Enabling the use of lithium metal anodes is a critical step required to dramatically increase the energy density of rechargeable batteries. However, dendrite growth in lithium metal batteries, and a lack of fundamental understanding of the factors governing this growth, is a limiting factor preventing their adoption. Herein we present the effect of battery cycling temperature, ranging from 90 to 120 • C, on dendrite growth through a polystyrene-block-poly(ethylene oxide)-based electrolyte. This temperature range encompasses the glass transition temperature of polystyrene (107 • C). A slight increase in the cycling temperature of symmetric lithium-polymer-lithium cells from 90 to 105 • C results in a factor of five decrease in the amount of charge that can be passed before short circuit. Synchrotron hard X-ray microtomography experiments reveal a shift in dendrite location from primarily within the lithium electrode at 90 • C, to primarily within the electrolyte at 105 • C. Rheological measurements show a large change in mechanical properties over this temperature window. Time-temperature superposition was used to interpret the rheological data. Dendrite growth characteristics and cell lifetimes correlate with the temperature-dependent shift factors used for time-temperature superposition. Our work represents a step toward understanding the factors that govern lithium dendrite growth in viscoelastic electrolytes. Energy density and safety are two parameters that drive current research for improved rechargeable lithium batteries in applications such as electric vehicles and personal electronics.1 Many groups around the world are working on innovative battery chemistries, such as lithiumsulfur 2-5 and lithium-air, 3,[6][7][8] in an effort to improve battery energy density. Virtually all approaches that affect a substantial increase of the energy density of rechargeable batteries beyond that of lithiumion batteries require the use of a lithium metal anode. 4,9 Gallagher et al. show that coupling a lithium metal anode with currently available lithium cathodes results in energy densities that are three to six times larger than existing batteries used in electric vehicles. Likewise, lithium-sulfur and lithium-air chemistries rely on lithium metal anodes for improved energy density; battery energy densities obtained using a conventional graphite anode with sulfur and air cathodes are similar to those of traditional lithium ion batteries.
10The adoption of rechargeable lithium metal anode batteries has been hindered, however, by the formation of dendrites during battery cycling. 1,11,12 Upon repeated stripping and deposition, lithium metal deposits unevenly on the anode, creating protrusions that grow and eventually short the cell.13 Not only is the battery then unusable, but the flammable nature of typical liquid and gel electrolytes based on alkyl carbonates can result in catastrophic failure.1,14 Uncontrolled deposition of lithium metal can also take place in a conventional lithium-ion cell with a graphitic anode if t...