Influence of the cold sintering process and post annealing on the microstructure and Li-ion conductivity of LiTa2PO8 solid electrolyte

Kim, Hyeonjin; Choi, Soo Jung; Peck, Dong‐Hyun; Yoon, Soon-Do

doi:10.1016/j.ceramint.2022.10.107

Cited by 8 publications

(7 citation statements)

References 19 publications

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“…50,51 As reported by previous researchers, the microstructure can affect the ionic conductivity of inorganic compounds. 52,53 The large size of the electrolyte is detrimental to the conduction of Li + . Additionally, the conductivities of electrolytes synthesized under different ball-to-powder mass ratios display a tendency to initially increase and then decrease (Figure 4d).…”

Section: Resultsmentioning

confidence: 99%

High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

Shi,

Yao,

Xiang

et al. 2024

ACS Sustainable Chem. Eng.

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The combined advantages of good mechanical deformability, high Li + conductivity, and strong compatibility with 4 V-class cathodes make halide solid-state electrolytes promising candidates for high-energy all-solid-state lithium−metal batteries (ASSLMBs). Among these, the cost-effective Li 2 ZrCl 6 has garnered significant attention due to the non-inclusion of rare-earth metals. However, the conventional one-step ball-milling synthesized Li 2 ZrCl 6 always exhibits an ionic conductivity lower than 5 × 10 −4 S cm −1 in most literature. Here, a simple optimized two-step ball-milling strategy is adopted to achieve a high Li + conductivity of nearly 1 × 10 −3 S cm −1 at 30 °C for Li 2 ZrCl 6 . Simultaneously, the effects of rotational speed and ball-to-powder mass ratio on the structure and ionic conductivity of Li 2 ZrCl 6 are investigated. The Li + migration pathways in electrolytes are also studied by bond valence site energy (BVSE) calculations. Moreover, the application potential of the modified Li 2 ZrCl 6 electrolyte in ASSLMBs assembled with the LiCoO 2 cathode and the lithium−indium alloy anode has been studied. The ASSLMBs exhibit an initial discharge capacity of 123.4 mA h g −1 at room temperature (0.1 C) and a capacity retention of 71% after 50 cycles. Therefore, this study introduces an effective strategy for synthesizing high-performance halide electrolytes, thus facilitating the practical implementation of halide-based ASSLMBs.

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Section: Resultsmentioning

confidence: 99%

High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

Shi,

Yao,

Xiang

et al. 2024

ACS Sustainable Chem. Eng.

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“…As shown in Figure 2a−f, the surface and cross-sections of the pellets exhibit a dense structure, and the particles were well connected with each other, resulting in the high density of the pellet. This implies that the Li 2 O− B 2 O 3 −Li 2 SO 4 solution evaporates and supersaturates to form an intermediate phase around and between the LTPO particles as an interface during the CSP, 16 leading to the aggregation and adhesion of particles. This high extent of adhesion between the particles and the resulting high-density microstructure possibly improves the ionic conductivity of the grain boundary.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…However, LTPO pellets prepared using CSP still exhibited a lower total ionic conductivity of 1.05 × 10 −5 S/cm compared to that of the high-temperature sintered pellet. 16 In this study, to achieve the ionic conductivity comparable to LTPO ceramic electrolytes obtained via high-temperature sintering, we attempted to introduce heterogeneous amorphous phases into the LTPO particle interface by modifying the composition of the CSP solution. Among them, it determined that the amorphous form of the Li ■ EXPERIMENTAL SECTION Preparation of the LTPO Powder.…”

Section: ■ Introductionmentioning

confidence: 99%

“…LTPO powder was prepared via a solid-state reaction, as detailed in a previous study. 16 Li 2 CO 3 (99.0%; Sigma-Aldrich), Ta 2 O 5 (99.9%, Alfa Aesar), and NH 4 H 2 PO 4 (98.0%, Sigma-Aldrich) as raw materials were mixed in an alumina mortar in a stoichiometric ratio of Li−Ta−P = 1:2:1. This mixture of reagents was heated at 600 °C for 6 h and 1050 °C for 6 h under an air atmosphere.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Moreover, the intermediate amorphous phase between the LTPO particles was found to help form Li-ion migration pathways, which significantly improved the total ionic conductivity of LTPO prepared using CSP compared to LTPO simply pressed into a pellet. However, LTPO pellets prepared using CSP still exhibited a lower total ionic conductivity of 1.05 × 10 –5 S/cm compared to that of the high-temperature sintered pellet . In this study, to achieve the ionic conductivity comparable to LTPO ceramic electrolytes obtained via high-temperature sintering, we attempted to introduce heterogeneous amorphous phases into the LTPO particle interface by modifying the composition of the CSP solution.…”

Section: Introductionmentioning

confidence: 99%

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Effect of the Li₂O–B₂O₃–Li₂SO₄ Amorphous Boundary Layer on the Ionic Conductivity and Humidity Stability of the LiTa₂PO₈ Solid Electrolyte

Kim

Choi

Nam

et al. 2023

ACS Appl. Energy Mater.

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Recently, a Li-ion solid electrolyte material LiTa 2 PO 8 (LTPO) which exhibits a high bulk ionic conductivity of 1.6 × 10 −3 S/cm and a total ionic conductivity of 2.5 × 10 −4 S/ cm was developed. In a previous study, we sintered the LTPO pellet, which has a high relative density of 82% and a total ionic conductivity of 1.05 × 10 −5 S/cm at room temperature via a cold sintering process (CSP). In this study, to achieve the ionic conductivity comparable to LTPO ceramic electrolytes obtained via high-temperature sintering, a Li 2 O−B 2 O 3 −Li 2 SO 4 amorphous layer was formed at the interface between LTPO particles via the CSP, and the microstructure and electrochemical properties of LTPO with the Li 2 O−B 2 O 3 −Li 2 SO 4 amorphous layer were investigated. Moreover, humidity acceleration tests were conducted to confirm the chemical stability of the pellet under ambient humidity conditions. It was found that pellets of LTPO prepared via the CSP exhibited a relative density of 85−87%, which is comparable to the density of high-temperature sintered pellets, and high adhesion between LTPO particles was observed due to the Li 2 O−B 2 O 3 −Li 2 SO 4 amorphous layer forming a particle interface. LTPO pellets with the Li 2 O−B 2 O 3 −Li 2 SO 4 amorphous boundary layer exhibited a high grain boundary ionic conductivity of 7.47 × 10 −5 S/cm, a total ionic conductivity of 1.07 × 10 −4 S/cm, and an extremely low activation energy of 0.215 eV. After humidity acceleration testing, the pellets showed good chemical stability against humidity, and the grain boundary and total ionic conductivities were increased by approximately 1.3 times to 9.21 × 10 −5 and 1.38 × 10 −4 S/cm, respectively. These results provide evidence that introducing an amorphous layer at the particle interface is a solution to the issues associated with low grain boundary ionic conductivity in ceramic-based solid electrolytes.

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Cold sintering of perovskite‐based mixed conducting membrane for oxygen separation

Zhou,

Fan,

Jiang

et al. 2024

AIChE Journal

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Cold sintering has attracted significant attention as its remarkably rapid densification process at low sintering temperatures leads to considerable energy savings. However, the sintering behaviors of cold‐sintered perovskite ceramics remain poorly understood and lack precise control over material microstructure. Here, we fabricated dense SrCo0.8Fe0.2O3−δ (SCF) ceramic oxygen permeation membranes by cold sintering. Adding an appropriate ratio of sub‐micron SCF particles can better bridge the sintering interspaces between micron particles, generate amorphous phase through “dissolution‐precipitation,” and aid in the initial densification. The average relative density of SCF membranes undergoes a significant increase to 95.9% after cold sintering and post‐annealing at 900°C, which is much lower than the temperature required for conventional high‐temperature solid‐state sintering (>1200°C). The oxygen permeation flux of the prepared SCF perovskite membrane reaches 2.8 mL min−1 cm−2, which proves that this method has the potential to be an excellent sintering technique for dense perovskite ceramic membranes.

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Influence of the cold sintering process and post annealing on the microstructure and Li-ion conductivity of LiTa2PO8 solid electrolyte

Cited by 8 publications

References 19 publications

High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

Effect of the Li₂O–B₂O₃–Li₂SO₄ Amorphous Boundary Layer on the Ionic Conductivity and Humidity Stability of the LiTa₂PO₈ Solid Electrolyte

Cold sintering of perovskite‐based mixed conducting membrane for oxygen separation

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Influence of the cold sintering process and post annealing on the microstructure and Li-ion conductivity of LiTa2PO8 solid electrolyte

Cited by 8 publications

References 19 publications

High-Conductivity Li2ZrCl6 Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

High-Conductivity Li2ZrCl6 Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

Effect of the Li2O–B2O3–Li2SO4 Amorphous Boundary Layer on the Ionic Conductivity and Humidity Stability of the LiTa2PO8 Solid Electrolyte

Cold sintering of perovskite‐based mixed conducting membrane for oxygen separation

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Product

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High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

High-Conductivity Li₂ZrCl₆ Electrolytes via an Optimized Two-Step Ball-Milling Method for All-Solid-State Lithium–Metal Batteries

Effect of the Li₂O–B₂O₃–Li₂SO₄ Amorphous Boundary Layer on the Ionic Conductivity and Humidity Stability of the LiTa₂PO₈ Solid Electrolyte