Optimization of Al2O3 and Li3BO3 Content as Sintering Additives of Li7−x
                     La2.95Ca0.05ZrTaO12 at Low Temperature

Rosero-Navarro, Nataly Carolina; Miura, Akira; Higuchi, Mikio; Tadanaga, Kiyoharu

doi:10.1007/s11664-016-4924-4

Cited by 33 publications

(12 citation statements)

References 21 publications

(39 reference statements)

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“…One of the most popular glass used as an additive material seems to be Li3BO3, denoted later as LBO, due to its low glass transition and melting temperatures. N. C. Rosero-Navarro et al [31,32] studied the composites based on garnet-type material and formed in the system Li7La3ZrxM1-xO12 -Li3BO3 (M = Nb, Ta). They reported that the value of ionic conductivity of ceramic Li7La3Zr2O12 (LLZO) sintered at 900°C is relatively low, ca.…”

Section: Introductionmentioning

confidence: 99%

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Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Kwatek

Ślubowska

Trébosc

et al. 2020

Journal of Alloys and Compounds

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The existing solid electrolytes for lithium ion batteries suffer from low total ionic conductivity, which restricts its usefulness for the lithium-ion battery technology. Among them, the NASICON-based materials, such as Li1.3Al0.3Ti1.7(PO4)3 (LATP) exhibit low total ionic conductivity due to highly resistant grain boundary phase. One of the possible approaches to efficiently enhance their total ionic conductivity is the formation of a composite material. Herein, the Li2.9B0.9S0.1O3.1 glass, called LBSO hereafter, was chosen as an additive material to improve the ionic properties of the ceramic Li1.3Al0.3Ti1.7(PO4)3 base material. The properties of this Li1.3Al0.3Ti1.7(PO4)3-xLi2.9B0.9S0.1O3.1 (0  x  0.3) system have been studied by means of high temperature X-ray diffractometry (HTXRD), 7 Li, 11 B, 27 Al and 31 P magic angle spinning nuclear magnetic resonance spectroscopy (MAS NMR), thermogravimetry (TG), scanning electron microscopy (SEM), impedance spectroscopy (IS) and density methods. We show here that the introduction of the foreign LBSO phase enhances their electric properties. This study reveals several interesting correlations between the apparent density, the microstructure, the composition, the sintering temperature and the ionic conductivity. Moreover, the electrical properties of the composites will be discussed in the terms of the bricklayer model (BLM). The highest value of σtot = 1.5 × 10 −4 S•cm −1 has been obtained for LATP-0.1LBSO material sintered at 800°C.

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Section: Introductionmentioning

confidence: 99%

“…Therefore, to obtain highly conductive material, another approach has been proposed. It is based on the addition of some foreign phase into the base matrix in order to lower the grain boundary resistance [24][25][26][27][28][29][30][31][32][33].…”

Section: Introductionmentioning

confidence: 99%

Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Kwatek

Ślubowska

Trébosc

et al. 2020

Journal of Alloys and Compounds

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“…Garnet-type Li +ion-conducting Li 7 La 3 Zr 2 O 12 -based ceramics have been prepared by sintering at about 700-900°C with several additives such as Li 3 BO 3 23-25 and lithium borosilicate based glasses. 26,27 These liquid-phase sintered ceramics show high conductivities approaching those of high-temperature-sintered ceramics (generally 1100-1200°C). Moreover, these sintering techniques do not require expensive apparatus like hot-pressing or spark plasma sintering.…”

Section: Introductionmentioning

confidence: 99%

Liquid‐phase sintering of highly Na⁺ ion conducting Na₃Zr₂Si₂PO₁₂ ceramics using Na₃BO₃ additive

et al. 2017

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Na3Zr2Si2PO12 (NASICON) is a promising material as a solid electrolyte for all‐solid‐state sodium batteries. Nevertheless, one challenge for the application of NASICON in batteries is their high sintering temperature above 1200°C, which can lead to volatilization of light elements and undesirable side reactions with electrode materials at such high temperatures. In this study, liquid‐phase sintering of NASICON with a Na3BO3 (NBO) additive was performed for the first time to lower the NASICON sintering temperature. A dense NASICON‐based ceramic was successfully obtained by sintering at 900°C with 4.8 wt% NBO. This liquid‐phase sintered NASICON ceramic exhibited high total conductivity of ~1 × 10−3 S cm−1 at room temperature and low conduction activation energy of 28 kJ mol−1. Since the room‐temperature conductivity is identical to that of conventional high‐temperature‐sintered NASICON, NBO was demonstrated as a good liquid‐phase sintering additive for NASICON solid electrolyte. In the NASICON with 4.8 wt% NBO ceramic, most of the NASICON grains directly bonded with each other and some submicron sodium borates segregated in particulate form without full penetration to NASICON grain boundaries. This characteristic composite microstructure contributed to the high conductivity of the liquid‐phase sintered NASICON.

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“…The activation energy is 0.31 eV (estimated from log(σT) vs 1/T), which is a typical value for the cubic garnet LLZ solid electrolyte doped with calcium and tantalum. 23,36 The ionic conductivity and activation energy of the LS/LLCZT/LS pellet suggest that lithium silicate does not significantly affect the electrical properties of the LLCZT pellet.…”

Section: Resultsmentioning

confidence: 97%

“…The LLCZT solid electrolyte was synthesized by the liquid-phase process, following a similar protocol described in a previous report. 23 LiNO 3 (99%, Kanto Chemical Co.), La(NO 3 ) 3 •6H 2 O (99.9%, Kanto Chemical Co.), Ca(NO 3 ) 2 (99%, Wako), Zr(OC 4 H 9 ) 4 (85% in butanol, Wako), Ta(OC 2 H 5 ) 5 (99.9%, High Purity Chemicals), and Al(OCHCH 3 C 2 H 5 ) 3 (95.0%, Kanto Chemical Co.) were used as precursors. The ethyl acetoacetate (EAC, 99.0%, Kanto Chemical Co.) was used as a stabilizing agent for the alkoxides.…”

Section: Methodsmentioning

confidence: 99%

Significant Reduction in the Interfacial Resistance of Garnet-Type Solid Electrolyte and Lithium Metal by a Thick Amorphous Lithium Silicate Layer

Rosero-Navarro

Kajiura

Jalem

et al. 2020

ACS Appl. Energy Mater.

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The poor ionic and electronic contacts between electrodes and the electrolyte is a critical problem in the fabrication of all-solid-state lithium batteries based on garnet-type oxide solid electrolytes. The interfacial resistance with lithium metal anode has been widely studied because the use of lithium metal anodes can provide energy storage systems with the largest specific energy. Here, an amorphous lithium silicate interlayer is proposed to obtain a low interfacial resistance of the garnet solid electrolyte with lithium metal. The lithium silicate layer is deposited on the garnet solid electrolyte by a liquid-phase process followed by heat treatment, and metallic lithium is put on the modified surface by just pressing, without heat treatment. This approach achieves a low interfacial resistance of 44 Ω cm 2 and a stable dissolution/deposition cycling behavior at a current density of up to 0.5 mA cm −2 . A quasi-solid-state battery constructed with the garnet solid electrolyte modified with the lithium silicate layer, lithium metal, and LiNi 1/3 Co 1/3 Mn 1/3 O 2 electrode shows a stable cycling performance at 25 °C (124 mAh g −1 after 100 cycles). Thermodynamic calculations suggest that the effective contact between lithium metal and lithium silicate is created by the formation of Li−Si phases at the interface.

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Optimization of Al2O3 and Li3BO3 Content as Sintering Additives of Li7−x La2.95Ca0.05ZrTaO12 at Low Temperature

Cited by 33 publications

References 21 publications

Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Liquid‐phase sintering of highly Na⁺ ion conducting Na₃Zr₂Si₂PO₁₂ ceramics using Na₃BO₃ additive

Significant Reduction in the Interfacial Resistance of Garnet-Type Solid Electrolyte and Lithium Metal by a Thick Amorphous Lithium Silicate Layer

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Optimization of Al2O3 and Li3BO3 Content as Sintering Additives of Li7−x La2.95Ca0.05ZrTaO12 at Low Temperature

Cited by 33 publications

References 21 publications

Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Impact of Li2.9B0.9S0.1O3.1 glass additive on the structure and electrical properties of the LATP-based ceramics

Liquid‐phase sintering of highly Na+ ion conducting Na3Zr2Si2PO12 ceramics using Na3BO3 additive

Significant Reduction in the Interfacial Resistance of Garnet-Type Solid Electrolyte and Lithium Metal by a Thick Amorphous Lithium Silicate Layer

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Liquid‐phase sintering of highly Na⁺ ion conducting Na₃Zr₂Si₂PO₁₂ ceramics using Na₃BO₃ additive