Cross‐Scale Decoupling Kinetic Processes in Lithium‐Ion Batteries Using the Multi‐Dimensional Distribution of Relaxation Time

Advanced Science, vol. 11, pp. e2406934

Abstract

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.

Authors 7

1. Xue Cai corresponding Aachen Center for Ageing

   Beijing Jiaotong University · RWTH Aachen University

   Affiliation as printed

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) Campus‐Boulevard 89 52074 Aachen Germany

   National Active Distribution Network Technology Research Center Beijing Jiaotong University Beijing 100044 China

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL), Campus-Boulevard 89, 52074 Aachen, Germany

   National Active Distribution Network Technology Research Center, Beijing Jiaotong University, Beijing, 100044 China

2. Caiping Zhang corresponding

   Beijing Jiaotong University

   Affiliation as printed

   National Active Distribution Network Technology Research Center Beijing Jiaotong University Beijing 100044 China

   National Active Distribution Network Technology Research Center, Beijing Jiaotong University, Beijing, 100044 China

3. Haijun Ruan corresponding

   Imperial College London · Coventry University

   Affiliation as printed

   Centre for E‐Mobility and Clean Growth Research Coventry University Coventry CV1 5FB UK

   Dyson School of Design Engineering Imperial College London London SW7 2AZ UK

   Centre for E-Mobility and Clean Growth Research, Coventry University, Coventry, CV1 5FB UK

   Dyson School of Design Engineering, Imperial College London, London, SW7 2AZ UK

4. Zeping Chen

   Beijing Jiaotong University

   Affiliation as printed

   National Active Distribution Network Technology Research Center Beijing Jiaotong University Beijing 100044 China

   National Active Distribution Network Technology Research Center, Beijing Jiaotong University, Beijing, 100044 China

5. Linjing Zhang

   Beijing Jiaotong University

   Affiliation as printed

   National Active Distribution Network Technology Research Center Beijing Jiaotong University Beijing 100044 China

   National Active Distribution Network Technology Research Center, Beijing Jiaotong University, Beijing, 100044 China

6. Dirk Uwe Sauer corresponding Aachen Center for Ageing

   Forschungszentrum Jülich · Helmholtz-Institute Münster · RWTH Aachen University

   Affiliation as printed

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) Campus‐Boulevard 89 52074 Aachen Germany

   Helmholtz Institute Münster (HI MS) IEK‐12 Forschungszentrum Jülich Germany

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL), Campus-Boulevard 89, 52074 Aachen, Germany

7. Weihan Li corresponding Aachen Center for Ageing

   RWTH Aachen University

   Affiliation as printed

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) Campus‐Boulevard 89 52074 Aachen Germany

   Center for Ageing, Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL), Campus-Boulevard 89, 52074 Aachen, Germany