To non‐destructively resolve and diagnose the degradation mechanisms of lithium‐ion batteries (LIBs), it is necessary to cross‐scale decouple complex kinetic processes through the distribution of relaxation times (DRT). However, LIBs with low interfacial impedance render DRT unreliable without data processing and closed‐loop validation. This study proposes a hierarchical analytical framework to enhance timescale resolution and reduce uncertainty, including interfacial impedance reconstruction and multi‐dimensional DRT analysis. Interfacial impedance is reconstructed by eliminating simulated inductive and diffusive impedance based on a high‐fidelity frequency‐domain model. Multi‐dimensional DRT decouples solid electrolyte interphase (SEI) and charge transfer (CT) processes by the reversibility of electrochemical reactions with state of charge (SOC) to characterize electrode kinetic evolution driven by SOC and temperature through timescales and peak area. The findings reveal that reconstructed impedance improves the accuracy of identified time constants by ≈20%. Cross‐scale DRT results reveal that SOCs below 10% at 25 °C effectively distinguish electrode kinetics due to the high correlation between cathodic CT and SOC. Kinetic metrics characterize that anodic SEI or CT are different control steps limiting the low‐temperature performance of different cells. This work underscores the potential of the proposed framework for non‐destructive diagnostics of kinetic evolution.

The mechanism revelation of performance decrease and fast-charging limitation of lithium-ion batteries at low temperatures is indispensable to optimize battery design and develop fast-charging methods. In this article, an electrochemical model-based quantitative analysis method is proposed to uncover the dominant reason for performance decrease and fast-charging limitation of batteries at low temperatures. The highly important dynamic parameters are carefully determined by the experimental data from the checked three-electrode battery and optimized by the genetic algorithm, rather than directly taken from the references. Validation results confirm that the electrochemical model can well reproduce battery behaviors under different conditions and that identified parameters are accurate. The quantitative analysis indicates that the sluggish diffusion in cathode and anode electrodes is the principal reason for battery available capacity loss. Battery available power attenuation is primarily attributed to the increased film resistance of anode and the reduced exchange current density of cathode, and it is substantially independent of the reduced diffusivity. The comparison result from the lithium-plating-prevention charging current reveals that the increased film resistance of the anode is responsible for the predominant limitation of low-temperature fast-charging, despite the most change in the exchange current density of the anode. This quantitative revelation breaks through the traditional understanding from the qualitative analysis that performance decrease and fast-charging limitation of batteries at low temperatures are highly associated with the degree of the change of characteristic parameters.

Lithium-ion batteries (LIBs) have the advantages of high energy/power densities, low self-discharge rate, and long cycle life, and thus are widely used in electric vehicles (EVs). However, at low temperatures, the peak power and available energy of LIBs drop sharply, with a high risk of lithium plating during charging. This poor performance significantly impacts the application of EVs in cold weather and dramatically limits the promotion of EVs in high-latitude regions. This challenge recently attracted much attention, especially investigating the performance decrease for LIBs at low temperatures, and exploring the solutions; however, limited reviews exist on this topic. Here, we thoroughly review the state-of-the-arts about battery performance decrease, modeling, and preheating, aiming to drive effective solutions for addressing the low-temperature challenge of LIBs. We outline the performance limitations of LIBs at low temperatures and quantify the significant changes in (dis)charging performance and resistance of LIBs at low temperatures. The various models considering low-temperature influencing factors are also tabulated and summarized, with the modeling improvement for describing low-temperature performance highlighted. Furthermore, we categorize the existing heating methods, and the metrics such as heating rate, energy consumption, and lifetime impact are highlighted to provide fundamental insights into the heating methods. Finally, the limits of current research on low-temperature LIBs are outlined, and an outlook on future research direction is provided.