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Dendrite formation during electrodeposition while charging lithium metalbatteries compromises their safety. While high shear modulus solid-ionconductors (SICs) have been prioritized to resolve pressure-driveninstabilities that lead to dendrite propagation and cell shorting, it isunclear whether these or alternatives are needed to guide uniform lithiumelectrodeposition, which is intrinsically density-driven. Here, we show thatSICs can be designed within a universal chemomechanical paradigm to accesseither pressure-driven dendrite-blocking or density-driven dendrite-suppressingproperties, but not both. This dichotomy reflects the competing influence ofthe SICs mechanical properties and partial molar volume of Li+ relative tothose of the lithium anode on plating outcomes. Within this paradigm, weexplore SICs in a previously unrecognized dendrite-suppressing regime that areconcomitantly soft, as is typical of polymer electrolytes, but featureatypically low Li+ partial molar volume, more reminiscent of hard ceramics. Liplating mediated by these SICs is uniform, as revealed using synchrotron hardx-ray microtomography. As a result, cell cycle-life is extended, even whenassembled with thin Li anodes and high-voltage NMC-622 cathodes, where 20percent of the Li inventory is reversibly cycled.

Universal Chemomechanical Design Rules for Solid-Ion Conductors to Prevent Dendrite Formation in Lithium Metal Batteries