A Brush-like Li-Ion Exchange Polymer as Potential Artificial Solid Electrolyte Interphase for Dendrite-Free Lithium Metal Batteries

Artificial polymeric solid electrolyte interfaces (APSEIs) are an emerging material that enables use of a lithium metal anode as a lithium metal battery technique with high energy density. However, the poor ionic conductivity, low lithium transference number, and bad compatibity with lithium metal anode lead to a large dissipative loss of energy capacity. Here we report that, by properly constructing a brush-like structure in cellulose nanofibril (CNF) based APSEIs, a good ion-aggregation morphology with interconnected ionic conducting channels can be built, such that the Li-ion conduction in the APSEI layer becomes highly efficient. The optimal approach to constructing such an ionic highway is proved computationally using coarse-grained molecular dynamics (CGMD) simulations and implemented experimentally based on transmission electron microscopy (TEM) and atomic force microscopy (AFM). In addition, Li-ion exchange structures and hydroxyl-abundant structures endow the APSEIs with good ability to suppress dendrite growth and excellent compatibility with the anode surface.