Molecular Level Investigations of Structural and Chemical Evolution of Interfacial Processes Relevant to Energy Storage Systems
EMSL Project ID
49321
Abstract
The objectives of this proposal are to understand the reactions occurring at the electrode/electrolyte interphases in lithium-oxygen (Li-O2) batteries, and to investigate the transform mechanisms of lithium nickel manganese cobalt oxide (NMC) cathode materials for Li-ion batteries during synthesis processes. In nonaqueous Li-O2 batteries, recent reports indicated that the battery cycling can be performed via LiOH formation and decomposition by adding water and LiI as additives in electrolytes or through LiO2 by using Ir-decorated graphene electrode, both of which are different from the traditional pathway of formation of Li2O2. However, the proposed mechanism for cycling LiOH is not convincing and there is no direct experimental XRD evidence for LiO2. We also found that the temperature below and above 0 degrees C has significant effects on the discharge behaviors of the Li-O2 battery but the true mechanisms are unclear. Therefore, the investigations in Li-O2 batteries will be focused on (1) the mechanisms of oxygen reduction reaction (ORR) at the air electrode/electrolyte interphase in the temperature ranges below and above 0?C, (2) the effects of selected catalysts and moisture with and without LiI additive in electrolytes on ORR and oxygen evolution reaction (OER) at air electrode/electrolyte interphases and the cycling stability of related Li-O2 cells, and (3) the Li/electrolyte interphases during Li-O2 operations. In Li-ion batteries, the studies include (1) the phase transformation and Ni segregation in Li-rich Mn-rich (LMR) layered cathode materials during synthesis process to find out the Ni-segregation layer formation process, (2) the phase transformation mechanisms and morphological changes of Ni-rich LiNixMnyCozO2 (NMC) cathode materials during synthesis to find out the optimized calcination temperature for cathode materials synthesis, and (3) the conditions that the NMC particles start to form cracks and show deteriorated cycling stability when cycled to high voltages. All of the work is leveraged with the strong capabilities in PNNL including energy storage materials, characterizations and computational calculations.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2018-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
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Stress-Tolerant Nanoporous Germanium Nanofibers for Long Cycle Life Lithium Storage with High Structural Stability
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Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes
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Minimizing Polysulfide Shuttle Effect in Lithium-Ion Sulfur Batteries by Anode Surface Passivation
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Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries
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Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition
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High‐Voltage Lithium‐Metal Batteries Enabled by Localized High‐Concentration Electrolytes
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Dendrite‐Free and Performance‐Enhanced Lithium Metal Batteries through Optimizing Solvent Compositions and Adding Combinational Additives
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Pushing the limit of layered transition metal oxide cathodes for high-energy density rechargeable Li ion batteries
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Enhanced Cyclability of Lithium–Oxygen Batteries with Electrodes Protected by Surface Films Induced via In Situ Electrochemical Process
Liu B., W. Xu, J. Tao, P. Yan, J. Zheng, M.H. Engelhard, and D. Lu, et al. 2018. "Enhanced Cyclability of Lithium-Oxygen Batteries with Electrodes Protected by Surface Films Induced via In-Situ Electrochemical Process." Advanced Energy Materials 8, no. 11:1702340. PNNL-SA-128613. doi:10.1002/aenm.201702340
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Harnessing the concurrent reaction dynamics in active Si and Ge to achieve high performance lithium-ion batteries
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Stability of polymeric separators in lithium metal batteries in a low voltage environment
Li X, J Tao, D Hu, MH Engelhard, W Zhao, J Zhang, and W Xu. 2018. "Stability of Polymeric Separators in Lithium Metal Batteries in a Low Voltage Environment." Journal of Materials Chemistry A 6(12):5006-5015. doi:10.1039/C7TA11259A
Facet-Dependent Rock-Salt Reconstruction on the Surface of Layered Oxide Cathodes
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Extremely Stable Sodium Metal Batteries Enabled by Localized High-Concentration Electrolytes
Zheng J, S Chen, W Zhao, J Song, MH Engelhard, and J Zhang. 2018. "Extremely Stable Sodium Metal Batteries Enabled by Localized High-Concentration Electrolytes." ACS Energy Letters 3(2):315-321. doi:10.1021/acsenergylett.7b01213
Revealing the Reaction Mechanism of Na–O2 Batteries using Environmental Transmission Electron Microscopy
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Guided Lithium Metal Deposition and Improved Lithium Coulombic Efficiency through Synergistic Effects of LiAsF6 and Cyclic Carbonate Additives
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Li+-Desolvation Dictating Lithium-Ion Battery’s Low-Temperature Performances
Li Q, D Lu, J Zheng, S Jiao, L Luo, C Wang, K Xu, J Zhang, and W Xu. 2017. "Li+-Desolvation Dictating Lithium-Ion Battery's Low-Temperature Performances." ACS Applied Materials & Interfaces 9(49):42761-42768. doi:10.1021/acsami.7b13887
Suppressing Lithium Dendrite Growth by Metallic Coating on a Separator
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Rock-Salt Growth-Induced (003) Cracking in a Layered Positive Electrode for Li-Ion Batteries
Zhang H, F Omenya, P Yan, L Luo, MS Whittingham, C Wang, and G Zhou. 2017. "Rock-salt Growth Induced (003) Cracking in Layered Positive Electrode for Li-ion Batteries." ACS Energy Letters 2(11):2607-2615. doi:10.1021/acsenergylett.7b00907
Temperature Dependence of the Oxygen Reduction Mechanism in Nonaqueous Li–O2 Batteries
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Formation of an Anti-Core–Shell Structure in Layered Oxide Cathodes for Li-Ion Batteries
Zhang H, F Omenya, MS Whittingham, C Wang, and G Zhou. 2017. "Formation of an Anti-core-shell Structure in Layered Oxide Cathode for Li-ion Batteries." ACS Energy Letters 2(11):2598-2606. doi:10.1021/acsenergylett.7b00921
Atomic Resolution Structural and Chemical Imaging Revealing the Sequential Migration of Ni, Co, and Mn upon the Battery Cycling of Layered Cathode
Yan P, J Zheng, J Zhang, and C Wang. 2017. "Atomic Resolution Structural and Chemical Imaging Revealing the Sequential Migration of Ni, Co and Mn upon Battery Cycling of Layered Cathode." Nano Letters 17(6):3946-3951. doi:10.1021/acs.nanolett.7b01546
The roles of oxygen non-stoichiometry on the electrochemical properties of oxide-based cathode materials
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Structural Transformations in High-Capacity Li2Cu0.5Ni0.5O2 Cathodes
Ruther R, AS Pandian, P Yan, JN Weker, C Wang, and J Nanda. 2017. "Structural Transformations in High Capacity Li2Cu0. 5Ni0. 5O2 Cathodes." Chemistry of Materials 29(7):2997-3005. doi:10.1021/acs.chemmater.6b05442
Revealing the reaction mechanisms of Li–O2 batteries using environmental transmission electron microscopy
Luo L ,Liu B ,Song S ,Xu W ,Zhang J ,Wang C 2017. "Revealing The Reaction Mechanisms of Li-O2 Batteries Using Environmental Transmission Electron Microscopy" Nature Nanotechnology 12():535-540. 10.1038/nnano.2017.27
Wide-Temperature Electrolytes for Lithium-Ion Batteries
Li Q ,Jiao S ,Luo L ,Ding M S,Zheng J ,Cartmell S S,Wang C ,Xu K ,Zhang J ,Xu W 2017. "Wide temperature electrolytes for lithium-ion batteries" ACS Applied Materials & Interfaces 9(22):18826-18835. 10.1021/acsami.7b04099
Revisiting the Corrosion of the Aluminum Current Collector in Lithium-Ion Batteries
Ma T ,Xu GL ,Li Y ,Wang L ,He X ,Zheng J ,Liu J ,Engelhard M H,Zapol P ,Curtiss L A,Jorne J ,Amine K ,Chen Z 2017. "Revisiting the Corrosion of Aluminum Current Collector in Lithium-Ion Batteries" The Journal of Physical Chemistry Letters 8(5):1072-1077. 10.1021/acs.jpclett.6b02933