Preparation method of low-resistivity garnet type modified LLZO solid electrolyte

A solid electrolyte, garnet-type technology, applied in the direction of electrolytes, circuits, electrical components, etc., can solve the problems of large interface impedance, high operating costs, high material costs, etc., to improve the conductivity of grain boundaries, reduce DC and AC resistivity , Improve the effect of mixing efficiency

Active Publication Date: 2021-09-07
WANXIANG 123 CO LTD
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Problems solved by technology

[0003] However, the above scheme also has some disadvantages. For example, the nano-LLZO prepared in the patent CN201710797774.5 has a large specific surface area and a large interface impedance; in the patent CN201910885634.2, ion sputtering coating is used to reduce the interface resistance, and the operation cost is high, which cannot meet the scale. Application requirements; patent CN202010894341.3 fills the three-dimensional pores of LLZO with flexible organic materials, but in order to achieve uniform filling of organic materials, the three-dimensional porous LLZO matrix used needs to maintain a certain porosity, the material cost is high, and lithium ions are in the interface. The molecular-level transport process is still limited, and the side reaction between water and LLZO materials cannot be avoided, which has certain technical limitations.

Method used

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  • Preparation method of low-resistivity garnet type modified LLZO solid electrolyte

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preparation example Construction

[0025] A preparation method of low-resistivity garnet-type modified LLZO solid electrolyte, comprising the following steps:

[0026] 1) Preparation of Al / Ga doped modified LLZO solid electrolyte: Li 2 CO 3 (purity 99.9%, add 5-15% excess Li 2 CO 3 to compensate for Li loss during sintering), La 2 o 3 (purity 99.9%), ZrO 2 (purity 99.9%), Ga 2 o 3 (purity 99.9%), Al 2 o 3 (purity 99.9%) as raw material, according to the required stoichiometric ratio into the three-dimensional high-energy vibration ball mill (the total doping amount of Ga and Al in LLZO is not more than 5wt%), the inner wall of the ball mill is made of zirconia, and the grinding balls are steel balls , tungsten carbide ball, polyaminopeptide ball, the ratio of ball to material is 20-50:40-80, ball milling at room temperature for 5-10 minutes, and sintering in air at 300-400°C for 1-3 hours to promote different Interfacial compatibility between raw materials, cooling to room temperature at a rate of 10...

Embodiment 1

[0029] Preparation of Al / Ga-doped modified LLZO solid electrolyte: Li 2 CO 3 (purity 99.9%, add 10% excess Li 2 CO 3 to compensate for Li loss during sintering), La2 o 3 (purity 99.9%), ZrO 2 (purity 99.9%), as a raw material, according to the required stoichiometric ratio into the three-dimensional high-energy vibration ball mill, the inner wall of the ball mill is made of zirconia, the grinding balls are tungsten carbide balls, the ball-material ratio is 25:45, ball milling at room temperature for 10 minutes, Sinter in air at 400°C for 3 hours to promote interfacial compatibility between different raw materials, cool to room temperature at a rate of 10°C / min, continue ball milling and mixing for 10 minutes, and sinter anaerobically at 1000°C for 8 hours at 400Mpa to increase crystallization Degree and density, LLZO solid electrolyte was prepared, with an average particle size of 0.5-1.0 μm.

Embodiment 2

[0031] The difference from Example 1 is: 2% Al doping is carried out, and the Al-containing raw material is Al 2 o 3 (purity 99.9%).

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Abstract

The invention relates to the field of lithium batteries, and discloses a preparation method of a low-resistivity garnet type modified LLZO solid electrolyte. The method comprises the following steps: 1) adding raw materials into a three-dimensional high-energy vibration ball mill for ball milling after batching, sintering in air at 300-400 DEG C after ball milling, cooling, continuing ball milling, and performing anaerobic sintering under 300-500 Mpa and 900-1100 DEG C to prepare an Al/Ga doped modified LLZO solid electrolyte; and 2) uniformly mixing polypropylene carbonate and acetone, adding lithium perchlorate for fully dissolving, adding the Al/Ga doped modified LLZO solid electrolyte, continuously performing ultrasonic mixing uniformly, and sintering a finished product at a low temperature of 100-250 DEG C under 300-400 Mpa. The method disclosed by the invention can be used for remarkably reducing the actual resistivity of the LLZO solid electrolyte and is beneficial to application of the LLZO solid electrolyte in a solid battery.

Description

technical field [0001] The invention relates to the field of lithium batteries, in particular to a method for preparing a low-resistivity garnet-type modified LLZO solid electrolyte. Background technique [0002] Inflammability and leakage are the main problems of liquid electrolytes in lithium-ion batteries. Replacing liquid electrolytes with solid electrolytes can solve the above safety problems. Garnet-type lanthanum lithium zirconate Li 7 La 3 Zr 2 o 12 (LLZO) is considered to be one of the most important candidates for oxide electrolytes due to its high ionic conductivity, good thermal and chemical stability at room temperature. However, the contact resistance between LLZO and the electrode is large. In order to meet the performance requirements of solid lithium batteries, the conductivity of LLZO needs to be further improved. For example, the patent application number CN201910885634.2 discloses a low barrier garnet structure solid electrolyte for lithium batteries...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M10/0562H01M10/0525
CPCH01M10/0562H01M10/0525H01M2300/0071Y02E60/10
Inventor 宫娇娇陈军黄建根郑利峰
Owner WANXIANG 123 CO LTD
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