Silicon oxide interface-linked high-strength porous carbon material, preparation method, application and battery

Abstract

The application provides a high-strength porous carbon material linked by a silicon oxide interface, a preparation method, application and battery. The preparation method comprises the following steps: (1) spray granulation is performed on a mixture containing sub-micron anthracite particles, phenolic resin and pitch to obtain granulated particles; (2) a mixed solution containing the granulated particles, organosilicon and a catalyst is reacted to obtain modified particles coated with an organosilicon hydrolysis film on the surface; (3) the modified particles coated with the organosilicon hydrolysis film on the surface are carbonized to obtain a porous silicon oxide coated carbonized composite material; and (4) the porous silicon oxide coated carbonized composite material is activated by water vapor under a heated state to form pores. The high-strength porous carbon material linked by a silicon oxide interface prepared by the application has high mechanical strength, and when applied to a sodium ion battery, has high initial efficiency and capacity, and excellent cycle stability.

Description

Technical Field

[0001] This invention specifically relates to a high-strength porous carbon material with silicon oxide interface linkage, its preparation method, applications, and batteries. Background Technology

[0002] Carbon-based composite materials, due to their excellent electrical conductivity, structural plasticity, and sodium storage performance, have become the mainstream research direction and application material in the field of battery anodes. Currently, traditional carbon-based anode materials mostly use phenolic resins, coconut shell carbon, and other raw materials to prepare porous carbon matrices. However, these raw materials are expensive, and pure carbon matrices suffer from insufficient structural stability and low ion transport efficiency, making it difficult to meet the energy storage application requirements of high-rate charge-discharge and long-cycle applications, thus limiting their large-scale application in the high-end battery field. At the same time, in order to improve the energy storage performance of materials, the industry generally uses elements such as silicon and aluminum for doping modification. However, conventional doping processes are prone to problems such as particle agglomeration and uneven distribution, which further affect the electrochemical performance of the electrode.

[0003] To reduce production costs, the industry is gradually exploring the use of low-cost raw materials such as coal to prepare carbon-based composite materials for anodes. Coal-based raw materials have advantages such as abundant reserves, high carbon conversion rate, and low cost, and can achieve efficient resource utilization, which is in line with the development trend of the green energy storage industry. However, existing coal-based raw materials generally have problems such as large particles and low reactivity, making it difficult to form a uniform and stable carbon matrix through conventional processes. After traditional crushing processes, the resulting powder is prone to agglomeration, with poor flowability and formability. During high-temperature carbonization and activation, the material structure is prone to collapse and the channels are prone to collapse, making it difficult to effectively increase the specific surface area. This fails to provide sufficient channels for ion transport, thus affecting the rate performance and cycle life of the battery, making it difficult to meet the usage requirements of power batteries, long-term energy storage, and other scenarios. Summary of the Invention

[0004] This invention addresses the shortcomings of existing preparation techniques by providing a high-strength porous carbon material with silica-interface linkages, its preparation method, applications, and batteries. The high-strength porous carbon material with silica-interface linkages prepared by this invention exhibits high mechanical strength and demonstrates high initial efficiency and capacity, as well as excellent cycle stability, when applied to sodium-ion batteries.

[0005] This invention uses natural anthracite containing silicon and aluminum as the matrix. It leverages the inherent silicon and aluminum components in the coal to form in-situ rigid sites at high temperatures, optimizing interfacial conductivity and strength. Ultrafine grinding enhances the dispersibility and interfacial reactivity of the raw materials. A phenolic resin / asphalt composite binder system and spray granulation form regularly shaped, dense spherical precursors, providing a stable structural substrate for subsequent coating and high-temperature reactions. In-situ hydrolysis of organosilicon forms a uniform silica coating layer on the particle surface, enabling interfacial bonding between the silicon source and the carbon matrix. High-temperature carbonization then yields… The precursor is transformed into a rigid carbon framework, and the coating layer is transformed into a porous silica shell. The synergistic enhancement effect of inorganic oxides and coal-based silica-alumina minerals is used to suppress pore collapse and structural deformation during high-temperature activation. Finally, multi-level interconnected pores are constructed by water vapor activation etching to improve the specific surface area and ion transport channels of the material. At the same time, relying on the synergistic effect of in-situ silica-alumina doping and core-shell structure, the material is endowed with high porosity, structural stability and excellent electrochemical compatibility, thereby obtaining a high-strength porous carbon material with silica interface linkages with outstanding comprehensive performance.

[0006] The present invention solves the above-mentioned technical problems through the following technical solutions: This invention provides a method for preparing a high-strength porous carbon material with silica interface linkages, comprising the following steps: (1) Spray granulation is performed on a mixture containing submicron anthracite particles, phenolic resin and asphalt to obtain granulated particles; (2) The mixture containing the granulated particles, organosilicon and catalyst is reacted to obtain modified particles with an organosilicon hydrolysis film coated on the surface. (3) The modified particles coated with the organosilicon hydrolysis film are carbonized to obtain a porous silica-coated carbonized composite material. (4) The porous silica-coated carbonized composite material is activated by steam under heating to create pores, thereby obtaining a high-strength porous carbon material with silica interface linkage.

[0007] In step (1), the particle size D of the submicron anthracite particles 50 It can be 100nm-1000nm, preferably 200-800nm, such as 300nm, 400nm, 450nm, 500nm, 600nm or 700nm.

[0008] In step (1), the method for preparing the submicron anthracite particles preferably includes the following steps: grinding and pulverizing the anthracite raw material.

[0009] The grinding process is generally carried out in a sand mill. The grinding speed can be 1500-4000 r / min, for example 2500 r / min, 2800 r / min, 3000 r / min or 3500 r / min; the grinding time can be 2-8 hours, for example 2 hours, 4 hours or 6 hours; the grinding balls used in the grinding process can be made of materials commonly used in the field, such as zirconia beads; the diameter of the grinding balls can be 0.2-20 mm, for example 0.5 mm, 0.7 mm, 1 mm, 2 mm, 5 mm, 8 mm, 10 mm or 15 mm; the ball-to-material ratio can be (2-20):1, for example 3:1, 6:1, 8:1 or 10:1, where the ball-to-material ratio refers to the mass ratio of the grinding balls to the material to be ground.

[0010] The sand milling can be performed using a wet sand milling method. When using the wet sand milling method, the added solvent can be conventional in the art, such as ethanol and / or deionized water. The mass ratio of the anthracite raw material to the solvent can be 1:(0.5-1.5), for example, 1:0.8, 1:1, or 1:1.2.

[0011] After milling, drying is generally required. This drying can be carried out in a dryer; the drying temperature can be 70-100℃; and the drying time can be 6-24 hours. If wet milling is used, solid-liquid separation is generally required before drying. This solid-liquid separation can be performed by centrifugation.

[0012] In step (1), the phenolic resin accounts for 10%-70% of the mass percentage of the submicron anthracite particles, for example, 15%, 20%, 30%, 40%, 45%, 48%, 55%, 60%, or 65%. The asphalt accounts for 10%-50% of the mass percentage of the submicron anthracite particles, for example, 15%, 20%, 25%, 30%, 32%, 35%, 40%, or 45%.

[0013] In step (1), the reactants and solvent are generally mixed and formulated into a slurry before spray granulation. The solvent in the mixture containing submicron anthracite particles, phenolic resin, and asphalt can be conventional in the art, such as anhydrous ethanol. The ratio of the sum of the mass of the submicron anthracite particles, phenolic resin, and asphalt to the volume of the solvent can be (1-4) kg / L, for example, 1.5 kg / L, 2 kg / L, 2.25 kg / L, 2.5 kg / L, or 3 kg / L.

[0014] In step (1), the spray granulation is generally carried out in a spray dryer. During the spray granulation process, the inlet air temperature can be 160-220℃, for example 180℃, 190℃ or 200℃; the outlet air temperature can be 80-110℃, for example 90℃, 95℃ or 100℃; the spray pressure can be 0.1-0.4 MPa, for example 0.2 MPa or 0.3 MPa; the nozzle diameter can be 0.4-1mm, for example 0.5mm, 0.7mm or 0.8mm; and the feed rate can be 10-30 L / h, for example 15 L / h, 20 L / h or 25 L / h.

[0015] In step (1), after spray granulation, sieving is generally required. The particle size D of the granulated particles after sieving is... 50 The micrometer size can be 1-15 μm, preferably 3-10 μm. Drying is generally required before sieving.

[0016] In step (2), the organosilicon generally refers to an organosilicon compound that can generate silicon dioxide through hydrolysis or alcoholysis, preferably including one or more of tetraethyl orthosilicate, methyl orthosilicate and methyltriethoxysilane.

[0017] In step (2), the mass ratio of the granulated particles to the volume of the organosilicon can be (5-30) g / mL, for example, 8 g / mL, 10 g / mL, 12 g / mL, 13.6 g / mL, 15 g / mL, 20 g / mL or 25 g / mL; the mass ratio of the granulated particles to the volume of the solvent in the mixture containing the granulated particles, organosilicon and catalyst can be (0.5-1.5) g / mL, for example, 0.8 g / mL, 1 g / mL or 1.2 g / mL.

[0018] In step (2), the catalyst can be a conventional acid or alkaline solution, preferably an acid solution. The catalyst is preferably added dropwise.

[0019] The acid solution may be hydrochloric acid and / or acetic acid. The concentration of the hydrochloric acid may be 0.1-1 mol / L, for example 0.2 mol / L, 0.5 mol / L, or 0.8 mol / L. The alkaline solution may be ammonia. The volume ratio of the acid solution to the organosilicon may be 1:(5-15), for example 1:6, 1:7.3, 1:8, 1:10, or 1:12.

[0020] The solvent in the mixture containing the granulated particles, organosilicon and catalyst may be anhydrous ethanol and / or deionized water.

[0021] In some specific embodiments, the solvent in the mixture containing the granulated particles, organosilicon and catalyst is a mixture of anhydrous ethanol and deionized water in a volume ratio of (2-7):1 (e.g., 4:1, 5.5:1 or 6:1).

[0022] In step (2), the reaction is generally carried out under normal pressure. The temperature of the reaction can be 20-35℃, for example 25℃; the reaction time can be 4-12h, for example 6h or 8h; the reaction is generally carried out in a mixed state; the mixing method is generally stirring.

[0023] In step (2), solid-liquid separation, washing and drying are generally required after the reaction is completed.

[0024] In step (3), the carbonization is generally carried out in a tube furnace; the carbonization is generally carried out in an inert atmosphere. The carbonization temperature can be 600-900℃, for example 650℃, 700℃, 750℃, 800℃ or 850℃; the carbonization time can be 1.5-6h, for example 1.5h, 2h, 2.5h, 3h or 4h.

[0025] In step (4), the heating temperature can be 650-1000℃, for example 700℃, 750℃, 800℃, 820℃, 850℃, 900℃, or 950℃. The steam activation pore-forming can be carried out in a rotary kiln or a tube furnace. The steam activation pore-forming time can be 30-150 min, for example 45 min, 60 min, 75 min, 90 min, 100 min, or 120 min.

[0026] In step (4), during the process of water vapor activation and pore formation, the partial pressure of water vapor can be 15%-40%, for example 20%, 22.8%, 25% or 30%. The partial pressure of water vapor refers to the percentage of water vapor pressure in the total gas pressure inside the reactor. The total gas pressure inside the reactor is generally slightly higher than atmospheric pressure, preferably 0.102-0.11 MPa, for example 0.105 MPa or 0.108 MPa. The water vapor flow rate can be 0.5-3 g / min, for example 0.8 g / min, 1 g / min, 1.2 g / min, 1.5 g / min or 2 g / min.

[0027] In step (4), the process of activating pores with water vapor preferably includes the following steps: placing the porous silica-coated carbonized composite material in a reactor, heating it to the target heating temperature under inert gas protection, and then introducing water vapor to activate and create pores.

[0028] The water vapor can be introduced into the reaction system in a conventional manner in the art. For example, the feed rate of liquid water is first controlled by a precision metering pump to enter the vaporization chamber, and the liquid water is heated into stable saturated water vapor. Then, the steam flow rate is monitored in real time by a water vapor mass flow meter to ensure that it is introduced into the reaction system at a stable rate.

[0029] The inert gas can be conventional in the art, such as nitrogen. The flow rate of the inert gas can be 1000-3000 mL / min, for example 1500 mL / min, 2000 mL / min or 2500 mL / min.

[0030] The present invention also provides a high-strength porous carbon material with silica interface linkages prepared by the preparation method described above.

[0031] The present invention also provides an application of a high-strength porous carbon material with silica interface linkages as described above in a battery.

[0032] The present invention also provides a battery comprising a positive electrode, a negative electrode and an electrolyte, wherein the negative electrode comprises a high-strength porous carbon material with silicon oxide interface bonding as described above.

[0033] In this invention, the battery may be a sodium-ion battery.

[0034] Based on common knowledge in the field, the above-mentioned preferred conditions can be combined arbitrarily to obtain various preferred embodiments of the present invention.

[0035] The reagents and raw materials used in this invention are all commercially available.

[0036] The positive and progressive effects of this invention are as follows: The high-strength porous carbon material with silica interface linkage prepared by this invention has high mechanical strength and exhibits high initial efficiency and capacity, as well as excellent cycle stability when applied to sodium-ion batteries. Attached Figure Description

[0037] Figure 1 This is a scanning electron microscope image of the high-strength porous carbon material with silica interface bonding prepared in Example 1. Detailed Implementation

[0038] The present invention is further illustrated below by way of embodiments, but the invention is not limited to the scope of the embodiments described herein. Experimental methods in the following embodiments that do not specify specific conditions were performed according to conventional methods and conditions, or as selected according to the product instructions. Example 1

[0039] Step (1): Ultrafine grinding of raw materials: Industrial anthracite (Ningxia Rujigou standard anthracite) was selected as raw material. 5 kg of anthracite raw material was put into a horizontal sand mill (Shanghai Rujia, model RTSM-20) for wet sand grinding. Zirconia beads with a diameter of 0.7 mm were used as grinding media and ethanol was used as dispersion media. The mass ratio of ethanol to anthracite was 1:1, and the ball-to-material ratio (mass ratio of zirconia beads to anthracite) was 6:1. The sand milling speed was 2800 r / min and the sand milling time was 4 h. After sand milling, a high-speed centrifuge (Hunan Xiangyi TG16-WS) was used for solid-liquid separation. The separated filter cake was placed in a forced-air drying oven (Shanghai Yiheng DHG-9070A) and dried at 85℃ for 12 h to obtain the median particle size D. 50 Anthracite submicron particles with a diameter of 450 nm; Step (2): Preparation of composite matrix particles by spray granulation: Take 2.5 kg of the above-mentioned anthracite submicron particles, mix with 1.2 kg of phenolic resin (model PF-660, solid content ≥98%), 0.8 kg of medium-temperature asphalt (industrial grade, softening point 85℃, Shanxi Coking), add 2 L of anhydrous ethanol (analytical grade, Sinopharm), place in a magnetic stirrer (Beijing Saidekais SC-MS-I) and stir at room temperature for 2.5 h to form a uniform mixed suspension. Send the suspension to a spray granulator (Jiangsu Jinluyuan LPG-5 type) for spray granulation. Set the inlet air temperature to 190℃, the outlet air temperature to 95℃, the nozzle diameter to 0.7 mm, the spray pressure to 0.3 MPa, the feed rate to 20 L / h, and the hot air velocity to 2 m / s. After spraying, the material is vacuum dried at 85℃ for 6 h, and then the particle size D is collected by sieving. 50 Spray-granulated particles of 3-10 μm; Step (3): Surface silica coating modification: Weigh 3 kg of spray-granulated particles and disperse them in 2.5 L of anhydrous ethanol. Add 220 mL of tetraethyl orthosilicate (analytical grade, Aladdin reagent), 450 mL of deionized water, and 30 mL of dilute hydrochloric acid (0.5 mol / L, prepared with analytical grade hydrochloric acid) as hydrolysis catalyst. Stir the reaction in a sealed container at room temperature for 6 h. After the reaction is completed, filter the mixture, wash it three times with anhydrous ethanol, and dry it to obtain modified particles with a uniformly coated silicate hydrolysis film on the surface. Step (4): Carbonization treatment: The modified particles are spread evenly on an alumina crucible and placed in a tube furnace (Hefei Kejing OTF-1200X). High-purity nitrogen (purity 99.999%, Nanjing Special Gas) is introduced as a protective gas. The nitrogen flow rate is 60 mL / min. The temperature is raised to 750℃ at a rate of 5℃ / min. The carbonization is carried out at a constant temperature for 2.5 h. The mixture is then naturally cooled to room temperature to obtain a porous silica film-coated carbonized particle composite material. Step (5): Steam activation and pore formation: The composite material was placed in an atmosphere rotary furnace (Bangshida BJXG-66-10). High-purity nitrogen (99.999%) was introduced as a protective gas throughout the experiment. The nitrogen flow rate was set to 2000 mL / min. The furnace was kept at a normal pressure with a slight positive pressure (0.105 MPa) to ensure atmosphere stability and isolate it from the outside air. After heating to 820℃ at a heating rate of 5℃ / min, saturated steam was introduced for activation and pore formation. The constant steam flow rate was 1.2 g / min. The activation holding time was 90 min, and the steady-state steam partial pressure was maintained at 22.8%. After activation, the material was cooled to room temperature under a nitrogen atmosphere to finally obtain a high-strength porous carbon material with silica interface linkage. During the steam introduction process, the feed rate of liquid water was first controlled by a precision metering pump to enter the vaporization chamber and heated into stable saturated steam. The steam flow rate was then monitored in real time by a steam mass flow meter to ensure a stable introduction rate of 1.2 g / min. Example 2

[0040] Compared with Example 1, except that the amount of phenolic resin added in step (2) is adjusted to 0.5 kg, all other operations and conditions are the same as in Example 1. Example 3

[0041] Compared with Example 1, except that the amount of phenolic resin added in step (2) was adjusted to 1.5 kg, all other operations and conditions were the same as in Example 1. Example 4

[0042] Compared with Example 1, except that the amount of medium-temperature asphalt added in step (2) is adjusted to 0.5 kg, the other operations and conditions are the same as in Example 1. Example 5

[0043] Compared with Example 1, except that the amount of medium-temperature asphalt added in step (2) is adjusted to 1 kg, the other operations and conditions are the same as in Example 1. Example 6

[0044] Compared with Example 1, except that the amount of tetraethyl orthosilicate added in step (3) was adjusted to 150 mL, all other operations and conditions were the same as in Example 1. Example 7

[0045] Compared with Example 1, except that the amount of tetraethyl orthosilicate added in step (3) was adjusted to 300 mL, all other operations and conditions were the same as in Example 1. Example 8

[0046] Compared with Example 1, except that the carbonization temperature in step (4) is adjusted to 650°C, all other operations and conditions are the same as in Example 1. Example 9

[0047] Compared with Example 1, except that the carbonization temperature in step (4) is adjusted to 850°C, all other operations and conditions are the same as in Example 1. Example 10

[0048] Compared with Example 1, except that the carbonization time in step (4) is adjusted to 1.5h, all other operations and conditions are the same as in Example 1. Example 11

[0049] Compared with Example 1, except that the carbonization time in step (4) is adjusted to 4h, the other operations and conditions are the same as in Example 1. Example 12

[0050] Compared with Example 1, except that the activation temperature in step (5) is adjusted to 700°C, all other operations and conditions are the same as in Example 1. Example 13

[0051] Compared with Example 1, except that the activation temperature in step (5) is adjusted to 900°C, all other operations and conditions are the same as in Example 1. Example 14

[0052] Compared with Example 1, except that the activation time in step (5) is adjusted to 60 min, all other operations and conditions are the same as in Example 1. Example 15

[0053] Compared with Example 1, except that the activation time in step (5) is adjusted to 120 min, all other operations and conditions are the same as in Example 1.

[0054] Comparative Example 1 Compared with Example 1, except that phenolic resin is not added in step (2), all other operations and conditions are the same as in Example 1.

[0055] Comparative Example 2 Compared with Example 1, except that medium-temperature asphalt is not added in step (2), all other operations and conditions are the same as in Example 1.

[0056] Comparative Example 3 Compared with Example 1, except that step (3) is not performed, all other operations and conditions are the same as in Example 1.

[0057] Comparative Example 4 Compared with Example 1, except that step (5) is not performed, all other operations and conditions are the same as in Example 1. Effect Example

[0058] (1) Characterization of material properties Figure 1 This is a scanning electron microscope image of the high-strength porous carbon material with silica interface bonding prepared in Example 1.

[0059] The high-strength porous carbon materials with silica interface linkages prepared in Examples 1-15 and Comparative Examples 1-4 were tested using an ASAP2020 surface area and pore size analyzer. The test results are shown in Table 1.

[0060] (2) Electrochemical performance testing Negative electrode preparation: The high-strength porous carbon materials with silicon oxide interface bonding prepared in Examples 1-15 and Comparative Examples 1-4 were subjected to half-cell tests. The test method was as follows: hard carbon material, superconducting carbon black (SuperP), and PVDF were prepared in a mass ratio of 8:1:1, uniformly mixed using a homogenizer, and then coated onto a copper foil current collector and dried overnight in a vacuum oven at 90°C. Subsequently, the obtained electrode was cut into circular battery electrode sheets with a diameter of 12 mm for later use, with an average mass loading of 2 mg / cm². -2 .

[0061] The sodium-ion battery uses a sodium metal sheet as the counter electrode, a single layer of glass fiber as the separator, and a nickel foam disc. The electrolyte is a 1M NaPF6 diethylene glycol dimethyl ether solution. After assembly, the battery was allowed to stand for 8 hours for aging. Constant current charge / discharge tests were performed on a LAND CT2001A battery testing system at 1C = 1000 mAh / g, with a voltage range of 0.001 to 3.0 Vvs. Na / Na + The test results are shown in Table 1: Table 1

[0062] As shown in Table 1, the high-strength porous carbon material with silica interface linkage prepared in this invention has a high specific surface area and exhibits high specific capacity and excellent cycle stability when applied to sodium-ion batteries.

[0063] While specific embodiments of the present invention have been described above, those skilled in the art should understand that these are merely illustrative examples, and the scope of protection of the present invention is defined by the appended claims. Those skilled in the art can make various changes or modifications to these embodiments without departing from the principles and essence of the present invention, but all such changes and modifications fall within the scope of protection of the present invention.

Claims

1. A method for preparing a high-strength porous carbon material with silica interface bonding, characterized in that, Includes the following steps: (1) A mixture containing submicron anthracite particles, phenolic resin and asphalt is spray-granulated to obtain granulated particles; (2) The mixture containing the granulated particles, organosilicon and catalyst is reacted to obtain modified particles with an organosilicon hydrolysis film coated on the surface. (3) The modified particles coated with the organosilicon hydrolysis film on the surface are carbonized to obtain a porous silica-coated carbonized composite material. (4) The porous silica-coated carbonized composite material is activated by steam under heating to create pores, thereby obtaining a high-strength porous carbon material with silica interface linkage.

2. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, In step (1), the particle size D of the submicron anthracite particles 50 The range is 100nm-1000nm, preferably 200-800nm, such as 300nm, 400nm, 450nm, 500nm, 600nm or 700nm; And / or, in step (1), the method for preparing the submicron anthracite particles includes the following steps: grinding and pulverizing the anthracite raw material.

3. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, Step (1) satisfies one or more of the following conditions: (1) The phenolic resin accounts for 10%-70% of the mass of the submicron anthracite particles, for example, 15%, 20%, 30%, 40%, 45%, 48%, 55%, 60% or 65%; (2) The asphalt accounts for 10%-50% of the mass of the submicron anthracite particles, for example, 15%, 20%, 25%, 30%, 32%, 35%, 40% or 45%; (3) Before spray granulation, the reactants and solvents need to be mixed and prepared into a slurry; (4) The solvent in the mixture containing submicron anthracite particles, phenolic resin and asphalt is anhydrous ethanol; (5) The ratio of the sum of the mass of the submicron anthracite particles, phenolic resin and asphalt to the volume of the solvent is (1-4) kg / L, for example 1.5 kg / L, 2 kg / L, 2.25 kg / L, 2.5 kg / L or 3 kg / L.

4. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, Step (1) satisfies one or more of the following conditions: (1) During the spray granulation process, the air inlet temperature is 160-220℃, for example 180℃, 190℃ or 200℃; (2) During the spray granulation process, the outlet air temperature is 80-110℃, for example 90℃, 95℃ or 100℃; (3) During the spray granulation process, the spray pressure is 0.1-0.4 MPa, for example 0.2 MPa or 0.3 MPa; (4) During the spray granulation process, the feed rate is 10-30 L / h, for example 15 L / h, 20 L / h or 25 L / h; (5) After the spray granulation is completed, sieving is required; the particle size D of the granulated particles after sieving is... 50 The preferred size is 1-15 μm, and the more preferred size is 3-10 μm.

5. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, Step (2) satisfies one or more of the following conditions: (1) The organosilicon includes one or more of tetraethyl orthosilicate, methyl orthosilicate and methyltriethoxysilane; (2) The ratio of the mass of the granulated particles to the volume of the organosilicon is (5-30) g / mL, for example, 8 g / mL, 10 g / mL, 12 g / mL, 13.6 g / mL, 15 g / mL, 20 g / mL or 25 g / mL; (3) The ratio of the mass of the granulated particles to the volume of the solvent in the mixture containing the granulated particles, organosilicon and catalyst is (0.5-1.5) g / mL, for example 0.8 g / mL, 1 g / mL or 1.2 g / mL; (4) The catalyst is an acid solution or an alkaline solution, preferably an acid solution; Preferably, the acid solution is hydrochloric acid and / or acetic acid; the concentration of the hydrochloric acid is preferably 0.1-1 mol / L, for example 0.2 mol / L, 0.5 mol / L or 0.8 mol / L; the volume ratio of the acid solution to the organosilicon is preferably 1:(5-15), for example 1:6, 1:7.3, 1:8, 1:10 or 1:12; the solvent in the mixture containing the granulated particles, organosilicon and catalyst is preferably anhydrous ethanol and / or deionized water.

6. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, The preparation method satisfies one or more of the following conditions: (1) In step (2), the reaction temperature is 20-35℃, for example 25℃; (2) In step (2), the reaction time can be 4-12 hours, for example 6 hours or 8 hours; (3) In step (3), the carbonization temperature is 600-900℃, for example 650℃, 700℃, 750℃, 800℃ or 850℃; (4) In step (3), the carbonization time is 1.5-6h, for example 1.5h, 2h, 2.5h, 3h or 4h.

7. The method for preparing high-strength porous carbon material with silica interface bonding as described in claim 1, characterized in that, Step (4) satisfies one or more of the following conditions: (1) The heating temperature is 650-1000℃, for example 700℃, 750℃, 800℃, 820℃, 850℃, 900℃ or 950℃; (2) The time for water vapor activation to form pores is 30-150 min, for example 45 min, 60 min, 75 min, 90 min, 100 min or 120 min; (3) During the process of water vapor activation and pore formation, the partial pressure of water vapor is 15%-40%, for example, 20%, 22.8%, 25% or 30%; (4) During the process of water vapor activation and pore formation, the water vapor flow rate is 0.5-3 g / min, for example 0.8 g / min, 1 g / min, 1.2 g / min, 1.5 g / min or 2 g / min; (5) The process of water vapor activation and pore formation includes the following steps: placing the porous silica-coated carbonized composite material in a reactor, heating it to the target heating temperature under inert gas protection, and then introducing water vapor for activation and pore formation.

8. A high-strength porous carbon material with silica interface linkage prepared by a method for preparing a high-strength porous carbon material with silica interface linkage as described in any one of claims 1-7.

9. The application of a high-strength porous carbon material with silica interface bonding as described in claim 8 in a battery.

10. A battery comprising a positive electrode, a negative electrode, and an electrolyte, wherein the negative electrode comprises a high-strength porous carbon material with silicon oxide interfacial bonding as claimed in claim 10.

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