Building Organic/Inorganic Hybrid Interphases for Fast Interfacial Transport in Rechargeable Metal Batteries

Abstract

We report a facile in situ synthesis that utilizes readily accessible SiCl cross-linking chemistry to create durable hybrid solid-electrolyte interphases (SEIs) on metal anodes. Such hybrid SEIs composed of Si-interlinked OOCOR molecules that host LiCl salt exhibit fast charge-transfer kinetics and as much as five-times higher exchange current densities, in comparison to their spontaneously formed analogues. Electrochemical analysis and direct optical visualization of Li and Na deposition in symmetric Li/Li and Na/Na cells show that the hybrid SEI provides excellent morphological control at high current densities (3-5 mA cm ) for Li and even for notoriously unstable Na metal anodes. The fast interfacial transport attributes of the SEI are also found to be beneficial for Li-S cells and stable electrochemical cycling was achieved in galvanostatic studies at rates as high as 2 C. Our work therefore provides a promising approach towards rational design of multifunctional, elastic SEIs that overcome the most serious limitations of spontaneously formed interphases on high-capacity metal anodes.

Metal Organic Framework Derivative Improving Lithium Metal Anode Cycling

“…The corresponding N 1s depth profile shows that Li 3 N, a good Li ion conductor, is distributed throughout the SEI layer (Figure 3l). Such an organic/inorganic well‐mixed SEI combining mechanical strength and ionic conductivity can mitigate the uneven Li ion flux and suppress dendrite formation during Li plating/stripping, thus promoting stable cycling of the Li metal electrode . In contrast, the SEI layer of the control cell only contains a thin and nonuniform layer of Li 3 N and organic species (Figure 3i,j), inferior in both structural flexibility and ionic conductivity, which is likely caused by uneven distribution/decomposition of LiNO 3 and solvent on the electrode surface.…”

A compact inorganic layer for robust anode protection in lithium‐sulfur batteries

“…40,41 Additives react irreversibly with Li anode to form in situ protective layer, in which the role of inorganic components is realized. [42][43][44][45] However, the sacrificial nature of the film-forming additives cripples their effects during long-term cycling. Constructing a robust ex situ protective layer emerges as another effective way to protect Li anode.…”

A Diffusion‐‐Reaction Competition Mechanism to Tailor Lithium Deposition for Lithium‐Metal Batteries

“…Comprehensive electrochemical characterizations were performed to evaluate the kinetics of Li migrating beneath the SEI. [18] The Tafel slopes of all samples were probed and obtained from the cyclic voltammetry (CV) profiles in Figure 3 a. The exchange current density (j 0 ) are calculated from the corresponding Tafel plots to reflect charge-transfer kinetics in SEI formed in different electrolytes.…”