CN105621383A - Preparation method of macroporous carbon - Google Patents
Preparation method of macroporous carbon Download PDFInfo
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Abstract
The invention provides a preparation method of macroporous carbon. Composition of the carbon material contains amorphous carbon element which has three-stage pores. The preparation method of the carbon material contains the following steps: mixing calcium carbonate and alkali lye and stirring, mixing calcium carbonate obtained after filtration and heat treatment and water and sugars, stirring and carrying out ultrasonic treatment, drying the mixture, processing the mixture in nitrogen atmosphere to obtain a substance, mixing the substance and an acid solution, and washing and drying so as to obtain the carbon material. According to the method, expensive organic additives are not used, operation steps are simple and feasible, and production cost is low.
Description
Technical field
The invention belongs to porous inorganic material synthesis field, the specifically preparation method of a kind of macropore material with carbon element.
Background technology
Classification according to IUPAC, porous material can be divided into three major types: large pore material (direct > 50nm), mesoporous material (2nm��directly��50nm) and poromerics (direct < 2nm). Due to poromerics and mesoporous material Industrial Catalysis with the field such as separate and apply with succeeding, so being always up research and the focus of application. In recent years, compensate for conventional small pore molecular sieve along with large pore material in the field such as bulky molecular catalysis, separation and mesoporous material is difficult to the shortcoming that allows macromole to enter within duct, and the advantage that some other physical chemical characteristics embodies, the sight of the researcher attracted gradually, becomes the popular domain of research.
" utilize SiO2Opal prepares high specific surface area three-dimensional ordered big hole carbon " (Nanjing Aero-Space University's journal; 2005; 37(5): 593-593) adopting colloid crystal templating to prepare three-dimensional ordered macroporous carbon, preparation process is: (1) first adopts Stobber method synthesis single dispersing SiO2Colloid micro ball, then through centrifuge washing, ethanol disperses, and stands at normal temperatures and pressures 10��30 days, by SiO2Microsphere is self-assembled into orderly opal structure under gravity, then dry 12h at 120 DEG C. (2) use the space of sucrose filling template and the process of repetition carbonization again, prepare macropore material with carbon element.
" double-template method synthesising mesoporous/macropore second hole road carbon material " (Acta PhySico-Chimica Sinica, 2007,23 (5):
757-760) adopting colloid crystal templating to prepare mesopore/macropore second hole road material with carbon element, its preparation method is: first prepare close to monodispersed silica spheres according to Stober method, and under gravity self assembly and form template; Preparing phenol resin oligomer again to dissolve, and by Organic substance mixing such as itself and ethanol, PluronicF127, be then immersed in silica template, room temperature is placed to solution exsiccation; Then being polymerized completely by phenolic resin, carbonization under nitrogen protection atmosphere, and namely obtain mesopore/macropore second hole road material with carbon element with after Fluohydric acid. removing silicon dioxide, the diameter macropores of material with carbon element is about 230nm, and mesopore diameter is about 10nm.
CN102295281A, a kind of method preparing graded porous carbon for template with hollow mesoporous silicon sphere, phenolic resin alcoholic solution is impregnated in the mesopore orbit of hollow mesoporous silicon sphere, then by phenolic resin primary solidification, deep and firmization, carbonization and elimination template, finally it is prepared for having the graded porous carbon of macropore, mesoporous, micropore. Wherein template is hollow mesoporous silicon sphere, and hollow mesoporous silicon sphere has hollow core and mesoporous wall, and hollow core aperture is 300-800nm, and mesoporous wall is about 25-60nm. The aperture of the graded porous carbon of preparation is 300-800nm, and wall thickness is 25-60nm.
CN103482597A, the preparation method of a kind of middle macropore carbon, resin is mixed with firming agent, is heating and curing; With pore creating material and mixed with proppants after being pulverized by solidifying substance, being pressed into precast body then high temperature cabonization, macropore carbon in preparation after being sufficiently mixed, its macropore diameter is at 50nm-10 ��m again. Wherein pore creating material is polyvinyl alcohol, polyvinyl butyral resin, poly-phthalimide resin, and effect is to manufacture macropore, and aperture can change carbonaceous material and pore creating material ratio, and temperature, pressing pressure and material proportion regulate; Proppant is graphite powder, activated carbon powder, NACF, CNT or graphite fibre, and effect is to stop the base shrinks in carbonisation to a certain extent, makes the pore structure of porous charcoal tend towards stability and add large aperture.
Existing large pore material, although especially existing a lot of the disclosing of the preparation method of macropore carbon is reported, but still has some defects to need to overcome, and the template assemblies of such as colloid crystal templating is consuming time long, and preparation cost is high, it is difficult to industrialized production; The macropore ratio of the large pore material that some technology obtains and content are too low, and macropore diameter is generally higher than 200nm, and the excessive using value in aperture is relatively low, and pore diameter range is difficult to prepare at 100��200nm macropore with high using value. Therefore, studying novel, especially the preparation method of the macropore carbon of Cheap highly effective just has very real meaning.
Summary of the invention
For the deficiencies in the prior art, the preparation method that the present invention provides a kind of macropore material with carbon element, material with carbon element provided by the invention has abundant pore structure, and preparation method is simple, and production cost is low.
The present invention provides a kind of macropore material with carbon element, and described material with carbon element has the feature that constituent is amorphous carbon element, has two-stage duct, and wherein the aperture in first order duct is 30��60nm, and the aperture in duct, the second level is 100��200nm; Total specific surface area is 50��150m2/g��
The preparation method of macropore carbon of the present invention, comprises the following steps:
(1) being mixed with alkali liquor by calcium carbonate, stir process at 50��90 DEG C, then filter, the solid matter being filtrated to get is heat treatment 1��3h at 300��500 DEG C;
(2) will mix with water and glucide through the calcium carbonate after step (1) processes, stir 10��60min, then ultrasonic Treatment 1��10h;
(3) solution obtained of step (2) is removed, in the way of droplet splashing, the equipment containing solution, collect the droplet that sputters, then dry at 50��80 DEG C, finally it is placed in nitrogen atmosphere at 700��1000 DEG C carbonization treatment 3��10h;
(4) material that step (3) obtains is mixed homogeneously with acid solution, at 50��200 DEG C, process 1��10h, be washed out drying;
(5) material step (4) obtained in a nitrogen atmosphere, at 700��1000 DEG C of high-temperature process 3��10h, namely prepares macropore material with carbon element.
In preparation method of the present invention, calcium carbonate described in step (1) is nano-calcium carbonate, and the particle diameter of described nano-calcium carbonate is 30��50nm.
In preparation method of the present invention, alkali liquor described in step (1) is one or both in sodium hydroxide, potassium hydroxide, and described concentration of lye is 0.01��0.1mol/L, and the mass ratio of calcium carbonate and alkali liquor is 1:5��1:50, it is preferable that 1:10��1:20.
In preparation method of the present invention, glucide described in step (2) is one or both in sucrose, glucose, calcium carbonate, glucide, water mass ratio be 0.1��2:1:10��33, it is preferred to 0.2��1:1:13��26.
In preparation method of the present invention, solution described in step (3) removes, in the way of droplet splashing, the equipment containing solution, described splashing mode is specifically as follows quickly to stir solution and makes solution splash out with the form of droplet, or under stirring, with high velocity air through solution, splash out with droplet form by solution; The mode of the droplet that described collection splashes out is collect with filter paper or filter cloth.
In preparation method of the present invention, the carbonization treatment described in step (3) carries out in nitrogen atmosphere, and nitrogen flow rate is 10��50mL/min, it is preferred to 15��40mL/min.
In preparation method of the present invention, carbonization treatment heating rate described in step (3), more than 10 DEG C/min, heats up with constant heating rate.
In preparation method of the present invention, the carbonization described in step (3) is process 4��8h at 800��950 DEG C.
In preparation method of the present invention, the acid solution described in step (4) is hydrochloric acid or nitric acid, and the mass concentration of acid solution is 20��60%.
In preparation method of the present invention, the treatment conditions described in step (4) are process 2��7h at 100��180 DEG C.
In preparation method of the present invention, washing described in step (4) for distilled water wash, described dries as 5��15h dry at 100��140 DEG C.
Macropore carbon provided by the invention has abundant macropore, can be used as catalyst carrier, adsorbent, chromatographic column filler, it is possible to as the synthesis masterplate of inorganic organic material.
Compared with prior art, macropore material with carbon element provided by the invention and preparation method thereof has the advantage that
(1) present invention provides macropore carbon to have the physicochemical characteristic of uniqueness, has two-stage duct, and wherein the aperture integrated distribution scope in first order duct is 30��60nm, and the aperture integrated distribution scope in duct, the second level is the macropore duct of 100��200nm. Such pore passage structure is very beneficial for the transmission diffusion of macromolecular substances, has prominent advantage in bulky molecular catalysis process and adsorption separation process.
(2) in the inventive method, using through base extraction and heat treated calcium carbonate as hard template, required multistage pore canal material with carbon element can be obtained, adopt the inventive method pretreatment calcium carbonate, the Surface electric property that can make calcium carbonate changes, the calcium carbonate promoting a part of single dispersing form is assembled, and makes several calcium carbonate particle assemble and forms miniature coherent condition, in order to forms the template needed for macropore duct; And remaining calcium carbonate still keeps monodisperse status, it is possible to as the template needed for medium duct. And finally by material with carbon element being carried out high-temperature process to reduce the surface area of material, reach the effect of reconciliation statement area and pore structure, it is also possible to improve the mechanical strength of material. The preparation method of macropore carbon of the present invention is simple, and topmost being characterized by does not use expensive poisonous organic formwork agent or additive, and cost is low.
(3) in the inventive method, by controlling the ratio of various material, ultrasonic, stirring, the operating procedure such as roasting, control the dispersity of calcium carbonate particle (including single dispersing and miniature state of aggregation). Especially the mode of operation of step (3), splash out with droplet form to collect by step (2) described solution and be then dried process again, saccharide and calcium carbonate particle can be made to be in Homogeneous phase mixing state all the time, avoid saccharide to be separated with calcium carbonate, calcium carbonate particle can be assembled in a large number, cannot forming template, the material with carbon element prepared is that aperture is less than the common microporous activated carbon of 2nm.
Accompanying drawing explanation
Fig. 1 is the SEM photograph of the material with carbon element of embodiment 1 synthesis.
Detailed description of the invention
Below by specific embodiment, the preparation method of material with carbon element of the present invention is described in detail, but is not limited to embodiment. In embodiment, the granularity of calcium carbonate used is about 40nm, and manufacturer is Hangzhou Wanjing New Material Co., Ltd..
Embodiment 1
(1) 2g calcium carbonate is mixed with 30mL0.02mol/L sodium hydroxide solution, at 70 DEG C, stir 2h; Then being filtered, the solid sample obtained is heat treatment 2h at 350 DEG C;
(2) calcium carbonate obtained to step (1) adds 50mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min;
(3) solution that step (2) obtains quickly is stirred, the equipment containing solution is sputtered with the form of droplet, and the droplet splashing out is collected with filter paper, then the droplet collected is dried under 70 DEG C of conditions, finally sample is placed in tube furnace, passing into nitrogen, nitrogen flow rate is 30mL/min; With 12 DEG C/min from room temperature to 900 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 900 DEG C with 5 DEG C/min, constant temperature 5h, namely to prepare material with carbon element, be numbered CL1, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Embodiment 2
(1) 2.5g calcium carbonate is mixed with 30mL0.02mol/L sodium hydroxide solution, at 70 DEG C, stir 2h; Then being filtered, the solid sample obtained processes 1h at 400 DEG C;
(2) calcium carbonate obtained to step (1) adds 50mL distilled water and 3g sucrose, ultrasonic Treatment 4h after stirring 30min;
(3) solution that step (2) obtains quickly is stirred, sputter the equipment containing solution with the form of droplet, and collect the droplet splashing out with filter paper, then the droplet collected is dried under 60 DEG C of conditions; Finally being placed in tube furnace by sample, pass into nitrogen, nitrogen flow rate is 30mL/min; With 13 DEG C/min from room temperature to 800 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 900 DEG C with 3 DEG C/min, constant temperature 5h, namely to prepare macropore material with carbon element, be numbered CL2, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Embodiment 3
(1) 1.5g calcium carbonate is mixed with 50mL0.05mol/L sodium hydroxide solution, under 70 DEG C of conditions, stir 2h; Then being filtered, the solid sample obtained is dry 2.5h under 500 DEG C of conditions;
(2) calcium carbonate obtained to step (1) adds 70mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min.
(3) solution that step (2) obtains quickly is stirred, sputter the equipment containing solution with the form of droplet, and collect the droplet splashing out with filter paper, then the droplet collected is dried under 70 DEG C of conditions; Finally being placed in tube furnace by sample, pass into nitrogen, nitrogen flow rate is 20mL/min; With 11 DEG C/min from room temperature to 900 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 140 DEG C of conditions, process 6h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 950 DEG C with 6 DEG C/min, constant temperature 5h, namely to prepare macropore material with carbon element, be numbered CL3, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Embodiment 4
(1) 3g calcium carbonate is mixed with 60mL0.02mol/L sodium hydroxide solution, under 70 DEG C of conditions, stir 1h; Then being filtered, the solid sample obtained processes 1.5h under 360 DEG C of conditions;
(2) calcium carbonate obtained to step (1) adds 50mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min;
(3) solution that step (2) obtains quickly is stirred, sputter the equipment containing solution with the form of droplet, and collect the droplet splashing out with filter paper, then the droplet collected is dried under 60 DEG C of conditions; Finally being placed in tube furnace by sample, pass into nitrogen, nitrogen flow rate is 15mL/min; With 15 DEG C/min from room temperature to 750 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the salpeter solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 800 DEG C with 5 DEG C/min, constant temperature 7h, namely to prepare macropore material with carbon element, be numbered CL4, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Embodiment 5
(1) 5g calcium carbonate is mixed with 80mL0.02mol/L sodium hydroxide solution, under 60 DEG C of conditions, stir 2h; Then being filtered, the solid sample obtained processes 2h under 400 DEG C of conditions;
(2) calcium carbonate obtained to step (1) adds 50mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min;
(3) solution that step (2) obtains quickly is stirred, sputter the equipment containing solution with the form of droplet, and collect the droplet splashing out with filter cloth, then the droplet collected is dried at 60 DEG C; Finally being placed in tube furnace by sample, pass into nitrogen, nitrogen flow rate is 30mL/min; With 15 DEG C/min from room temperature to 850 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 850 DEG C with 3 DEG C/min, constant temperature 4h, namely to prepare macropore material with carbon element, be numbered CL5, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Comparative example 1
(1) by 2g calcium carbonate, 50mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min;
(2) solution that step (2) obtains quickly is stirred, sputter the equipment containing solution with the form of droplet, and collect the droplet splashing out with filter paper, then the droplet collected is dried under 70 DEG C of conditions; Finally being placed in tube furnace by sample, pass into nitrogen, nitrogen flow rate is 30mL/min; With 12 DEG C/min from room temperature to 900 DEG C, constant temperature 5h;
(3) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 900 DEG C with 3 DEG C/min, constant temperature 5h, namely to prepare material with carbon element, be numbered CL6, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Comparative example 2
(1) 2g calcium carbonate is mixed with 30mL0.02mol/L sodium hydroxide solution, under 70 DEG C of conditions, stir 2h; Then being filtered, the solid sample obtained processes 2h under 350 DEG C of conditions;
(2) calcium carbonate obtained to step (1) adds 50mL distilled water and 3g sucrose, ultrasonic Treatment 5h after stirring 30min;
(3) mixture step (2) prepared is dry under 70 DEG C of conditions; Being subsequently placed in tube furnace, pass into nitrogen, nitrogen flow rate is 30mL/min; With 12 DEG C/min from room temperature to 900 DEG C, constant temperature 5h;
(4) material that step (3) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(5) being placed in tube furnace by the sample that step (4) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 900 DEG C with 3 DEG C/min, constant temperature 5h, namely to prepare material with carbon element, be numbered CL7, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Comparative example 3
(1) 2g calcium carbonate, 50mL distilled water and 3g sucrose are mixed, ultrasonic Treatment 5h after stirring 30min;
(2) mixture step (1) prepared is dry under 70 DEG C of conditions. Being placed in tube furnace again, pass into nitrogen, nitrogen flow rate is 30mL/min; With 12 DEG C/min from room temperature to 900 DEG C, constant temperature 5h.
(3) material that step (2) obtains is mixed homogeneously with the hydrochloric acid solution of 50mL50%, under 150 DEG C of conditions, process 5h, be finally washed with water to neutrality, dry 10h under 100 DEG C of conditions;
(4) being placed in tube furnace by the sample that step (3) obtains, pass into nitrogen, nitrogen flow rate is 30mL/min; It is warming up to 900 DEG C with 5 DEG C/min, constant temperature 5h, to prepare material with carbon element, be numbered CL8, the duct at different levels aperture integrated distribution of gained sample and reference area result are in Table 1.
Table 1 embodiment and comparative example gained sample physico-chemical property
Can be drawn by embodiment and comparative example result, the inventive method can prepare high-quality macropore carbon, and do not adopt the operating procedure of the present invention, when same material proportion, the material with carbon element of preparation is common micro-pore carbon material or meso-porous carbon material, does not contain macroporous structure.
Claims (16)
1. a preparation method for macropore carbon, described macropore carbon constituent is amorphous carbon element, has three grades of ducts, wherein the aperture in first order duct is 3��5nm, the aperture in duct, the second level is 30��60nm, and the aperture in third level duct is 100��200nm, and total specific surface area is 500��1000m2/ g; Described preparation method comprises the following steps:
(1) being mixed with alkali liquor by calcium carbonate, stir process at 50��90 DEG C, then filter, the solid matter being filtrated to get is heat treatment 1��3h at 300��500 DEG C;
(2) will mix with water and glucide through the calcium carbonate after step (1) processes, after stirring 10��60min, ultrasonic Treatment 1��10h;
(3) solution obtained of step (2) is removed, in the way of droplet splashing, the equipment containing solution, collect the droplet that sputters, then dry at 50��80 DEG C, finally it is placed in nitrogen atmosphere at 700��1000 DEG C carbonization treatment 3��10h;
(4) material that step (3) obtains is mixed homogeneously with acid solution, at 50��200 DEG C, process 1��10h, be washed out drying;
(5) material step (4) obtained is in a nitrogen atmosphere, at 700��1000 DEG C of high-temperature process 3��10h.
2. the preparation method described in claim 1, it is characterised in that: calcium carbonate described in step (1) is nano-calcium carbonate.
3. the preparation method described in claim 2, it is characterised in that: described in step (1), the particle diameter of nano-calcium carbonate is 30��50nm.
4. the preparation method described in claim 1, it is characterised in that: alkali liquor described in step (1) is one or both in sodium hydroxide, potassium hydroxide.
5. the preparation method described in claim 1, it is characterised in that: concentration of lye described in step (1) is 0.01��0.1mol/L.
6. the preparation method described in claim 1, it is characterised in that: in step (1), calcium carbonate is 1:5��1:50 with the mass ratio of alkali liquor, it is preferable that 1:10��1:20.
7. the preparation method described in claim 1, it is characterised in that: glucide described in step (2) is one or both in sucrose, glucose.
8. the preparation method described in claim 1, it is characterised in that: calcium carbonate described in step (2), glucide, water mass ratio be 0.1��2:1:10��33, it is preferred to 0.2��1:1:13��26.
9. the preparation method described in claim 1, it is characterized in that: the solution described in step (3) removes, in the way of droplet splashing, the equipment containing solution, described splashing mode is quickly stir solution to make solution splash out with the form of droplet, or splashes out with droplet form by solution through solution with high velocity air under stirring.
10. the preparation method described in claim 1, it is characterised in that: the mode collecting the droplet splashing out described in step (3) is collect with filter paper or filter cloth.
11. the preparation method described in claim 1, it is characterised in that: the carbonization treatment described in step (3) carries out in nitrogen atmosphere, and nitrogen flow rate is 10��50mL/min, it is preferred to 15��40mL/min.
12. the preparation method described in claim 1, it is characterised in that: described in step (3), carbonization treatment heating rate is more than 10 DEG C/min.
13. the preparation method described in claim 1, it is characterised in that: carbonization treatment described in step (3) heats up with constant heating rate.
14. the preparation method described in claim 1, it is characterised in that: the acid solution described in step (4) is hydrochloric acid or nitric acid.
15. the preparation method described in claim 1, it is characterised in that: the mass concentration of the acid solution described in step (4) is 20��60%.
16. the preparation method described in claim 1, it is characterised in that: washing described in step (4) for distilled water wash, described dries as 5��15h dry at 100��140 DEG C.
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| CN113474285A (en) * | 2019-04-02 | 2021-10-01 | 贺利氏电池科技有限公司 | Method for preparing porous carbonaceous material, porous carbonaceous material and catalyst made of said material |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109928379A (en) * | 2017-12-15 | 2019-06-25 | 中国石油化工股份有限公司 | Two-stage duct carbon material and preparation method thereof |
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| CN109928381A (en) * | 2017-12-15 | 2019-06-25 | 中国石油化工股份有限公司 | A kind of macropore carbon and preparation method thereof |
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| CN109928381B (en) * | 2017-12-15 | 2020-09-11 | 中国石油化工股份有限公司 | Macroporous carbon and preparation method thereof |
| CN113474285A (en) * | 2019-04-02 | 2021-10-01 | 贺利氏电池科技有限公司 | Method for preparing porous carbonaceous material, porous carbonaceous material and catalyst made of said material |
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