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Mixed ion-electron conductor with garnet structure and application thereof in energy storage device

A technology of mixed ions and electronic conductors, which is applied in the direction of hybrid capacitor electrolytes, electrical components, electrochemical generators, etc., can solve the problems of low interface surface resistance, electronic conductance is not too high, etc., to improve power density, eliminate interface resistance, high lithium The effect of ionic conductivity

Inactive Publication Date: 2020-06-23
BEIJING UNIV OF CHEM TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] So far, there is no interface modification material that can meet all the following requirements to suppress the interfacial dendrites between Li metal and garnet: (1) While having intrinsically high ionic conductivity, it maintains a low contact with Li metal. (2) has a uniform electronic conductance, which makes the interface electric field evenly distributed, promotes the uniform deposition and detachment of lithium, and reduces the possibility of nucleation of lithium atoms; (3) the electronic conductance of the interface is not too high (excluding metal ), preventing electron injection into the garnet electrolyte

Method used

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  • Mixed ion-electron conductor with garnet structure and application thereof in energy storage device
  • Mixed ion-electron conductor with garnet structure and application thereof in energy storage device
  • Mixed ion-electron conductor with garnet structure and application thereof in energy storage device

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Embodiment 1

[0056] The mixed ion-electron conductor material of garnet structure refers to the material with figure 1 The stoichiometric ratio of the structure and the doped garnet structure of the non-stoichiometric ratio, and the crystal structure is synthesized by heat treatment (including heating, quenching, annealing), mechanical ball milling, and liquid phase method, and the derived crystalline phase and amorphous phase and a crystalline-amorphous mixed phase. The material system includes a composite phase containing garnet-type mixed conductor materials, including organic and inorganic lithium ion conductors, and electronic conductors / semiconductors. The mixed conductor of the present invention has high ion-electronic conductivity, high stability with electrode and electrolyte materials and small interfacial resistance. The diffusion coefficient of lithium ions determines the ion conductivity, the ion channel and the Arrhenius curve of ion conductivity with temperature as shown in...

Embodiment 2

[0057] Embodiment 2 (Li 6.75 La 3 Zr 1.6875 Ti 0.0625 Ta 0.25 o 12 )

[0058] Anhydrous LiNO 3 ,La(NO 3 ) 3 ·6H 2 O,ZrC 16 h 36 o 4 , TaC 10 h 25 o 5 and TiC 12 h 28 o 4 as raw material, according to Li 6.75 La 3 Zr 1.6875 Ti 0.0625 Ta 0.25 o 12 The stoichiometric ratio of the drug was weighed. TaC 10 h 25 o 5 ,, ZrC 16 h 36 o 4 , TiC 12 h 28 o 4 Disperse in absolute ethanol to obtain solution 1, then La(NO 3 ) 3 ·6H 2 O, LiNO 3 (10wt% excess) was dissolved in deionized water to obtain solution 2; solution 2 was added dropwise into solution 1 to fully hydrolyze the tantalum salt, zirconium salt and titanium salt, and mix evenly with a magnetic stirrer. The obtained gel solution was evaporated to dryness at 150° C., and the obtained dry gel was transferred to an alumina crucible, and treated at 500° C. for 1 hour to remove organic matter. The obtained powder is fully ground, pressed into tablets, covered with mother powder, and calcined at ...

Embodiment 3

[0059] Embodiment 3 (Li 6.7+δ Al 0.1 La 3 Zr 1.75 Ti 0.25 o 12 )

[0060] Take LiOH·H 2 O,La 2 o 3 ,ZrO 2 , TiO 2 and Al(OH) 3 As a raw material, heat (200-500°C) to remove moisture. Mole ratio of raw materials to LiOH·H 2 O:La 2 o 3 :ZrO 2 :TiO 2 :Al(OH) 3 = 6.7:3:1.75:0.25:0.1 mixed with ZrO 2 Balls, ball milled for 1 hour to mix the raw materials evenly. Then the uniformly mixed powder was pressed into tablets, placed in an alumina crucible, covered with mother powder, and calcined in air at 950°C for 12 hours. Grind to obtain a cubic phase powder. Re-press the sheet, cover the mother powder, and sinter at 1100°C for 5 hours to obtain a dense ceramic sheet lithium ion conductor. The ceramic sheet is in contact with metallic lithium, which can intercalate lithium in situ to generate a mixed conductor Li 6.7+δ Al 0.1 La 3 Zr 1.75 Ti 0.25 o 12 (0<δ≤0.25).

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Abstract

The invention relates to a mixed ion-electron conductor with a garnet structure and application of the mixed ion-electron conductor in an energy storage device. The general formula of the conductor is(LimM)xLa3(Zr<1-a>Xa)2O12, wherein m is greater than 0 and less than or equal to 1, n is greater than or equal to 0 and less than or equal to 0.5, the sum of m and n is less than or equal to 1, and xis greater than or equal to 3 and less than or equal to 7.5; M comprises at least one element selected from H, Na, K, Rb, Mg, Ca, Sr, Ba, Y, La, Ti, Zr, Zn, B, Al, Ga, In, C, Si, Ge, P, S and Se; a is greater than or equal to 0 and less than 1; and X comprises at least one element selected from Ta, Hf, V, Nb, Ta, Cr, Mo, W, Mn, Fe, Co, Ni, Si, Ge, Sn, Pb, As, Sb and Se. The conductor provided bythe invention has high ionic conductivity and electronic conductivity, and can be applied to an electrode / electrolyte interface layer in a battery or a capacitor, a positive electrode layer and a negative electrode layer. The mixed ion-electron conductor can be applied to a lithium ion battery, a rechargeable metal lithium battery, a lithium flow battery and a lithium ion capacitor, and the energystorage devices have wide application.

Description

Technical field [0001] The present invention relates to a mixed ion-electron conductor (mixed conductor) material, a composite mixed conductor material containing the mixed conductor material, and its application in energy storage devices. Background technique [0002] Lithium-ion secondary batteries have good overall performance and are widely used in large-scale energy storage, electric vehicles, consumer electronics and other industries. Therefore, people have put forward higher requirements for their safety performance, energy density and power density. Compared with traditional organic electrolytes, inorganic solid electrolytes are non-flammable and have the possibility of matching high-energy-density metallic lithium anodes. They have received widespread attention in the development of next-generation high-energy-density lithium batteries. For all-solid-state batteries, the kinetic limit of the solid-solid interface is the biggest challenge limiting its application (K....

Claims

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Application Information

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IPC IPC(8): H01M10/0562H01M10/052H01M10/0525H01M8/18H01G11/56
CPCH01G11/56H01M8/188H01M10/052H01M10/0525H01M10/0562Y02E60/10Y02E60/13Y02E60/50
Inventor 高健周伟东
Owner BEIJING UNIV OF CHEM TECH
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