WO2025251852A1 - 一种用于形成耐压无溢胶自粘结涂层的涂料、硅钢及电机铁心 - Google Patents

一种用于形成耐压无溢胶自粘结涂层的涂料、硅钢及电机铁心

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Publication number
WO2025251852A1
WO2025251852A1 PCT/CN2025/094624 CN2025094624W WO2025251852A1 WO 2025251852 A1 WO2025251852 A1 WO 2025251852A1 CN 2025094624 W CN2025094624 W CN 2025094624W WO 2025251852 A1 WO2025251852 A1 WO 2025251852A1
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WO
WIPO (PCT)
Prior art keywords
coating
silicon steel
epoxy resin
motor core
inorganic particulate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
PCT/CN2025/094624
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English (en)
French (fr)
Inventor
李国保
李登峰
王妮
王波
王志成
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Baoshan Iron and Steel Co Ltd
Original Assignee
Baoshan Iron and Steel Co Ltd
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Filing date
Publication date
Application filed by Baoshan Iron and Steel Co Ltd filed Critical Baoshan Iron and Steel Co Ltd
Publication of WO2025251852A1 publication Critical patent/WO2025251852A1/zh
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D1/00—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D163/00—Coating compositions based on epoxy resins; Coating compositions based on derivatives of epoxy resins
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
    • C09D7/40—Additives
    • C09D7/60—Additives non-macromolecular
    • C09D7/61—Additives non-macromolecular inorganic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/18—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances
    • H01B3/30—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02K—DYNAMO-ELECTRIC MACHINES
    • H02K1/00—Details of the magnetic circuit
    • H02K1/06—Details of the magnetic circuit characterised by the shape, form or construction
    • H02K1/12—Stationary parts of the magnetic circuit

Definitions

  • This disclosure relates to a coating, silicon steel, and motor core, and more particularly to a coating, silicon steel, and motor core for use in self-adhesive coatings.
  • Self-bonded laminated cores are prone to adhesive overflow during hot-pressing curing, especially under the following process conditions: large coating thickness, high curing pressure, high temperature and/or long holding time.
  • the thickness of the silicon steel substrate used for self-adhesive coatings in mass production is generally between 0.35 and 0.65 mm, while the thickness of high-grade silicon steel substrates is usually less than or equal to 0.30 mm, and the thickness of silicon steel substrates used in drive motors is generally between 0.20 and 0.27 mm.
  • the thinner the substrate the higher the proportion of coating within the unit core, and the more prone it is to glue overflow during hot pressing. Therefore, it is necessary to optimize the coating formulation and its production process to enhance the glue-free performance of the coated products.
  • silicon steel laminated cores typically require a high stacking factor during manufacturing.
  • the core is prone to axial expansion.
  • the degree of expansion is aggravated by the greater the pressure applied during the initial hot pressing, the thinner the substrate, and the thicker the coating. This also makes it difficult to control the dimensional consistency between different batches, thus affecting the core performance.
  • the self-adhesive coating absorbs some of the pressure as an elastomer during the first hot pressing process, and shrinks as a whole after the physical bonding between the sheets is achieved and the curing reaction is completed.
  • the core is heated again without pressure constraint, the residual stress in the coating is released, causing the axial dimension of the core to elastically rebound and expand.
  • One of the objectives of this disclosure is to provide an improved coating that, by introducing effective inorganic particulate matter into a conventional purely organic self-adhesive coating system, enhances coating stiffness and reduces coating elasticity, achieving pressure resistance without adhesive overflow, and ensuring excellent bond strength and coating processability.
  • the coating of this invention is particularly suitable for forming self-adhesive coatings with pressure resistance and no adhesive overflow.
  • the effective components of the coating include an organic component and an inorganic particulate component.
  • the organic component includes an epoxy resin and an epoxy resin curing agent.
  • the epoxy resin includes macromolecular epoxy resin and small molecule epoxy resin.
  • the inorganic particulate component includes nano-sized fumed oxide particles and nano-sized silica particles.
  • the organic component has a mass percentage content of 86% to 99% in the effective components, preferably 90% to 99%, more preferably 94% to 99%, and most preferably 96% to 99%.
  • the effective components of the coating disclosed herein consist of the aforementioned organic components and the aforementioned inorganic particulate components.
  • macromolecular epoxy resin refers to epoxy resin with an epoxy equivalent of 1500 to 10000 g/eq.
  • small molecule epoxy resin refers to epoxy resin with an epoxy equivalent of 100 to 1000 g/eq.
  • the macromolecular epoxy resin undergoes endothermic stretching during heating and shrinking during cooling through its chain groups, thereby forming effective physical entanglement between the layers and enhancing adhesion.
  • the small-molecule epoxy resin undergoes an exothermic reaction during film formation and forms a secondary cross-linked structure with the macromolecular epoxy resin, improving the rigidity and adhesion strength of the coating.
  • the epoxy groups combine with functional groups in the curing agent during the ring-opening reaction, enhancing the mechanical strength and corrosion resistance of the coating.
  • the surface of the nano-sized fumed oxide particles in the inorganic particulate component possesses a large number of highly reactive hydroxyl groups.
  • These particles along with organic film-forming agents containing polar groups such as amine and hydroxyl groups in the coating, can form a three-dimensional flocculated network structure through hydrogen bonds and van der Waals forces, thereby enhancing the adhesion toughness and structural stability of the coating and helping to suppress adhesive overflow during hot-pressing curing.
  • the introduction of such particles can also lead to a decrease in the compatibility of the coating system, manifested as increased coating viscosity and easy surface skinning. If commercially available fumed oxide powder is used directly and dispersed in the coating, it may be difficult to improve the adhesion strength of the self-adhesive coating and result in significant coating skinning, precipitation, and other unstable phenomena.
  • nano-sized silica particles are further introduced into the coating disclosed herein. These particles can fill the intermolecular gaps in the coating, improving the density and rigidity of the coating; the long carbon chains of the modifier can form steric hindrance, improving the compatibility and stability between the inorganic dispersion and the coating system, thereby significantly reducing the viscosity of the coating, increasing the coating's wetting ability on the silicon steel substrate, and improving the coating processing performance.
  • the epoxy equivalent of the macromolecular epoxy resin is 1500 to 10000 g/eq.
  • the epoxy equivalent of the small molecule epoxy resin is 100 to 1000 g/eq.
  • the small molecule epoxy resin has a mass percentage content of 15-30% in the organic components.
  • the epoxy resin curing agent has a mass percentage content of 2-8% in the organic components.
  • the epoxy resin may be one type of epoxy resin, such as bisphenol A, bisphenol F or phenolic epoxy resin, preferably selected from two or more of bisphenol A, bisphenol F and phenolic epoxy resin.
  • the gaseous oxide particles may be selected from at least one of SiO2 , Al2O3 , TiO2 , ZnO, and ZrO2 .
  • the epoxy resin curing agent is selected from one or more of amine, acid anhydride, and resin curing agents.
  • the median particle size D50 of the fumed oxide particles is 7-40 nm, and the specific surface area is 50-300 m2 /g.
  • fumed oxide particles are mixed with organic components in the coating and act like rivets during the manufacturing process of motor cores, thereby enhancing the toughness and adhesion of the coating.
  • the particle size and specific surface area of the fumed oxide particles need to be reasonably controlled.
  • the median particle size D50 of the fumed oxide particles is too small, their specific surface area increases significantly.
  • the mutual attraction of surface charges leads to agglomeration, reducing surface energy and inhibiting the thermal motion of the particle molecular chains. This hinders the formation of a network structure by the organic film-forming substances, resulting in a decrease in the adhesion strength of the coating.
  • the median particle size D50 of the fumed oxide particles is too large, it easily causes the coating volume to shrink, resulting in poor wetting and spreading properties of the coating, and ultimately, unevenly distributed circular spot defects appear on the surface of the coated steel plate. Therefore, in the coating of this invention, it is preferable to control the median particle size D50 of the fumed oxide particles in the range of 7–40 nm and the specific surface area in the range of 50–300 m2 /g.
  • the particle size of the silica particles is 8-12 nm.
  • the SiO2 sol particles in the coating are too small, a large number of microbubbles are introduced during high-speed dispersion. During subsequent coating and heat treatment, the bursting of these bubbles can cause burr-like protrusions on the sample surface, increasing the brittleness of the coating and thus deteriorating its adhesive strength. Conversely, if the SiO2 sol particles in the coating are too large, the specific surface area decreases, preventing the modifier from fully contacting the particle surface to form an adhesion layer. Simultaneously, as the particle size increases, the total potential energy decreases, and Brownian motion between particles will cause spontaneous gel formation, making the coating prone to precipitation and sedimentation. Therefore, in the coating of this invention, the particle size of the silica particles is controlled to be 8-12 nm.
  • the mass percentage of the gaseous oxide particles in the inorganic particulate matter component is not particularly limited, but is preferably 12.5 to 75.0%, more preferably 20 to 50%, more preferably 35.0 to 50%, and most preferably 35.0 to 42.5%.
  • the higher the mass percentage of fumed oxide particles in the inorganic particulate matter component the better the effect on improving the coating adhesion.
  • excessively high content can lead to reduced storage stability of the coating, deterioration of coating processing performance, and increased susceptibility to coating defects. Therefore, in the coating of the present invention, it is preferable to control the mass percentage of fumed oxide particles in the inorganic particulate matter component to be 12.5% to 75.0%, more preferably to be 20% to 50%.
  • the median particle size D50 of the inorganic particulate component is not particularly limited, but is preferably 11-53 ⁇ m, more preferably 25-45 ⁇ m.
  • the coarse-end particle size D90 is not particularly limited, but is preferably 45-134 ⁇ m, more preferably 60-100 ⁇ m.
  • Another objective of this disclosure is to provide a silicon steel that, while ensuring the basic properties of self-adhesive coatings such as bonding strength and insulation, can withstand high pressure and has no glue overflow during hot pressing of laminated iron cores, thus enabling the manufacture of high-efficiency iron cores with high stacking coefficients.
  • this disclosure provides a silicon steel comprising a silicon steel substrate and a coating formed by the aforementioned coating material applied to the surface of the silicon steel substrate.
  • the coating material is formed by applying the coating material of the present invention to the surface of the silicon steel substrate and baking and heating the coated silicon steel substrate.
  • the thickness of the silicon steel substrate is ⁇ 0.65mm.
  • the thickness of the silicon steel substrate is 0.15 to 0.3 mm.
  • the single-sided dry film thickness of the coating is 0.5 to 5.0 ⁇ m.
  • Another object of this disclosure is to provide a high-adhesion motor core with a high stacking factor, which exhibits no glue overflow in the coating when subjected to hot pressing at 0.5 to 10 MPa and has a high adhesion strength of ⁇ 2 N/mm.
  • this disclosure provides an electric motor core made of silicon steel of the present invention.
  • the stacking coefficient F% of the motor core of the present invention is (98-0.06 ⁇ h/H+0.23 ⁇ P)%; where P represents the pressure between the stacked silicon steel sheets (inter-sheet pressure), in MPa; H represents the thickness of the silicon steel substrate, in mm; and h represents the sum of the dry film thicknesses of the double-sided coating on each silicon steel sheet, in ⁇ m.
  • the stacking factor of the motor core of the present invention is ⁇ 97%.
  • the motor core of the present invention does not overflow glue when subjected to hot pressing at 0.5 to 10 MPa.
  • the bonding strength of the coating of the motor core of the present invention is ⁇ 2N/mm, preferably ⁇ 3N/mm, when subjected to hot pressing at 0.5 to 10MPa.
  • the coating, silicon steel, and motor core of the present invention have the following advantages and beneficial effects:
  • the coating of this invention can be used to form a self-adhesive coating on the surface of silicon steel sheets. While ensuring the basic properties of self-adhesive coatings such as bonding strength and insulation, it also possesses good pressure resistance and adhesive overflow control. This coating can withstand high pressure without adhesive overflow during hot pressing of laminated iron cores, enabling the manufacture of high-efficiency iron cores with a high stacking factor, and has significant practical value.
  • the motor core of the present invention When the motor core of the present invention is subjected to hot pressing at 0.5 to 10 MPa, no glue overflow occurs in the coating, and more preferably, it can exhibit a high bonding strength of ⁇ 2 N/mm.
  • the coating of this invention can stably achieve a stacking factor of ⁇ 97% for the resulting coated silicon steel laminated core. It is particularly suitable for high-viscosity, non-overflowing, and high-stacking-factor self-adhesive coating products on thin-gauge silicon steel substrates, enabling better manufacturing and utilization of the application advantages of high-efficiency motor cores.
  • Figure 1 shows the trend of the bonding strength of the coating of the motor core of the present invention with the change of the content ratio of organic or inorganic components in the coating.
  • Figure 2 shows the trend of the bonding strength of the coating of the motor core of the present invention with the change of the content of gas phase oxide particles in the coating.
  • Figure 3 shows the variation trend of the stacking coefficient F of the motor core of the present invention under different pressure conditions between silicon steel sheets.
  • the “active ingredient” of a coating refers to the substance that directly participates in the formation of the coating and imparts functionality to it in the formulation, as opposed to solvents, dispersion media or other inert substances.
  • the epoxy equivalent can be determined by conventional methods in the art, such as in accordance with GB/T 4612-2008.
  • the median particle size D50 refers to the particle size value corresponding to a cumulative distribution percentage of 50% in the particle size distribution, which can be determined by conventional methods in the field, such as laser particle size analysis.
  • coarse-end particle size D90 refers to the particle size value corresponding to a cumulative distribution percentage of 90% in the particle size distribution, which can be determined by conventional methods in the field, such as laser particle size analysis.
  • the single-sided dry film thickness of the coating refers to the coating thickness formed on a single surface after drying or curing.
  • the stacking factor F of the motor core refers to the ratio between the actual core height after pressing and the theoretical total thickness of all metals, which is determined according to GB/T 19289 (or IEC 60404-13) standard.
  • no excess adhesive in motor core refers to the phenomenon that the coating does not overflow, flow, or spill onto the outside of the core during the hot pressing process of motor core manufacturing.
  • the bond strength of the coating on the motor core is determined according to DIN EN 1464.
  • Tables 1-1, 1-2 and 1-3 list the mass fractions and mass ratios of each component in the coatings used in Examples 1-13 and the comparative coatings used in Comparative Example 1.
  • the inorganic particulate component in the coating is a dispersion suspension obtained by dispersing two types of nanoparticles with different properties: hydrophilic fumed oxide powder and silica sol.
  • the preparation process is as follows:
  • Step 1 Hydrophilic gaseous oxide powder is prepared using a high-temperature hydrolysis method with an oxyhydrogen flame.
  • the gaseous oxide is selected from metal oxides such as SiO2 , Al2O3 , TiO2 , ZnO, and ZrO2 .
  • the particle size of the gaseous oxide is controlled by adjusting the amount of metal halide additives, ensuring that the ratio of halide to hydrogen and air is within the range of 1:(0.3–1.7):(8–20).
  • the gas velocity at the nozzle in the hydrolysis furnace is 5–15 m/s; the furnace temperature is 1000–1800°C; the cooling medium temperature is 70–110°C; and the dispersion solvent, in addition to pure water, can be two or more mixtures of ethylene glycol, glycerol, n-butanol, isobutanol, isopropanol, and ethylene glycol methyl ether.
  • gaseous oxide particles with a median particle size D50 of 7–40 nm, a specific surface area of 50–300 m2 /g, and hydrophilic groups such as -OH hydroxyl groups on the particle surface are prepared.
  • Step 2 Preparation of silica sol using the sol-gel method. Silicon-based tetraethyl orthosilicate, alcohol, and distilled water were added to a flask at a volume ratio of 15:(110–320):10. The oil bath temperature was set to 70°C and the stirring speed to 150 rpm. Then, 0.5–3% (v/v) of surfactant was added, and stirring was continued to obtain a relatively clear microemulsion. Next, an alkaline catalyst (v/v) of 10–25 was added dropwise over 5 minutes. After 1.5–2 hours, the emulsion became clear and transparent, and the reaction was complete. The product was centrifuged and washed with distilled water. Then, the silica sol was surface-modified using a modifier under ultrasonic conditions, ultimately obtaining a SiO2 particle size of 10 ⁇ 2 nm in the silica sol.
  • the alkaline catalyst can control the particle size in the sol, and amines and ammonia can be selected;
  • the alcohol can be methanol, ethanol, propanol, or pentanol;
  • the surfactant inhibits the rapid growth of particles to obtain nano-sized silica sol, and ammonium chloride or sodium dodecylbenzene sulfonate can be selected;
  • the modifier can be fatty alcohol, amine, fatty acid, or siloxane.
  • Step 3 Add the aforementioned gaseous oxide powder into SiO2 sol. If necessary, add a certain amount of pure water and additives to adjust the solid content of the mixture to 5-30%. Disperse the mixture for 60-180 minutes at a shear rate of 7-25 m/s. During the process, an ice bath is required to control the liquid temperature to ⁇ 40°C to obtain the final form of inorganic particle dispersion suspension.
  • the above-mentioned coating is applied to both sides of a silicon steel substrate with a thickness of 0.15-0.65 mm, and the dry film thickness on each side is controlled between 0.5-5.0 ⁇ m.
  • the coating liquid is applied to the surface of B25AV1300 high-grade silicon steel sheet/coil using a two-roll or three-roller coating machine, and cured by baking in an open flame oven or infrared drying oven to obtain silicon steel sheet.
  • the dry film thickness on each side can preferably be controlled between 1-3 ⁇ m.
  • the production speed of the coated strip can be controlled between 80-200 mpm, the corresponding baking heating time can be controlled between 18-45 s, and the temperature of the coated steel sheet can be controlled between 210-280°C.
  • silicon steel is stacked into a core, which is then hot-pressed and cured in a tooling fixture to obtain a shaped core.
  • the inter-laminate pressure load can be controlled between 0.5 and 10 MPa, and the core is held at 160–250°C for 10–240 minutes.
  • Table 2 lists the relevant process parameters of the motor cores of Examples 1-13 and the comparative motor core of Comparative Example 1 in the above manufacturing process.
  • the motor cores of Examples 1-13 and the comparative motor core of Comparative Example 1 were subjected to performance tests, including testing the adhesion strength of their coatings, stacking factor, and excess adhesive during hot pressing.
  • the test results are listed in Table 3.
  • the specific test methods are as follows:
  • Coating adhesion strength The adhesion strength of the motor cores of Examples 1-13 and the control motor core of Comparative Example 1 was tested according to DIN EN 1464.
  • Glue overflow test Observe whether glue overflows when the motor core is subjected to hot pressing at 0.5-10MPa.
  • Stacking factor The stacking factor is determined according to GB/T 19289 (or IEC 60404-13) standard.
  • Stacking factor F% (98 - 0.06 ⁇ h / H + 0.23 ⁇ P)%; where P represents the pressure between the laminated silicon steel sheets, in MPa; H represents the thickness of the silicon steel substrate, in mm; and h represents the sum of the dry film thicknesses of the double-sided coating on each silicon steel sheet, in ⁇ m.
  • Table 3 lists the relevant performance test results of the motor cores of Examples 1-13 and the comparative motor core of Comparative Example 1.
  • Figure 1 shows the trend of the bonding strength of the coating of the motor core of the present invention with the change of the content ratio of organic or inorganic components in the coating.
  • Figure 1 shows coatings with different organic component ratios (fixed fumed oxide particles account for 35-40% of the total inorganic particulate matter) applied to the surface of B25AV1300 high-grade silicon steel coils.
  • the coatings were then cured in a single baking process using an open flame oven or infrared drying oven at 210-280°C to obtain coated silicon steel samples in state B, with the dry film thickness on each surface controlled at 2.5 ⁇ m.
  • Coated steel sheet laminate samples were prepared according to the DIN EN 1464 bond strength test standard and subjected to a second hot-press curing process to obtain coated samples in state C.
  • the state C hot-pressing process involved an inter-sheet load pressure of 3 MPa and a holding time of 200°C for 60 min.
  • the figure shows that a coating with a certain bond strength can be obtained when the organic component ratio in the coating is ⁇ 90%, with the highest bond strength at 96%. Considering both bond performance and adhesive overflow, an organic component ratio of 90-99% is optimal.
  • the motor cores prepared in Examples 1-13 did not have any glue overflow when subjected to hot pressing at 0.5 to 10 MPa.
  • Figure 2 shows the trend of the bonding strength of the coating of the motor core of the present invention with the change of the content of gas phase oxide particles in the coating.
  • the coating adhesion performance gradually improves with the increase of the mass percentage of fumed oxide particles in the inorganic particulate matter component. Therefore, in a more preferred embodiment, the mass percentage of fumed oxide particles in the inorganic particulate matter component is controlled to be 20-50%.
  • the mass percentage of fumed oxide particles in the inorganic particulate matter component is lower than this range, therefore its adhesion strength is slightly inferior to that of Examples 1-10.
  • the mass percentage of fumed oxide particles in the inorganic particulate matter component is higher than this range; excessively high fumed oxide particle content may degrade the storage stability of the coating.
  • Example 11 does not meet the preferred embodiment of this disclosure, and its bonding strength is slightly inferior to that of Examples 1-10.
  • Figure 3 shows the variation trend of the stacking coefficient F of the motor core of the present invention under different pressure conditions between silicon steel sheets.
  • the thinner the substrate the smaller the stacking factor of the laminated steel blocks.
  • the laminated core can achieve a high stacking factor of ⁇ 97%.

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Abstract

本发明涉及一种用于形成耐压无溢胶自粘结涂层的涂料，其溶剂为水，其有效成分包含有机组分和无机颗粒物组分，有机组分包含环氧树脂以及环氧树脂固化剂；环氧树脂包含大分子环氧树脂和小分子环氧树脂；无机颗粒物组分包含纳米级的气相氧化物颗粒和纳米级的二氧化硅颗粒；有机组分在有效成分中的质量百分含量为90～99％。本发明还涉及一种硅钢，其包含硅钢基材和涂覆在硅钢基材表面上由所述涂料形成的涂层。本发明还涉及一种高叠装系数的高粘结性电机铁心，其由上述硅钢制得。

Description

一种用于形成耐压无溢胶自粘结涂层的涂料、硅钢及电机铁心 技术领域
本公开涉及一种涂料、硅钢及电机铁心，尤其涉及一种用于自粘结涂层的涂料、硅钢及电机铁心。
背景技术
自粘结叠层铁心在热压固化过程中存在易发生溢胶的问题，尤其在以下工艺条件下更为明显：涂层膜厚较大、固化压强较高、温度较高和/或保压时间较长。
目前批量生产中所用自粘结涂层适配的硅钢基材厚度一般在0.35～0.65mm之间，而高等级硅钢基材厚度通常小于或等于0.30mm，驱动电机用硅钢基材厚度一般在0.20～0.27mm之间。在其他工艺参数大致相同的条件下，基材越薄，单位铁心内涂层所占比例越高，越容易在热压成型过程中出现溢胶现象。因此，需要优化涂层配方及其生产工艺，强化涂层产品的无溢胶性能。
此外，为提高电机运行效率，硅钢叠层铁心在制造成型过程中通常需实现较高的叠装系数。然而，硅钢基材越薄，所需涂层厚度相对越高，往往会导致叠装系数下降。
在现有技术中，提高叠装系数的常用方式是增加固化压力。铁心经过一次热压固化成型后，轴向尺寸会发生一定程度的收缩，该收缩通常较小且较为可控，可通过提前设定散片堆叠高度或总重量加以补偿，满足最终尺寸要求。
然而，部分扁线电机铁心在热压固化后仍需对轴向两端面进行滴漆处理，以增强端面绝缘性能。该滴漆的固化工艺通常需在150～200℃下加热30～60min，相当于对铁心进行了二次加热。
由于在二次加热过程中铁心轴向两端既未施加压力也未设置限位约束，铁心容易发生轴向尺寸膨胀现象。且膨胀程度会随着一次热压给压越大、基材越薄、涂层越厚而加剧，同时也导致不同批次间尺寸一致性难以控制，进而影响铁心性能。
产生这一现象的原因在于：自粘结涂层在第一次热压过程中作为弹性体材料吸收了部分压力，在实现片间物理贴合并完成固化反应后整体发生收缩。当铁心再次加热而无压力约束时，涂层中的残余应力被释放，导致铁心轴向尺寸发生弹性回弹膨胀。
发明内容
本公开的目的之一在于提供一种改进的涂料，该涂料通过在传统的纯有机体系的自粘结涂料中引入有效的无机颗粒物，增强了涂层刚度并降低了涂层弹性，实现了产品耐压无溢胶、且保证了优良的粘结强度和涂布加工性能。本发明的涂料特别适用于形成具有耐压无溢胶性能的自粘结涂层。
为了实现上述目的，本公开提供了一种涂料，其溶剂为水，所述涂料的有效成分包含有机组分和无机颗粒物组分，所述有机组分包含环氧树脂以及环氧树脂固化剂，所述环氧树脂包含大分子环氧树脂和小分子环氧树脂，所述无机颗粒物组分包含纳米级的气相氧化物颗粒和纳米级的二氧化硅颗粒，所述有机组分在所述有效成分中的质量百分含量为86～99％，优选90～99％，更优选94％～99％，最优选96％～99％。
优选地，本公开涂料的有效成分由上述有机组分和上述无机颗粒物组分组成。
在本公开中，大分子环氧树脂是指环氧当量为1500～10000g/eq的环氧树脂。
在本公开中，小分子环氧树脂是指环氧当量为100～1000g/eq的环氧树脂。
在本公开中，大分子环氧树脂通过其链状基团在加热过程中发生吸热伸展，在冷却过程中收缩，从而在片层之间形成有效的物理缠结，增强粘结力；小分子环氧树脂在成膜过程中发生放热反应，并与大分子环氧树脂形成二次交联结构，提高了涂层的刚性和粘结强度。此外，环氧基团在开环反应中与固化剂中的官能团结合，增强了涂层的机械强度和耐腐蚀性。
此外，在本公开的涂料中，无机颗粒物组分中的纳米级气相氧化物颗粒的表面存在大量活性较高的羟基。这些颗粒与涂料中含有胺基、羟基等极性基团的有机成膜物可通过氢键和范德华力形成三维絮凝网状结构，从而增强涂层的粘结韧性和结构稳定性，有助于抑制热压固化过程中的溢胶现象。然而，该类颗粒的引入也会造成涂料体系的相容性下降，表现为涂料粘稠度增高和表面易结皮的问题。若直接使用市售的气相氧化物粉末并将其分散于涂料中，可能难以提升自粘结涂层的粘结强度，且导致明显的涂料结皮、析出等不稳定现象。
为克服上述问题，本公开的涂料中进一步引入了纳米级的二氧化硅颗粒。该类颗粒可填充涂料中的分子间空隙，提高涂层的致密性和刚度；改性剂的长碳链可形成空间位阻，提升无机分散体与涂料体系的相容稳定性，从而显著降低涂料的粘稠度，增加涂料对硅钢基板的浸润能力，提高涂布加工性能。
优选地，在本发明的涂料中，所述大分子环氧树脂的环氧当量为1500～10000g/eq。
优选地，在本发明的涂料中，所述小分子环氧树脂的环氧当量为100～1000g/eq。
优选地，在本发明的涂料中，所述小分子环氧树脂在有机组分中的质量百分含量为15～30％。
优选地，在本发明的涂料中，所述环氧树脂固化剂在有机组分中的质量百分含量为2～8％。
在本发明的涂料中，所述环氧树脂可使用一种类型的环氧树脂，例如双酚A、双酚F或酚醛环氧树脂，优选选自双酚A、双酚F、酚醛环氧树脂中的两种以上。
优选地，在本发明的涂料中，所述气相氧化物颗粒可以选自SiO2、Al2O3、TiO2、ZnO、ZrO2中的至少一种。
优选地，在本发明的涂料中，所述环氧树脂固化剂选自胺类、酸酐类、树脂类固化剂中的一种或多种。
优选地，在本发明的涂料中，所述气相氧化物颗粒的中值粒径D50为7～40nm，比表面积为50～300m2/g。
在本公开中，气相氧化物颗粒在涂料中与有机组分混合，在电机铁心制造过程中起到类似铆钉的作用，从而增强涂层的韧性和粘结性。为了确保其增强效果，需合理控制气相氧化物颗粒的粒径和比表面积。当气相氧化物颗粒的中值粒径D50过小时，其比表面积显著增大，颗粒表面电荷相互吸引导致团聚，表面能降低，会抑制胶粒分子链的热运动，妨碍有机成膜物质形成网状结构，导致涂层的粘结强度降低。相反，当气相氧化物颗粒的中值粒径D50过大时，容易引起涂膜体积收缩，导致涂料的润湿铺展性不佳，最终涂层钢板表面出现不均匀分布的圆斑状缺陷。因此，在本发明的涂料中，优选将气相氧化物颗粒的中值粒径D50控制在7～40nm范围内，比表面积控制在50～300m2/g范围内。
此外，为进一步改善涂层的结构稳定性和涂布加工性能，优选地，在本发明的涂料中，所述二氧化硅颗粒的粒径为8～12nm。
在本公开中，若涂料所含SiO2溶胶颗粒过小，在高速分散过程中引入大量微气泡，在后续涂布及热处理过程中，气泡破裂会导致样片表面产生毛刺状突起，增加涂层脆性，从而劣化涂料的粘结强度；反之，若涂料所含SiO2溶胶颗粒过大，比表面积减小，致使改性剂不能充分与颗粒表面接触形成附着层，同时随着粒径增大，总位能降低，颗粒之间的布朗运动将使粒子自发形成凝胶，使涂料易发生析出和沉降的问题。因此，在本发明的涂料中，将二氧化硅颗粒的粒径控制为8-12nm。
在本发明的涂料中，所述气相氧化物颗粒在无机颗粒物组分中的质量百分含量并无特别限制，优选为12.5～75.0％，还优选为20～50％，更优选35.0～50％，最优选35.0～42.5％。
在本公开中，气相氧化物颗粒在无机颗粒物组分的质量百分含量越高，提升涂层粘结性能的效果越好。然而，过高的含量会导致涂料的存储稳定性降低、涂布加工性能劣化并易引发涂层缺陷。因此，在本发明的涂料中，优选将气相氧化物颗粒在无机颗粒物组分中的质量百分含量控制为12.5～75.0％，更优选控制为20～50％。
在本发明的涂料中，所述无机颗粒物组分的中值粒径D50并无特别限制，优选为11～53μm，更优选25～45μm，粗端粒径D90并无特别限制，优选为45-134μm，更优选为60～100μm。
在本公开中，无机颗粒物组分的中值粒径D50越小，涂料中的颗粒度越细，涂层表面光泽度越好、抗划伤、耐化学品性越强，但粘结性能越差；无机颗粒物组分的粗端粒径D90越大，涂料中颗粒度越粗，涂层点线状漏涂、划伤和涂层不均等缺陷概率加大，粘结性能也会变差。
本公开的另一目的在于提供一种硅钢，该硅钢在保证粘结强度、绝缘性等自粘结涂层基本性能的基础上，还能在叠层铁心热压成型时耐受较高压强且无溢胶，可制造出高叠装系数的高效能铁心。
为了实现上述目的，本公开提供了一种硅钢，其包括硅钢基材和涂覆在所述硅钢基材表面上的由上述涂料形成的涂层，所述涂层可通过用本发明涂料涂覆硅钢基材表面并对涂覆的硅钢基材进行烘烤加热而形成。
优选地，在本发明的硅钢中，所述硅钢基材的厚度≤0.65mm。
优选地，在本发明的硅钢中，所述硅钢基材的厚度为0.15～0.3mm。
优选地，在本发明的硅钢中，所述涂层的单面干膜厚度为0.5～5.0μm。
本公开的又一目的在于提供一种高叠装系数的高粘结性电机铁心，该铁心在经受0.5～10MPa热压成型时涂层无溢胶，且具有≥2N/mm的高粘结强度。
为了实现上述目的，本公开提供了一种由本发明硅钢制得的电机铁心。
优选地，本发明电机铁心的叠装系数F％＝(98-0.06×h/H+0.23×P)％；其中P表示叠层硅钢片之间的压强(片间压强)，单位为MPa；H表示硅钢基材的厚度，单位为mm；h表示每片硅钢的双面涂层干膜厚度之和，单位为μm。
优选地，本发明电机铁心的叠装系数≥97％。
优选地，本发明的电机铁心在经受0.5～10MPa热压成型时无溢胶。
更优选地，本发明的电机铁心在经受0.5～10MPa热压成型时涂层的粘结强度≥2N/mm，优选≥3N/mm。
相较于现有技术，本发明的涂料、硅钢和电机铁心具有如下优点以及有益效果：
本发明的涂料可用于在硅钢片表面形成自粘结涂层，在保证粘结强度、绝缘性等自粘结涂层基本性能的基础上，还具备良好的耐压性能和溢胶控制能力。该涂料在叠层铁心热压成型时可耐受较高压强而不发生溢胶，可制造出叠装系数高的高效能铁心，具有显著的实用价值。
本发明的电机铁心在经受0.5～10MPa热压成型时涂层无溢胶现象发生，并且更优选地能发挥出≥2N/mm的高粘结强度。
本发明的涂料在双面涂层总厚度为1～10μm、压强≥1MPa的合适固化成型工艺下，所形成的涂层硅钢叠层铁心可稳定实现≥97％的叠装系数。特别适用于薄规格硅钢基材的高粘性、无溢胶、高叠装系数的自粘结涂层产品，能更好地制造和发挥出高效能电机铁心的应用优势。
附图说明
图1显示了本发明电机铁心的涂层的粘结强度随涂料中有机组分或无机组分含量比例变化的趋势关系。
图2显示了本发明电机铁心的涂层的粘结强度随涂料中气相氧化物颗粒含量变化的趋势关系。
图3显示了本发明电机铁心在不同硅钢片间压强条件下的叠装系数F的变化趋势。
具体实施方式
除非另有定义，否则本文使用的所有技术和科学术语具有与本公开所属领域的普通技术人员的通常理解相同的含义。
在本文中，涂料的“有效成分”是指是指在配方中直接参与形成涂层、赋予涂层功能性的物质成分，区别于溶剂、分散介质或其他惰性物质。
在本文中，环氧当量可通过本领域常规方法测定，如依据GB/T 4612-2008进行测定。
在本文中，中值粒径D50是指在颗粒粒径分布中，累积分布百分比为50％所对应的粒径值，可通过本领域常规方法测定，如激光粒度分析法。
在本文中，粗端粒径D90是指在颗粒粒径分布中，累积分布百分比为90％所对应的粒径值，可通过本领域常规方法测定，如激光粒度分析法。
在本文中，涂层的单面干膜厚度是指单个表面在干燥或固化后形成的涂层厚度。
在本文中，电机铁心的叠装系数F是指铁心压装后的实际铁心高度与理论全金属厚度总和之间的比值，依据GB/T 19289(或IEC 60404-13)标准进行测定。
在本文中，电机铁心无溢胶是指在电机铁心制造过程中，涂料在热压成型时不发生涂料溢出、流动或溢出至铁心外部的现象。
在本文中，电机铁心的涂层的粘结强度依据DIN EN 1464测定。
下面将结合具体的实施例对本公开的涂料、硅钢和电机铁心做进一步的解释和说明，然而该解释和说明并不对本公开的技术方案构成不当限定。
实施例1-13和对比例1
采用下述步骤制得实施例1-13及对比例1的涂料、硅钢和电机铁心：
(1)配制涂料，表1-1、表1-2和表1-3列出了实施例1-13中采用的涂料和对比例1中采用的对比涂料中各组分的质量份数及质量比。
表1-1.



在一些实施方式中，涂料中的无机颗粒物组分是由亲水性气相氧化物粉体和二氧化硅溶胶这两类不同性质的纳米颗粒经分散加工而得的分散体悬浊液，其制备过程如下：
步骤一：采用氢氧焰高温水解法制备亲水性气相氧化物粉体，该气相氧化物选自SiO2、Al2O3、TiO2、ZnO、ZrO2金属氧化物。在制备过程中，调节金属卤化物的添加剂的量来控制气相氧化物的颗粒粒径，使卤化物与氢气、空气的用量比在1：(0.3～1.7)：(8～20)范围内。合成器水解炉内喷嘴处气体流速为5～15m/s；合成器炉温1000～1800℃；冷却介质温度70～110℃；分散溶剂除纯水外，还可选择乙二醇、丙三醇、正丁醇、异丁醇、异丙醇、乙二醇甲醚中的两种或两种以上的混合物。
按上述工艺，制备中值粒径D50为7～40nm，比表面积为50～300m2/g，颗粒表面存在-OH羟基等亲水性基团的气相氧化物颗粒。
步骤二：采用溶胶-凝胶法制备二氧化硅溶胶。将硅源正硅酸乙酯、醇、蒸馏水按15：(110～320)：10的体积比投料到烧瓶中，设置油浴温度70℃、搅拌速度150rpm，再加入0.5～3％体积比的表面活性剂，持续搅拌得到较清澈的微乳液，之后在5min内逐滴向其中滴入10～25体积比的碱性催化剂，1.5～2小时后乳液变得澄清透明，反应结束。用蒸馏水对产物进行离心、洗涤，再使用改性剂在超声条件下对硅溶胶进行表面改性，最终获得硅溶胶中SiO2颗粒粒径尺寸为10±2nm。
其中的碱性催化剂可控制溶胶中的颗粒粒径，可选择胺类和氨水；醇可以选择甲醇、乙醇、丙醇、戊醇；表面活性剂抑制粒子快速长大而获得纳米级的硅溶胶，可选择氯化铵、十二烷基苯磺酸钠；改性剂可选用脂肪醇、胺、脂肪酸、硅氧烷。
步骤三：将前述气相氧化物粉体投入到SiO2溶胶中，视需要可再加入一定量的纯水和助剂，把混合液的固含量调整为5～30％，在剪切速率7～25m/s条件下分散60～180min，过程中需冰浴控制液体温度<40℃，得到最终形式的无机颗粒分散体悬浊液。
(2)将上述涂料双面涂布于0.15～0.65mm厚度的硅钢基材，每面干膜厚度控制在0.5～5.0μm之间涂液被两辊或三辊式辊涂机涂敷于B25AV1300高牌号硅钢板卷表面，采用明火烘烤炉或红外干燥炉的烘烤工艺处理固化获得硅钢卷材。在一些实施方式中，每面干膜厚度可以优选地控制在1～3μm之间。可以将涂层带钢生产速度控制在80～200mpm之间，对应烘烤加热时间控制为18～45s，涂层钢板温度控制为210～280℃。
(3)硅钢经过剪冲加工后叠装成铁心，在工装夹具内经受热压固化后获得成型铁心。其中，铁心热压的固化工艺中，片间压强负载可以控制在0.5～10MPa之间，在160～250℃保温10～240min。此外，为实现可稳定生产出高叠装系数的高粘结性电机铁心，叠层硅钢片间压强P(MPa)、硅钢基材H(mm)、每片硅钢的双面涂层干膜厚度之和h(μm)需符合以下公式关系：叠装系数F％＝(98-0.06×h/H+0.23×P)％.
表2列出了实施例1-13的电机铁心和对比例1的对比电机铁心在上述制造流程中的相关工艺参数。
表2.
对得到的实施例1-13的电机铁心和对比例1的对比电机铁心进行性能测试，包括测试其涂层的粘结强度、叠装系数和热压成型制造时的溢胶情况，并将测试结果列于表3中。其中，测试方法具体如下：
涂层的粘结强度：按照DIN EN 1464对实施例1-13的电机铁心和对比例1的对比电机铁心进行粘结强度测试。
溢胶测试：观察电机铁心在经受0.5～10MPa热压成型时是否溢胶。
叠装系数：叠装系数依据GB/T 19289(或IEC 60404-13)标准进行测定。叠装系数F％＝(98-0.06×h/H+0.23×P)％；其中P表示叠层硅钢片之间的压强，单位为MPa；H表示硅钢基材的厚度，单位为mm；h表示每片硅钢的双面涂层干膜厚度之和，单位为μm。
表3列出了实施例1-13的电机铁心和对比例1的对比电机铁心的相关性能测试结果。
表3.
图1显示了本发明电机铁心的涂层的粘结强度随涂料中有机组分或无机组分含量比例变化的趋势关系。
图1显示了不同有机组分占比的涂料(固定气相氧化物颗粒占所有无机颗粒物组分的质量比例为35～40％)，将其涂敷于B25AV1300高牌号硅钢板卷表面，采用明火烘烤炉或红外干燥炉在210～280℃板温条件下进行一次烘烤固化获得B状态的涂层硅钢试样，控制每表面涂层的干膜厚度为2.5μm。按DIN EN 1464粘结强度测试标准来制备涂层钢片叠层样块，并作二次热压固化获得C状态的涂层试样，C态热压工艺为片间负载压强3MPa，200℃保温60min。该图显示，涂料中的有机组分占比≥90％时，才可获得一定粘结强度的涂层性能，且在96％时的粘结强度最高；综合考虑粘结性能和溢胶情况，涂料中有机组分占比90～99％最佳。
从上述表3中也可以看出，实施例1-13制得的电机铁心在经受0.5～10MPa热压成型时均无溢胶。
图2显示了本发明电机铁心的涂层的粘结强度随涂料中气相氧化物颗粒含量变化的趋势关系。
从图2可以看出，随着气相氧化物颗粒在无机颗粒物组分的质量百分含量的提升，涂层粘结性能逐渐提升，因此在更优选的实施例中，控制气相氧化物颗粒在无机颗粒物组分的质量百分含量占比为20～50％。本公开实施例12中的气相氧化物颗粒在无机颗粒物组分的质量百分含量占比低于该范围，因此其粘结强度稍逊于实施例1-10。实施例13中的气相氧化物颗粒在无机颗粒物组分的质量百分含量占比高于该范围，气相氧化物颗粒含量过高有可能会劣化涂料存储稳定性。
此外，实施例11的无机颗粒物的粒径不满足本公开的优选方案，其粘结强度稍逊于实施例1-10。
图3显示了本发明电机铁心在不同硅钢片间压强条件下的叠装系数F的变化趋势。
从图3可以看出，基材板厚越薄，叠层钢块的叠装系数就越小，当双面干膜厚度≤6μm、且片间压强≥3MPa时，叠层铁心可实现≥97％的高叠装系数。
本公开中提及的所有出版物、专利申请、专利以及其它参考文献均通过引用全文的方式并入本文。
虽然通过参照本公开的某些优选实施方式，已经对本公开进行了图示和描述，但本领域的普通技术人员应该明白，以上内容是结合具体的实施方式对本公开所作的进一步详细说明，不能认定本公开的具体实施只局限于这些说明。本领域技术人员可以在形式上和细节上对其作各种改变，包括做出若干简单推演或替换，而不偏离本公开的精神和范围。

Claims (21)

  1. 一种涂料，其溶剂为水，所述涂料的有效成分包含有机组分和无机颗粒物组分，其中：
    所述有机组分包含环氧树脂以及环氧树脂固化剂，所述环氧树脂包含大分子环氧树脂和小分子环氧树脂；
    所述无机颗粒物组分包含纳米级的气相氧化物颗粒和纳米级的二氧化硅颗粒；
    所述有机组分在所述有效成分中的质量百分含量为86～99％，优选90～99％。
  2. 如权利要求1所述的涂料，其中，所述有效成分由所述有机组分和所述无机颗粒物组分组成。
  3. 如权利要求1或2所述的涂料，其中，所述大分子环氧树脂的环氧当量为1500～10000g/eq。
  4. 如权利要求1至3中任一项所述的涂料，其中，所述小分子环氧树脂的环氧当量为100～1000g/eq。
  5. 如权利要求1至4中任一项所述的涂料，其中，所述小分子环氧树脂在有机组分中的质量百分含量为15～30％，所述环氧树脂固化剂在有机组分中的质量百分含量为2～8％。
  6. 如权利要求1至5中任一项所述的涂料，其中，所述环氧树脂选自双酚A、双酚F、酚醛环氧树脂中的两种以上。
  7. 如权利要求1至6中任一项所述的涂料，其中，所述气相氧化物颗粒选自SiO2、Al2O3、TiO2、ZnO、ZrO2中的至少一种。
  8. 如权利要求1至7中任一项所述的涂料，其中，所述环氧树脂固化剂选自：胺类、酸酐类和树脂类固化剂中的至少一种。
  9. 如权利要求1至8中任一项所述的涂料，其中，所述气相氧化物颗粒的中值粒径D50为7～40nm，比表面积为50～300m2/g。
  10. 如权利要求1至9中任一项所述的涂料，其中，所述二氧化硅颗粒的粒径为8～12nm。
  11. 如权利要求1至10中任一项所述的涂料，其中，所述气相氧化物颗粒在无机颗粒物组分中的质量百分含量为20～50％。
  12. 如权利要求1至11中任一项所述的涂料，其中，所述无机颗粒物组分的中值粒径D50为25～45μm，粗端粒径D90为60～100μm。
  13. 一种硅钢，其包括硅钢基材和涂覆在所述硅钢基材表面上由权利要求1-12中任一项所述的涂料形成的涂层。
  14. 如权利要求13所述的硅钢，其中，所述硅钢基材的厚度≤0.65mm。
  15. 如权利要求13或14所述的硅钢，其中，所述硅钢基材的厚度为0.15～0.3mm。
  16. 如权利要求13至15中任一项所述的硅钢，其中，所述涂层的单面干膜厚度为0.5～5.0μm。
  17. 一种电机铁心，其中，所述电机铁心由权利要求13至16中任一项所述的硅钢制得。
  18. 如权利要求17所述的电机铁心，其中，所述电机铁心的叠装系数F％＝(98-0.06×h/H+0.23×P)％，
    其中，P表示叠层硅钢片之间的压强，单位为MPa；H表示硅钢基材的厚度，单位为mm；h表示每片硅钢的双面涂层干膜厚度之和，单位为μm。
  19. 如权利要求18所述的电机铁心，其中，所述叠装系数F≥97％。
  20. 如权利要求17至19中任一项所述的电机铁心，其中，所述电机铁心在经受0.5～10MPa热压成型时无溢胶。
  21. 如权利要求17至20中任一项所述的电机铁心，其中，所述电机铁心在经受0.5～10MPa热压成型时涂层的粘结强度≥2N/mm、优选≥3N/mm。
PCT/CN2025/094624 2024-06-06 2025-05-13 一种用于形成耐压无溢胶自粘结涂层的涂料、硅钢及电机铁心 Pending WO2025251852A1 (zh)

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