A Two-Parameter Space to Tune Solid Electrolytes for Lithium Dendrite Constriction

[Image: see text] Li dendrite penetration, and associated microcrack propagation, at high current densities is one main challenge to the stable cycling of solid-state batteries. The interfacial decomposition reaction between Li dendrite and a solid electrolyte was recently used to suppress Li dendrite penetration through a novel effect of “dynamic stability”. Here we use a two-parameter space to classify electrolytes and propose that the effect may require the electrolyte to occupy a certain region in the space, with the principle of delicately balancing the two property metrics of a sufficient decomposition energy with the Li metal and a low critical mechanical modulus. Furthermore, in our computational prediction prepared using a combination of high-throughput computation and machine learning, we show that the positions of electrolytes in such a space can be controlled by the chemical composition of the electrolyte; the compositions can also be attained by experimental synthesis using core–shell microstructures. The designed electrolytes following this principle further demonstrate stable long cycling from 10 000 to 20 000 cycles at high current densities of 8.6–30 mA/cm(2) in solid-state batteries, while in contrast the control electrolyte with a nonideal position in the two-parameter space showed a capacity decay that was faster by at least an order of magnitude due to Li dendrite penetration.