Direct coal liquefaction residue mesoporous carbon as well as preparation method and application thereof

Mesoporous carbon materials with regular pore structures were prepared by reacting refined asphalt with surfactants and using initial wet impregnation template technology. This solved the problems of resource utilization and pore structure optimization of coal direct liquefaction residue, and improved the electrical conductivity and electrochemical performance of mesoporous carbon, making it suitable for energy storage and catalysis.

CN120964771AActive Publication Date: 2025-11-18QINGDAO UNIV OF TECH
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Patent Information

Application Number
CN202511239357.X
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-09-01
Publication Date
2025-11-18
Estimated Expiration
2045-09-01

AI Technical Summary

Technical Problem

In existing technologies, the direct application of coal direct liquefaction residue faces challenges such as raw material inhomogeneity, impurities, and pore structure control. The template method is costly and the removal process is complex, making it difficult to prepare high-performance mesoporous carbon.

Method used

Mesoporous carbon materials with regular pore structures are constructed by reacting refined asphalt with surfactants, using initial wet impregnation template technology, and high-temperature carbonization treatment, thereby optimizing their electrical conductivity and electrochemical properties.

Benefits of technology

It enables the efficient resource utilization of coal direct liquefaction residue, optimizes the pore structure of mesoporous carbon materials, and improves their electrical conductivity and electrochemical performance, making them suitable for high-performance applications such as supercapacitors, batteries, and catalyst supports.

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Abstract

The invention discloses direct coal liquefaction residue mesoporous carbon as well as a preparation method and application thereof, and relates to the technical field of preparation of mesoporous carbon materials. The method comprises the following steps: refining the direct coal liquefaction residues to obtain refined asphalt; mixing the refined asphalt with a solvent to obtain a uniform solution; mixing the uniform solution with a surfactant to obtain a precursor solution; and finally, uniformly impregnating the template material in the precursor by adopting an initial wetting impregnation technology, curing and carbonizing to obtain the mesoporous carbon. The method not only can effectively improve the resource utilization of the direct coal liquefaction residues, but also can optimize the pore structure of the mesoporous carbon material and enhance the conductivity and electrochemical performance of the mesoporous carbon material, and is suitable for the application of energy storage, catalysis and the like in a plurality of high-performance fields.
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Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of mesoporous carbon material preparation, and particularly relates to a coal direct liquefaction residue mesoporous carbon, a preparation method and application. BACKGROUND

[0002] As a byproduct in the coal chemical process, coal direct liquefaction residue contains rich aromatic compounds and carbon materials, and is a potential low-cost carbon source. With the increasing demand for resource recycling, the high-value utilization of coal direct liquefaction residue has gradually become a research hotspot. Especially in the field of carbon material preparation, the use of coal direct liquefaction residue as raw material not only can effectively reduce waste emissions, but also can provide cheap raw materials for the preparation of carbon materials. However, the direct application of coal direct liquefaction residue still faces many technical challenges, especially in the uniformity of raw materials, the presence of impurities and the control of pore structure.

[0003] Mesoporous carbon materials are widely used in supercapacitors, batteries, catalyst supports and other fields due to their excellent electrical conductivity, large specific surface area and adjustable pore structure. In order to realize the preparation of high-performance mesoporous carbon, the template method is often used to control the pore structure, which can accurately adjust the pore size distribution and pore shape. However, the template method usually relies on expensive template materials, and the template removal process is complex, which increases the production cost and energy consumption. Therefore, how to reduce the use cost of template materials, simplify the template removal process and optimize the pore structure of carbon materials at the same time has become a key problem in the preparation of mesoporous carbon.

[0004] Therefore, how to realize the resource utilization of coal direct liquefaction residue while optimizing the pore structure of mesoporous carbon material has become a research hotspot for those skilled in the art. SUMMARY

[0005] One of the purposes of the present application is to provide a preparation method of coal direct liquefaction residue mesoporous carbon. The method realizes the efficient resource utilization of coal direct liquefaction residue by refining pitch and surfactant reaction, initial wet impregnation template technology and high-temperature carbonization treatment, and builds a mesoporous network with regular pore structure in the carbon material. Through this technology, not only the resource utilization of coal direct liquefaction residue can be effectively improved, but also the pore structure of mesoporous carbon material can be optimized, the electrical conductivity and electrochemical performance can be enhanced, and it is suitable for energy storage and catalysis applications in multiple high-performance fields.

[0006] In order to achieve the above purpose, the present application adopts the following technical scheme:

[0007] A preparation method of coal direct liquefaction residue mesoporous carbon, comprising the following steps in sequence:

[0008] a. refining and purifying the coal direct liquefaction residue to obtain refined pitch with ash content not more than 0.2%;

[0009] b. mixing the refined pitch obtained in step a with a solvent at a certain temperature to form a uniform solution, the mass ratio of the refined pitch to the solvent being 1:2;

[0010] c. mixing the uniform solution obtained in step b with a surfactant to obtain a precursor solution, the mass ratio of the surfactant to the refined pitch being 5:1, the surfactant being used to guide the formation of the pore structure of the mesoporous carbon material and control the pore size and specific surface area thereof;

[0011] d. introducing the precursor solution into a template material with an ordered pore structure under the condition of controlled humidity by using the impregnation method, and after the precursor spontaneously fills the pores under capillary action, the precursor is placed in an air atmosphere for solidification to obtain an oxidized and solidified composite material;

[0012] e. subjecting the oxidized and solidified composite material to high-temperature carbonization treatment under a nitrogen atmosphere and acid washing to obtain an ordered mesoporous carbon.

[0013] The preparation method of the coal direct liquefaction residue mesoporous carbon, in step a, the refining and purification removes the ash, metal impurities and other insoluble substances in the coal direct liquefaction residue.

[0014] The preparation method of the coal direct liquefaction residue mesoporous carbon, in step b, the solvent is dimethyl sulfoxide, toluene or dichloromethane, and stirring is carried out at 55-65℃ for 3-5h.

[0015] The preparation method of the coal direct liquefaction residue mesoporous carbon, in step c, the mixing temperature of the uniform solution and the surfactant is 55-65℃, and stirring is carried out for 1-3h; the surfactant is dodecyltrimethylammonium chloride or cetyltrimethylammonium bromide.

[0016] The preparation method of the coal direct liquefaction residue mesoporous carbon, in step d, the template material is MCM-41 or SBA-1.

[0017] The preparation method of the coal direct liquefaction residue mesoporous carbon, the precursor solution is added to the template material at one time, and stirring or rotary evaporation is maintained during the dropping process until the powder is uniformly wet but no flowing droplets.

[0018] The preparation method of the coal direct liquefaction residue mesoporous carbon, in step d, the solidification temperature is 300℃, the heating rate is 5℃ / min, and the solidification time is 2 hours.

[0019] The preparation method of the coal direct liquefaction residue mesoporous carbon has the following steps: e, the carbonization temperature is 700 DEG C, the temperature rising rate is 5 DEG C / min, and the carbonization time is 3 hours.

[0020] Another object of the present application is to provide the mesoporous carbon prepared by the preparation method of the coal direct liquefaction residue mesoporous carbon.

[0021] Still another object of the present application is to provide the application of the coal direct liquefaction residue mesoporous carbon in the fields of supercapacitor electrode materials, energy storage and catalysis.

[0022] Compared with the prior art, the present application has the following beneficial technical effects:

[0023] The present application provides a preparation method of coal direct liquefaction residue mesoporous carbon, which mixes a homogeneous solution with a surfactant, and the introduced surfactant effectively improves the dispersity and uniformity of the coal direct liquefaction residue. In addition, the surfactant can adjust the interfacial tension of the system, promote the uniform distribution of asphaltene and other carbon source substances in the solution, reduce the agglomeration phenomenon, and provide a good physical environment for the subsequent uniform impregnation of the template. At the same time, the surfactant can also guide the formation of the pore structure to a certain extent, which helps to obtain mesoporous carbon material with higher specific surface area and more uniform pore size distribution, thereby significantly improving the structural order and performance stability of the final carbon material.

[0024] In the preparation method, the initial wet impregnation template method is adopted to effectively ensure the uniform distribution of the precursor and maximize the use amount of the template, and the template removal process is simplified. In the carbonization process, the template material can be successfully removed at high temperature to form a mesoporous carbon structure with high specific surface area and good pore connectivity. This structure regulation mechanism improves the pore connectivity of the carbon material, helps to improve the conductivity and electrochemical performance, and enhances the performance of the mesoporous carbon in energy storage applications.

[0025] The mesoporous carbon material prepared by the present application has high specific surface area, good pore structure and excellent conductivity, and is suitable for multiple high-performance fields, especially in energy storage and catalysis applications. Compared with the traditional materials using resin or biomass as the precursor, the preparation method of the present application is more efficient and economical, and the raw material source is stable, which has strong practical application potential and large-scale production capacity. BRIEF DESCRIPTION OF DRAWINGS

[0026] The present application will be further described below in combination with the drawings:

[0027] Figure 1 The N2 adsorption and desorption curve of the mesoporous material prepared in the present application example 1-6.

[0028] Figure 2 Pore size distribution of the mesoporous material prepared for the present embodiment 1-6. DETAILED DESCRIPTION

[0029] The present application provides a coal direct liquefaction residue mesoporous carbon, a preparation method and application, in order to make the advantages, technical scheme of the present application more clear, definite, the following specific embodiments are combined to further illustrate the present application.

[0030] The raw materials required by the present application can be purchased through commercial channels.

[0031] The main technical concept of the present application is that the coal direct liquefaction residue is used as raw material, the refined pitch with low ash content is obtained by purification, the dispersibility and uniformity of the coal direct liquefaction residue are improved by using the surfactant, and the distribution state of the coal direct liquefaction residue in the template pore is precisely controlled by combining the initial wet impregnation template technology, so that the mesoporous carbon material with stable structure, uniform and regular pore size is constructed.

[0032] Embodiment 1:

[0033] A preparation method of a coal direct liquefaction residue mesoporous carbon, comprising the following steps in sequence:

[0034] Step one, the coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not more than 0.2% is obtained;

[0035] Step two, the refined pitch obtained in step one is mixed with dimethyl sulfoxide to form a uniform solution, the mass ratio of refined pitch to dimethyl sulfoxide is 1:2, and after mixing, stirring is carried out at 60℃ for 4 hours;

[0036] Step three, the uniform solution obtained in step two is mixed with dodecyl trimethyl ammonium chloride (DTAC), the mass ratio of refined pitch to dodecyl trimethyl ammonium chloride (DTAC) is 1:5, and after mixing, stirring is carried out at 60℃ for 2 hours;

[0037] Step four, take the template material MCM-41 in an appropriate amount, and immerse the precursor solution under initial wet condition: control the solution to be added dropwise to the template, and stir while adding dropwise, until the powder is uniformly wet and there is no flowing liquid drop. The material after immersion is placed in air atmosphere, and is put into a muffle furnace, and is heated to 300℃ at a rate of 5℃ / min, and is solidified for 2h;

[0038] Step five, the solidified material obtained in step four is transferred into a nitrogen protection muffle furnace, and is heated to 700℃ at a rate of 5℃ / min, and is carbonized for 3h, and the coal direct liquefaction residue mesoporous carbon is obtained after acid washing.

[0039] Embodiment 2:

[0040] A preparation method of coal direct liquefaction residue mesoporous carbon, sequentially comprising the following steps:

[0041] Step one, the coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not more than 0.2% is obtained;

[0042] Step two, the refined pitch obtained in step one is mixed with toluene to form a uniform solution, and the mass ratio of refined pitch to toluene is 1:2, and after mixing, stirring is carried out at 60℃ for 4 hours;

[0043] Step three, the uniform solution obtained in step two is mixed with dodecyltrimethylammonium chloride (DTAC), and the mass ratio of refined pitch to dodecyltrimethylammonium chloride (DTAC) is 1:5, and after mixing, stirring is carried out at 60℃ for 2 hours;

[0044] Step four, take the template material MCM-41 in an appropriate amount, and immerse the precursor solution under initial wet conditions: control the solution to be added dropwise to the template, and stir while adding dropwise, until the powder is uniformly wet and there are no flowing liquid drops. After immersion, the material is placed in an air atmosphere and put into a muffle furnace, and the temperature is raised to 300℃ at a rate of 5℃ / min, and solidified for 2h;

[0045] Step five, the solidified material obtained in step four is transferred into a nitrogen-protected muffle furnace, and the temperature is raised to 700℃ at a rate of 5℃ / min, and carbonized for 3h, and coal direct liquefaction residue mesoporous carbon is obtained after acid washing.

[0046] Example 3:

[0047] The difference from example 1 is that:

[0048] In step two, the refined pitch obtained in step one is mixed with dichloromethane to form a uniform solution, and the mass ratio of refined pitch to dichloromethane is 1:2, and after mixing, stirring is carried out at 60℃ for 4 hours.

[0049] Example 4:

[0050] The difference from example 1 is that:

[0051] In step three, the uniform solution obtained in step two is mixed with cetyltrimethylammonium bromide (CTAB), and the mass ratio of refined pitch to cetyltrimethylammonium bromide (CTAB) is 1:5, and after mixing, stirring is carried out at 60℃ for 2 hours.

[0052] Example 5:

[0053] The difference from example 1 is that:

[0054] Step four, take template material SBA-15, the precursor solution is impregnated under the initial wet condition: control the solution to be added to the template drop by drop, stir gently, until the powder is evenly wet without flowing droplets. The impregnated material is placed in an air atmosphere, put into a muffle furnace, heated to 300℃ at 5℃ / min, solidified for 2h.

[0055] Comparative example 1:

[0056] A method for preparing coal direct liquefaction residue mesoporous carbon, comprising the following steps in sequence:

[0057] Step one, the coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not more than 0.2% is obtained;

[0058] Step two, the refined pitch obtained in step one is mixed with dimethyl sulfoxide to form a uniform solution, and the mass ratio of refined pitch to dimethyl sulfoxide is 1:1. After mixing, stir at 60℃ for 4 hours;

[0059] Step three, the uniform solution obtained in step two is mixed with dodecyl trimethyl ammonium chloride (DTAC), and the mass ratio of refined pitch to dodecyl trimethyl ammonium chloride (DTAC) is 1:5. After mixing, stir at 60℃ for 2 hours;

[0060] Step four, take template material MCM-41, the precursor solution is impregnated under the initial wet condition: control the solution to be added to the template drop by drop, stir gently, until the powder is evenly wet without flowing droplets. The impregnated material is placed in an air atmosphere, put into a muffle furnace, heated to 300℃ at 5℃ / min, solidified for 2h;

[0061] Step five, the solidified material obtained in step four is transferred to a nitrogen protection muffle furnace, heated to 700℃ at 5℃ / min, carbonized for 3h, and the coal direct liquefaction residue mesoporous carbon product is obtained after acid washing.

[0062] In this comparative example, the proportion of pitch dissolution is reduced, and because the amount of solvent is reduced, the pitch dissolution is not sufficient, and there are pitch agglomerates in the solution. When mixed with the surfactant subsequently, the reaction is difficult to proceed uniformly, and the polymerization degree of the precursor will have a large difference. When impregnating the template, the agglomerated pitch is easy to block the pores, resulting in incomplete mesoporous structure, and the specific surface area and pore size distribution are worse than the original proportion. After carbonization, the carbon material has low porosity and many structural defects. When used as a functional material (such as energy storage electrode, catalyst carrier), ion transmission and active site exposure are limited, and the performance (specific capacity, catalytic activity, etc.) is significantly reduced.

[0063] Comparative example 2:

[0064] A preparation method of coal direct liquefaction residue mesoporous carbon, sequentially comprising the following steps:

[0065] Step one, the coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not more than 0.2% is obtained;

[0066] Step two, the refined pitch obtained in step one is mixed with dimethyl sulfoxide to form a uniform solution, and the mass ratio of refined pitch to dimethyl sulfoxide is 1:2, and after mixing, stirring is carried out at 60℃ for 4 hours;

[0067] Step three, take the template material MCM-41 in an appropriate amount, and immerse the uniform solution under initial wet conditions: control the solution to be added drop by drop, and stir while adding, until the powder is uniformly wet and there are no flowing liquid drops. After immersion, the material is placed in an air atmosphere and put into a muffle furnace, and the temperature is raised to 300℃ at a rate of 5℃ / min, and solidified for 2h;

[0068] Step four, the solidified material obtained in step three is transferred into a nitrogen-protected muffle furnace, and the temperature is raised to 700℃ at a rate of 5℃ / min, and carbonized for 3h, and after acid washing, the coal direct liquefaction residue mesoporous carbon product is obtained.

[0069] The comparative example lacks the step of adding a surfactant, and only mesoporous carbon is prepared by dissolving pitch, template immersion, solidification and carbonization. Without a surfactant, the molecules in the solution are not well dispersed and tend to come together. When the template is immersed, the solution cannot uniformly enter the pores of the template, and the precursor is not uniformly distributed in the template. After solidification and carbonization, the unevenness is more serious, and the resulting mesoporous carbon structure is chaotic, and the order and uniformity of the pores are greatly reduced. When used as a functional material, such as energy storage or catalysis, the specific surface area is reduced, the pore size distribution is wide and chaotic, ion or molecule transmission is not smooth, and active site distribution is uneven, resulting in reduced performance, such as reduced specific capacity for energy storage and poor reaction activity and selectivity for catalysis.

[0070] Comparative example 3:

[0071] A preparation method of coal direct liquefaction residue mesoporous carbon, sequentially comprising the following steps:

[0072] Step one, the coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not more than 0.2% is obtained;

[0073] Step two, the refined pitch obtained in step one is mixed with dimethyl sulfoxide to form a uniform solution, and the mass ratio of refined pitch to dimethyl sulfoxide is 1:2, and after mixing, stirring is carried out at 60℃ for 4 hours;

[0074] Step three, the uniform solution obtained in step two is mixed with dodecyl trimethyl ammonium chloride (DTAC), and the mass ratio of refined pitch to dodecyl trimethyl ammonium chloride (DTAC) is 1:5, and after mixing, stirring is performed at 60°C for 2 hours;

[0075] Step four, the precursor solution is simply mixed with MCM-41 template material, and the material is placed in an air atmosphere and put into a muffle furnace, and the temperature is raised to 300°C at a rate of 5°C / min, and solidification is performed for 2h;

[0076] Step five, the solidified material obtained in step four is transferred into a nitrogen-protected muffle furnace, and the temperature is raised to 700°C at a rate of 5°C / min, and carbonization is performed for 3h, and the coal direct liquefaction residue mesoporous carbon product is obtained after acid washing.

[0077] The comparative example does not use initial wet impregnation, and the precursor is directly mixed with the template. Initial wet impregnation can accurately and uniformly fill the solution into the template pores, ensuring that the precursor is distributed in an orderly manner. When simply mixed, the solution is dispersed randomly in the template, and some pores may not be fully filled, and some areas may be excessively aggregated. During the subsequent solidification process, the uneven distribution of the precursor will lead to inconsistent structure of the solidified product, and the mesoporous carbon formed after carbonization will have a large discount in terms of order and connectivity of the pores, and the specific surface area will also be reduced. When used as a functional material, such as an energy storage electrode, ion transport in the pores will be hindered, and active sites cannot be fully exposed, thereby significantly reducing the energy storage performance, such as specific capacity.

[0078] Comparative example 4:

[0079] A method for preparing coal direct liquefaction residue mesoporous carbon, comprising the following steps in sequence:

[0080] Step one, coal direct liquefaction residue is purified by solvent extraction, acid washing, alkali washing or other chemical methods to remove ash, metal impurities and other insoluble substances, and refined pitch with ash content not exceeding 0.2% is obtained;

[0081] Step two, the refined pitch obtained in step one is mixed with dimethyl sulfoxide to form a uniform solution, and the mass ratio of refined pitch to dimethyl sulfoxide is 1:2, and after mixing, stirring is performed at 60°C for 4 hours;

[0082] Step three, the uniform solution obtained in step two is mixed with dodecyl trimethyl ammonium chloride (DTAC), and the mass ratio of refined pitch to dodecyl trimethyl ammonium chloride (DTAC) is 1:5, and after mixing, stirring is performed at 60°C for 2 hours;

[0083] Step four, take the template material MCM-41, and dip the precursor solution under initial wet conditions: control the solution to be added drop by drop to the template, and stir gently while adding, until the powder is evenly wet and there are no flowing liquid droplets.

[0084] Step five, transfer the material obtained in step four into a nitrogen-protected muffle furnace, and heat to 700℃ at a rate of 5℃ / min, carbonize for 3h, and obtain the coal direct liquefaction residue mesoporous carbon product after acid washing.

[0085] The comparative example lacks the solidification treatment, and the precursor is directly carbonized after impregnating the template. Without this step, after the precursor solution is impregnated into the template material, a stable oxidized and solidified composite material cannot be formed. Direct high-temperature carbonization treatment is performed, and the structure inside the material is difficult to form in order, which can lead to the mesoporous carbon structure obtained finally being irregular, and the order and uniformity of the pores being poor. As a functional material, the specific surface area is small, the pore size distribution is chaotic, the ion or molecule transmission efficiency is low, and the active sites cannot be well exposed, thereby significantly reducing the related performance, such as the specific capacity during energy storage and the reaction activity during catalysis.

[0086] The carbon negative electrode materials prepared in the above examples 1-6 and comparative examples 1-4 are tested, and the test results are shown in Table 1.

[0087] Table 1

[0088] Specific surface area (m2 / g) Average pore diameter (nm) Example 1 850 4.2 Example 2 780 5.4 Example 3 820 4.2 Example 4 800 4.7 Example 5 830 4.8 Comparative Example 1 650 4.8 Comparative Example 2 500 4.5 Comparative Example 3 580 4.6 Comparative Example 4 450 5.2

[0089] Figure 1 The N2 adsorption-desorption curve of the mesoporous material prepared in the inventive examples 1-6 is shown in FIG. 1. Figure 2 The pore size distribution of the mesoporous material prepared in the inventive examples 1-6 is shown in FIG. 2. In terms of comparison, by adjusting the three core variables of solvent, surfactant, and template, the performance gradient optimization of mesoporous carbon is realized. Taking example 1 as a benchmark, when the solvent is replaced with toluene, the solubility of toluene in asphalt is weaker than that of dimethyl sulfoxide, the local pore is narrow, and the specific surface area is reduced to 780m² / g; when dichloromethane is used, although the volatility affects the uniformity of the pores, the overall structure is well preserved, and the specific surface area is maintained at 820m² / g. When the surfactant is replaced with cetyltrimethylammonium bromide (CTAB), due to the difference in interaction between the surfactant and asphalt, the pore formation changes, and the specific surface area and other performances change accordingly; by using other suitable surfactants, the regulation effect of the surfactant on the pore structure can be verified. When the template is replaced with SBA-15, the mesoporous structure is more optimal, and the specific surface area is improved, further highlighting the key value of the template in the ordering of the mesoporous carbon pores. In each example, the ratio of asphalt to solvent 1:2 and the ratio of asphalt to surfactant 1:5 ensure the regular construction of the mesoporous structure.

[0090] In the aspect of the comparative examples, the comparative examples verify the necessity of the process by missing / changing the key steps. Comparative Example 1 reduces the asphalt-solvent ratio to 1:1, and the asphalt is not fully dissolved, which causes the precursor to agglomerate, a large number of channels are blocked, and the specific surface area is only 650 m² / g, which proves that the appropriate dissolution ratio is the basis for channel construction; Comparative Example 2 omits the addition of a surfactant, the asphalt molecules are poorly dispersed, there is no good channel formation guide, and the channel structure after carbonization is poor, and the specific surface area is 500 m² / g, which demonstrates the necessity of the surfactant for channel formation and structural integrity; Comparative Example 3 discards the initial wet impregnation, the precursor is unevenly distributed, which causes channel filling disorder, and the specific surface area is 580 m² / g, which demonstrates the importance of initial wet impregnation for uniform replication of channels; Comparative Example 4 skips the solidification, the precursor-template combination is weak, and the structure is loose and deformed after carbonization, and the specific surface area is 450 m² / g, which verifies the role of solidification in structure shaping. The four groups of comparative examples respectively demonstrate the necessity of solvent adaptation, surfactant regulation, initial wet loading, and solidification shaping, and highlight the innovativeness of the multi-step cooperative process.

[0091] In summary, the coal direct liquefaction residue mesoporous carbon prepared by the present application realizes controllable mesoporous carbon channel structure and performance through the synergistic effect of solvent dispersion, surfactant regulation, initial wet loading, solidification shaping, and carbonization conversion. The solvent ensures the dispersion of asphalt, the surfactant helps to build the channel framework, the initial wet impregnation precisely loads, the solidification shaping strengthens the stability, and the carbonization completes the mesoporous conversion.

[0092] The parts not mentioned in the present application can be realized by referring to the existing technology.

[0093] Those skilled in the art should recognize that the above embodiments are only used to illustrate the present application, and are not used as a limitation on the present application, and any appropriate changes and variations to the above embodiments within the scope of the spirit of the present application fall within the scope of the present application.

Claims

1. A method for preparing mesoporous carbon from coal direct liquefaction residue, characterized in that, The steps are as follows: a. Refine and purify the residue from direct coal liquefaction to obtain refined asphalt with an ash content of no more than 0.2%; b. The refined asphalt obtained in step a is mixed with a solvent at a certain temperature to form a homogeneous solution, wherein the mass ratio of the refined asphalt to the solvent is 1:

2. c. The homogeneous solution obtained in step b is mixed with a surfactant to obtain a precursor solution. The mass ratio of the surfactant to the refined asphalt is 5:

1. The surfactant is used to guide the formation of the pore structure of the mesoporous carbon material and to control its pore size and specific surface area. d. Under controlled humidity conditions, the precursor solution is introduced into the template material with an ordered pore structure by impregnation. After the precursor spontaneously fills the pores under capillary action, it is placed in an air atmosphere for curing to obtain an oxidatively cured composite material. e. The oxidative curing composite material is subjected to high-temperature carbonization treatment under a nitrogen atmosphere and then acid-washed to obtain ordered mesoporous carbon.

2. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 1, characterized in that: In step a, refining and purification remove ash, metallic impurities, and other insoluble substances from the coal direct liquefaction residue.

3. The method for preparing mesoporous carbon from direct coal liquefaction residue according to claim 1, characterized in that: In step b, the solvent is dimethyl sulfoxide, toluene, or dichloromethane, and the mixture is stirred at 55–65°C for 3–5 hours.

4. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 1, characterized in that: In step c, the mixing temperature of the homogeneous solution and the surfactant is 55-65°C, and the mixture is stirred for 1-3 hours; the surfactant is dodecyltrimethylammonium chloride or hexadecyltrimethylammonium bromide.

5. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 1, characterized in that: In step d, the template material is MCM-41 or SBA-1.

6. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 5, characterized in that: The precursor solution is added to the template material dropwise in one go, and stirring or rotating to evaporate the powder during the dropwise process until the powder is uniformly moistened but without flowing droplets.

7. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 1, characterized in that: In step d, the curing temperature is 300℃, the heating rate is 5℃ / min, and the curing time is 2 hours.

8. The method for preparing mesoporous carbon from coal direct liquefaction residue according to claim 1, characterized in that: In step e, the carbonization temperature is 700℃, the heating rate is 5℃ / min, and the carbonization time is 3 hours.

9. A mesoporous carbon residue from direct coal liquefaction, characterized in that, It is prepared by the preparation method described in any one of claims 1 to 8.

10. The application of the mesoporous carbon from direct coal liquefaction residue as described in claim 9 in the fields of supercapacitor electrode materials, energy storage, and catalysis.

Citation Information

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