Abstract
Understanding the cause of lithium dendrites formation and propagation is essential for developing practical all-solid-state batteries. Li dendrites are associated with mechanical stress accumulation and can cause cell failure at current densities below the threshold suggested by industry research (i.e., >5 mA/cm2). Here, we apply a MHz-pulse-current protocol to circumvent low-current cell failure for developing all-solid-state Li metal cells operating up to a current density of 6.5 mA/cm2. Additionally, we propose a mechanistic analysis of the experimental results to prove that lithium activity near solid-state electrolyte defect tips is critical for reliable cell cycling. It is demonstrated that when lithium is geometrically constrained and local current plating rates exceed the exchange current density, the electrolyte region close to the defect releases the accumulated elastic energy favouring fracturing. As the build-up of this critical activity requires a certain period, applying current pulses of shorter duration can thus improve the cycling performance of all-solid-solid-state lithium batteries.
| Originalsprache | Englisch |
|---|---|
| Aufsatznummer | 2432 |
| Seitenumfang | 12 |
| Fachzeitschrift | Nature Communications |
| Jahrgang | 14.2023 |
| DOIs | |
| Publikationsstatus | Veröffentlicht - 27 Apr. 2023 |
Bibliographische Notiz
Funding Information:D.R. acknowledges financial support by the Austrian Federal Ministry for Digital and Economic Affairs, the National Foundation for Research, Technology and Development and the Christian Doppler Research Association (Christian Doppler Laboratory for Solid-State Batteries). Moreover, V.R. would like to thank the Austrian Marshall Plan Foundation for sponsoring parts of this project. P.F. and M.L.-M. acknowledge the European Research Council under the European Union’s Horizon 2020 Program (FP/2014–2020)/ERC Grant Agreement (771834—POPCRYSTAL). The CSnanoXRD experiments were performed on beamline ID13 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to Manfred Burghammer at the ESRF for providing assistance in using beamline ID13 and to Pavan Badami at Argonne National Laboratory for providing calcined LLZTO powder for preliminary test measurements.
Funding Information:
D.R. acknowledges financial support by the Austrian Federal Ministry for Digital and Economic Affairs, the National Foundation for Research, Technology and Development and the Christian Doppler Research Association (Christian Doppler Laboratory for Solid-State Batteries). Moreover, V.R. would like to thank the Austrian Marshall Plan Foundation for sponsoring parts of this project. P.F. and M.L.-M. acknowledge the European Research Council under the European Union’s Horizon 2020 Program (FP/2014–2020)/ERC Grant Agreement (771834—POPCRYSTAL). The CSnanoXRD experiments were performed on beamline ID13 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to Manfred Burghammer at the ESRF for providing assistance in using beamline ID13 and to Pavan Badami at Argonne National Laboratory for providing calcined LLZTO powder for preliminary test measurements.
Publisher Copyright:
© 2023, The Author(s).