Method for preparing spinnable mesophase pitch through coal pitch hydrocatalysis-hydrogen supply treatment

A technology for mesophase pitch and coal pitch, which is applied in the field of coal pitch hydrogen catalysis-hydrogen-donating treatment to prepare spinnable mesophase pitch, can solve the problem that it is difficult to effectively improve the molecular structure and composition of pitch, difficult to regulate the formation and transformation of mesophase pitch, Solid catalysts are difficult to avoid problems such as carbon deposition, and achieve the effects of high mesophase content, excellent spinnability and good quality

Active Publication Date: 2020-01-17
郑州中科新兴产业技术研究院
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

This method has problems such as the need to remove quinoline insolubles many times, the severity of catalytic hydrogenation is high, and the solid catalyst is difficult to avoid carbon deposition.
Patent CN85105609A proposes a coal tar pitch hydrogenation method, using a fixed-bed metal-supported solid catalyst, which has low catalytic hydrogenation activity and weak hydrogenation ability, and it is difficult to effectively improve the molecular structure and composition of pitch, and there are multiple removals of quinoline insolubles A step of
Patent CN107760348A thermally polymerizes the refined coal liquefaction residue in the presence of a hydrogen donor and under the protection of nitrogen to obtain mesophase pitch. However, since the coal liquefaction residue is composed of fused-ring aromatics with a high degree of polymerization and condensation, the It is difficult to control the formation and conversion of mesophase pitch by hydrogenation modification of hydrogen donor

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0027] A method for preparing spinnable mesophase pitch by hydrogen catalysis-hydrogen supplying treatment of coal tar pitch, the steps are as follows:

[0028] (1) Add medium-temperature coal tar pitch and sublimed sulfur into the stirred reactor at a mass ratio of 100:0.1, and carry out hydrogenation on coal tar pitch at a reaction temperature of 380°C, a reaction hydrogen pressure of 1 MPa, a reaction time of 4 hours, and a stirring rate of 200 rpm. Catalytic treatment, after the reaction, vacuum distillation to remove low boiling point fractions to obtain primary hydrogenated pitch, vacuum distillation heating temperature 380 ℃, absolute pressure 0.5kPa.

[0029] (2) Put primary hydrogenated pitch and tetrahydronaphthalene into the stirred reactor at a mass ratio of 1:5, and hydrogenate the pitch at a reaction temperature of 390°C, a reaction hydrogen pressure of 0.5 MPa, a reaction time of 8 hours, and a stirring rate of 200 rpm. Catalysis-hydrogen supply synergistic trea...

Embodiment 2

[0034] A method for preparing spinnable mesophase pitch by hydrogen catalysis-hydrogen supplying treatment of coal tar pitch, the steps are as follows:

[0035] (1) Add high-temperature coal tar pitch and mercaptan into the stirred reactor at a mass ratio of 100:2, and perform hydrogenation on coal tar pitch under the conditions of reaction temperature 440°C, reaction hydrogen pressure 4MPa, reaction time 1h, stirring rate 50rpm Catalytic treatment, after the reaction, vacuum distillation to remove low boiling fractions to obtain primary hydrogenated pitch, vacuum distillation heating temperature 320 ° C, absolute pressure 1kPa.

[0036] (2) Put primary hydrogenated pitch and tetrahydronaphthalene into the stirred reactor at a mass ratio of 1:0.5, and perform hydrogenation catalysis on the pitch under the conditions of reaction temperature 450°C, reaction hydrogen pressure 6MPa, reaction time 1h, stirring rate 150rpm -Hydrogen supply synergistic treatment. After the reaction, ...

Embodiment 3

[0040] A method for preparing spinnable mesophase pitch by hydrogen catalysis-hydrogen supplying treatment of coal tar pitch, the steps are as follows:

[0041] (1) Add medium-temperature coal tar pitch and carbon disulfide into the stirred reactor at a mass ratio of 100:0.5, and conduct hydrogen catalytic treatment of coal tar pitch under the conditions of reaction temperature 400°C, reaction hydrogen pressure 2 MPa, reaction time 3 h, stirring rate 150 rpm After the reaction, the low-boiling point fraction was removed by vacuum distillation to obtain primary hydrogenated pitch. The vacuum distillation heating temperature was 360°C and the absolute pressure was 10kPa.

[0042] (2) Add primary hydrogenated pitch and decahydronaphthalene into the stirred reactor at a mass ratio of 1:3, and perform hydrogenation catalysis on the pitch at a reaction temperature of 400°C, a reaction hydrogen pressure of 3 MPa, a reaction time of 4 hours, and a stirring rate of 50 rpm. -Hydrogen su...

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Abstract

The invention discloses a method for preparing spinnable mesophase pitch through coal pitch hydrocatalysis-hydrogen supply treatment. The method comprises the following steps: (1) adding aids into coal pitch, promoting primary inorganic mineral to form a dispersed catalyst in situ under the high-temperature hydrogen condition, performing hydrocatalysis treatment on the coal pitch, performing reduced pressure distillation after reaction to remove a fraction with low boiling point to obtain primary hydrogenated pitch; (2) adding a hydrogen supply agent into the primary hydrogenated pitch, performing hydrocatalysis-hydrogen supply cooperative treatment under the high-temperature hydrogen condition, and performing reduced pressure distillation to remove a fraction with low boiling point to obtain secondary hydrogenated pitch; (3) removing a quinoline insoluble substance from the secondary hydrogenated pitch to obtain refined hydrogenated pitch; and (4) performing thermal polymerization reaction on the refined hydrogenated pitch to obtain the spinnable mesophase pitch. Through hydrocatalysis-hydrogen supply combined treatment, formation and transformation of the mesophase pitch can be effectively regulated and controlled; and the obtained spinnable mesophase pitch has excellent quality, moderate softening point and high mesophase content and can be applied to preparation of high-performance pitch-based carbon fiber.

Description

technical field [0001] The invention relates to the field of carbon material preparation and processing, in particular to a method for preparing spinnable mesophase pitch by hydrogen catalysis-hydrogen supplying treatment of coal tar pitch. Background technique [0002] Mesophase pitch is an anisotropic carbonaceous substance composed of a variety of flat disk-shaped condensed ring aromatics. It is often used as an excellent carbon precursor for high-performance carbon materials. Its raw materials are coal tar pitch, petroleum pitch and heavy aromatics. compounds etc. High-quality mesophase pitch is the precursor for preparing high-performance pitch-based carbon fibers. Mesophase pitch-based carbon fibers have significant advantages such as high thermal conductivity and high modulus, and are widely used in aerospace, aviation, sports, entertainment, transportation and other fields. [0003] The regulation of the molecular structure and composition of raw pitch is a key fact...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C10C3/02
CPCC10C3/023
Inventor 杜俊涛聂毅郏慧娜张敏鑫孙一凯吕家贺马江凯郑双双
Owner 郑州中科新兴产业技术研究院
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