Electrochemical Tracking of Lithium Metal Anode Surface Evolution via Voltage Relaxation Analysis.
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| Title: | Electrochemical Tracking of Lithium Metal Anode Surface Evolution via Voltage Relaxation Analysis. |
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| Authors: | Min, Yu-Jeong1 (AUTHOR), Shin, Heon-Cheol1 (AUTHOR) hcshin@pusan.ac.kr |
| Source: | Energies (19961073). Jan2026, Vol. 19 Issue 1, p187. 18p. |
| Subjects: | Lithium cell electrodes, Surface dynamics, Interface dynamics, Charge transfer, Equivalent electric circuits, Electrochemical analysis |
| Abstract: | The surface morphology of lithium metal electrodes evolves markedly during cycling, modulating interfacial kinetics and increasing the risk of dendrite-driven internal short circuits. Here, we infer this morphological evolution from direct-current (DC) signals by analyzing open-circuit voltage (OCV) transients after constant current interruptions. The OCV exhibits a rapid initial decay followed by a transition to a slower long-time decay. With repeated plating, this transition shifts to earlier times, thereby increasing the contribution of long-term relaxation. We quantitatively analyze this behavior using an equivalent circuit with a transmission-line model (TLM) representing the electrolyte-accessible interfacial region of the electrode, discretized into ten depth-direction segments. Tracking segment-wise changes in resistances and capacitances with cycling enables morphology estimation. Repeated plating strongly increases the double-layer area near the current collector, while the charge-transfer-active surface shifts toward the separator side, showing progressively smaller and eventually negative changes toward the current-collector side. Together with the segment-resolved time constants, these trends indicate that lithium deposition becomes increasingly localized near the separator-facing surface, while the interior becomes more tortuous, consistent with post-mortem observations. Overall, the results demonstrate that DC voltage-relaxation analysis combined with a TLM framework provides a practical route to track lithium metal electrode surface evolution in Li-metal-based cells. [ABSTRACT FROM AUTHOR] |
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| Database: | Engineering Source |
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| Abstract: | The surface morphology of lithium metal electrodes evolves markedly during cycling, modulating interfacial kinetics and increasing the risk of dendrite-driven internal short circuits. Here, we infer this morphological evolution from direct-current (DC) signals by analyzing open-circuit voltage (OCV) transients after constant current interruptions. The OCV exhibits a rapid initial decay followed by a transition to a slower long-time decay. With repeated plating, this transition shifts to earlier times, thereby increasing the contribution of long-term relaxation. We quantitatively analyze this behavior using an equivalent circuit with a transmission-line model (TLM) representing the electrolyte-accessible interfacial region of the electrode, discretized into ten depth-direction segments. Tracking segment-wise changes in resistances and capacitances with cycling enables morphology estimation. Repeated plating strongly increases the double-layer area near the current collector, while the charge-transfer-active surface shifts toward the separator side, showing progressively smaller and eventually negative changes toward the current-collector side. Together with the segment-resolved time constants, these trends indicate that lithium deposition becomes increasingly localized near the separator-facing surface, while the interior becomes more tortuous, consistent with post-mortem observations. Overall, the results demonstrate that DC voltage-relaxation analysis combined with a TLM framework provides a practical route to track lithium metal electrode surface evolution in Li-metal-based cells. [ABSTRACT FROM AUTHOR] |
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| ISSN: | 19961073 |
| DOI: | 10.3390/en19010187 |
