High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Han, Fudong; Westover, Andrew S.; Yue, Jie; Fan, Xiulin; Wang, Fei; Chi, Miaofang; Leonard, Donovan N.; Dudney, Nancy J.; Wang, Howard; Wang, Chunsheng

doi:10.1038/s41560-018-0312-z

Cited by 1,332 publications

(1,309 citation statements)

References 59 publications

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“…This is very important to produce practical Li metal batteries. In a very recent literature, Wang et al pointed out that high electronic conductivity is the origin of lithium dendrite formation within SSEs . In the case of Li–Al–O SSE, Al 3+ is a strong hard acid while O 2− is a strong hard base.…”

Section: Resultsmentioning

confidence: 99%

A Li–Al–O Solid‐State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

Xie

Xing

Huang

et al. 2019

Adv Funct Materials

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Using a solid‐state electrolyte (SSE) to stabilize the Li metal anode is widely considered a promising route to develop next‐generation high energy density lithium batteries. Here, a new polycrystalline aluminate‐based SSE (named Li–Al–O SSE) with good capability is introduced to protect Li metal. The SSE is formed on the Li metal surface via a chemical reaction between LiOH and triethylaluminum (TEAL) with the existence of LiTFSI‐based electrolyte. It is a continuous film that consists of polycrystalline LiAlO2, Li3AlO3, Al2O3, Li2CO3, LiF, and some organic compounds. Such Li–Al–O SSE possesses a room‐temperature ionic conductivity as high as 1.42 × 10−4 S cm−1. Meanwhile, it effectively protects the Li anode from the corrosion of H2O, O2, and organic solvent, and suppresses the growth of Li dendrite. With the protection of the Li–Al–O SSE, the cycle life of Li|Li symmetric cell and Li|O2 cell is substantially elongated, indicating that the SSE exhibits an excellent protective effect under both inert and oxidizing circumstances.

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Section: Resultsmentioning

confidence: 99%

A Li–Al–O Solid‐State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

Xie

Xing

Huang

et al. 2019

Adv Funct Materials

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“…Furthermore, all ceramic solid ion conductors with high modulus can act both as the separator and the electrolyte to suppress dendritic growth 32. However, these more robust blocking separators often only serve to delay dendritic penetration and the subsequent shorting can result in an even more violent failure 33…”

Section: Figurementioning

confidence: 92%

Draining Over Blocking: Nano‐Composite Janus Separators for Mitigating Internal Shorting of Lithium Batteries

et al. 2020

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Catastrophic battery failure due to internal short is extremely difficult to detect and mitigate. In order to enable the next‐generation lithium‐metal batteries, a “fail safe” mechanism for internal short is highly desirable. Here, a novel separator design and approach is introduced to mitigate the effects of an internal short circuit by limiting the self‐discharge current to prevent cell temperature rise. A nano‐composite Janus separator—with a fully electronically insulating side contacting the anode and a partially electronically conductive (PEC) coating with tunable conductivity contacting the cathode—is implemented to intercept dendrites, control internal short circuit resistance, and slowly drain cell capacity. Galvanostatic cycling experiments demonstrate Li‐metal batteries with the Janus separator perform normally before shorting, which then results in a gradual increase of internal self‐discharge over >25 cycles due to PEC‐mitigated shorting. This is contrasted by a sudden voltage drop and complete failure seen with a single layer separator. Potentiostatic charging abuse tests of Li‐metal pouch cells result in dendrites completely penetrating the single‐layer separator causing high short circuit current and large cell temperature increase; conversely, negligible current and temperature rise occurs with the Janus separator where post mortem electron microscopy shows the PEC layer successfully intercepts dendrites.

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“…Moreover, the exploitation of alternative electrode chemistries, such as Li metal for LIBs, has been hindered by the intrinsically limited properties of LEs . For these reasons, the solidification of electrolytes with non‐flammable and single‐ion conducting inorganic solid electrolytes (SEs) is highly desired . Among various SE material candidates, the highest ionic conductivities comparable to those of LEs (≈10 mS cm −1 at room temperature) have been achieved for sulfide SEs (e.g., Li 10 GeP 2 S 12 : 12 mS cm −1 , Li 7 P 3 S 11 : 17 mS cm −1 , Li 5.5 PS 4.5 Cl 1.5 : 12 mS cm −1 ).…”

Section: Introductionmentioning

confidence: 99%

Ni‐Rich Layered Cathode Materials with Electrochemo‐Mechanically Compliant Microstructures for All‐Solid‐State Li Batteries

Jung

Kim

et al. 2019

Advanced Energy Materials

176

104

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While Ni‐rich cathode materials combined with highly conductive and mechanically sinterable sulfide solid electrolytes are imperative for practical all‐solid‐state Li batteries (ASLBs), they suffer from poor performance. Moreover, the prevailing wisdom regarding the use of Li[Ni,Co,Mn]O2 in conventional liquid electrolyte cells, that is, increased capacity upon increased Ni content, at the expense of degraded cycling stability, has not been applied in ASLBs. In this work, the effect of overlooked but dominant electrochemo‐mechanical on the performance of Ni‐rich cathodes in ASLBs are elucidated by complementary analysis. While conventional Li[Ni0.80Co0.16Al0.04]O2 (NCA80) with randomly oriented grains is prone to severe particle disintegration even at the initial cycle, the radially oriented rod‐shaped grains in full‐concentration gradient Li[Ni0.75Co0.10Mn0.15]O2 (FCG75) accommodate volume changes, maintaining mechanical integrity. This accounts for their different performance in terms of reversible capacity (156 vs 196 mA h g−1), initial Coulombic efficiency (71.2 vs 84.9%), and capacity retention (46.9 vs 79.1% after 200 cycles) at 30 °C. The superior interfacial stability for FCG75/Li6PS5Cl to for NCA80/Li6PS5Cl is also probed. Finally, the reversible operation of FCG75/Li ASLBs is demonstrated. The excellent performance of FCG75 ranks at the highest level in the ASLB field.

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High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Cited by 1,332 publications

References 59 publications

A Li–Al–O Solid‐State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

A Li–Al–O Solid‐State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

Draining Over Blocking: Nano‐Composite Janus Separators for Mitigating Internal Shorting of Lithium Batteries

Ni‐Rich Layered Cathode Materials with Electrochemo‐Mechanically Compliant Microstructures for All‐Solid‐State Li Batteries

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