Operando Interaction and Transformation of Metastable Defects in Layered Oxides for Na‐Ion Batteries

Author:

Gorobtsov Oleg Yu.1ORCID,Hirsh Hayley2,Zhang Minghao2,Sheyfer Dina3,Nguyen Long Hoang Bao2,Matson Stephanie D.1,Weinstock Daniel1,Bouck Ryan1,Wang Ziyi1,Cha Wonsuk3,Maser Jörg3,Harder Ross3,Meng Ying Shirley24ORCID,Singer Andrej1ORCID

Affiliation:

1. Department of Materials Science and Engineering Cornell University Ithaca NY 14853 USA

2. Department of NanoEngineering University of California San Diego La Jolla CA 92093 USA

3. Advanced Photon Source Argonne National Laboratory Argonne IL 60439 USA

4. Pritzker School of Molecular Engineering The University of Chicago Chicago IL 60637 USA

Abstract

AbstractNon‐equilibrium defects often dictate the macroscopic properties of materials. They largely define the reversibility and kinetics of processes in intercalation hosts in rechargeable batteries. Recently, imaging methods have demonstrated that transient dislocations briefly appear in intercalation hosts during ion diffusion. Despite new discoveries, the understanding of impact, formation and self‐healing mechanisms of transient defects, including and beyond dislocations, is lacking. Here, operando X‐ray Bragg Coherent Diffractive Imaging (BCDI) and diffraction peak analysis capture the stages of formation of a unique metastable domain boundary, defect self‐healing, and resolve the local impact of defects on ionic diffusion in NaxNi1−yMnyO2 intercalation hosts in a charging sodium‐ion battery. Results, applicable to a wide range of layered intercalation materials due to the shared nature of framework layers, elucidate new dynamics of transient defects and their connection to macroscopic properties, and suggest how to control the nanostructure dynamics.

Funder

National Science Foundation

Argonne National Laboratory

Publisher

Wiley

Subject

General Materials Science,Renewable Energy, Sustainability and the Environment

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