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Lithium Ion Electrolytes and Lithium Ion Cells With Good Low Temperature Performance
There is provided in one embodiment of the invention an electrolyte for use in a lithium ion electrochemical cell. The electrolyte comprises a mixture of an ethylene carbonate (EC), an ethyl methyl carbonate (EMC), an ester cosolvent, and a lithium salt. The ester cosolvent comprises methyl propionate (MP), ethyl propionate (EP), methyl butyrate (MB), ethyl butyrate (EB), propyl butyrate (PB), or butyl butyrate (BB). The electrochemical cell operates in a temperature range of from about -60 C to about 60 C. In another embodiment there is provided a lithium ion electrochemical cell using the electrolyte of the invention.
Fundamentals of Rechargeable Lithium ion and Beyond Lithium Ion Batteries
A very brief introduction to batteries is provided, with a focus on lithium-ion batteries and the common materials.
Lithium loss, resistance growth, electrode expansion, gas evolution, and Li plating: Analyzing performance and failure of commercial large-format NMC-Gr lithium-ion pouch cells
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Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries
Abstract Among various rechargeable batteries, the lithium-ion battery (LIB) stands out due to its high energy density, long cycling life, in addition to other outstanding properties. However, the capacity of LIB drops dramatically at low temperatures (LTs) below 0 °C, thus restricting its applications as a reliable power source for electric vehicles in cold climates and equipment used in the aerospace. The electrolyte engineering has proved to be one of the most effective approaches to mitigate LIB performance degradation at LTs. In this review, we summarize the important factors contributing to the deterioration in Li + transport and capacity utilization at LTs while systematically categorize the solvents, salts and additives reported in the literature. Strategies to improve the Li + transport kinetics, in the bulk electrolyte and across the interphases, are discussed. In particular, the formation mechanism of solid electrolyte interphase and its functionality for LT electrolytes are analyzed. Perspectives on the future evolution of this area are also provided. Graphical abstract
Polymers in Lithium‐Ion and Lithium Metal Batteries
Abstract Lithium‐ion batteries play a significant role in modern electronics and electric vehicles. However, current Li‐ion battery chemistries are unable to satisfy the increasingly heightened expectations regarding energy demand and reliability. To boost the overall energy density while ensuring the safety of Li batteries, researchers have focused on alternative battery materials, such as silicon, sulfur, and Li metal. These represent promising avenues, although numerous obstacles (e.g., Si cracking, polysulfide shuttling, Li dendrites, etc.) must be tackled before batteries based on these materials can enter mass production and penetrate the mainstream market. Polymers are a class of materials that are widely used in current battery systems; however, many novel polymer chemistries may offer better performance and reliability than the current ones, and even overcome the issues of the above‐mentioned new battery materials. In this review, selected polymeric materials for solving these issues are categorized into four parts: polymer electrolytes, polymer artificial solid‐electrolyte interphases, binders, and separators. Both the current progress and the characterization methods are included. Potential future directions of energy materials research are pointed out as well.
Lithium-rich layered titanium sulfides: Cobalt- and Nickel-free high capacity cathode materials for lithium-ion batteries
Abstract not provided
Unravelling high-temperature stability of lithium-ion battery with lithium-rich oxide cathode in localized high-concentration electrolyte
Lithium (Li)-rich manganese (Mn)-rich oxide (LMR) cathode materials, despite of the high specific capacity up to 250 mAh g-1 suffer from instability of cathode/electrolyte interfacial layer at high working voltages, causing continuous voltage decay and capacity fading, especially at elevated temperatures. In various battery systems, localized high-concentration electrolytes (LHCEs) have been widely reported as a promising candidate to form effective electrode/electrolyte interphases. Here, an optimized LHCE is studied in graphite (Gr)-based full cells being cycled at 25, 45 and 60 °C with the reference of a conventional LiPF6-based electrolyte. It is revealed that the LHCE can effectively suppress continuous electrolyte decompositions and mitigate the dissolution of Mn ions due to the formation of more protective electrode/electrolyte interphases on both anode and cathode, which, in turn, lead to significantly improved cycling stability and enhanced rate capability under the selected temperatures. The mechanistic understanding on the failure of the conventional LiPF6-containing electrolyte and the function of the LHCE in Gr||LMR cells under high temperatures provides valuable perspectives of electrolyte development for practical application of LMR cathodes in high energy density batteries over a wide temperature range.
Development of lithium ion conducting interface between lithium metal and a lithium ion conducting ceramic using block polymers
The lithium-air (Li-air) technology developed by EDF uses an air electrode which works with an aqueous electrolyte, which prevent the use of unprotected lithium metal electrode. A Li+ ionic conductor glass ceramic is used to separate the aqueous electrolyte compartment from the negative lithium electrode. However, this glass-ceramic is not stable in contact with lithium, it is thus necessary to add a protective buffer layer. In another hand, this protection should ideally resist to lithium dendritic growth. It is in this context that this research project which has as goal the development of a protective buffer layer based on block copolymer electrolytes (BCE) between the lithium metal and the lithium ionic conductor ceramic, for lithium-air battery. In a first part, the BCE is studied in lithium-lithium symmetric cells, in order to determine their electrochemical properties such as ionic conductivity, steady state transference number, and finally their resistance to dendritic growth during cycling. Several characterization techniques were employed and especially hard X-ray micro-tomography to analyze the lithium morphology before and after cycling. For single-ion BCE, we expect to suppress dendritic growth, however, we report here for the first time, the visualization of a homogeneous growth of lithium but the formation of dense lithium objects. In another part, the composite BCE-ceramic is studied by electrochemical impedance spectroscopy (EIS). The cycling of lithium-composite-lithium symmetric cells and the analysis of the EIS measurement after each cycle permit to determine if the dendrites have cross the protective layer and are in contact with the ceramic. Besides, the quantification of the polarization loss at the interface polymer-ceramic is evaluated by polarization experiments. This contribution is found to be small.
Energy, greenhouse gas, and water life cycle analysis of lithium carbonate and lithium hydroxide monohydrate from brine and ore resources and their use in lithium ion battery cathodes and lithium ion batteries
Life cycle analyses (LCAs) were conducted for battery-grade lithium carbonate (Li 2 CO 3 ) and lithium hydroxide monohydrate (LiOH·H 2 O) produced from Chilean brines (Salar de Atacama) and Australian spodumene ores. The LCA was also extended beyond the production of Li 2 CO 3 and LiOH·H 2 O to include battery cathode materials as well as full automotive traction batteries to observe the effect that the lithium production pathways had on these end products. The LCA here covers material, water, and energy flows associated with lithium acquisition; lithium concentration; production of lithium chemicals, battery cathode powders, and batteries; and associated transportation activities along the supply chain. Based on battery cathode material, the difference in lithium source represents a difference of up to 20% for NMC811 cathode greenhouse gases (GHGs) and up to 45% for NMC622 cathode GHGs. For full batteries, this represents a difference of up to 9% for NMC811 batteries and 20% for NMC622 batteries. Production of Li 2 CO 3 from brine-based resources had less life cycle GHG emissions and freshwater consumption per tonne of Li 2 CO 3 than Li 2 CO 3 from ore-based resources. And LiOH·H 2 O produced from brine-based lithium also had less life cycle GHG emissions and freshwater consumption per tonne of LiOH·H 2 O than LiOH·H 2 O from ore-based resources.
Impact of Residual Lithium on the Adoption of High-Nickel Layered Oxide Cathodes for Lithium-Ion Batteries
High-nickel layered oxide cathodes are becoming appealing for lithium-ion batteries employed in portable electronics and electric vehicles because of their higher energy density, low or no cobalt content, and ability to be manufactured with existing infrastructure. However, high-nickel layered oxides are plagued by the formation of residual lithium species, such as LiOH and Li 2 CO 3 , on the surface, which are detrimental to the manufacturing process and performance. Despite the problems residual lithium causes for the industry, academia mainly focuses on the safety risks and electrochemical impacts of residual lithium. In this Perspective, we examine the residual lithium problem through a lens of its impact on cathode slurry instability and large-scale manufacturing of high-nickel layered oxides. Additionally, methods of measuring residual lithium are discussed from the perspective of their accuracy as well as practicality in the manufacturing process. Furthermore, we hope that this Perspective would encourage the academic endeavor to consider the practical obstacles caused by residual lithium on the industrialization of high-nickel layered oxides and their mitigation, while attempting to improve their electrochemical performance and safety through doping, surface modifications, or other approaches.
3D Printed TiO 2 Negative Electrodes for Sodium-Ion and Lithium-ion Batteries using Vat Photopolymerization
Additive manufacturing, also called 3D printing, represents a unique approach to develop three dimensional shape-conformable batteries with enhanced electrodes, specific surface area, improved ion diffusion, and power. For the first time, the formulation of a composite photocurable resin loaded with battery electrochemically active components was designed to feed a vat photopolymerization (VPP) 3D printer. In direct alignment with NASA’s Artemis mission goals to develop sustainable lunar energy storage infrastructure necessary to support long-term human operations, TiO 2 was here selected as an active material for the negative electrode for sodium-ion and lithium-ion batteries due to its abundance on the lunar surface. The TiO 2 loading in the composite photocurable resin and in the resulting VPP-printed negative electrode was increased as high as possible to enhance the electrochemical performance, while simultaneously ensuring the printability and acceptable mechanical strength for sample handling. The effect of thermal post-processing on the electrical, electrochemical and mechanical performance is reported. Finally, a configurational study is implemented to identify the impact of two different electrode designs (cubic and gyroid lattice unit cells) on the electrochemical performance. This work addresses the difficulties related to the introduction of solid particles within a VPP photocurable resin and the need for a compromise between the electrochemical performances and printability to obtain fully functional VPP-printed electrodes.
High-rate cathode CrSSe based on anion reactions for lithium-ion batteries
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Modeling Extreme Deformations in Lithium Ion Batteries
A simultaneously coupled modeling approach to study the electrochemical and thermal behavior of lithium-ion batteries under large mechanical deformation has been developed. The thermo-electrochemical pseudo-2D (P2D) battery model is coupled with a mechanical material model. Mechanical, thermal, and electrochemical models are implemented as user-defined sub-routines in the commercial multi-physics code LS-DYNA. The mechanical strain experienced by anode, cathode and separator results in thickness and porosity changes in each layer which in turn influences electrochemical behavior. The evolution of concentration profiles and cell potential are studied under different mechanical loading conditions. Internal short-circuits caused by mechanical deformation and corresponding physical behaviors are also elucidated. We discuss the competing effects of improved transport at higher temperature due to the internal short-circuit versus a drop in the effective ionic conductivity and electrolyte diffusivity due to mechanical deformation.
Lithium-Ion Batteries with Lithium Manganese Iron Phosphate Cathodes and Lithium Titanate Anodes: Linking Electrode Dynamics to Cell Performance
This study examines the electrochemical performance, impedance behavior, and aging mechanisms of lithium-ion cells pairing lithium manganese iron phosphate (LiMn 0.6 Fe 0.4 PO 4 , LMFP64) cathodes with lithium titanate (Li 4 Ti 5 O 12 , LTO) anodes. LMFP64 half-cells display distinct Fe and Mn redox plateaus at ∼3.5 and ∼4.1 V, respectively, and deliver excellent rate capability. Three-electrode measurements show that LMFP64 dominates cell impedance, which changes sharply across the Fe–Mn redox transition and decreases with increasing temperature (30 °C–50 °C). Voltage hysteresis arises mainly from the cathode, with higher C-rates shortening redox plateaus and broadening the transition region. Elevated temperature lowers impedance, especially near the Mn-redox and transition regions, but accelerates capacity fade. Post-cycling analyses of electrodes confirm structural stability of LMFP64 and indicate loss of lithium inventory (LLI) as the source of capacity fade. This LLI causes potential slippage between the LMFP64 and LTO electrodes, which decreases the Fe-redox plateau width. Long-term cycling highlights the critical role of electrode overhang: cathode overhang mitigates capacity fade by buffering lithium loss, whereas anode overhang cells experience faster capacity decline due to uncompensated lithium depletion. These results clarify LMFP64/LTO battery impedance evolution, thermal effects, and degradation pathways and provide insights for their applications in electric vehicles.
Lithium-ion battery physics and statistics-based state of health model
A pseudo-2d model using COMSOL Multiphysics® software is developed to simulate performance and performance degradation of Li-ion batteries consisting of layered and olivine cathodes with graphite anode when subjected to peak shaving grid service. Multiple degradation pathways are considered, including solid electrolyte interphase (SEI) formation and breakdown at the anode, cathode dissolution and its synergistic effect on SEI formation at the anode. The model is validated by simulating commercial cylindrical cell performance. A global model is developed to simulate performance across all chemistries, along with individual chemistry models using global model parameters as initial values. There is good agreement between these models for various optimization parameters such as SEI equilibrium potential, cathode dissolution exchange current density, solvent diffusivity in the SEI and SEI ionic conductivity. To circumvent time constraints related to the COMSOL model, a 0d global model is developed which fits data well and provides more clarity on differences in cathode dissolution exchange current density. Again, good agreement for various optimization parameters is obtained among the COMSOL global & individual chemistry models and the 0-d model. The lessons learned from the physics-based model is used to develop a top down statistics-based model using current, voltage and anode volumetric change per mole lithium intercalated, along with their interactions as degradation predictors. This model predicts out of sample degradation for multiple grid services and electric vehicle drive cycle with high accuracy and provides the pathway to develop an efficient battery management system combining machine learning and findings from physics-based computationally intensive algorithms.
Insights into lithium ion deposition on lithium metal surfaces
Lithium metal is among the most promising anodes for the next generation of batteries due to its high theoretical energy density and high capacity. Challenges such as extreme reactivity and lithium dendrite formation have kept lithium metal anodes away from practical applications. However, the underlying mechanisms of Li ion deposition from the electrolyte solution onto the anode surface are still poorly understood due to their inherent complexity. In this work, density functional theory calculations and thermodynamic integration via constrained molecular dynamics simulations are conducted to study the electron and ion transfer between lithium metal slab and the electrolyte in absence of an external field. Here, we explore the effect of the solvent chemistry and structure, distance of the solvated complex from the surface, anion–cation separation, and concentration of Li-salts on the deposition of lithium ions from the electrolyte phase onto the surface. Ethylene carbonate (EC), 1,2-dimethoxyethane (DME), 1,3-dioxolane (DOL), and mixtures of them are used as solvents. These species compete with the salt anion and the Li cation for electron transfer from the surface. It is found that the structure and properties of the solvation shell around the lithium cation has a great influence on the ability of the cation to diffuse as well as on its surrounding electron environment. DME molecules allow easier motion of the lithium ion compared with EC and DOL molecules. The slow growth approach allows the study of energy barriers for the ion diffusion and desolvation during the deposition pathway. This method helps elucidating the underlying mechanisms on lithium-ion deposition and provides a better understanding of the early stages of Li nucleation.