Improvement of life-time is an important issue in the development of Li-ion batteries. Aging mechanisms limiting the life-time can efficiently be characterized by physico-chemical analysis of aged cells with a variety of complementary methods. This study reviews the state-of-the-art literature on Post-Mortem analysis of Li-ion cells, including disassembly methodology as well as physicochemical characterization methods for battery materials. A detailed scheme for Post-Mortem analysis is deduced from literature, including pre-inspection, conditions and safe environment for disassembly of cells, as well as separation and post-processing of components. Special attention is paid to the characterization of aged materials including anodes, cathodes, separators, and electrolyte. More specifically, microscopy, chemical methods sensitive to electrode surfaces or to electrode bulk, and electrolyte analysis are reviewed in detail. The techniques are complemented by electrochemical measurements using reconstruction methods for electrodes built into half and full cells with reference electrode. The changes happening to the materials during aging as well as abilities of the reviewed analysis methods to observe them are critically discussed. Li-ion batteries are currently used in everyday objects such as smart-phones, power tools and tablet computers as well as in the growing fields of light electric vehicles (LEVs), unmanned aerial vehicles (UAVs), battery electric vehicles (BEVs), hybrid electric vehicles (HEVs), and plug-in hybrid electric vehicles (PHEVs). [1][2][3][4] Furthermore, the rise of renewable energy sources like wind and solar power, which are only intermittently available, demands reliable and highly flexible stationary energy storage solutions, which provide high capacities and predictable life-times. 2,5Aging of Li-ion batteries is a general problem for manufacturers as they have to guarantee long-term reliability of their products. For state-of-the-art cells, degradation effects on the material level lead to capacity fade and resistance increase on the cell level. The aging state of a battery is often characterized by the state-of-health (SOH) in % according to 3,16,22,[29][30][31] SO H(t) = discharge capacity (t) discharge capacity (t = 0)[1]where t represents the aging time. In general, one has to differentiate between cycling 7,16,18,21,[23][24][25]32 and calendar aging. 7,19,[21][22][23][24]27 Since commercial Li-ion cells can be subject to calendar aging in the time between manufacturing and delivery, it is good practice to measure the discharge capacity at t = 0 for each cell that undergoes an aging test. Since the discharge capacity depends mainly on temperature, depth-of-discharge (DOD), and discharge current, the SOH is usually monitored by regular check-ups with defined parameter sets, 7,16,21,23,24 which can vary depending on the application. Typically, a temperature of 25• C, 16,22,24 DOD of 100%, 16,21 and discharge rates of 1C 7,16,21,22,24 or lower 23 are used in check-ups. The performance dec...
Nowadays, the electric vehicle is one of the most promising alternatives for sustainable transportation. However, the battery, which is one of the most important components, is the main contributor to environmental impact and faces recycling issues. In order to reduce the carbon footprint and to minimize the overall recycling processes, this paper introduces the concept of re-use of electric vehicle batteries, analyzing some possible second-life applications.\ud Methods\ud First, the boundaries of the life cycle assessment of an electric vehicle are defined, considering the use of the battery in a second-life application. To perform the study, we present eight different scenarios for the second-life application. For each case, the energy, the efficiency, and the lifetime of the battery are calculated. Additionally, and based on the global warming potential, the environmental impact of the electric vehicle and its battery on a second-life application is determined for each scenario. Finally, an environmentally focused discussion on battery electrodes and research trends is presented.\ud Results and discussion\ud For the selected scenarios, the second life of the battery varies from 8 to 20 years depending on the application and the requirements. It has been observed that the batteries connected to the electricity grid for energy arbitrage storage have the highest impact per provided kilowatt hour. On the contrary, the environmental benefit comes from applications working with renewable energy sources and presenting a longer lifetime. We pointed out that a correlation between cycling conditions and degradation mechanisms of the electrode materials is compulsory for proper use of the electric vehicle battery in a second-life application.\ud Conclusions\ud To limit the environmental impact, batteries should be associated with renewable energy sources in stationary applications. However, it is more profitable to re-use Li-ion batteries than to use new lead-acid batteries. Although many batteries applied for electric vehicles use graphite-based anodes, the latter may not be the most suitable for the second-life application. A better understanding of Li-ion battery degradation during the second-life application is required for the different existing chemistries.Postprint (author's final draft
Application of Li-ion batteries for transportation not only requires long cycling life but also the preservation of the electrochemical performance during the resting period. For certain car usage this resting time could be predominant compared with the cycling activity and is referred to as calendar aging. To understand the aging mechanisms during calendar aging, an extensive post-mortem study was conducted on commercial 16 Ah NMC/graphite pouch cells stored at 5, 25, 45, and 60 °C. The post-mortem analyses were performed in parallel within three separate laboratories across Europe. They included visual inspection and structural and microstructural analysis along with a combination of analytical techniques to determine accurately the composition of positive (NMC) and negative (graphite) electrodes and the electrolyte. A direct correlation was established between the calendar-aging temperature and the degradation of the cells. The measurements revealed a severe deterioration phenomenon for the electrodes aged at 45 and 60 °C. These results are explained by the formation of a resistive interface on top of the negative electrodes due to a continuous and heterogeneous growth of a surface layer. Electrochemical impedance spectroscopy and electrochemical measurements confirm the resistance increase during cell degradation. At high temperatures, this occasionally leads to a Li deposition phenomenon. Nonetheless, we revealed that this degradation process does not affect the bulk structure of the materials but only the surface of the particles.
Nanoparticulate Fe2O3 and Fe2O3/C composites with different carbon proportions have been prepared for anode application in lithium ion batteries (LIBs). Morphological studies revealed that particles of Fe2O3 in the composites were well-dispersed in the matrix of amorphous carbon. The properties of the γ-Fe2O3 nanoparticles and the correlation with the particle size and connectivity were studied by electron paramagnetic resonance, magnetic, and Mössbauer measurements. The electrochemical study revealed that composites with carbon have promising electrochemical performances. These samples yielded specific discharge capacities of 1200 mAh/g after operating for 100 cycles at 1C. These excellent results could be explained by the homogeneity of particle size and structure as well as the uniform distribution of γ-Fe2O3 nanoparticles in the in situ generated amorphous carbon matrix.
Four LiMn0.8Fe0.1M0.1PO4/C (M = Fe, Co, Ni, Cu) cathode materials have been synthesized via a freeze-drying method. The samples have been characterized by powder X-ray diffraction, transmission electron microscopy, magnetic susceptibility, and electrochemical measurements. The composition and effective insertion of the transition-metal substituents in LiMnPO4 have been corroborated by elemental analysis, the evolution of the crystallographic parameters, and the magnetic properties. The morphological characterization of the composites has demonstrated that the phosphate nanoparticles are enclosed in a matrix of amorphous carbon. Among them, LiMn0.8Fe0.1Ni0.1PO4/C is the most promising cathode material, providing a good electrochemical performance in all aspects: high voltage and specific capacity values, excellent cyclability, and good rate capability. This result has been attributed to several factors, such as the suitable morphology of the sample, the good connection afforded by the in situ generated carbon, and the amelioration of the structural stress provided by the presence of Ni(2+) and Fe(2+) in the olivine structure.
Nanoparticulate NiO and NiO/C composites with different carbon proportions have been prepared for anode application in lithium and sodium ion batteries. Structural characterization demonstrated the presence of metallic Ni in the composites. Morphological study revealed that the NiO and Ni nanoparticles were well dispersed in the matrix of amorphous carbon. The electrochemical study showed that the lithium ion batteries (LIBs), containing composites with carbon, have promising electrochemical performances, delivering specific discharge capacities of 550 mAh/g after operating for 100 cycles at 1C. These excellent results could be explained by the homogeneity of particle size and structure, as well as the uniform distribution of NiO/Ni nanoparticles in the in situ generated amorphous carbon matrix. On the other hand, the sodium ion battery (NIB) with the NiO/C composite revealed a poor cycling stability. Post-mortem analyses revealed that this fact could be ascribed to the absence of a stable Solid Electrolyte Interface (SEI) or passivation layer upon cycling.
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