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Preparation method and application of double-layer oxide solid electrolyte

A solid electrolyte and solid electrolyte technology, applied in the field of batteries, can solve the problems of high interface impedance, large battery polarization, poor cycle performance, etc., and achieve the effect of excellent working cycle stability

Inactive Publication Date: 2019-08-23
QINGDAO UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The researchers used the solid-state sintering method to construct a composite positive electrode based on the inorganic electronic conductor ITO and the inorganic ionic conductor LBO, which can realize the charge and discharge of solid-state lithium batteries at room temperature. However, the high interface impedance between the inorganic particles leads to large polarization of the battery. Poor cycle performance

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  • Preparation method and application of double-layer oxide solid electrolyte
  • Preparation method and application of double-layer oxide solid electrolyte
  • Preparation method and application of double-layer oxide solid electrolyte

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preparation example Construction

[0026] The invention provides a method for preparing a double-layer oxide solid electrolyte, the method comprising:

[0027] (1) Prepare a dense garnet-type (Garnet) LLZO ceramic electrolyte layer by vacuum hot pressing: put the lithium lanthanum zirconium oxide solid electrolyte powder into a mold, and compact it on a tablet machine at 1-5 Mpa; Pressurize 5-10 Mpa in a vacuum atmosphere in a vacuum hot-pressing furnace, hold at 1140°C for 0.5-6 hours, and heat up at a rate of 1-10°C / min; after the sintering is completed, cut and grind it into a disc to obtain a dense LLZO Ceramic electrolyte layer; the ionic conductivity of the LLZO ceramic electrolyte layer is 1.6×10-3S / cm, the thickness is 0.3-1 mm, and the relative density is greater than 99.6%.

[0028](2) Prepare porous LATP solid electrolytes by sol-gel method, such as solid electrolytes with NASICON structure or perovskite structure: mix the reactant precursors according to the stoichiometric ratio of each solid electr...

Embodiment 1

[0033] The preparation method of the double-layer oxide solid electrolyte of this embodiment includes:

[0034] (1) Preparation of Garnet-type lithium lanthanum zirconium oxide (LLZO) ceramic electrolyte layer:

[0035] The chemical formula is Li prepared by solid state reaction method 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Lithium lanthanum zirconium oxide solid electrolyte powder, its preparation steps include: according to the molar ratio of Li, La, Zr, Ta is 6.4:3:1.4:0.6, select LiOH, La 2 o 3 , ZrO 2 and Ta 2 o 5 LiOH is used as a raw material with an excess of 5% LiOH, ball milled in alcohol for 24 hours and then dried; then calcined at 900°C for 10 hours with a heating rate of 4°C / min, after the sintering is completed, the powder is crushed and sieved to obtain Li 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Powder (LLZO), which is sieved to obtain LLZO powder with a particle size of 5 μm;

[0036] The LLZO ceramic electrolyte layer was prepared by vacuum hot pressing method. The LL...

Embodiment 2

[0042] The preparation method of the double-layer oxide solid electrolyte of this embodiment includes:

[0043] (1) Preparation of Garnet-type lithium lanthanum zirconium oxide (LLZO) ceramic electrolyte layer:

[0044] The chemical formula is Li prepared by solid state reaction method 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Lithium lanthanum zirconium oxide solid electrolyte powder, its preparation steps include: according to the molar ratio of Li, La, Zr, Ta is 6.4:3:1.4:0.6, select LiOH, La 2 o 3 , ZrO 2 and Ta 2 o 5 LiOH is used as a raw material with an excess of 5% LiOH, ball milled in alcohol for 24 hours and then dried; then calcined at 900°C for 10 hours with a heating rate of 4°C / min, after the sintering is completed, the powder is crushed and sieved to obtain Li 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Powder (LLZO), which is sieved to obtain LLZO powder with a particle size of 5 μm;

[0045] The LLZO ceramic electrolyte layer was prepared by vacuum hot pressing method, the LL...

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Abstract

The invention discloses a preparation method and application of a double-layer oxide solid electrolyte. A double-layer LLZO / LATP multifunctional oxide solid electrolyte comprises a dense LLZO ceramicelectrolyte layer and a porous LATP solid electrolyte layer. The dense LLZO electrolyte layer is stable to a metal lithium negative electrode and prevents corrosion of the metal lithium negative electrode by seawater. The porous LATP solid electrolyte layer is stable to seawater and air and provides an ionic conductive framework for the air positive electrode reaction. The double-layer oxide solidelectrolyte can be used for preparing a lithium seawater battery pack. The lithium seawater battery comprises the LLZO / LATP multifunctional oxide solid electrolyte, a lithium negative electrode packaged in a dense garnet electrolyte layer and an air positive electrode material having an ion / electron conductive network. Compared with the present lithium seawater battery, the structure design of the lithium seawater battery is more suitable for complicated seawater condition and has better working stability.

Description

technical field [0001] The invention relates to the technical field of batteries, in particular to a preparation method and application of a double-layer oxide solid electrolyte. Background technique [0002] Lithium seawater batteries use metal lithium as the negative electrode and seawater as the positive electrode. It is a new energy system that obtains electrical energy by controlling the electrochemical reaction between lithium and seawater. The battery system can be directly injected into seawater or directly placed in seawater to generate electricity, and has far-reaching application prospects in the fields of deep-sea autonomous underwater vehicles and marine buoy power supplies that require high battery life. [0003] As one of the core components of lithium seawater batteries, the solid electrolyte is the key to achieving high safety and high cycle stability of the battery, while the porous electrode on the positive side needs to have high ion conductivity, wide vo...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M6/18H01M12/06
CPCH01M6/185H01M6/188H01M12/06H01M2300/0071
Inventor 郭向欣赵宁石川毕志杰黄玮麟
Owner QINGDAO UNIV
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