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Lithium-ion batteries can last many years but sometimes exhibit rapid, nonlinear degradation that severely limits battery lifetime. In this work, we review prior work on "knees" in lithium-ion battery aging trajectories. We first review definitions for knees and three classes of "internal state trajectories" (termed snowball, hidden, and threshold trajectories) that can cause a knee. We then discuss six knee "pathways", including lithium plating, electrode saturation, resistance growth, electrolyte and additive depletion, percolation-limited connectivity, and mechanical deformation -- some of which have internal state trajectories with signals that are electrochemically undetectable. We also identify key design and usage sensitivities for knees. Finally, we discuss challenges and opportunities for knee modeling and prediction. Our findings illustrate the complexity and subtlety of lithium-ion battery degradation and can aid both academic and industrial efforts to improve battery lifetime., Comment: Submitted to the Journal of the Electrochemical Society

This manuscript presents an algorithm for individual Lithium-ion (Li-ion) battery cell state of charge (SOC) estimation in a large-scale battery pack under minimal sensing, where only pack-level voltage and current are measured. For battery packs consisting of up to thousands of cells in electric vehicle or stationary energy storage applications, it is desirable to estimate individual cell SOCs without cell local measurements in order to reduce sensing costs. Mathematically, pure series connected cells yield dynamics given by ordinary differential equations under classical full voltage sensing. In contrast, parallel--series connected battery packs are evidently more challenging because the dynamics are governed by a nonlinear differential--algebraic equations (DAE) system. The majority of the conventional studies on SOC estimation for battery packs benefit from idealizing the pack as a lumped single cell which ultimately lose track of cell-level conditions and are blind to potential risks of cell-level over-charge and over-discharge. This work explicitly models a battery pack with high fidelity cell-by-cell resolution based on the interconnection of single cell models, and examines the observability of cell-level state with only pack-level measurements. A DAE-based state observer with linear output error injection is formulated, where the individual cell SOC and current can be reconstructed from minimal number of pack sensing. The mathematically guaranteed asymptotic convergence of differential and algebraic state estimates is established by considering local Lipschitz continuity property of system nonlinearities. Simulation results for Graphite/NMC cells illustrate convergence for cell SOCs, currents, and voltages.

Electrochemical energy storage is central to modern society -- from consumer electronics to electrified transportation and the power grid. It is no longer just a convenience but a critical enabler of the transition to a resilient, low-carbon economy. The large pluralistic battery research and development community serving these needs has evolved into diverse specialties spanning materials discovery, battery chemistry, design innovation, scale-up, manufacturing and deployment. Despite the maturity and the impact of battery science and technology, the data and software practices among these disparate groups are far behind the state-of-the-art in other fields (e.g. drug discovery), which have enjoyed significant increases in the rate of innovation. Incremental performance gains and lost research productivity, which are the consequences, retard innovation and societal progress. Examples span every field of battery research , from the slow and iterative nature of materials discovery, to the repeated and time-consuming performance testing of cells and the mitigation of degradation and failures. The fundamental issue is that modern data science methods require large amounts of data and the battery community lacks the requisite scalable, standardized data hubs required for immediate use of these approaches. Lack of uniform data practices is a central barrier to the scale problem. In this perspective we identify the data- and software-sharing gaps and propose the unifying principles and tools needed to build a robust community of data hubs, which provide flexible sharing formats to address diverse needs. The Battery Data Genome is offered as a data-centric initiative that will enable the transformative acceleration of battery science and technology, and will ultimately serve as a catalyst to revolutionize our approach to innovation., Comment: corrected author list

Solid electrolytes are widely considered as the enabler of lithium metal anodes for safe, durable, and high energy density rechargeable lithium-ion batteries. Despite the promise, failure mechanisms associated with solid-state batteries are not well-established, largely due to limited understanding of the chemomechanical factors governing them. We focus on the recent developments in understanding solid-state aspects including the effects of mechanical stresses, constitutive relations, fracture, and void formation, and outline the gaps in the literature. We also provide an overview of the manufacturing and processing of solid-state batteries in relation to chemomechanics. The gaps identified provide concrete directions towards the rational design and development of failure-resistant solid-state batteries., Comment: 49 pages, 10 figures

Improvements in rechargeable batteries are enabling several electric urban air mobility (UAM) aircraft designs with up to 300 miles of range with payload equivalents of up to 7 passengers. We find that novel UAM aircraft consume between 130 Wh/passenger-mile up to ~1,200 Wh/passenger-mile depending on the design and utilization, relative to an expected consumption of over 220 Wh/passenger-mi for terrestrial electric vehicles and 1,000 Wh/passenger-mile for combustion engine vehicles. We also find that several UAM aircraft designs are approaching technological viability with current Li-ion batteries, based on the specific power-and-energy while rechargeability and lifetime performance remain uncertain. These aspects highlight the technological readiness of a new segment of transportation., Comment: 3 pages, 2 figures, 1 supplementary information file

Electrodeposition and stripping are fundamental electrochemical processes for metals and have gained importance in rechargeable Li-ion batteries due to lithium metal electrodes. The electrode kinetics associated with lithium metal electrodeposition and stripping is crucial in determining performance at fast discharge and charge which is important for electric vertical take-off and landing (eVTOL) aircraft and electric vehicles (EV). In this work, we show the use of Marcus-Hush-Chidsey (MHC) kinetics to accurately predict the Tafel curve data from the work of Boyle et al. We discuss the differences in predictions of reorganization energies from the Marcus-Hush and the MHC models for lithium metal electrodes in four solvents. The MHC kinetic model is implemented and open-sourced within Cantera. Using the reaction kinetic model in a pseudo-2D battery model with a lithium anode paired with a LiFePO$_4$ cathode, we show the importance of accounting for the MHC kinetics and compare it to the use of Butler-Volmer (BV) and Marcus-Hush kinetic models. We find that significant deviation in the overpotentials associated with reaction kinetics for the two different rate laws for conditions of fast discharge and charge relevant for eVTOL and EV respectively., Comment: 10 pages, 5 figures, 2 pages of Supplementary Information

Development of Urban Air Mobility (UAM) concepts has been primarily focused on electric vertical takeoff and landing aircraft (eVTOLs), small aircraft which can land and takeoff vertically, and which are powered by rechargeable (typically lithium-ion) batteries. Design, analysis, and operation of eVTOLs requires fast and accurate prediction of Li-ion battery performance throughout the lifetime of the battery. eVTOL battery performance modeling must be particularly accurate at high discharge rates to ensure accurate simulation of the high power takeoff and landing portions of the flight. In this work, we generate a battery performance and thermal behavior dataset specific to eVTOL duty cycles. We use this dataset to develop a battery performance and degradation model (Cellfit) which employs physics-informed machine learning in the form of Universal Ordinary Differential Equations (U-ODE's) combined with an electrochemical cell model and degradation models which include solid electrolyte interphase (SEI) growth, lithium plating, and charge loss. We show that Cellfit with U-ODE's is better able to predict battery degradation than a mechanistic battery degradation model. We show that the improved accuracy of the degradation model improves the accuracy of the performance model. We believe that Cellfit will prove to be a valuable tool for eVTOL designers., Comment: 38 pages, 5 figures, 8 pages of Supplementary information

Weight, computational load, sensor load, and possibly higher drag may increase the energy use of automated electric vehicles (AEVs) relative to human-driven electric vehicles (EVs), although this increase may be offset by smoother driving. We use a vehicle dynamics model to show that automation is likely to impose a minor penalty on EV range and have negligible effect on battery longevity. As such, while some commentators have suggested that the power and energy requirements of automation mean that the first automated vehicles (AVs) will be gas-electric hybrids, we conclude that this need not be the case. We also find that drivers need to place only a modest value on the time saved by automation for its benefits to exceed direct costs., Comment: 25 pages, 4 figures, 14 pages of Supporting Information

There has been considerable interest in the electrification of freight transport, particularly heavy-duty trucks to downscale the greenhouse-gas (GHG) emissions from the transportation sector. However, the economic competitiveness of electric semi-trucks is uncertain as there are substantial additional initial costs associated with the large battery packs required. In this work, we analyze the trade-off between the initial investment and the operating cost for realistic usage scenarios to compare a fleet of electric semi-trucks with a range of 500 miles with a fleet of diesel trucks. For the baseline case with 30% of fleet requiring battery pack replacements and a price differential of US\$50,000, we find a payback period of about 3 years. Based on sensitivity analysis, we find that the fraction of the fleet that requires battery pack replacements is a major factor. For the case with 100% replacement fraction, the payback period could be as high as 5-6 years. We identify the price of electricity as the second most important variable, where a price of US$0.14/kWh, the payback period could go up to 5 years. Electric semi-trucks are expected to lead to savings due to reduced repairs and magnitude of these savings could play a crucial role in the payback period as well. With increased penetration of autonomous vehicles, the annual mileage of semi-trucks could substantially increase and this heavily sways in favor of electric semi-trucks, bringing down the payback period to around 2 years at an annual mileage of 120,000 miles. There is an undeniable economic case for electric semi-trucks and developing battery packs with longer cycle life and higher specific energy would make this case even stronger., Comment: 12 pages, 3 figures, 1 table, 5 pages of SI

Electric Vehicles (EVs), like all modern vehicles, are entirely controlled by electronic devices embedded within networks that are exposed to the threat of cyberattacks. Cyber vulnerabilities are magnified with EVs due to unique risks associated with EV battery packs. Current batteries have well-known issues with specific energy, cost and fire-related safety risks. In this study, we develop a systematic framework to assess the impact of cyberattacks on EVs. While the current focus of automotive cyberattacks is on short-term physical safety, it is crucial to consider long-term cyberattacks that aim to cause financial losses through accrued impact, especially in the context of EVs. Faulty components of battery management systems such as a compromised voltage regulator could lead to cyberattacks that can overdischarge or overcharge the battery. Overdischarge could lead to failures such as internal shorts in the timescale of minutes through cyberattacks that compromise energy-intensive EV subsystems like auxiliary components. Attacks that overcharge the pack could shorten the lifetime of a new battery pack to less than a year. Further, such attacks also pose physical safety risks via the triggering of thermal (fire) events. Attacks on auxiliary components lead to battery drain, which could be up to 20% of the state-of-charge per hour. Lastly, we develop a heuristic for the stealthiness of a cyberattack to augment traditional threat models. The methodology presented here will help in building the foundational principles of electric vehicle cybersecurity: a nascent but critical topic in the coming years., Comment: 23 pages, 3 figures, 1 table, 9 pages of Supporting Information