Break-Even Analysis of All-Solid-State Batteries with Li-Garnet Solid Electrolytes

Kravchyk, Kostiantyn V.; Okur, Faruk; Kovalenko, Maksym V.

doi:10.1021/acsenergylett.1c00672

Cited by 40 publications

(29 citation statements)

References 61 publications

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“…The previous λ estimates are for typical 1 mm-thick LLZO pellets. To increase energy density, it is ideal to reduce the solid electrolyte thickness to hundreds or tens of microns . At those scales, our discussions remain relevant as the ion exchange thickness can be scaled with t .…”

Section: Resultsmentioning

confidence: 99%

“…To increase energy density, it is ideal to reduce the solid electrolyte thickness to hundreds or tens of microns. 93 At those scales, our discussions remain relevant as the ion exchange thickness can be scaled with t. For thin solid electrolytes, the layer thickness is likely to be a significant fraction of t. This will increase σ T inside of the pellet (via eq 11) and reduce σ c in the surface layer.…”

Section: Macroscopic Residual Compressive Stressmentioning

confidence: 99%

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Tradeoff between the Ion Exchange-Induced Residual Stress and Ion Transport in Solid Electrolytes

et al. 2022

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Rapid filament growth of lithium is limiting the commercialization of solid-state lithium metal anode batteries. Recent work demonstrated that lithium filaments grow into pre-existing or nascent cracks in the solid electrolyte, suggesting that increasing the fracture toughness of the solid electrolytes will inhibit filament penetration. It has been suggested that introducing residual compressive stresses at the surface of the solid electrolyte can provide this additional fracture toughness. One of the ways to induce these residual compressive stresses is by exchanging lithium ions (Li+) with larger isovalent ions such as potassium (K+). On the other hand, incorporation of too much potassium can alter the lithium-ion diffusion pathway and lower the diffusivity, thus limiting the performance of the solid-state electrolyte. Using multiscale modeling methods, we optimize this tradeoff and predict that exchanging 3.4% potassium ions up to a depth twice the grain sizes in Li7La3Zr2O12 solid electrolyte can induce a maximum residual compressive stress of around 1.1 GPa, corresponding to an increase in fracture strength by ∼8 times, while lowering the diffusivity in the ion-exchanged region by a factor of 5 at room temperature. The reduction of lithium diffusivity is due to K+-induced stress and (mainly) blockage of lithium ion pathways in the shallow ion-exchanged layer.

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Section: Resultsmentioning

confidence: 99%

Section: Macroscopic Residual Compressive Stressmentioning

confidence: 99%

Tradeoff between the Ion Exchange-Induced Residual Stress and Ion Transport in Solid Electrolytes

et al. 2022

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“…CCD is a crucial parameter for evaluating the efficacy of SEs and electrode–SE interfaces to suppress dendrites in ASSLBs. Several emerging SEs have been explored, including Li stuffed garnets, Li superionic conductor (LISICON)-type (Li 14 ZnGe 4 O 16 ), thio-LISICON (Li 4‑ x M 1‑ x P x S 4 (M = Ge, Si); Li 10 GeP 2 S 12 ), argyrodites (Li 6 PS 5 X (X = Cl, Br, I)), Na superionic conductor (NASICON)-type (Li 1+ x Al x Ge 2‑ x (PO 4 ) 3 , Li 1+ x Al x Ti 2‑ x (PO 4 ) 3 ), sulfide electrolytes, solid polymer electrolytes (SPEs), and lithium phosphorus oxynitride (LiPON). The nature of interfaces and the interfacial composition and structure between electrode–SE interfaces necessitate thorough research.…”

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confidence: 99%

Critical Current Densities for High-Performance All-Solid-State Li-Metal Batteries: Fundamentals, Mechanisms, Interfaces, Materials, and Applications

Sarkar

Thangadurai

2022

ACS Energy Lett.

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All-solid-state lithium batteries (ASSLBs) are considered promising next-generation energy storage devices due to their safety and high volumetric energy densities. However, achieving the key U.S. DOE milestone of a power density of 33 kW L −1 appears to be a significant hurdle in current ASSLBs. One of the main reasons is that advancements in solid electrolyte (SE) conductivity have been prioritized over the critical current density (CCD) when employing an elemental Li anode. Several aspects of Li electrode-and SE interface-based difficulties must be resolved before commercialization. Here, we very deeply analyze some crucial parameters that effectively restrict Li dendrite formation while achieving high CCD. Mechanistic explanations are provided to comprehend the critical relationship between a cell failure and development of Li dendrites. The latest progress is discussed in achieving higher CCD in emerging SE structures, including Li-stuffed garnets, Na superionic conductors (NASICONs), Li sulfides, and lithium phosphorus oxynitride (LiPON). Furthermore, primary strategies for improving CCDs by tailoring SE design and stabilizing interfaces are proposed for advanced ASSLBs.

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“…Li–garnet solid-state batteries (SSBs) have attracted a great deal of attention due to their nonflammability, nontoxicity, and potential to achieve significantly higher energy and power densities compared to those of conventional Li-ion batteries. − Research that began in 2007 and focused primarily on improving the Li-ion conductivity of Li 7 La 3 Zr 2 O 12 (LLZO) has since evolved into the development of Li–garnet SSBs, encompassing aspects of the LLZO/Li interface, , the electrochemical voltage window of LLZO, − and compatibility with current cathode chemistries. − Nevertheless, an analysis of the literature shows that there is still no clear opinion in the research community on the configuration of future Li–garnet SSBs. In particular, opinions differ on the design of the LLZO-based anode layer that accounts for (i) the dynamic expansion and shrinkage of the Li metal (from up to 5–25 μm for the area capacity of 1–5 mAh cm –2 ) and (ii) the probability of void formation at the Li/LLZO interface.…”

mentioning

confidence: 99%

“…The combination of LLZO thickness and porosity, allowing us to attain energy densities of 250, 275, 300, and 350 Wh kg −1 , is shown as dashed lines. Another important curve, shown in blue, represents the minimum required combination of LLZO thickness and porosity that results in a pore volume of approximately 0.0017 cm 3 . This pore volume theoretically allows for the complete plating of Li within the LLZO scaffold for a given areal capacity of 3.5 mAh cm −2 .…”

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confidence: 99%

Li–Garnet Solid-State Batteries with LLZO Scaffolds

et al. 2022

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Break-Even Analysis of All-Solid-State Batteries with Li-Garnet Solid Electrolytes

Cited by 40 publications

References 61 publications

Tradeoff between the Ion Exchange-Induced Residual Stress and Ion Transport in Solid Electrolytes

Tradeoff between the Ion Exchange-Induced Residual Stress and Ion Transport in Solid Electrolytes

Critical Current Densities for High-Performance All-Solid-State Li-Metal Batteries: Fundamentals, Mechanisms, Interfaces, Materials, and Applications

Li–Garnet Solid-State Batteries with LLZO Scaffolds

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