CN-122011014-A - All-solid-state battery interface optimizer with lithium ion conduction and flame retardance functions and preparation method thereof

CN122011014ACN 122011014 ACN122011014 ACN 122011014ACN-122011014-A

Abstract

The invention discloses an all-solid-state battery interface optimizer with double functions of lithium ion conduction and flame retardance and a preparation method thereof, and the structure of the all-solid-state battery interface optimizer is shown as a formula (I), wherein m is more than or equal to 1 and less than or equal to 4, n is more than or equal to 1 and less than or equal to 3, x is more than or equal to 1 and less than or equal to 3, and m, n and x are integers. The bi-functional all-solid-state battery interface optimizer PPD is synthesized by chemical reaction of raw materials of phosphorus pentachloride, diamine and alcohol ether, and lithium salt (such as LiTFSI) is needed to be doped before use to provide lithium ion conductivity. The interface optimizing agent has the advantages of good lithium ion conductivity, flame resistance, fluidity, wettability and the like. The invention synthesizes the interface optimizing agent by a one-pot one-step method, has simple process, good reproducibility, good controllability and low cost, and is expected to realize the preparation of the all-solid-state battery with high safety, high energy density and low cost when being applied to the all-solid-state battery interface optimizing agent.

Inventors

HAN DONGMEI
HUANG CHENG
MENG YUEZHONG
ZHONG LEI
XIAO MIN
WANG SHUANJIN
HUANG SHENG
XU YAN
QIU JUNCHENG

Assignees

中山大学

Dates

Publication Date: 20260512
Application Date: 20260121

Claims (7)

1. An all-solid-state battery interface optimizing agent with double functions of lithium ion conduction and flame retardance has the structure shown in a formula (I), wherein m is more than or equal to 1 and less than or equal to 4, n is more than or equal to 1 and less than or equal to 3, x is more than or equal to 1 and less than or equal to 3, and m, n and x are integers; 。
2. the method for preparing the all-solid-state battery interface optimizer with lithium ion conduction and flame retardance functions as set forth in claim 1, which is characterized by comprising the following steps: S1, adding phosphorus pentachloride and tetrahydrofuran into a three-necked flask, taking out after sealing, placing the three-necked flask in a low-temperature reactor, stirring the three-necked flask and the phosphorus pentachloride with a stirring paddle at-20 ℃ until the three-necked flask is dispersed, then diluting diamine, alcohol ether and triethylamine into absolute dry tetrahydrofuran, placing the absolute dry tetrahydrofuran into a constant pressure funnel, slowly dropwise adding the absolute dry tetrahydrofuran into the three-necked flask, and reacting the absolute dry tetrahydrofuran with the three-necked flask at-20 ℃ under the protection of nitrogen for 3 hours to obtain an intermediate product; S2, filtering and rotary steaming the intermediate product to remove redundant raw materials and byproducts, pouring the intermediate product into a separating funnel, repeatedly extracting with water and ethyl acetate, dissolving the redundant raw materials in water at the moment and dissolving most of target products in ethyl acetate, taking an upper organic phase, removing residual ethyl acetate and water through rotary steaming and vacuumizing, and adding LiTFSI to obtain the all-solid-state battery interface optimizing agent.
3. The method of claim 2, wherein the molar ratio of phosphorus pentachloride to diamine is 1 (1-3), the molar ratio of phosphorus pentachloride to alcohol ether is 1 (2-4), and the mixed solution of diamine, alcohol ether and triethylamine is added dropwise over about 2 hours.
4. The method according to claim 2, wherein the diamine is one of diethylamine, dipropylamine and dibutylamine.
5. The method of claim 2, wherein the alcohol ether is one or more of ethylene glycol monomethyl ether, diethylene glycol monomethyl ether, triethylene glycol monomethyl ether, tetraethylene glycol monomethyl ether.
6. The preparation method of claim 2, wherein the molar ratio of water to ethyl acetate is 1 (1-3), the number of repeated extractions is 2, and the mass fraction of LiTFSI in the all-solid-state battery interface optimizing agent is 30%.
7. Use of an all-solid-state battery interface optimizer having both lithium ion conduction and flame retardance functions of claim 1 in an all-solid-state battery.

Description

All-solid-state battery interface optimizer with lithium ion conduction and flame retardance functions and preparation method thereof Technical Field The invention belongs to the technical field of synthesis of all-solid-state battery interface optimizers, and particularly relates to an all-solid-state battery interface optimizer with double functions of lithium ion conduction and flame retardance and a preparation method thereof. Background In recent years, events such as explosion and ignition of lithium ion batteries have been reported, and safety problems have become a problem to be solved in further large-scale lithium ion batteries. Solid state batteries are an effective way to address the potential safety hazards of lithium batteries, but the incompatibility of the inside and between the components of solid state batteries affects the performance of the batteries. The method for optimizing the interface is to add a small amount of liquid, and the common liquid is alkyl carbonate compounds such as diethyl carbonate (DEC), ethylene Carbonate (EC) and the like, but the alkyl carbonate compounds are all low-flash-point and high-volatility organic solvents and are inflammable and explosive. Flame-retardant liquids such as triethyl phosphate, trimethyl phosphate, etc. have also been developed and studied, but various kinds of liquids cannot be considered in terms of wettability, lithium ion conductivity, flame resistance and low cost, and therefore, development and application of an all-solid-state battery interface optimizer having both lithium ion conductivity and flame retardance have been demanded. The method for synthesizing the all-solid-state battery interface optimizer with the functions of lithium ion conduction and flame retardance, which contains nitrogen and phosphorus elements, through phosphorus pentachloride, diamine and alcohol ether has not been reported yet. Disclosure of Invention In order to solve the defects and shortcomings of the prior art, the invention aims to provide an all-solid-state battery interface optimizer (PPD) with double functions of lithium ion conduction and flame retardance, which can solve the problem of incompatibility between the inside of each part and each part of an all-solid-state battery, and has the advantages of simple process, good reproducibility, good controllability and low cost. In order to achieve the above purpose, the present invention adopts the following technical scheme: the full-solid battery interface optimizing agent with the double functions of lithium ion conduction and flame retardance has the structure shown in a formula (I), wherein m is more than or equal to 1 and less than or equal to 4, n is more than or equal to 1 and less than or equal to 3, x is more than or equal to 1 and less than or equal to 3, and m, n and x are integers. The preparation method of the all-solid-state battery interface optimizing agent with the dual functions of lithium ion conduction and flame retardance comprises the following steps: S1, adding phosphorus pentachloride and tetrahydrofuran into a three-necked flask, taking out after sealing, placing the three-necked flask in a low-temperature reactor, stirring the three-necked flask and the phosphorus pentachloride with a stirring paddle at-20 ℃ until the three-necked flask is dispersed, then diluting diamine, alcohol ether and triethylamine into absolute dry tetrahydrofuran, placing the absolute dry tetrahydrofuran into a constant pressure funnel, slowly dropwise adding the absolute dry tetrahydrofuran into the three-necked flask, and reacting the absolute dry tetrahydrofuran with the three-necked flask at-20 ℃ under the protection of nitrogen for 3 hours to obtain an intermediate product; S2, filtering and rotary steaming the intermediate product to remove redundant raw materials and byproducts, pouring the intermediate product into a separating funnel, repeatedly extracting with water and ethyl acetate, dissolving the redundant raw materials in water at the moment and dissolving most of target products in ethyl acetate, taking an upper organic phase, removing residual ethyl acetate and water through rotary steaming and vacuumizing, and adding LiTFSI to obtain the all-solid-state battery interface optimizing agent. Preferably, the molar ratio of phosphorus pentachloride to diamine is 1 (1-3), the molar ratio of phosphorus pentachloride to alcohol ether is 1 (2-4), and the mixed solution of diamine, alcohol ether and triethylamine is dropwise added within about 2 hours. Preferably, the diamine is one of diethylamine, dipropylamine and dibutylamine. Preferably, the alcohol ether is one or more of ethylene glycol monomethyl ether, diethylene glycol monomethyl ether, triethylene glycol monomethyl ether and tetraethylene glycol monomethyl ether. Preferably, the molar ratio of water to ethyl acetate is 1 (1-3), the number of repeated extraction is 2, and the mass fraction of LiTFSI in the all-solid-state battery inte