CN113948677B - Silicon-alkene negative plate capable of being directly used for preparing lithium ion battery and preparation and application thereof - Google Patents

Silicon-alkene negative plate capable of being directly used for preparing lithium ion battery and preparation and application thereof Download PDF

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CN113948677B
CN113948677B CN202111208327.4A CN202111208327A CN113948677B CN 113948677 B CN113948677 B CN 113948677B CN 202111208327 A CN202111208327 A CN 202111208327A CN 113948677 B CN113948677 B CN 113948677B
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silylene
less
silicon
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lithium ion
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CN113948677A (en
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张校刚
王华兰
贺文杰
刘雪
李岩
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Nanjing University of Aeronautics and Astronautics
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/134—Electrodes based on metals, Si or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H01M4/623—Binders being polymers fluorinated polymers
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Abstract

The invention discloses a silylene negative plate capable of being directly used for preparing a lithium ion battery, a preparation method thereof and application thereof in preparing the lithium ion battery. The preparation method comprises the following steps: (1) Mixing and dispersing a silicon precursor, conductive carbon black and a binder in a solvent, performing ultrasonic treatment and stirring to form slurry, coating the slurry on a current collector, and performing vacuum drying to remove the solvent to obtain an electrode plate; the silicon precursor is CaSi 2 Or MgSi 2 (ii) a (2) Taking a platinum wire as a cathode or an anode, inserting the platinum wire into an electrolyte containing inorganic acid and an organic solvent, taking the electrode slice prepared in the step (1) as the anode or the cathode, constructing an electrochemical reaction cell, carrying out electrochemical reaction, cleaning the surface of the electrode slice after the reaction is finished, and carrying out vacuum drying to obtain a silicon-alkene negative electrode slice which can be directly used for preparing a lithium ion battery; the conditions of the electrochemical reaction are as follows: 1mA/cm 2 The current density is not less than 300mA/cm 2 The reaction time is less than or equal to 300min and is less than or equal to 1 min.

Description

Silicon-alkene negative plate capable of being directly used for preparing lithium ion battery and preparation and application thereof
Technical Field
The invention relates to the field of preparation of two-dimensional silylene materials, in particular to a silylene negative plate capable of being directly used for preparing a lithium ion battery and preparation and application thereof.
Background
Silicon and carbon belong to the group IVA of the periodic table of elements, and like graphene, silylene is also a layered material with a honeycomb structure, being the thinnest two-dimensional form of silicon. Unlike graphene, the six silicon atoms of the graphene on the honeycomb surface are not strictly in the same plane, but constitute a folded and bent "chair-shaped" structure. The silicon alkene layer can be used for inserting lithium ions, the lattice constant of the silicon alkene is larger than that of graphite, and the theoretical capacity of the silicon alkene serving as a lithium ion battery cathode can be about three times of that of the graphite. Van der Waals force between the silicon alkene layers ensures that the structure of the silicon alkene is not damaged in the charging and discharging process, so that the problem of huge volume expansion caused by charging and discharging of the traditional silicon electrode material is solved, and the stability and the cycle frequency of the battery taking the silicon alkene as the cathode material are greatly improved. In addition, the silylene has strong spin orbit coupling, can open a larger energy gap at a Dirac point, realizes observable quantized spin Hall effect, is also very suitable for a novel transistor, is convenient to integrate into electronic equipment, is compatible with the existing silicon semiconductor industry, and therefore has extremely wide application prospect.
As early as 1994, a two-dimensional layered structure of silicon was predicted (Phys Rev B1994, 50, 14916). Guzm n-Verri and Lew Yan Voon in 2007 named silicon materials in two-dimensional layered structures as silylene (Phys Rev B2007, 76, 075131). Ciraci et al in 2009 demonstrated that two-dimensional silylene can exist stably by theoretical calculations (Phys Rev Lett,2009,102, 236804.). The epitaxial growth method is the first method for preparing the silicon alkene which is also used at present, namely heating a silicon target under a vacuum condition, evaporating silicon atoms and depositing the silicon atoms on a special substrate material such as Ag single crystal and the like. The evaporated silicon atoms are subjected to strong silicon/silver interface interaction when the silylene is generated on the substrate, and the warping degree of the layered silylene is changed, namely, part of the silicon atoms rise and part of the silicon atoms fall, so that few layers of the silylene are formed. However, early studies of the preparation of silylene on the Ag (001) and Ag (110) planes only allowed for silylene nanoribbons of limited width, and the prepared silylene unit cells became large and less symmetrical, destroying the dirac-fermi character of silylene, thus affecting the performance of silylene (surfsci 2007,601,262-7.Appl Phys Lett 2010,96,183102.Appl Phys Lett 2011,98,081909.Appl Phys Lett 2010,96, 261905.). Until 2012, vogt et al in Ag (1)11 Large area of single layer of silylene was successfully prepared on the face and the stable presence of the single layer of silylene was experimentally verified (Phys Rev Lett 2012,108, 155501.). Meanwhile, the scholars have prepared large-area single-layer silylene and multi-layer silylene on the Ag (111) surface. Then, the scholars on other substrates (ZrB) 2 、ZrC、Ir、Ru、MoS 2 ) Silenes, e.g. ZrB, are also prepared 2 (Phys Rev Let 2012,108, 24501), zrC (J Phys Chem C2014, 118, 23049), ir (Nano Lett 2013,13, 685), ru (Nano Lett.2017,17, 1161) and MoS 2 (Adv Mater 2014,26,2096)。
In 2006, hideyuki Nakano firstly tried to prepare silylene by a chemical method, and Mg-doped CaSi 2 (CaSi 1.85 Mg 0.15 ) And hydrochloric acid as raw materials, the reaction time is as long as 10 days, but the generation rate of the silylene is only 1% (Angew. Chem. Int. Ed.2006,45, 6303-6306). KaSi by Ritsuko Yaokawa et al 2016 2 And ionic liquids [ BMIM][BF 4 ](1-butyl-3-methylimidazolium tetrafluoroborate) at 300 ℃ for 15h 4 - Decomposition to F - Into CaSi 2 Interlayer preparation of CaSi 2 F x (0 ≦ x ≦ 2.3), since Si bonded to Ca was substituted with F having a stronger electronegativity, si liberated from the original honeycomb structure reconstructed into a double-layered structure, and thus, a double-layered silylene was prepared (nat. Commun.2016,7, 10657). 2018 Yuxi Xu in acetonitrile solvent at normal temperature 2 And CaSi 2 The reaction produced a few layers of silylene (adv. Mater.2018,30, 1800838).
Patent CN105439148A in 2015 discloses a method for preparing silylene. Processing silicon block into concave cone-shaped silicon target, mounting on sputtering target of cesium sputtering negative ion source, sputtering silicon target with cesium ions, and sputtering the resultant Si 2 Cluster negative ion beam is led out from the extraction hole of the anode and cluster negative ion Si 2 After being accelerated by a suction electrode voltage, the sample is uniformly deposited on an Ag (111) substrate through a scanning electric field, the sample is placed in a vacuum chamber, ar is added + And sputtering the surface by ions, and then annealing the sample under ultrahigh vacuum to complete the preparation of the silylene. 2016 patent CN 106554016A discloses a method for preparing a silicon alkene film by mechanical stripping. Two-dimensional material (hexagonal boron nitride, di)Molybdenum sulfide, tungsten disulfide, molybdenum diselenide and graphene) cover the surface of the silicon (111) passivated by the metal (Ag, au, mo, cu and Ti) film, and after being treated at the high temperature of 750-1050 ℃ for 2-4 hours, the silicon element is diffused to the interface of the metal film and the two-dimensional material and is cooled to the room temperature; dispersing a sample in a solvent with a surfactant, enabling polar molecules to easily enter an interface between metal and a substrate, increasing friction between the metal and the substrate through ultrasonic stirring, and stripping the silylene and the two-dimensional material from the silicon substrate to obtain the silylene film. Patent CN 110600688A in 2019 discloses a method for preparing SiCl serving as a silicon source by taking ionic liquid as a medium 4 And a method for preparing the silylene-copper-silylene composite material by electrodepositing bivalent copper. The concentration of the divalent copper in the ionic liquid is 0.002-0.003 mol/L, and the potential of electrodeposition is-1.9 to-2.1V.
Although various methods for preparing silylene have been developed, the method for preparing high-quality silylene, which has low cost and high efficiency and can adapt to various application occasions in the future, is still very short and is also a great problem and challenge at present.
Disclosure of Invention
Aiming at the technical problems of low silicon alkene yield, high cost, difficulty in batch preparation, long reaction time for preparing silicon alkene by a chemical method, low product quality, low silicon alkene yield prepared by a mechanical stripping method, low efficiency and the like in the preparation of silicon alkene by an epitaxial growth method, the invention provides a preparation method of a silicon alkene negative plate which can be directly used for preparing a lithium ion battery, and the preparation method is a novel method for preparing a two-dimensional silicon alkene material.
A preparation method of a silicon alkene negative plate which can be directly used for preparing a lithium ion battery comprises the following steps:
(1) Mixing and dispersing a silicon precursor, conductive carbon black and a binder in a solvent, performing ultrasonic treatment and stirring to form slurry, coating the slurry on a current collector, and performing vacuum drying to remove the solvent to obtain an electrode plate;
the silicon precursor is CaSi 2 Or MgSi 2 ；
(2) Taking a platinum wire as a cathode or an anode, inserting the platinum wire into an electrolyte containing inorganic acid and an organic solvent, taking the electrode slice prepared in the step (1) as the anode or the cathode, constructing an electrochemical reaction cell, carrying out electrochemical reaction, cleaning the surface of the electrode slice after the reaction is finished, and carrying out vacuum drying to obtain the silylene negative electrode slice which can be directly used for preparing the lithium ion battery;
the conditions of the electrochemical reaction are as follows: 1mA/cm 2 The current density is not less than 300mA/cm 2 The reaction time is less than or equal to 300min and is less than or equal to 1 min.
In a preferred example, the binder is one of polyvinylidene fluoride, polysaccharide, carboxymethyl cellulose, polyacrylic acid and polyacrylonitrile.
The mass ratio of the silicon precursor to the conductive carbon black to the binder is a: b:1, wherein preferably, a is more than or equal to 7 and less than or equal to 15, b is more than or equal to 1 and less than or equal to 3, further preferably, a is more than or equal to 7 and less than or equal to 12, and b is more than or equal to 1 and less than or equal to 2.
In a preferred embodiment, in step (1), the solvent is nitrogen methyl pyrrolidone.
In a preferred embodiment, the current collector is one of copper foil, carbon-plated copper foil, foam copper, carbon paper and carbon cloth.
In the step (2), the following preferred technical scheme can be adopted:
the inorganic acid is one of hydrochloric acid, sulfuric acid, nitric acid, hydrofluoric acid and phosphoric acid;
the organic solvent is an alcohol solvent;
the volume ratio of the inorganic acid to the organic solvent is 1.
In a preferred example, in the step (2), the conditions of the electrochemical reaction are: 1mA/cm 2 The current density is not less than 100mA/cm 2 The reaction time is less than or equal to 120min and is less than or equal to 1 min.
The existing epitaxial growth preparation method of the silylene is generally realized under the conditions of high temperature and high vacuum of hundreds of even thousands of degrees, a noble metal substrate is used, the silylene needs to be subjected to post-treatment to stabilize the silylene, the preparation process is complex and tedious, the production period is long, and the cost is very high. The existing mechanical stripping method of the silylene has low yield and low efficiency, and is not suitable for the requirement of large-scale industrial production. The chemical preparation method has the disadvantages of long reaction time, poor quality of the prepared silylene, poor experimental reproducibility and the like. The development of a novel preparation method of the silylene with simplicity, low cost, high efficiency and high quality becomes an urgent need to promote the application of the silylene. The invention provides a method for preparing silylene by an electrochemical method, the obtained negative plate can be directly used as a negative electrode to be applied to a lithium ion battery, and high-quality silylene is successfully prepared at normal temperature in one step by setting constant current density and reaction time on electrochemical equipment. The method avoids using a noble metal substrate and a high-temperature high-vacuum environment, greatly shortens the reaction time, effectively reduces the cost and improves the yield and the quality of the silylene. On the basis, the application of the silylene prepared by the electrochemical method as an active ingredient in the lithium ion battery cathode material is realized.
The invention also provides the silylene negative plate which is prepared by the preparation method and can be directly used for preparing the lithium ion battery.
The invention also provides application of the silicon-alkene negative plate in preparation of a lithium ion battery.
Compared with the prior art, the invention has the main advantages that:
1) The invention provides a novel electrochemical preparation method of simple, efficient, low-cost and high-quality silylene, which does not need to use a noble metal substrate, avoids high-temperature and high-vacuum reaction conditions, can be completed within minutes to several hours at normal temperature, prepares the silylene with the nanoscale thickness, greatly reduces the preparation cost and simplifies the preparation process.
2) Compared with the traditional method for preparing the silicon alkene, the silicon alkene prepared by the method provided by the invention has good quality and high yield, and provides a high-performance key material for the next generation lithium ion battery technology and the electronic field.
3) The electrochemical method for preparing the silylene has high process safety, good reproducibility and environmental protection, and is expected to be applied to industrial large-scale batch preparation.
Drawings
FIG. 1 is a graph showing the constant current density electrochemical reaction operation in example 4;
FIG. 2 is a SEM photograph of the silylene prepared in examples 1-6;
in fig. 3, a is a graph of the charge and discharge performance of the first 1 to 2 turns of the negative silicon-ene sheet prepared in example 3 at a current density of 100mA/g, and b is a graph of the coulombic efficiency of the first 1 to 100 turns of the negative silicon-ene sheet prepared in example 3 at a current density of 100 mA/g.
Detailed Description
The invention is further described with reference to the following drawings and specific examples. It should be understood that these examples are for illustrative purposes only and are not intended to limit the scope of the present invention. The following examples are conducted under conditions not specified, usually according to conventional conditions, or according to conditions recommended by the manufacturer.
An electrochemical reaction cell constructed in accordance with the following examples, comprising:
a base on which a current collector is placed;
the reaction tank is arranged on the current collector and has a hollow cylindrical structure, and the upper end and the lower end of the reaction tank are open; the hollow part of the reaction tank is used for filling electrolyte, the bottom end of the electrolyte is contacted with the current collector after the electrolyte is filled, and a platinum wire is inserted into the electrolyte.
Example 1
(1) Preparing an electrode foil: mixing CaSi 2 Mixing and dispersing conductive carbon black and polyvinylidene fluoride in N-methyl pyrrolidone according to the mass ratio of 7;
(2) Construction of an electrochemical reaction cell: taking a platinum wire as a cathode or an anode, inserting the platinum wire into electrolyte of a reaction tank, taking an electrode foil prepared in the step (1) as the anode or the cathode, placing the electrode foil between the reaction tank and a base, and taking the electrolyte as hydrochloric acid: ethanol =1:10 (v/v) constructing an electrochemical reaction tank by using the mixed solution; the HCl concentration in the hydrochloric acid is 37wt%;
(3) Carrying out an electrochemical reaction: setting the current density to be 10mA/cm on an electrochemical workstation 2 And the reaction time is 5min, after the reaction is finished, the surface of the electrode foil is cleaned by absolute ethyl alcohol, and the electrode foil is placed in a vacuum drying oven for drying, so that the silicon-alkene negative plate which can be directly used for preparing the lithium ion battery is obtained. Prepared siliconA scanning electron micrograph of the alkene is shown in FIG. 2 a.
Example 2
The only difference from example 1 is that the reaction time in step (3) is 10min, the rest steps and conditions are the same, and the scanning electron micrograph of the prepared silylene is shown in fig. 2 b.
Example 3
The difference from the example 1 is only that the carbon-plated copper foil is adopted as the current collector in the step (1), and the current density in the step (3) is 50mA/cm 2 And the rest steps and conditions are the same, and the scanning electron micrograph of the prepared silylene is shown in figure 2 c.
Example 4
The difference from example 1 is only that the current collector in step (1) adopts carbon paper, the constant current density electrochemical reaction working curve in step (3) is shown in figure 1, and the current density is 50mA/cm 2 The reaction time is 10min, the rest steps and conditions are the same, and the scanning electron micrograph of the prepared silylene is shown in FIG. 2 d.
Example 5
The difference from the example 1 is only that the carbon cloth is adopted as the current collector in the step (1), and the current density in the step (3) is 100mA/cm 2 And the rest steps and conditions are the same, and the scanning electron micrograph of the prepared silylene is shown in figure 2 e.
Example 6
The difference from the example 1 is only that the carbon cloth is adopted as the current collector in the step (1), and the current density in the step (3) is 100mA/cm 2 The reaction time is 10min, the rest steps and conditions are the same, and the scanning electron micrograph of the prepared silylene is shown in figure 2 f.
The electrochemical reaction parameters and the basic performance parameters of the silylene negative electrode sheet of examples 1-6, which can be directly used for preparing lithium ion batteries, are shown in table 1 below. The 90% silylene radial dimension parameter index represents that 90% silylene radial dimensions are concentrated in the corresponding range. The 90% silylene thickness parameter index represents that the 90% silylene thickness is concentrated in the corresponding range.
TABLE 1
Figure BDA0003307747830000071
Application example
The negative silylene plates prepared in examples 1 to 6 were directly used to make lithium ion batteries: cutting the silicon alkene negative pole piece into small round pieces, compacting the small round pieces on a tablet press under 10MPa, stacking the battery in an argon-protected glove box according to the sequence of the positive pole shell, the silicon alkene negative pole piece, the electrolyte, the diaphragm, the lithium piece, the foam nickel and the negative pole shell, and sealing the battery by using a sealing machine. Electrolyte adopts 1.0M LiPF 6 [ EC-EMC-DEC-FEC (EC: EMC: DEC =1 (volume ratio): 1, wherein EC: ethylene carbonate, EMC: ethyl methyl carbonate, DEC: diethyl carbonate, FEC: ethylene carbonate). The diaphragm is Celgare 2400 type porous PP diaphragm and the battery case model is CR2025. And detecting a charge and discharge curve of the battery by using the charge and discharge equipment. At a current density of 50mA/cm 2 Taking the negative silylene sheet prepared at the reaction time of 5min (i.e., the negative silylene sheet prepared in example 3) as an example, the charge-discharge curve is shown in fig. 3a, and the coulombic efficiency is shown in fig. 3 b. The first discharge specific capacity of the battery is 1614mAh/g, the coulombic efficiency is 9%, the second circle discharge specific capacity is 470mAhg, the coulombic efficiency is increased to 41%, the discharge specific capacity is 211mAh/g after 100 circles of charge-discharge cycles, and the coulombic efficiency value is gradually increased and finally approaches 100%.
As can be seen from examples 1 to 6, table 1 and FIG. 2, the silylene prepared by the electrochemical method of the present invention has uniform size, and the radial size and thickness of 90% of the silylene can be ensured to be in a more concentrated range. The thickness of the obtained silicon alkene has a certain relation with electrochemical reaction parameters, and the thickness of the obtained silicon alkene sheet layer is gradually reduced along with the increase of the current density. From the application example and fig. 3, it can be seen that the silylene prepared by the electrochemical method has good electrochemical performance when used as the negative electrode material of the lithium ion battery, and after the activation of the first several cycles of charge and discharge, the battery has high coulombic efficiency and good cycle performance.
The electrochemical preparation method of the silylene negative plate has the characteristics of mild preparation conditions, simplicity in operation, rapidness in reaction, low cost, high yield, high product quality, small volume effect in the charging and discharging process, excellent electrochemical lithium storage performance and the like.
Furthermore, it should be understood that various changes and modifications can be made by one skilled in the art after reading the above description of the present invention, and equivalents also fall within the scope of the invention as defined by the appended claims.

Claims (9)

1. A preparation method of a silicon-alkene negative plate directly used for preparing a lithium ion battery is characterized by comprising the following steps:
(1) Mixing and dispersing a silicon precursor, conductive carbon black and a binder in a solvent, performing ultrasonic treatment and stirring to form slurry, coating the slurry on a current collector, and performing vacuum drying to remove the solvent to obtain an electrode plate;
the silicon precursor is CaSi 2 Or MgSi 2 ；
(2) Taking a platinum wire as a cathode or an anode, inserting the platinum wire into an electrolyte containing inorganic acid and an organic solvent, taking the electrode slice prepared in the step (1) as the anode or the cathode, constructing an electrochemical reaction cell, carrying out electrochemical reaction, cleaning the surface of the electrode slice after the reaction is finished, and carrying out vacuum drying to obtain the silylene negative electrode slice which can be directly used for preparing the lithium ion battery;
the conditions of the electrochemical reaction are as follows: 1mA/cm 2 The current density is not less than 300mA/cm 2 The reaction time is less than or equal to 300min and is less than or equal to 1 min.
2. The method according to claim 1, wherein the binder is one of polyvinylidene fluoride, polysaccharide, carboxymethyl cellulose, polyacrylic acid, and polyacrylonitrile.
3. The preparation method of claim 1, wherein the mass ratio of the silicon precursor to the conductive carbon black and the binder is a: b:1, wherein a is greater than or equal to 7 and less than or equal to 15, and b is greater than or equal to 1 and less than or equal to 3.
4. The method according to claim 1, wherein in the step (1), the solvent is N-methylpyrrolidone.
5. The method of claim 1, wherein the current collector is one of a copper foil, a carbon-plated copper foil, a copper foam, a carbon paper, and a carbon cloth.
6. The production method according to claim 1, wherein in the step (2):
the inorganic acid is one of hydrochloric acid, sulfuric acid, nitric acid, hydrofluoric acid and phosphoric acid;
the organic solvent is an alcohol solvent;
the volume ratio of the inorganic acid to the organic solvent is 1.
7. The method according to claim 1, wherein in the step (2), the conditions of the electrochemical reaction are: 1mA/cm 2 The current density is not less than 100mA/cm 2 The reaction time is less than or equal to 120min and is less than or equal to 1 min.
8. The negative silylene plate prepared by the preparation method according to any one of claims 1 to 7 and directly used for preparing a lithium ion battery.
9. The use of the negative silylene sheet of claim 8 in the preparation of a lithium ion battery.
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