Solid–Liquid Electrolyte as a Nanoion Modulator for Dendrite-Free Lithium Anodes

Rechargeable lithium (Li) metal batteries are considered the most promising of Li-based energy storage technologies. However, tree-like dendrite produced by irregular Li+ electrodeposition restricts it wide applications. Herein, based on a cation-microphase-regulation strategy, we create solid-liquid electrolytes (SLEs) by absorbing commercial liquid electrolytes into polyethylene glycol (PEG) engineered nanoporous Al2O3 ceramic membranes. By means of molecular dynamics simulations and comprehensive experiments, we show that Li ions are regulated and promoted in the two microphases, the channel phase and nonchannel phase, respectively. The channel phase can achieve homogeneous Li+ flux distribution by multiple mechanisms, including its uniform array of nanochannels and ability to suppress lateral dendrite growth by its high modulus. In the nonchannel phase, PEG chains swollen by electrolyte facilitate desolvation and fast conduction of Li+. As a result, the studied SLEs exhibit high ionic conductivity, low interfacial resistance, and the unique ability to stabilize deposition at the Li anode. By means of galvanostatic cycling studies in symmetric Li cells and Li/Li4Ti5O12 cells, we further show that the materials open a path to Li metal batteries with excellent cycling performance.