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3.3 Panel 3 Report — In Pursuit of Long Lifetime and Reliability: Time-Dependent Phenomena at Electrodes and Electrolytes Electrochemical storage devices do not last forever. Failure mechanisms differ depending on the device chemistry, mode of use, and details of storage. Electrochemical cells may degrade gradually, or experience “sudden death” events that result in catastrophic failure, which can present safety hazards. These failure mechanisms are many and varied, but result in shorter device cycle lives and lifespans than generally desired. Premature failure is common to all types of devices, but the issues are particularly well delineated for lithium-ion batteries, as outlined below. These findings broadly illustrate the challenges involved in attempting to understand the key and often inter-related factors that influence device lifetimes and the commensurate need to develop solutions for them. The evolution of rechargeable lithium batteries dates back to the 1950s when Carl Wagner began the discussion of fast ionic conduction in solids.1 In the 1960s, the work was expanded to studies of topotactic reactions in certain unique crystal structures, and in the 1970s, to the concept of intercalation of alkali ions into these structures as cathode materials for rechargeable alkali metal batteries.2 In the 1980s, commercialization of intercalation electrode-based cell designs was pursued, and in the 1990s, early lithium-ion batteries with a “rocking-chair” functional concept were successfully commercialized.3 In the 2000s, the energy density and costs of the lithium-ion battery cells were progressively improved with significant market penetration, and in the present day, mature cell designs are being adopted to consumer electronics, electric vehicles, and electrical grid energy storage applications. 3.3.1 CURRENT STATUS AND RECENT ADVANCES Despite astonishing improvement in the performance for lithium-ion batteries, the advancement of the technology continues to face significant challenges. There exists significant complexity associated with the long-term behavior of lithium-ion batteries either in storage or under use. For example, the same material composition used in the battery may exhibit different long-term behavior depending on the syntheses, electrode processing techniques, cell fabrication methods, and aging conditions. Thus, variability in performance cannot be easily traced back to its fundamental origins. In other words, the differences cannot be easily identified by the discrimination of materials variations in syntheses, electrode processing conditions, or cell fabrication methods. These issues highlight the need for basic understanding of such complexity at the systems level. This panel recognized the importance of degradation mechanisms in determining the viability of the energy storage systems. Major challenges for longer life for electric energy storage in a closed system with high energy density are developing the ability to probe, identify, and quantify unwanted reactions, which are often subtle and happen at the electrode/electrolyte interfaces, and unraveling the atomic-to-mesoscale mechanistic mysteries that appear to impose strong dynamic limits on storage reversibility and lifetime. The need to mitigate any irreversible changes during the charge-discharge cycle calls for operando and/or in situ characterization methods, as well as advanced modeling and simulation, that can reveal time-dependent behavior in both the electrodes and electrode/electrolyte interfaces. More specifically, this panel concluded that the following aspects are critically relevant to the improvement of energy storage performance: (i) electrochemical energy storage reversibility, stability, degradation, corrosion, and reliability issues; (ii) electrochemical-mechanical coupling phenomena; (iii) side reactions and subtle rate- NEXT GENERATION ELECTRICAL ENERGY STORAGE PANEL 3 REPORT 109PDF Image | Next Generation Electrical Energy Storage
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