The phantom menace of dynamic soft-shorts in solid-state battery research

Counihan, Michael J.; Chavan, Kanchan S.; Barai, Pallab; Powers, Devon J.; Zhang, Yuepeng; Srinivasan, Venkat; Tepavcevic, Sanja

doi:10.1016/j.joule.2023.11.007

Cited by 19 publications

(5 citation statements)

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“…The importance of Mode II has also been emphasized in electrolyte studies for solid-state batteries and its influence in molten Na batteries should be further explored (Han et al, 2019;Gorai et al, 2021;Wang et al, 2022;Shao et al, 2023). Detailed electrolyte studies utilizing unidirectional testing, conductivity vs. temperature series, and operando imaging would be beneficial to further understanding these important failure mechanisms (Fuchs et al, 2023;Counihan et al, 2024).…”

Section: Mode I and Ii Failure In Solid Electrolytesmentioning

confidence: 99%

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Hill,

Gross,

Percival

et al. 2024

Front. Batter. Electrochem.

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The need for clean, renewable energy has driven the expansion of renewable energy generators, such as wind and solar. However, to achieve a robust and responsive electrical grid based on such inherently intermittent renewable energy sources, grid-scale energy storage is essential. The unmet need for this critical component has motivated extensive grid-scale battery research, especially exploring chemistries “beyond Li-ion”. Among others, molten sodium (Na) batteries, which date back to the 1960s with Na-S, have seen a strong revival, owing mostly to raw material abundance and the excellent electrochemical properties of Na metal. Recently, many groups have demonstrated important advances in battery chemistries, electrolytes, and interfaces to lower material and operating costs, enhance cyclability, and understand key mechanisms that drive failure in molten Na batteries. For widespread implementation of molten Na batteries, though, further optimization, cost reduction, and mechanistic insight is necessary. In this light, this work provides a brief history of mature molten Na technologies, a comprehensive review of recent progress, and explores possibilities for future advancements.

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Section: Mode I and Ii Failure In Solid Electrolytesmentioning

confidence: 99%

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Hill,

Gross,

Percival

et al. 2024

Front. Batter. Electrochem.

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“…The entire process may be accelerated by the melting of Li dendrites, as internal short-circuiting is known for Joule heat generation. 41,43,44 When Li dendrites cannot be sustained by the mechanical deformation and infiltration of bulk Li, the cell voltage and stack pressure start to rise again in Stage IV (Figure 5 This proposed mechanism, which combines chemical reduction and electrochemical oxidation of NCA with macroscopic Li deformation, is supported by the increased full-cell resistance due to the severe chemical reactions between NCA and Li dendrites after the ninth discharge (Figure S13). As shown in Figure S14, galvanotactic electrochemical impedance spectra (GEIS) were also used to study the soft-shorting mechanism.…”

mentioning

confidence: 97%

“…This type of cell failure is not exclusive to our anode-free batteries, it has been reported in solid-state Li metal batteries, ,− commonly described as “soft shorting” or “shorting” due to Li dendrite formation. Combining semiquantitative impedance analysis and computational modeling, Counihan et al provided a very detailed study on the dynamic behavior of soft-shorting in Li metal based symmetric and half cells with polymer-ceramic composite electrolyte and highlights possible mechanisms of forming, unshorting, and reshorting during soft-shorting. The detailed mechanisms of soft-shorting in an anode-free full cell with a sulfide-based solid electrolyte, to our knowledge, have not been reported.…”

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confidence: 99%

“…During the early appearance of Li dendrites, their content is limited. Li dendrites chemically reduce the charged NCA, lowering the cathode potential . Once the dendrites are chemically reacted, the cathode potential increases again due to electrochemical charging (or oxidation) of NCA by the applied current, and SE also regains its function to transport lithium ions until the next dendrite-NCA contact, thereby resuming Li plating and the corresponding stack pressure increase.…”

mentioning

confidence: 99%

“…However, not all the plated Li infiltrates the SE because the pressure change does not drop to 0 MPa. The entire process may be accelerated by the melting of Li dendrites, as internal short-circuiting is known for Joule heat generation. ,, …”

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confidence: 99%

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Hydride-Based Interlayer for Solid-State Anode-Free Battery

Huang,

Zhang,

et al. 2024

ACS Energy Lett.

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Solid-state batteries (SSBs) are considered a promising approach to realizing an anode-free concept with high energy densities. However, the initial Coulombic efficiency (ICE) has remained insufficient for anode-free batteries using sulfide-based solid electrolytes (SEs). Herein, we incorporated a hydride-based interlayer, 3LiBH 4 -LiI (LBHI), between a typical sulfide SE, Li 6 PS 5 Cl, and the Cu current collector. By investigating the Li plating and stripping behaviors and the (electro)chemical stability between SEs and plated Li, we demonstrated that LBHI can effectively improve interfacial stability, leading to an ICE exceeding 94% in anode-free half cells. This interlayer also improves Coulombic efficiencies and specific capacities in anode-free full cells. Furthermore, the utilization of LBHI enables one to study Li plating behaviors without interference from interfacial (electro)chemical instabilities. The analysis of stack pressure evolution during electrochemical cycling reveals that soft shorting in SSBs arises from both dendrite formation and deformation, offering insights into further optimizing solidstate anode-free batteries.

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Single Atomic Cu‐C₃ Sites Catalyzed Interfacial Chemistry in Bi@C for Ultra‐Stable and Ultrafast Sodium‐Ion Batteries

Li,

Tang,

Wang

et al. 2024

Angewandte Chemie

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Regulating interfacial chemistry at electrode–electrolyte interface by designing catalytic electrode material is crucial and challenging for optimizing battery performance. Herein, a novel single atom Cu regulated Bi@C with Cu–C3 site (Bi@SA Cu–C) have been designed via the simple pyrolysis of metal–organic framework. Experimental investigations and theoretical calculations indicate the Cu–C3 sites accelerate the dissociation of P–F and C–O bonds in NaPF6–ether–based electrolyte and catalyze the formation of inorganic–rich and powerful solid electrolyte interphase. In addition, the Cu–C3 sites with delocalized electron around Cu trigger an uneven charge distribution and induce an in–plane local electric field, which facilitates the adsorption of Na+ and reduces the Na+ migration energy barrier. Consequently, the obtained Bi@SA Cu–C achieves a state–of–the–art reversible capacity, ultrahigh rate capability, and long–term cycling durability. The as–constructed full cell delivers a high capacity of 351 mAh g−1 corresponding to an energy density of 265 Wh kg−1. This work provides a new strategy to realize high–efficient sodium ion storage for alloy–based anode through constructing single–atom modulator integrated catalysis and promotion effect into one entity.

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The phantom menace of dynamic soft-shorts in solid-state battery research

Cited by 19 publications

References 73 publications

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Hydride-Based Interlayer for Solid-State Anode-Free Battery

Single Atomic Cu‐C₃ Sites Catalyzed Interfacial Chemistry in Bi@C for Ultra‐Stable and Ultrafast Sodium‐Ion Batteries

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The phantom menace of dynamic soft-shorts in solid-state battery research

Cited by 19 publications

References 73 publications

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Molten sodium batteries: advances in chemistries, electrolytes, and interfaces

Hydride-Based Interlayer for Solid-State Anode-Free Battery

Single Atomic Cu‐C3 Sites Catalyzed Interfacial Chemistry in Bi@C for Ultra‐Stable and Ultrafast Sodium‐Ion Batteries

Contact Info

Product

Resources

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Single Atomic Cu‐C₃ Sites Catalyzed Interfacial Chemistry in Bi@C for Ultra‐Stable and Ultrafast Sodium‐Ion Batteries