Rhombohedral Li1+xYxZr2-x(PO4)3 Solid Electrolyte Prepared by Hot-Pressing for All-Solid-State Li-Metal Batteries

NASICON-type solid electrolytes with excellent stability in moisture are promising in all-solid-state batteries and redox flow batteries. However, NASIOCN LiZr2(PO4)3 (LZP), which is more stable with lithium metal than the commercial Li1.3Al0.3Ti1.7(PO4)3, exhibits a low Li-ion conductivity of 10−6 S cm−1 because the fast conducting rhombohedral phase only exists above 50 °C. In this paper, the high-ionic conductive rhombohedral phase is stabilized by Y3+ doping at room temperature, and the hot-pressing technique is employed to further improve the density of the pellet. The dense Li1.1Y0.1Zr1.9(PO4)3 pellet prepared by hot-pressing shows a high Li-ion conductivity of 9 × 10−5 S cm−1, which is two orders of magnitude higher than that of LiZr2(PO4)3. The in-situ formed Li3P layer on the surface of Li1.1Y0.1Zr1.9(PO4)3 after contact with the lithium metal increases the wettability of the pellet by the metallic lithium anode. Moreover, the Li1.1Y0.1Zr1.9(PO4)3 pellet shows a relatively small interfacial resistance in symmetric Li/Li and all-solid-state Li-metal cells, providing these cells a small overpotential and a long cycling life.

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Li2(BH4)(NH2) Nanoconfined in SBA-15 as Solid-State Electrolyte for Lithium Batteries

Nanomaterials ◽

10.3390/nano11040946 ◽

2021 ◽

Vol 11 (4) ◽

pp. 946

Author(s):

Qianyi Yang ◽

Fuqiang Lu ◽

Yulin Liu ◽

Yijie Zhang ◽

Xiujuan Wang ◽

...

Keyword(s):

Solid State ◽

High Performance ◽

Coulombic Efficiency ◽

Specific Capacity ◽

Transference Number ◽

Electrochemical Stability ◽

Ion Conductivity ◽

Solid State Batteries ◽

Li Ion ◽

Conduction Properties

Solid electrolytes with high Li-ion conductivity and electrochemical stability are very important for developing high-performance all-solid-state batteries. In this work, Li2(BH4)(NH2) is nanoconfined in the mesoporous silica molecule sieve (SBA-15) using a melting–infiltration approach. This electrolyte exhibits excellent Li-ion conduction properties, achieving a Li-ion conductivity of 5.0 × 10−3 S cm−1 at 55 °C, an electrochemical stability window of 0 to 3.2 V and a Li-ion transference number of 0.97. In addition, this electrolyte can enable the stable cycling of Li|Li2(BH4)(NH2)@SBA-15|TiS2 cells, which exhibit a reversible specific capacity of 150 mAh g−1 with a Coulombic efficiency of 96% after 55 cycles.

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Highly Conjugated Three-Dimensional Covalent Organic Frame- works with Enhanced Li-ion Conductivity as Solid-State Electrolytes for High-Performance Lithium Metal Batteries

Journal of Materials Chemistry A ◽

10.1039/d1ta08771a ◽

2022 ◽

Author(s):

Shi Wang ◽

Xiang-Chun Li ◽

Tao Cheng ◽

Yuan-Yuan Liu ◽

Qiange Li ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

High Performance ◽

Three Dimensional ◽

Ion Conductivity ◽

Covalent Organic Frameworks ◽

Lithium Metal ◽

Lithium Metal Batteries ◽

Li Ion ◽

Solid State Electrolytes

Covalent organic frameworks (COFs) with well-tailored channels have the potential to efficiently transport ions yet remain to be explored. The ion transport capability is generally limited due to the lack...

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A solid-state dendrite-free lithium-metal battery with improved electrode interphase and ion conductivity enhanced by a bifunctional solid plasticizer

Journal of Materials Chemistry A ◽

10.1039/c9ta07165b ◽

2019 ◽

Vol 7 (33) ◽

pp. 19565-19572 ◽

Cited By ~ 6

Author(s):

Jun Peng ◽

Li-Na Wu ◽

Jin-Xia Lin ◽

Chen-Guang Shi ◽

Jing-Jing Fan ◽

...

Keyword(s):

Solid State ◽

Polymer Electrolyte ◽

Ion Conductivity ◽

Lithium Metal ◽

Ion Diffusion ◽

Interface Stability ◽

Li Ion ◽

Lithium Metal Battery ◽

Composite Solid

By adding a bifunctional plasticizer (SN) and an inorganic conductor (LAGP) to a PEO matrix, an inorganic–organic composite solid-state polymer electrolyte (SPE) was constructed to enhance Li-ion diffusion and interface stability.

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Mastering the interface for advanced all-solid-state lithium rechargeable batteries

Proceedings of the National Academy of Sciences ◽

10.1073/pnas.1615912113 ◽

2016 ◽

Vol 113 (47) ◽

pp. 13313-13317 ◽

Cited By ~ 138

Author(s):

Yutao Li ◽

Weidong Zhou ◽

Xi Chen ◽

Xujie Lü ◽

Zhiming Cui ◽

...

Keyword(s):

Solid State ◽

Solid Electrolyte ◽

Solid Electrolyte Interphase ◽

Rechargeable Batteries ◽

Ion Conductivity ◽

Rhombohedral Structure ◽

Interfacial Resistance ◽

Lithium Anode ◽

Metal Anode ◽

Li Ion

A solid electrolyte with a high Li-ion conductivity and a small interfacial resistance against a Li metal anode is a key component in all-solid-state Li metal batteries, but there is no ceramic oxide electrolyte available for this application except the thin-film Li-P oxynitride electrolyte; ceramic electrolytes are either easily reduced by Li metal or penetrated by Li dendrites in a short time. Here, we introduce a solid electrolyte LiZr2(PO4)3 with rhombohedral structure at room temperature that has a bulk Li-ion conductivity σLi = 2 × 10−4 S⋅cm−1 at 25 °C, a high electrochemical stability up to 5.5 V versus Li+/Li, and a small interfacial resistance for Li+ transfer. It reacts with a metallic lithium anode to form a Li+-conducting passivation layer (solid-electrolyte interphase) containing Li3P and Li8ZrO6 that is wet by the lithium anode and also wets the LiZr2(PO4)3 electrolyte. An all-solid-state Li/LiFePO4 cell with a polymer catholyte shows good cyclability and a long cycle life.

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(Invited) In Operando and in Situ techniques for Intercalation Compounds in Li-Ion and All-Solid-State Batteries

ECS Meeting Abstracts ◽

10.1149/ma2020-02116mtgabs ◽

2020 ◽

Vol MA2020-02 (1) ◽

pp. 16-16

Author(s):

Karim Zaghib ◽

Wen Zhu ◽

Shirin Kaboli ◽

Hendrix Demers ◽

Michel Trudeau ◽

...

Keyword(s):

Solid State ◽

Intercalation Compounds ◽

In Situ Techniques ◽

Solid State Batteries ◽

Li Ion ◽

All Solid State Batteries ◽

In Operando

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In Situ characterization of Reactive Lithium Metal Interfaces in Solid-State Batteries

ECS Meeting Abstracts ◽

10.1149/ma2020-025974mtgabs ◽

2020 ◽

Vol MA2020-02 (5) ◽

pp. 974-974

Author(s):

John A Lewis ◽

Francisco Javier Quintero Cortes ◽

Eugene Liu ◽

Jared Tippens ◽

Matthew T McDowell

Keyword(s):

Solid State ◽

Lithium Metal ◽

In Situ Characterization ◽

Solid State Batteries ◽

Metal Interfaces

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Blocking Lithium Dendrite Growth in Solid-State Batteries with an Ultrathin Amorphous Li-La-Zr-O Solid Electrolyte

10.21203/rs.3.rs-219404/v1 ◽

2021 ◽

Author(s):

Jordi Sastre ◽

Moritz Futscher ◽

Lea Pompizi ◽

Abdessalem Aribia ◽

Agnieszka Priebe ◽

...

Keyword(s):

Solid State ◽

Electronic Conductivity ◽

High Capacity ◽

External Pressure ◽

Lithium Metal ◽

Metallic Lithium ◽

Lithium Dendrites ◽

Lithium Garnet ◽

Solid State Batteries ◽

Lithium Dendrite

Abstract Lithium metal dendrites have become a roadblock in the realization of next-generation solid-state batteries with lithium metal as high-capacity anode. The presence of surface and bulk inhomogeneities with non-negligible electronic conductivity in crystalline electrolytes such as the lithium garnet Li7La3Zr2O12 (LLZO) facilitates the growth of lithium filaments, posing a critical safety risk. Here we explore the amorphous phase of LLZO (aLLZO) as a lithium dendrite shield owing to its grain-boundary-free microstructure, stability against metallic lithium, and high electronic insulation. We demonstrate that by tuning the lithium stoichiometry in sputtered aLLZO films, the ionic conductivity can be increased up to 10-7 S cm-1 while retaining an ultralow electronic conductivity of 10-14 S cm-1. In Li/aLLZO/Li symmetric cells, plating-stripping results in no degradation of the films and current densities up to 3.2 mA cm-2 can be applied with no signs of lithium penetration. The defect-free and conformal nature of the films enables microbatteries with an electrolyte thickness as low as 70 nm, which withstand charge-discharge at 0.2 mA cm-2 for over 500 cycles. Finally, we demonstrate that the application of aLLZO as a coating on crystalline LLZO lowers the interface resistance and significantly impedes the formation of lithium dendrites, increasing the critical current density of a symmetric cell up to 1.3 mA cm-2 at room temperature and without external pressure. The effectiveness of the amorphous Li-La-Zr-O as lithium dendrite blocking layer can accelerate the development of more powerful and safer solid-state batteries.

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In-situ electron holography charactering Li ions accumulation in the interface between electrode and solid-state-electrolyte

Journal of Materials Chemistry A ◽

10.1039/d1ta03517g ◽

2021 ◽

Author(s):

Yang Yang ◽

Jie Cui ◽

Hui-Juan Guo ◽

Xi Shen ◽

Yuan Yao ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

Charge Distribution ◽

Transport Mechanism ◽

Electron Holography ◽

Solid State Electrolyte ◽

Solid State Batteries ◽

Li Ion ◽

Solid State Electrolytes

Intensive understanding of the Li-ion transport mechanism in solid-state-electrolytes (SSEs) is crucial for the buildup of industrially scalable solid-state batteries. Here, we report the charge distribution near the electrode/SSEs interface...

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NASICON LiM2(PO4)3 electrolyte (M = Zr) and electrode (M = Ti) materials for all solid-state Li-ion batteries with high total conductivity and low interfacial resistance

Journal of Materials Chemistry A ◽

10.1039/c7ta08715b ◽

2018 ◽

Vol 6 (13) ◽

pp. 5296-5303 ◽

Cited By ~ 28

Author(s):

Hany El-Shinawi ◽

Anna Regoutz ◽

David J. Payne ◽

Edmund J. Cussen ◽

Serena A. Corr

Keyword(s):

Solid State ◽

Ionic Conductivities ◽

Total Conductivity ◽

Li Ion Batteries ◽

Interfacial Resistance ◽

Nasicon Type ◽

Solid State Batteries ◽

Li Ion ◽

All Solid State Batteries

All solid-state batteries based on NASICON-type LiM2(PO4)3 electrolyte phases are highly promising owing to their high ionic conductivities and chemical stabilities.

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