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Universal Chemomechanical Design Rules for Solid-Ion Conductors to Prevent Dendrite Formation in Lithium Metal Batteries
Materials Science · Submitted 15 Jan 2019
abstract compiled · 2026-09-23 · no language-model review
The authors' main claim Here, we show that SICs can be designed within a universal chemomechanical paradigm to access either pressure-driven dendrite-blocking or density-driven dendrite-suppressing properties, but not both.
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The abstract, sentence by sentence
Dendrite formation during electrodeposition while charging lithium metal batteries compromises their safety. While high shear modulus solid-ion conductors (SICs) have been prioritized to resolve pressure-driven instabilities that lead to dendrite propagation and cell shorting, it is unclear whether these or alternatives are needed to guide uniform lithium electrodeposition, which is intrinsically density-driven. Here, we show that SICs can be designed within a universal chemomechanical paradigm to access either pressure-driven dendrite-blocking or density-driven dendrite-suppressing properties, but not both. This dichotomy reflects the competing influence of the SICs mechanical properties and partial molar volume of Li+ relative to those of the lithium anode on plating outcomes. Within this paradigm, we explore SICs in a previously unrecognized dendrite-suppressing regime that are concomitantly soft, as is typical of polymer electrolytes, but feature atypically low Li+ partial molar volume, more reminiscent of hard ceramics. Li plating mediated by these SICs is uniform, as revealed using synchrotron hard x-ray microtomography. As a result, cell cycle-life is extended, even when assembled with thin Li anodes and high-voltage NMC-622 cathodes, where 20 percent of the Li inventory is reversibly cycled.
background contribution method result interpretation main claim
| # | sentence | role | the authors' own work | states the main conclusion | strength |
|---|---|---|---|---|---|
| s0 | Dendrite formation during electrodeposition while charging lithium metal batteries compromises their safety. | background 1.00 | 0.05 | 0.02 | asserted 1.00 |
| s1 | While high shear modulus solid-ion conductors (SICs) have been prioritized to resolve pressure-driven instabilities that lead to dendrite propagation and cell shorting, it is unclear whether these or alternatives are needed to guide uniform lithium electrodeposition, which is intrinsically density-driven. | gap 0.93 | 0.05 | 0.04 | asserted 0.59 |
| s2 | Here, we show that SICs can be designed within a universal chemomechanical paradigm to access either pressure-driven dendrite-blocking or density-driven dendrite-suppressing properties, but not both. | result 0.76 | 0.92 | 0.88 | asserted 1.00 |
| s3 | This dichotomy reflects the competing influence of the SICs mechanical properties and partial molar volume of Li+ relative to those of the lithium anode on plating outcomes. | interpretation 1.00 | 0.47 | 0.11 | asserted 1.00 |
| s4 | Within this paradigm, we explore SICs in a previously unrecognized dendrite-suppressing regime that are concomitantly soft, as is typical of polymer electrolytes, but feature atypically low Li+ partial molar volume, more reminiscent of hard ceramics. | contribution 0.91 | 0.84 | 0.10 | asserted 0.99 |
| s5 | Li plating mediated by these SICs is uniform, as revealed using synchrotron hard x-ray microtomography. | result 0.96 | 0.94 | 0.08 | asserted 1.00 |
| s6 | As a result, cell cycle-life is extended, even when assembled with thin Li anodes and high-voltage NMC-622 cathodes, where 20 percent of the Li inventory is reversibly cycled. | result 0.99 | 0.91 | 0.13 | asserted 1.00 |
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Original abstract
Dendrite formation during electrodeposition while charging lithium metal batteries compromises their safety. While high shear modulus solid-ion conductors (SICs) have been prioritized to resolve pressure-driven instabilities that lead to dendrite propagation and cell shorting, it is unclear whether these or alternatives are needed to guide uniform lithium electrodeposition, which is intrinsically density-driven. Here, we show that SICs can be designed within a universal chemomechanical paradigm to access either pressure-driven dendrite-blocking or density-driven dendrite-suppressing properties, but not both. This dichotomy reflects the competing influence of the SICs mechanical properties and partial molar volume of Li+ relative to those of the lithium anode on plating outcomes. Within this paradigm, we explore SICs in a previously unrecognized dendrite-suppressing regime that are concomitantly soft, as is typical of polymer electrolytes, but feature atypically low Li+ partial molar volume, more reminiscent of hard ceramics. Li plating mediated by these SICs is uniform, as revealed using synchrotron hard x-ray microtomography. As a result, cell cycle-life is extended, even when assembled with thin Li anodes and high-voltage NMC-622 cathodes, where 20 percent of the Li inventory is reversibly cycled.
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These include the use of artificial solid electrolyte interphase (SEI) [ref] , additives in liquid electrolytes [ref] , surface nanostructuring [ref] , solid polymer or inorganic electrolytes [ref] .
Design rules for liquid crystalline electrolytes for enabling dendrite-free lithium metal batteries · Introduction · 0.88
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