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NASICON (Na Super Ion Conductors) structure-based sodium ion solid electrolyte composite material and preparation method and application thereof

A solid electrolyte and composite material technology, which is applied to a sodium ion solid electrolyte composite material based on a NASICON structure and its preparation and application fields, achieves the effects of simple preparation process, good safety performance and excellent cycle performance

Active Publication Date: 2017-03-22
INST OF PHYSICS - CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

When x=2, (namely Na 3 Zr 2 Si 2 PO 12 ) has the highest ionic conductivity (Mater.Res.Bull., 1976,11:203-220), up to 10 at room temperature -4 S / cm, however, its ionic conductivity is far lower than that of liquid electrolytes, which has become a major factor limiting its application in all-solid-state batteries

Method used

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  • NASICON (Na Super Ion Conductors) structure-based sodium ion solid electrolyte composite material and preparation method and application thereof
  • NASICON (Na Super Ion Conductors) structure-based sodium ion solid electrolyte composite material and preparation method and application thereof
  • NASICON (Na Super Ion Conductors) structure-based sodium ion solid electrolyte composite material and preparation method and application thereof

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Embodiment 1

[0036] This embodiment is used to illustrate the sodium ion solid electrolyte composite material based on NASICON structure of the present invention, and its general formula is: xNa 3 La(PO 4 ) 2 / Na 3-2x Zr 2-x Si 2 P 1-2x o 12-8x , where 0

[0037] exist figure 1 The X-ray diffraction (X-ray diffraction, XRD) patterns of the sodium ion solid electrolyte composite materials with different composite ratios are given, wherein the diffraction peaks at the black solid circles correspond to Na 3 La(PO 4 ) 2 phase, other diffraction peaks correspond to NASICON phase.

[0038] The sodium ion solid electrolyte composite material can be applied to Na / S batteries, ZEBRA batteries, sodium ion all-solid-state batteries, sensors and the like.

[0039] The specific process of preparing the sodium ion solid electrolyte composite material based on the NASICON structure by using the solid-phase method described in the second aspect of the present invention and the sol-gel me...

Embodiment 2

[0041] This embodiment is used to illustrate the preparation of the sodium ion solid electrolyte composite material 0.05Na based on the NASICON structure by the solid-phase method described in the second aspect of the content of the present invention 3 La(PO 4 ) 2 / Na 2.9 Zr 1.95 Si 2 P 0.9 o 11.6 .

[0042] The required sodium stoichiometry 110wt% Na 2 CO 3 , ZrO 2 , La 2 o 3 (Heat treatment above 1000°C for 2 hours before use to remove adsorbed CO 2 ), SiO 2 , (NH 4 ) 2 HPO 4 Mix the ingredients in proportion to form a precursor; uniformly mix the precursor by ball milling to obtain a precursor powder; place the precursor powder in a muffle furnace and heat-treat it in an air atmosphere at 750°C for 12 hours; The pre-fired precursor powder was ground, pressed into tablets, and sintered at 1100° C. in an air atmosphere for 6 hours at a high temperature to obtain the ceramic sheet of the sodium ion solid electrolyte composite material.

[0043] Its powder X-ra...

Embodiment 3

[0046] In this embodiment, the sol-gel method described in the third aspect of the content of the present invention is used to prepare the sodium ion solid electrolyte composite material 0.15Na based on the NASICON structure 3 La(PO 4 ) 2 / Na 2.7 Zr 1.85 Si 2 P 0.7 o 10.8 .

[0047] Combine TEOS with H 2 O, ethanol is miscible with 1:10:20 molar ratio, adds citric acid (the molar ratio of citric acid and positive ion is 2:1), stirs and hydrolyzes 1h at 60 ℃, then adds the stoichiometric 115wt% of required sodium Sodium nitrate and stoichiometric zirconyl nitrate, lanthanum nitrate, and finally NH 4 h 2 PO 4 , heated up to 80°C and stirred to volatilize the water to obtain a gel precursor; put the gel precursor in an oven and bake at 200°C for 3 hours to obtain a xerogel; heat-treat the above xerogel at 550°C 5 hours; then sintering at 850°C for 12 hours; then grinding the pre-sintered precursor powder, and then sintering at 1200°C for 4 hours to obtain a sheet-shape...

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Abstract

The invention provides an NASICON (Na Super Ion Conductors) structure-based sodium ion solid electrolyte composite material and a preparation method and application thereof. The general formula of the sodium ion solid electrolyte composite material is (x)Na<3>La(PO<4>)<2> / Na<3-2x>Zr<2-x>Si<2>P<1-2x>O<12-8x>, wherein x is more than 0 but less than or equal to 0.5. The composite material is synthesized respectively by employing a traditional solid phase reaction method and a sol-gel method. The preparation method is simple and practical, is low in cost and can be suitably used for fabrication on a large scale. The sodium ion solid electrolyte composite material is excellent in thermal stability, is a non-pollution inorganic green material and can be used as a key part-solid electrolyte in a sodium all-solid-state battery. A secondary battery employing the sodium ion solid electrolyte material is excellent in cycle performance and good in safety performance, has a great practical value and can be used for solar power generation, wind power generation, intelligent peak regulation in a power grid, power station distribution, an emergency power supply or large-scale intelligent equipment of a communication base station.

Description

technical field [0001] The invention relates to a sodium-ion solid electrolyte composite material based on a NASICON structure, a preparation method thereof and an application thereof in an all-solid-state sodium-ion battery. Background technique [0002] Lithium-ion secondary batteries have the advantages of large specific energy density, wide operating temperature range, long charge and discharge life, small self-discharge, and no memory effect. Its mass energy density can reach 280Wh / kg, and it is considered to be the most promising chemical power supply. Since Sony commercialized it in 1990, it has not only occupied a dominant position in the field of 4C mobile consumer electronics such as notebook computers, mobile phones, video cameras, and digital cameras (Nature, 2002, 419 (6907): 553-555), but also in recent years It has shown remarkable development prospects in the fields of power batteries and energy storage batteries. [0003] However, the lithium resources on ...

Claims

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Application Information

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IPC IPC(8): H01M10/0565H01M10/0525
CPCH01M10/0525H01M10/0565Y02E60/10
Inventor 胡勇胜章志珍李泓陈立泉黄学杰
Owner INST OF PHYSICS - CHINESE ACAD OF SCI
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