Solid‐State NMR and MRI Spectroscopy for Li/Na Batteries: Materials, Interface, and In Situ Characterization

Abstract Enhancing the electrochemical performance of batteries, including the lifespan, energy, and power densities, is an everlasting quest for the rechargeable battery community. However, the dynamic and coupled (electro)chemical processes that occur in the electrode materials as well as at the electrode/electrolyte interfaces complicate the investigation of their working and decay mechanisms. Herein, the recent developments and applications of solid‐state nuclear magnetic resonance (ssNMR) and magnetic resonance imaging (MRI) techniques in Li/Na batteries are reviewed. Several typical cases including the applications of NMR spectroscopy for the investigation of the pristine structure and the dynamic structural evolution of materials are first emphasized. The NMR applications in analyzing the solid electrolyte interfaces (SEI) on the electrode are further concluded, involving the identification of SEI components and investigation of ionic motion through the interfaces. Beyond, the new development of in situ NMR and MRI techniques are highlighted, including their advantages, challenges, applications and the design principle of in situ cell. In the end, a prospect about how to use ssNMR in battery research from the perspectives of materials, interface, and in situ NMR, aiming at obtaining deeper insight of batteries with the assistance of ssNMR is represented.