Abstract
Solid-state Li-ion batteries with lithium anodes offer higher energy densities and are safer than conventional liquid electrolyte-based Li-ion batteries. However, the growth of lithium dendrites across the solid-state electrolyte layer leads to the premature shorting of cells and limits their practical viability. Here, using solid-state Li half-cells with metallic interlayers between a garnet-based lithium-ion conductor and lithium, we show that interfacial void growth precedes dendrite nucleation and growth. Specifically, void growth was observed at a current density of around two-thirds of the critical current density for dendrite growth. Computational calculations reveal that interlayer materials with higher critical current densities for dendrite growth also have the largest thermodynamic and kinetic barriers for lithium vacancy accumulation at their interfaces with lithium. Our results suggest that interfacial modification with suitable metallic interlayers decreases the tendency for void growth and improves dendrite growth tolerance in solid-state electrolytes, even in the absence of high stack pressures.
| Original language | English |
|---|---|
| Pages (from-to) | 1050-1056 |
| Number of pages | 7 |
| Journal | Nature Materials |
| Volume | 21 |
| Issue number | 9 |
| DOIs | |
| State | Published - Sep 2022 |
| Externally published | Yes |
Funding
This work was supported in part by grants from the Indian Space Research Organization (ISRO; grant no. ISTC/CSS/NPH/397), the Department of Heavy Industries (DHI), India, the Department of Science and Technology, India, through the DST-IISc Energy Storage Platform on Supercapacitors and Power Dense Devices under the MECSP-2K17 program (grant no. DST/TMD/MECSP/2K17/20) and by the Advanced Research Projects Agency-Energy Integration and Optimization of Novel Ion Conducting Solids (IONICS) programme (grant no. DE-AR0000774). V.R. acknowledges access to common facilities at CeNSE and SSCU. N.P.B.A. acknowledges the new faculty start-up grant (no. 12-0205-0618-77) provided by the Indian Institute of Science (IISc) and funding through the early career research award (grant no. ECR/2018/001047) of the Science and Engineering Research Board, Department of Science and Technology, India. The Extreme Science and Engineering Discovery Environment (XSEDE) is acknowledged for providing computational resources (award no. TG-CTS180061). This work was supported in part by grants from the Indian Space Research Organization (ISRO; grant no. ISTC/CSS/NPH/397), the Department of Heavy Industries (DHI), India, the Department of Science and Technology, India, through the DST-IISc Energy Storage Platform on Supercapacitors and Power Dense Devices under the MECSP-2K17 program (grant no. DST/TMD/MECSP/2K17/20) and by the Advanced Research Projects Agency-Energy Integration and Optimization of Novel Ion Conducting Solids (IONICS) programme (grant no. DE-AR0000774). V.R. acknowledges access to common facilities at CeNSE and SSCU. N.P.B.A. acknowledges the new faculty start-up grant (no. 12-0205-0618-77) provided by the Indian Institute of Science (IISc) and funding through the early career research award (grant no. ECR/2018/001047) of the Science and Engineering Research Board, Department of Science and Technology, India. The Extreme Science and Engineering Discovery Environment (XSEDE) is acknowledged for providing computational resources (award no. TG-CTS180061)41.