Engineering and characterization of interphases for lithium metal anodes

Abstract

Lithium metal is a very promising anode material for achieving high energy density for next generation battery systems due to its low redox potential and high theoretical specific capacity of 3860 mA h g⁻¹. However, dendrite formation and low coulombic efficiency during cycling greatly hindered its practical applications. The formation of a stable solid electrolyte interphase (SEI) on the lithium metal anode (LMA) holds the key to resolving these problems. A lot of techniques such as electrolyte modification, electrolyte additive introduction, and artificial SEI layer coating have been developed to form a stable SEI with capability to facilitate fast Li⁺ transportation and to suppress Li dendrite formation and undesired side reactions. It is well accepted that the chemical and physical properties of the SEI on the LMA are closely related to the kinetics of Li⁺ transport across the electrolyte–electrode interface and Li deposition behavior, which in turn affect the overall performance of the cell. Unfortunately, the chemical and structural complexity of the SEI makes it the least understood component of the battery cell. Recently various advanced in situ and ex situ characterization techniques have been developed to study the SEI and the results are quite interesting. Therefore, an overview about these new findings and development of SEI engineering and characterization is quite valuable to the battery research community. In this perspective, different strategies of SEI engineering are summarized, including electrolyte modification, electrolyte additive application, and artificial SEI construction. In addition, various advanced characterization techniques for investigating the SEI formation mechanism are discussed, including in situ visualization of the lithium deposition behavior, the quantification of inactive lithium, and using X-rays, neutrons and electrons as probing beams for both imaging and spectroscopy techniques with typical examples.