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Lithium-containing zirconium phosphate, calcined powder of same, and method for producing sintered body

A manufacturing method, lithium phosphoric acid technology, applied in chemical instruments and methods, phosphorus compounds, solid electrolytes, etc., can solve the problems of no clear regulations, no phosphoric acid concentration immobilization, etc., and achieve high temperature heat resistance and excellent mechanical strength.

Inactive Publication Date: 2019-02-05
DAIICHI KIGENSO KAGAKU KOGYO CO LTD +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0008] In Patent Document 2, the concentration (composition) of phosphoric acid is not particularly fixed, and there is no description of clearly defining a certain composition range, or focusing on the concentration of phosphoric acid.

Method used

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  • Lithium-containing zirconium phosphate, calcined powder of same, and method for producing sintered body
  • Lithium-containing zirconium phosphate, calcined powder of same, and method for producing sintered body
  • Lithium-containing zirconium phosphate, calcined powder of same, and method for producing sintered body

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1-1~1-15

[0078] Preparation of Li as starting material 2 CO 3 , ZrO 2 , CaCO 3 and NH 4 h 2 PO 4 , only change the amount of P and weigh the specified amount respectively, so that the composition shown in Table 1 can be reached after sintering.

[0079] Then, these weighed objects were put into a zirconia pot mill and mixed for 16 hours to obtain a mixed powder, which was calcined at 800° C. in an air atmosphere, and pulverized to obtain a calcined powder.

[0080] The calcined powder was molded at a pressure of 100 MPa, and then sintered at a temperature of 800 to 1500° C. shown in Table 1 to obtain a lithium-containing zirconium phosphate sintered body (sample).

[0081] All the lithium-containing zirconium phosphates shown in Table 1 were subjected to powder X-ray diffraction measurement, and as a result, the main constituent phases were all NASICON-type structures. figure 1 The powder X-ray diffraction pattern at room temperature of the lithium-containing zirconium phosphate...

Embodiment 2-1~2-8

[0083] Preparation of Li as starting material 2 CO 3 , ZrO 2 , CaCO 3 and NH 4 h 2 PO 4 , only changing the amount of Li and weighing the specified amount respectively, so that the composition shown in Table 2 can be reached after sintering.

[0084] Then, sample preparation and sample evaluation (powder X-ray diffraction measurement) were carried out in the same manner as in Example 1.

[0085] All the lithium-containing zirconium phosphates shown in Table 2 were subjected to powder X-ray diffraction measurement, and as a result, the main constituent phases were all NASICON-type structures.

Embodiment 3-1~3-6

[0087] Preparation of Li as starting material 2 CO 3 , ZrO 2 , CaCO 3 and NH 4 h 2 PO 4 , changing only M 1 The amounts of (Ca) were weighed in predetermined amounts so that the compositions shown in Table 3 were obtained after sintering.

[0088] Then, sample preparation and sample evaluation (powder X-ray diffraction measurement) were carried out in the same manner as in Example 1.

[0089] All the lithium-containing zirconium phosphates shown in Table 3 were subjected to powder X-ray diffraction measurement, and as a result, the main constituent phases were all NASICON-type structures.

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Abstract

The present invention provides: a lithium-containing zirconium phosphate having excellent high-temperature heat resistance and excellent mechanical strength, which is useful as an inorganic solid electrolyte material having lithium ion conductivity; a calcined powder of this lithium-containing zirconium phosphate; and a method for producing a sintered body. The present invention specifically provides a lithium-containing zirconium phosphate which is characterized in that (1) the composition ratio thereof satisfies Li:M1:M2:P = (1.0 to 1.7):(0.10 to 0.35):(2.0):(more than 3.00 but 3.50 or less); (2) M1 represents at least one element selected from the group consisting of Ca, Mg, Sr and Ba, and in cases where M1 represents two or more elements, the total composition ratio thereof is 0.10 to0.35, and (3) M2 represents Zr alone, or Zr and at least one element selected from the group consisting of Al, Sc, Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb and Lu, with the composition ratioof Zr in the composition ratio of M2 being 1.47 to 2.00.

Description

technical field [0001] The present invention relates to a lithium-containing zirconium phosphate useful as a lithium-ion conductive solid electrolyte material for an all-solid-state battery, and a method for producing its calcined powder and sintered body. Background technique [0002] At present, lithium-ion batteries used in portable electronic devices such as mobile phones and notebook computers are superior to other batteries in terms of energy density. applications in electric and hybrid vehicles. In addition, lithium-ion secondary batteries currently on the market mainly use organic electrolytes as electrolytes, but there are concerns about leakage or corrosion, and there are also problems such as flammability. [0003] As one of lithium ion conductive materials replacing it, there is an inorganic solid electrolyte using zirconium phosphate. Inorganic solid electrolytes are chemically and electrochemically safer materials than organic electrolyte solutions, and are c...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C01B25/45H01B1/06H01M10/0562
CPCC01B25/45H01B1/06H01M10/0562Y02E60/10C01P2002/72C01P2006/40H01M10/0525H01M2300/0068
Inventor 中岛靖中山享
Owner DAIICHI KIGENSO KAGAKU KOGYO CO LTD