Method for preparing mesophase carbon microspheres with emulsification-hydrogenation-thermal polymerization ternary coupled system

Abstract

The invention provides a method for preparing mesophase carbon microspheres with an emulsification-hydrogenation-thermal polymerization ternary coupled system and belongs to the technical field of preparation of mesophase carbon microspheres. The method comprises steps as follows: 1) an emulsification-hydrogenation-thermal polymerization ternary coupled solvent system is prepared from a hydrogen supply solvent, a modification catalyst and an emulsification solvent; 2) medium and low temperature coal tar asphalt with the fraction larger than 300 DEG C is added to the emulsification-hydrogenation-thermal polymerization ternary coupled solvent system, and mesophase asphalt is prepared; 3) the mesophase asphalt is subjected to extraction with an organic solvent, dried, pre-oxidized in the airatmosphere, carbonized in an N2 atmosphere and graphitized, and mesophase carbon microspheres are obtained. The preparation method of the mesophase carbon microspheres is a brand-new one-pot emulsification system, a good production environment is provided for growth of the mesophase carbon microspheres, and good sphericity degree, smooth surfaces, uniform size distribution and high graphitizationdegree of the prepared mesophase carbon microspheres are guaranteed.

Description

technical field

[0001] The invention relates to the technical field of preparation of mesophase carbon microspheres, in particular to a method for preparing mesophase carbon microspheres by using an emulsification-hydrogenation-thermal polymerization ternary coupling system. Background technique

[0002] Mesophase carbon microspheres are a nematic liquid crystal structure formed during the carbonization of polycyclic aromatic compounds (such as coal tar pitch, coal tar, petroleum pitch, naphthalene, etc.). In the initial stage of mesophase transformation, it is spherical due to the effect of surface tension. As time goes on, the mesophase spheres grow up and merge, and finally anisotropic mesophase pitch is obtained. Separating the small balls formed in the early stage of the mesophase transformation from the mother liquor by an appropriate method is the mesophase carbon microspheres. Mesocarbon microspheres have been widely used in high-performance carbon materials, cataly...

Examples

Embodiment 1

[0042] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0043] (1) According to the added amount of hydrogen donating solvent is 15.00wt%, the added amount of modified catalyst is 0.05wt%, and the added amount of emulsified solvent is 84.95wt%, and mixed to prepare emulsified-hydrogenation-thermal polymerization three-way coupling solvent system, wherein , the mass ratio of the modified catalyst is blue coke:coke:graphene:modifier=80:10:5:5.

[0044] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 40 and an aromaticity of 0.4, according to soft asphalt: three-way coupling Solvent system = 1:3 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, rising from normal temperature to 220°C, constant...

Embodiment 2

[0048] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0049] (1) According to the added amount of hydrogen-donating solvent is 12.00wt%, the added amount of modified catalyst is 0.5wt%, and the emulsified solvent is added to 100%, and mixed to prepare an emulsified-hydrogenation-thermal polymerization three-way coupled solvent system, wherein, modified The mass ratio of the active catalyst is blue carbon: coke: graphene: modifier = 75:5:15:5.

[0050] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 40 and an aromaticity of 0.4, according to soft asphalt: three-way coupling Solvent system = 1:4 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, from normal temperature to 200 ° C, constant t...

Embodiment 3

[0054] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0055] (1) According to the added amount of hydrogen-donating solvent is 10.00wt%, the added amount of modified catalyst is 0.01wt%, and the emulsified solvent is added to 100%, and mixed to prepare an emulsified-hydrogenation-thermal polymerization three-way coupled solvent system, wherein, modified The mass ratio of the active catalyst is blue carbon:coke:graphene:modifier=88.9:10:1:0.1.

[0056] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 70 and an aromaticity of 0.5, according to soft asphalt: three-way coupling Solvent system = 1:5 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, rising from normal temperature to 250°C, const...

technical field

[0001] The invention relates to the technical field of preparation of mesophase carbon microspheres, in particular to a method for preparing mesophase carbon microspheres by using an emulsification-hydrogenation-thermal polymerization ternary coupling system. Background technique

[0002] Mesophase carbon microspheres are a nematic liquid crystal structure formed during the carbonization of polycyclic aromatic compounds (such as coal tar pitch, coal tar, petroleum pitch, naphthalene, etc.). In the initial stage of mesophase transformation, it is spherical due to the effect of surface tension. As time goes on, the mesophase spheres grow up and merge, and finally anisotropic mesophase pitch is obtained. Separating the small balls formed in the early stage of the mesophase transformation from the mother liquor by an appropriate method is the mesophase carbon microspheres. Mesocarbon microspheres have been widely used in high-performance carbon materials, cataly...

Examples

Embodiment 1

[0042] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0043] (1) According to the added amount of hydrogen donating solvent is 15.00wt%, the added amount of modified catalyst is 0.05wt%, and the added amount of emulsified solvent is 84.95wt%, and mixed to prepare emulsified-hydrogenation-thermal polymerization three-way coupling solvent system, wherein , the mass ratio of the modified catalyst is blue coke:coke:graphene:modifier=80:10:5:5.

[0044] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 40 and an aromaticity of 0.4, according to soft asphalt: three-way coupling Solvent system = 1:3 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, rising from normal temperature to 220°C, constant...

Embodiment 2

[0048] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0049] (1) According to the added amount of hydrogen-donating solvent is 12.00wt%, the added amount of modified catalyst is 0.5wt%, and the emulsified solvent is added to 100%, and mixed to prepare an emulsified-hydrogenation-thermal polymerization three-way coupled solvent system, wherein, modified The mass ratio of the active catalyst is blue carbon: coke: graphene: modifier = 75:5:15:5.

[0050] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 40 and an aromaticity of 0.4, according to soft asphalt: three-way coupling Solvent system = 1:4 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, from normal temperature to 200 ° C, constant t...

Embodiment 3

[0054] The method for preparing mesophase carbon microspheres in this embodiment is specifically:

[0055] (1) According to the added amount of hydrogen-donating solvent is 10.00wt%, the added amount of modified catalyst is 0.01wt%, and the emulsified solvent is added to 100%, and mixed to prepare an emulsified-hydrogenation-thermal polymerization three-way coupled solvent system, wherein, modified The mass ratio of the active catalyst is blue carbon:coke:graphene:modifier=88.9:10:1:0.1.

[0056] (2) Put 2.5kg of medium and low temperature coal tar in a rectification kettle for distillation, and distill out soft asphalt with a distillate section at 330-420°C, with a softening point of 70 and an aromaticity of 0.5, according to soft asphalt: three-way coupling Solvent system = 1:5 ratio mixing, placed in a high-pressure reactor for three-stage heating reaction, that is, the first stage is dominated by emulsification and dispersion, rising from normal temperature to 250°C, const...

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