4.8 Article

Revealing the Solid-State Electrolyte Interfacial Stability Model with Na-K Liquid Alloy

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 29, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202203409

Keywords

Alkali Metal Batteries; Interfacial Chemistry; Liquid Metal Anode; Multi-Cation Anode; Solid-State Electrolyte

Funding

  1. Welch Foundation [F-1861]
  2. Camille-Dreyfus Teacher Scholar Award
  3. National Science Foundation, Division of Materials Research [1938833]
  4. Division Of Materials Research
  5. Direct For Mathematical & Physical Scien [1938833] Funding Source: National Science Foundation

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In this study, a Na-K liquid alloy with a charge selective interfacial layer was developed on a sodium super-ionic conductor solid-state electrolyte to achieve a long cycling life with small overpotential. A unique model containing a chemical decomposition domain and a kinetic decomposition domain was proposed, and two charge selection mechanisms were validated. This study provides an effective design for high-energy-density solid-state batteries and offers a novel approach to understand interfacial chemical processes.
In this work, the Na-K liquid alloy with a charge selective interfacial layer is developed to achieve an impressively long cycling life with small overpotential on a sodium super-ionic conductor solid-state electrolyte (NASICON SSE). With this unique multi-cation system as the platform, we further propose a unique model that contains a chemical decomposition domain and a kinetic decomposition domain for the interfacial stability model. Based on this model, two charge selection mechanisms are proposed with dynamic chemical kinetic equilibrium and electrochemical kinetics as the manners of control, respectively, and both are validated by the electrochemical measurements with microscopic and spectroscopic characterizations. This study provides an effective design for high-energy-density solid-state battery with alkali Na-K anode, but also presents a novel approach to understand the interfacial chemical processes that could inspire and guide future designs.

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