Polymerized organic-inorganic composite solid electrolyte and in-situ assembled all-solid-state battery

A solid electrolyte and all-solid-state battery technology, which is applied in the direction of composite electrolyte, electrolyte storage battery manufacturing, non-aqueous electrolyte storage battery, etc., can solve the problems of low conductivity and large interface resistance of all-solid-state batteries, and achieve reduced interface resistance and excellent battery performance , increase the effect of tightness

Active Publication Date: 2019-12-10
HUAZHONG UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] The invention solves the problems of low conductivity of polymer solid electrolyte and large interface resistance of all-solid-state b

Method used

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  • Polymerized organic-inorganic composite solid electrolyte and in-situ assembled all-solid-state battery
  • Polymerized organic-inorganic composite solid electrolyte and in-situ assembled all-solid-state battery
  • Polymerized organic-inorganic composite solid electrolyte and in-situ assembled all-solid-state battery

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Experimental program
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preparation example Construction

[0060] (1) Preparation of the liquid precursor: mix the liquid polymer monomer and the crosslinking agent uniformly according to the predetermined ratio, then add the solid organolithium salt and the initiator, and stir until completely dissolved. Then add the ceramic electrolyte filler and stir until it is uniformly dispersed to obtain a completely mixed and uniform liquid precursor;

[0061] (2) Preparation of active ceramic electrolyte filler: Add corresponding salts to ethylene glycol in sequence, then add citric acid monohydrate and stir to obtain a clear solution; heat the obtained clear solution to reflux, age, carbonize, and then undergo high temperature Calcination yields active nanoparticles. In some embodiments, for the heat treatment of the carbide, the heat treatment temperature is set at 600-900°C, the heating rate is 5°C / min, and the carbonization time is 24h-48h. Active ceramic electrolyte fillers can also be formed by solid-state reactions, or nanofibrous fil...

Embodiment 1

[0067] Preparation of the precursor: mix the polymer monomer polyethylene glycol dimethacrylate and the crosslinking agent tetraethylene glycol diacrylate in a ratio of 19:1, then add 1mol / L LiTFSI and 2wt% heat Initiator azobisisobutyronitrile until completely dissolved. The subsequent addition of 10 wt% ceramic electrolyte Li 6.25 Ga 0.25 La 3 Zr 2 o 12 Filler, stir until evenly dispersed, and then a completely mixed and uniform liquid precursor can be obtained. The precursor can form a solid electrolyte under thermal initiation.

[0068] as attached figure 1 As shown, the conductivity of the obtained solid electrolyte is 1.8×10 -4 S / cm; as attached figure 2 As shown, the electrochemical window of the solid electrolyte obtained in the present invention can reach more than 6V. as attached image 3 It was shown that the resulting electrolyte was assembled into a Li-Li symmetric battery, and at 0.5mA cm -2 Under a high current density, it can be cycled stably for mo...

Embodiment 2

[0076] Preparation of the precursor: mix the polymer monomer polyethylene glycol dimethacrylate and the crosslinking agent tetraethylene glycol diacrylate in a ratio of 4:1, then add 1mol / L LiTFSI and 2wt% heat Initiator azobisisobutyronitrile until completely dissolved. The subsequent addition of 10 wt% ceramic electrolyte Li 6.25 Ga 0.25 La 3 Zr 2 o 12 Filler, stir until evenly dispersed, and then a completely mixed and uniform liquid precursor can be obtained. The precursor can form a solid electrolyte under thermal initiation.

[0077] as attached figure 1 As shown, the conductivity of the obtained solid electrolyte is 1.2×10 -4 S / cm.

[0078] In situ curing assembled battery: take 10 μL of the obtained precursor, carefully drop on the LiNi 0.6 co 0.2 mn 0.2 o 2 Between the composite positive electrode and the lithium metal negative electrode, it was then carefully moved to a heating device at 100 °C to initiate polymerization. After 90s, the integrated lamina...

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Abstract

The invention relates to a polymerized organic-inorganic composite solid electrolyte and an in-situ assembled all-solid-state battery, and belongs to the technical field of ion battery preparation. The preparation method of the polymerized solid electrolyte comprises the following steps: fully and uniformly mixing a polymer monomer and a cross-linking agent, and adding an electrolyte salt and an initiator to obtain an electrolyte precursor; and initiating the electrolyte precursor to obtain the polymerized solid electrolyte. The in-situ assembled all-solid-state battery can be obtained by dropping the electrolyte precursor onto a positive electrode, covering the electrolyte precursor with a negative electrode, carrying out initiating and curing the electrolyte precursor. The room-temperature conductivity of the solid electrolyte reaches 1.6*10<-4>Scm<-1>, and the electrochemical window is greater than 6V. For the all-solid-state battery based on the solid electrolyte, the discharge capacity density is 145mAh/g at the charge-discharge rate of 0.5C, the discharge capacity is 176mAh/g at the charge-discharge rate of 0.1C, and the capacity retention ratio after 100 cycles at the charge-discharge rate of 0.5C is 88%.

Description

technical field [0001] The invention belongs to the technical field of ion battery preparation, and more specifically relates to a polymerized organic-inorganic composite solid electrolyte and an in-situ assembled all-solid-state battery. Background technique [0002] As a new type of energy storage device, lithium-ion batteries are widely used in mobile electronic devices and electric vehicles. At present, traditional commercial lithium-ion batteries mainly use liquid organic electrolytes, which are easy to cause serious safety problems such as combustion and leakage. At the same time, liquid electrolytes have poor stability and narrow electrochemical window, resulting in low energy density. Compared with liquid electrolytes, solid electrolytes have higher safety and thermal stability. At the same time, the solid electrolyte is stable to lithium metal and can well inhibit the growth of lithium dendrites. In addition, the solid electrolyte has a wider electrochemical wind...

Claims

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Application Information

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IPC IPC(8): H01M10/058H01M10/0565H01M10/0562H01M10/0525
CPCH01M10/0525H01M10/0562H01M10/0565H01M10/058H01M2300/0088Y02E60/10Y02P70/50
Inventor 郭新李卓
Owner HUAZHONG UNIV OF SCI & TECH
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