Lithium Dendrite in All-Solid-State Batteries: Growth Mechanisms, Suppression Strategies, and Characterizations

Cao, Daxian; Sun, Xiao; Li, Qiang; Natan, Avi; Xiang, Pengyang; Zhu, Hongli

doi:10.1016/j.matt.2020.03.015

Cited by 438 publications

(300 citation statements)

References 128 publications

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“…[ 1,5 ] Their elastic moduli could range from tens to hundreds of gigapascals, which are, in theory, more than enough to physically block the growth of Li dendrite penetration. [ 4,6,7 ] Unfortunately, Li penetration in such promising ceramic SEs as Li 7 La 3 Zr 2 O 12 (LLZO) is unexpectedly observed in experimental studies. [ 8–12 ] Li filaments are found at microstructural defects such as voids, cracks, and particularly along the grain boundary (GB), [ 8,13–15 ] suggesting that the microstructural impact on the Li penetration behavior is significant.…”

Section: Introductionmentioning

confidence: 99%

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Tantratian

Yan

Ellwood

et al. 2021

Advanced Energy Materials

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Lithium dendrite penetration has been widely evidenced in ceramic solid electrolytes (SEs), which are expected to suppress Li dendrite formation due to their ultrahigh elastic modulus. This work aims to reveal the mechanism of Li penetration in polycrystalline SEs through electro‐chemo‐mechanical phase‐field model, using Li7La3Zr2O12 (LLZO) as the model material. The results show the Li penetration patterns are influenced by both mechanical and electronic properties of the microstructures, i.e., grain boundaries (GBs). Li nucleates at the GB junctions on the Li/SE interface and propagates along the GB, at which the interfacial compressive stress is small due to the GB softening. Moreover, the excess trapped electrons at the GB may trigger isolated Li nucleation sites, abruptly increasing the Li penetration depth. High‐throughput simulations yield a phase map of Li penetration patterns under different trapped electrons concentrations and GB/grain elastic modulus mismatch. The map can quantitatively inform whether the mechanical or electronic properties dominate Li penetration morphologies, providing a strategy for the design of improved SE materials.

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Section: Introductionmentioning

confidence: 99%

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Tantratian

Yan

Ellwood

et al. 2021

Advanced Energy Materials

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“…As the cycling continues, the growing lithium dendrites pierce the separator, triggering a short circuit. Furthermore, the ohmic heat produced by this phenomenon can cause thermal runaway and disastrous battery failure (Finegan et al, 2017 ; Cao et al, 2020 ; Xiong et al, 2020 ).…”

Section: Introductionmentioning

confidence: 99%

Li7La3Zr2O12 Garnet Solid Polymer Electrolyte for Highly Stable All-Solid-State Batteries

et al. 2021

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All-solid-state batteries have gained significant attention as promising candidates to replace liquid electrolytes in lithium-ion batteries for high safety, energy storage performance, and stability under elevated temperature conditions. However, the low ionic conductivity and unsuitability of lithium metal in solid polymer electrolytes is a critical problem. To resolve this, we used a cubic garnet oxide electrolyte (Li7La3Zr2O12 – LLZO) and ionic liquid in combination with a polymer electrolyte to produce a composite electrolyte membrane. By applying a solid polymer electrolyte on symmetric stainless steel, the composite electrolyte membrane shows high ionic conductivity at elevated temperatures. The effect of LLZO in suppressing lithium dendrite growth within the composite electrolyte was confirmed through symmetric lithium stripping/plating tests under various current densities showing small polarization voltages. The full cell with lithium iron phosphate as the cathode active material achieved a highest specific capacity of 137.4 mAh g−1 and a high capacity retention of 98.47% after 100 cycles at a current density of 50 mA g−1 and a temperature of 60°C. Moreover, the specific discharge capacities were 137 and 100.8 mAh g−1 at current densities of 100 and 200 mA g−1, respectively. This research highlights the capability of solid polymer electrolytes to suppress the evolution of lithium dendrites and enhance the performance of all-solid-state batteries.

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“…These results may indicate that cycling at lower currents induces a slow degradation of the cell interfaces, evidenced by the large resistance as well as the high overpotential of the cell. However, at higher currents the failure of the cell is probably induced by the formation of dendrites [ 10 ], as observed from the sudden loss of capacity at C/5. The high current density is prone to favor dendritic Li metal during Li electrodeposition.…”

Section: Resultsmentioning

confidence: 99%

“…The replacement of the liquid organic electrolyte in conventional LIBs by solid electrolytes, considered as a solution to high-capacity lithium-metal anodes owing to their mechanical strength, in solid-state batteries (SSBs), offers outstanding high-energy and high-power densities as well as inherent safety [ 3 , 4 , 5 , 6 ]. However, far from being a reality, there are still many challenges to overcome on the use of lithium metal anodes for solid-state batteries [ 7 , 8 ]: most of the solid inorganic Li ion conductors are thermodynamically unstable [ 9 ] and dendrite growth is still a problem due to the inhomogeneous dissolution and subsequent deposition over cycling [ 8 , 10 , 11 , 12 ]. In addition, the continuous stripping and plating of Li metal needs to be fast enough to ensure their performance at an acceptable C-rate.…”

Section: Introductionmentioning

confidence: 99%

Designing Spinel Li4Ti5O12 Electrode as Anode Material for Poly(ethylene)oxide-Based Solid-State Batteries

et al. 2021

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The development of a promising Li metal solid-state battery (SSB) is currently hindered by the instability of Li metal during electrodeposition; which is the main cause of dendrite growth and cell failure at elevated currents. The replacement of Li metal anode by spinel Li4Ti5O12 (LTO) in SSBs would avoid such problems, endowing the battery with its excellent features such as long cycling performance, high safety and easy fabrication. In the present work, we provide an evaluation of the electrochemical properties of poly(ethylene)oxide (PEO)-based solid-state batteries using LTO as the active material. Electrode laminates have been developed and optimized using electronic conductive additives with different morphologies such as carbon black and multiwalled carbon nanotubes. The electrochemical performance of the electrodes was assessed on half-cells using a PEO-based solid electrolyte and a lithium metal anode. The optimized electrodes displayed an enhanced capability rate, delivering 150 mAh g−1 at C/2, and a stable lifespan over 140 cycles at C/20 with a capacity retention of 83%. Moreover, postmortem characterization did not evidence any morphological degradation of the components after ageing, highlighting the long-cycling feature of the LTO electrodes. The present results bring out the opportunity to build high-performance solid-state batteries using LTO as anode material.

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Lithium Dendrite in All-Solid-State Batteries: Growth Mechanisms, Suppression Strategies, and Characterizations

Cited by 438 publications

References 128 publications

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Li7La3Zr2O12 Garnet Solid Polymer Electrolyte for Highly Stable All-Solid-State Batteries

Designing Spinel Li4Ti5O12 Electrode as Anode Material for Poly(ethylene)oxide-Based Solid-State Batteries

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