16802 Phone: (814)-863-1287; (814) 867-1847 E-mail: dwang@psu.edu; mah49@psu.edu Start Date: January 1, 2011 Projected End Date: October 1, 2014 Objectives · Design, synthesize and test novel polymer binders with varying mechanical properties and surface linker groups for Si anodes · Synthesize and characterization of Si/SiO x -graphene nanocomposites, · Identify and evaluate the electrochemical performance of the Si/SiO x -graphene nanocomposites and the polymer binder. · Improve management of volume change characeristics of Si-based anodes, impede the capacity fading with enhanced capacity reliability, decrease initial irreversible capacity loss, and improve the specific capacity and coulombic efficiency of Si/SiO x -based anodes. Technical Barriers There are several technical barriers to developing Si/SiO x -based anodes for lithium-ion batteries including: · Poor capacity cycling · Large initial irreversible capacity and corresponding low coulombic efficiency · Need to add a high percentage of conductive carbon to obtain good rate (C/3) performance Technical Targets · Prepare Si nanoparticles with controlled particle size, and demonstrate Si-graphene nanocomposite anodes. · Synthesize and evaluate novel polymer binders with controlled SiO x binding groups and Li-conducting blocks. · Determine electrochemical properties of Si/SiO x nanoparticle, Si/SiO x -graphene nanocomposites and the polymer binders in lithium half cell. · Achieve stable reversible capacity in excess of ~1,000 mAh/g. · Obtain above 40% first cycle coulombic efficiency as well as 90% coulombic efficiency cycle to cycle. Accomplishments · Demonstrated Si nanoparticles with controlled diameter ranging from 5 nm to 20 nm and Si-graphene nanocomposite synthesis through solution synthesis approach. · Successful synthesis of Si nanoparticles with diameter ranging from 50-100 nm, and Si-graphene nanocomposites by using magnesiothermic reduction method. · Random and block copolymers with surface binding silanes have been synthesized. · Successful synthesis of a novel mechanically robust polymer binder (i.e., sulfonated Radel binder), which have been tested in battery cells for cycle performance and nearly equivalent performance to CMC/SBR. · As-prepared Si-graphene nanocomposites exhibit specific capacity in excess of ~1,000mAh/g with good cycling stability and rate capability. · The novel Si-graphene composites exhibit less than 20% first cycle irreversible loss as well as 90% coulombic efficiency cycle to cycle thereafter. Introduction An increase in energy and power densities of Li-ion cells depends in a decisive way on improvements in electrode materials performance. As the commercial anode, graphite has the theoretical capacity of 372 mAh/g, which is low relative to the requirement of high-energy application fields. Thus, the search for an alternative anode to replace graphite in Li-ion batteries has been underway for many years. So far, silicon has the highest theoretical Energy Storage R&D 576 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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Page 81 and 82: V.C.3 Search for New Anode Material
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Page 87 and 88: V.C.5 Development of High Capacity
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Page 117 and 118: V.C.12 Silicon Clathrates for Anode
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Page 121 and 122: V.C.13 Wiring Up Silicon Nanopartic
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Page 137 and 138: V.D.3 Molecular Dynamics Simulation
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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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