Conformal, Nanoscale ZnO Surface Modification of Garnet-Based Solid-State Electrolyte for Lithium Metal Anodes

Wang, Chengwei; Gong, Yunhui; Liu, Boyang; Fu, Kun; Yao, Yonggang; Hitz, Emily; Li, Yiju; Dai, Jiaqi; Xu, Shaomao; Luo, Wei; Wachsman, Eric D.; Hu, Liangbing

doi:10.1021/acs.nanolett.6b04695

Cited by 603 publications

(456 citation statements)

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“…Their elastic properties are listed in Table III. The different properties of the contact, such as elastic contact, adhesion or elastoplastic contact can be addressed by changing the initial and boundary conditions of Equation 22. Since both Li 3 PO 4 and LiCoO 2 are ceramic materials, the contact is considered to be elastic without adhesion in this study.…”

Section: After LImentioning

confidence: 99%

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Simulation of the Effect of Contact Area Loss in All-Solid-State Li-Ion Batteries

Tian

2017

J. Electrochem. Soc.

126

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Maintaining the physical contact between the solid electrolyte and the electrode is important to improve the performance of all-solidstate batteries. Imperfect contact can be formed during cell fabrication and will be worsened due to cycling, resulting in degradation of the battery performance. In this paper, the effect of imperfect contact area was incorporated into a 1-D Newman battery model by assuming the current and Li concentration will be localized at the contacted area. Constant current discharging processes at different rates and contact areas were simulated for a film-type Li|LiPON|LiCoO 2 all-solid-state Li-ion battery. The capacity drop was correlated with the contact area loss. It was found at lower cutoff voltage, the correlation is almost linear with a slope of 1; while at a higher cutoff voltage, the dropping rate is slower. To establish the relationship between the applied pressure and the contact area, Persson's contact mechanics theory was applied, as it uses self-affined surfaces to simplify the multi-length scale contacts in all-solid-state batteries. The contact area and pressure were computed for both film-type and bulk-type all-solid-state Li-ion batteries. The model is then used to suggest how much pressures should be applied to recover the capacity drop due to contact area loss. Conventional Li-ion batteries usually include a liquid electrolyte, which facilitates Li-ions transport between cathode and anode. However, the applications of Li-ion batteries are still limited by the flammability and narrow electrochemical window of the liquid electrolytes. 1-3During the past decades, several solid electrolytes 4-9 with the ionic conductivity close to the liquid electrolyte have been developed, thus enabled the development of all-solid-state batteries. The benefits of all-solid-state batteries are high energy density, non-flammability, and the large electrochemical window (if the solid electrolyte form stable interphase layers on electrode surface). 10,11However, a major bottleneck for all-solid-state Li-ion batteries lies at the high interfacial resistance due to two main factors, chemical effect and physical contact. 3 The chemical effect refers to the chemical changes at the solid-electrolyte/electrode interface that cause slower transport. The chemical changes include the interphase layer formation due to solid electrolyte decomposition, 11 and/or Li-ion depletion zone at the interface 12 (for example, LiPON/Li 2 CO 3 ). Physical contact induced impedance comes from the imperfect contact at the solid-electrolyte/electrode interface, which plays a more important role for batteries using solid-electrolytes than the conventional batteries employing liquid electrolytes. Liquid electrolytes can easily diffuse through the porous electrode and wet the electrode surface, so, any fracture and disconnection between solid particles will only cause electrical disconnection. However, for solid electrolytes, the fracture and disconnection will impede Li-ion transport, as well as electron transport. Thus...

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Section: After LImentioning

confidence: 99%

“…For elastic contact, P(σ, ξ) would be 0 when σ → ∞, when σ < 0 the P(σ, ξ) should be 0 as well since there is no adhesion. With the initial and boundary conditions, the stress distribution of Equation 22 can be solved, and the real contact area in Equation 21 can be further obtained by…”

Section: After LImentioning

confidence: 99%

Simulation of the Effect of Contact Area Loss in All-Solid-State Li-Ion Batteries

Tian

2017

J. Electrochem. Soc.

126

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“…Many approaches have been introduced to reduce the interfacial charge-transfer resistance between garnet-type SE and Li, including the introduction of thin film layers of Au [35], Si [36], Ge [37], Al 2 O 3 [38], and ZnO [39], or eliminating the secondary phases, such as LiOH and Li 2 CO 3 , by polishing the surface of SE and using multiple thermal treatments at specific temperatures before and after contact with Li [40][41][42]. However, a more simplified method to form the interface between garnet-type SE and the Li electrode would be preferable and further study is required of the relationship between the interfacial charge-transfer resistance and stability for Li deposition and dissolution reaction at the interface.…”

Section: Introductionmentioning

confidence: 99%

Formation and Stability of Interface between Garnet-Type Ta-doped Li7La3Zr2O12 Solid Electrolyte and Lithium Metal Electrode

et al. 2018

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Garnet-type Li 7-x La 3 Zr 2-x Ta x O 12 (LLZT) is considered a good candidate for the solid electrolyte in all-solid-state lithium batteries because of its reasonably high conductivity around 10 −3 S cm −1 at room temperature and stability against lithium (Li) metal with the lowest redox potential. In this study, we synthesized LLZT with a tantalum (Ta) content of 0.45 via a conventional solid-state reaction process and constructed a Li/LLZT/Li symmetric cell by attaching Li metal foils on the polished top and bottom surfaces of an LLZT pellet. We investigated the influence of heating temperatures and times on the interfacial charge-transfer resistance between LLZT and the Li metal electrode. In addition, the effect of the interface resistance on the stability for Li deposition and dissolution was examined using a galvanostatic cycling test. The lowest interfacial resistance of 25 Ω cm 2 at room temperature was obtained by heating at 175 • C (5 • C lower than the melting point of Li) for three to five hours. We confirmed that the current density at which the short circuit occurs in the Li/LLZT/Li cell via the propagation of Li dendrite into LLZT increases with decreasing interfacial charge transfer resistance.

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“…[3,4] However, the successful implementation of Li metal has been impeded due to the poor control of electrodeposition during the Li plating/stripping cycling, a consequence of which is the formation of mossy or dendritic lithium that can penetrate the separator, cause an internal short-circuit, and eventually lead to battery thermal runaway. [20][21][22][23][24] However, the performances at high current densities with high areal capacities over long cycling have not been fully explored. Moreover, unlike graphite anode that only have ≈10% volume change during lithiation/delithiation intercalation processes, Li metal is a "hostless" electrode with a virtually infinite volume change, resulting in significant internal stress accumulation, SEI collapse and high interfacial impedance upon prolonged cycling.…”

mentioning

confidence: 99%

High‐Rate and Large‐Capacity Lithium Metal Anode Enabled by Volume Conformal and Self‐Healable Composite Polymer Electrolyte

et al. 2019

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The widespread implementation of lithium‐metal batteries (LMBs) with Li metal anodes of high energy density has long been prevented due to the safety concern of dendrite‐related failure. Here a solid–liquid hybrid electrolyte consisting of composite polymer electrolyte (CPE) soaked with liquid electrolyte is reported. The CPE membrane composes of self‐healing polymer and Li + ‐conducting nanoparticles. The electrodeposited lithium metal in a uniform, smooth, and dense behavior is achieved using a hybrid electrolyte, rather than dendritic and pulverized structure for a conventional separator. The Li foil symmetric cells can deliver remarkable cycling performance at ultrahigh current density up to 20 mA cm −2 with an extremely low voltage hysteresis over 1500 cycles. A large areal capacity of 10 mAh cm −2 at 10 mA cm −2 could also be obtained. Furthermore, the Li|Li 4 Ti 5 O 12 cells based on the hybrid electrolyte achieve a higher specific capacity and longer cycling life than those using conventional separators. The superior performances are mainly attributed to strong adhesion, volume conformity, and self‐healing functionality of CPE, providing a novel approach and a significant step toward cost‐effective and large‐scalable LMBs.

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Conformal, Nanoscale ZnO Surface Modification of Garnet-Based Solid-State Electrolyte for Lithium Metal Anodes

Cited by 603 publications

References 47 publications

Simulation of the Effect of Contact Area Loss in All-Solid-State Li-Ion Batteries

Simulation of the Effect of Contact Area Loss in All-Solid-State Li-Ion Batteries

Formation and Stability of Interface between Garnet-Type Ta-doped Li7La3Zr2O12 Solid Electrolyte and Lithium Metal Electrode

High‐Rate and Large‐Capacity Lithium Metal Anode Enabled by Volume Conformal and Self‐Healable Composite Polymer Electrolyte

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