Building better all-solid-state batteries with Li-garnet solid electrolytes and metalloid anodes

Afyon, Semih; Kravchyk, Kostiantyn V.; Wang, Shutao; Broek, Jan van den; Hänsel, Christian; Kovalenko, Maksym V.; Rupp, Jennifer L. M.

doi:10.1039/c9ta04999a

Cited by 54 publications

(38 citation statements)

References 83 publications

(97 reference statements)

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“…The garnet‐type solid electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) [ 5 ] crystallizing with cubic symmetry definitely represent one of the frontrunners in the group of the most promising oxidic solid electrolytes. [ 6 ] With their outstanding ionic conductivity, [ 7 ] and their wide electrochemical stability window, they are envisaged to play an important role in both the development of volume‐type [ 8 ] and thin‐film batteries. [ 9 ] Of course, sulfide‐based electrolytes or thiophosphates show even higher conductivity values [ 10 ] but suffer from their air‐sensitivity and electrochemical instability.…”

Section: Introductionmentioning

confidence: 99%

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries

Philipp

Gadermaier

Posch

et al. 2020

Adv Materials Inter

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The next‐generation of all‐solid‐state lithium batteries need ceramic electrolytes with very high ionic conductivities. At the same time a negligible electronic conductivity σeon is required to eliminate self‐discharge in such systems. A non‐negligible electronic conductivity may also promote the unintentional formation of Li dendrites, being currently one of the key issues hindering the development of long‐lasting all‐solid‐state batteries. This interplay is suggested recently for garnet‐type Li7La3Zr2O12 (LLZO). It is, however, well known that the overall macroscopic electronic conductivity may be governed by a range of extrinsic factors such as impurities, chemical inhomogeneities, grain boundaries, morphology, and size effects. Here, advantage of Czochralski‐grown single crystals, which offer the unique opportunity to evaluate intrinsic properties of a chemically homogeneous matrix, is taken to measure the electronic conductivity σeon. Via long‐time, high‐precision potentiostatic polarization experiments an upper limit of σeon in the order of 5 × 10−10 S cm−1 (293 K) is estimated. This value is by six orders of magnitude lower than the corresponding total conductivity σtotal = 10−3 S cm−1 of Ga‐LLZO. Thus, it is concluded that the high values of σeon recently reported for similar systems do not necessarily mirror intragrain bulk properties of chemically homogenous systems but may originate from chemically inhomogeneous interfacial areas.

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Section: Introductionmentioning

confidence: 99%

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries

Philipp

Gadermaier

Posch

et al. 2020

Adv Materials Inter

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“…Solid inorganic electrolytes can also assist the use of high capacity electrode materials (e.g., sulfur [261] and vanadate [262] based cathodes), which have otherwise stability and safety issues in combination with the current liquid organic electrolytes. Many successful examples of all-solid batteries, especially for thin-film and minimal electrode loading applications, utilizing lithium phosphorus oxynitride (LiPON), [263] thio-LISICON (Li x A 1−y M y S 4 , A = Si, Ge and M = P, Al, Zn, Ga, Sb), [264] Al-doped Li 7 La 3 Zr 2 O 12 garnet structures, [265,266] Li 10 GeP 2 S 12 (LGPS) family, [267] and fast Li-ion conducting argyrodites Li 6 PS 5 X (X = Cl, Br, I), [268] have been demonstrated in literature. However, though good ionic conductivities in the range of ≈10 −4 S cm −1 [269,270] and theoretical capacities for the tested cathode or anode materials were demonstrated for inorganic solid electrolytes, their use in larger scale batteries and long-term applications are yet to be realized because of contact losses on the electrode/electrolyte interface by the volume work with the extended cycling.…”

Section: All-solid-state Batteriesmentioning

confidence: 99%

Sustainable Li‐Ion Batteries: Chemistry and Recycling

Piątek

Afyon

Budnyak

et al. 2020

Advanced Energy Materials

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208

153

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/aenm.202003456.footprint of LIBs by designing their components that are less toxic and more abundant, the inevitable recycling is still largely in disagreement with circular principles. [1,2] This review summarizes and critically assesses current LIB recycling technologies from a sustainable perspective in order to derive whether current solutions can be referred as green technologies. The structure of the present review contains an introduction to the historical evolution of Li-based storage devices and recent issues in the supply chain of critical raw materials (CRMs) (Section 1), before focusing on chemical recycling strategies. This section shall deliver the mandatory input parameters for the subsequent analysis of LIBs recycling technologies to the reader. The review's primary focus is on the chemical aspects of LIBs recycling rather than technological aspects of recycling, and we refer readers to recently published reviews for the latter. [3,4] The second section encompasses conventional recycling methods and includes besides published articles in peer-reviewed journal also recycling solutions that were patented. Given the high economic importance of recycling business models, it is not surprising that many prospective solutions are only available in form of patent applications rather than being published in scientific journals. The third section expands recycling to sustainable recycling that ensures both a reduced toxicity and a close to CO 2 -neutral process. The fourth section elucidates the impact of using renewable materials on the chemistry of recycling processes of LIBs. The fifth section spans the connection of LIBs recycling to future Li-based energy storage devices. The final section concludes with an outlook to the future of sustainable recycling. The review considers only previously reported work that either i) describes the experimental details or ii) offers a reference to patents that describe the experimental procedure. Although we do not neglect the importance of published reports that may not fulfill the abovementioned requirements, we strongly believe that the latter are necessary for the development of sustainable recycling process ensuring reproducibility. Technology of LIBsThe light molar weight of lithium (M = 6.94 g mol −1 and density ρ = 0.53 g cm −3 ) and the most negative potential among metals (−3.04 V vs standard hydrogen electrode) of the Li + /Li

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“…Generally, LLZO was prepared based on a modified solgel synthesis-combustion approach. Sub-micron-sized particles were obtained at 650 • C (Afyon et al, 2019). The resultant LLZO electrolyte pellets had relative densities of ∼87% and ionic conductivities of ∼0.5 × 10 −3 S/cm at room temperature.…”

Section: Castingmentioning

confidence: 99%

Recent Developments and Challenges in Hybrid Solid Electrolytes for Lithium-Ion Batteries

et al. 2020

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Lithium-ion batteries (LIBs) have attracted worldwide research interest due to their high energy density and long cycle life. Solid-state LIBs improve the safety of conventional liquid-based LIBs by replacing the flammable organic electrolytes with a solid electrolyte. Among the various types of solid electrolytes, hybrid solid electrolytes (HSEs) demonstrate great promise to achieve high ionic conductivity, reduced interfacial resistance between the electrolyte and electrodes, mechanical robustness, and excellent processability due to the combined advantages of both polymer and inorganic electrolyte. This article summarizes recent developments in HSEs for LIBs. Approaches for the preparation of hybrid electrolytes and current understanding of iontransport mechanisms are discussed. The main challenges including unsatisfactory ionic conductivity and perspectives of HSEs for LIBs are highlighted for future development. The present review provides insights into HSE development to allow a more efficient and target-oriented future endeavor on achieving high-performance solid-state LIBs.

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Building better all-solid-state batteries with Li-garnet solid electrolytes and metalloid anodes

Abstract: All-solid-state batteries provide new opportunities to realize safe, non-flammable, and temperature-tolerant energy storage and display a huge potential to be the core of future energy storage devices.

Cited by 54 publications

References 83 publications

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries

Sustainable Li‐Ion Batteries: Chemistry and Recycling

Recent Developments and Challenges in Hybrid Solid Electrolytes for Lithium-Ion Batteries

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Building better all-solid-state batteries with Li-garnet solid electrolytes and metalloid anodes

Abstract: All-solid-state batteries provide new opportunities to realize safe, non-flammable, and temperature-tolerant energy storage and display a huge potential to be the core of future energy storage devices.

Cited by 54 publications

References 83 publications

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li7La3Zr2O12: A Technologically Relevant Parameter for All‐Solid‐State Batteries

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li7La3Zr2O12: A Technologically Relevant Parameter for All‐Solid‐State Batteries

Sustainable Li‐Ion Batteries: Chemistry and Recycling

Recent Developments and Challenges in Hybrid Solid Electrolytes for Lithium-Ion Batteries

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Product

Resources

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The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries

The Electronic Conductivity of Single Crystalline Ga‐Stabilized Cubic Li₇La₃Zr₂O₁₂: A Technologically Relevant Parameter for All‐Solid‐State Batteries