Universal chemomechanical design rules for solid-ion conductors to prevent dendrite formation in lithium metal batteries
[2];
[4];
[5]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
- Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Mechanical Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Korea Inst. of Energy Research (KIER), Ulsan (South Korea). Ulsan Advanced Energy Technology R&D Center
- Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Dept. of Materials Science and Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry and Materials Sciences Division
Dendrite formation during electrodeposition while charging lithium metal batteries compromises their safety. Although high-shear-modulus (Gs) solid-ion conductors (SICs) have been prioritized to resolve the 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 SIC’s mechanical properties and the partial molar volume of Li+ $$(V_{\mathrm{Li}^+})$$ relative to those of the lithium anode (GLi and VLi) 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 an atypically low $$(V_{\mathrm{Li}^+})$$ that is more reminiscent of ‘hard’ ceramics. Li plating (1 mA cm-2; T = 20 °C) 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 (~30 µm) and either high-voltage NMC-622 cathodes (1.44 mAh cm-2) or high-capacity sulfur cathodes (3.02 mAh cm-2).
- Research Organization:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- USUSDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC02-05CH11231; AR0000774
- OSTI ID:
- 1631658
- Journal Information:
- Nature Materials, Vol. 19, Issue 7; ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing GroupCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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