Method for refining aromatic hydrocarbons by using microporous-mesoporous core-shell structure composite molecular sieve

A composite molecular sieve and core-shell structure technology, applied in the field of aromatics refining, can solve the problems of catalyst deactivation, catalyst pore blockage, etc., achieve the effect of optimizing reaction conditions, improving activity and activity stability

Active Publication Date: 2020-02-21
ZHEJIANG UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The research of patent CN 105413758 A shows that in the deene refining process with alumina and Y-type molecular sieve as the main component catalyst, metals such as Fe and Ni in the raw oil will gradually deposit on the catalyst, and the coke generated will also deposit on the catalyst. , leading to blockage of the catalyst pores and gradual deactivation of the catalyst

Method used

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  • Method for refining aromatic hydrocarbons by using microporous-mesoporous core-shell structure composite molecular sieve
  • Method for refining aromatic hydrocarbons by using microporous-mesoporous core-shell structure composite molecular sieve
  • Method for refining aromatic hydrocarbons by using microporous-mesoporous core-shell structure composite molecular sieve

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0045] Example 1: Preparation of ZrPO / HZSM-5 core-shell structure composite molecular sieve catalyst

[0046] (1) Synthesis of ZrPO / HZSM-5 core-shell structure composite molecular sieve powder with HZSM-5 microporous molecular sieve as the core and ZrPO mesoporous molecular sieve as the shell

[0047] According to the solid-to-liquid mass ratio of 1:10, 2.0g of inner core HZSM-5 microporous molecular sieve powder and triblock copolymer FI27(EO 106 PO 70 EO 106 ) ethanol solution was stirred and mixed, and stirred continuously at 30° C. for 10 h to obtain mixture A. According to the P to Zr molar ratio n P / n Zr =0.8, F127 and P+Zr molar ratio n F127 / (n P +n Zr )=0.014 ratio, dissolve 57.6g (4.57mmol) F127 with 600mL absolute ethanol, stir at 40°C for 30min to obtain F127 ethanol solution; dissolve 58.0g (180.0mmol) zirconium oxychloride with 300mL absolute ethanol , stirred at 40°C for 30min to obtain ethanol solution of zirconium oxychloride; then dissolved 20.2g (1...

Embodiment 2

[0050] Example 2: Al 0.25 Zr 0.75 Preparation of PO / Hβ core-shell structure composite molecular sieve catalyst

[0051] (1)Al 0.25 Zr 0.75 Synthesis of Composite Molecular Sieves with PO / Hβ Core-Shell Structure

[0052] According to the solid-to-liquid mass ratio of 1:30, 5.0 g of inner core microporous Hβ molecular sieve powder was stirred and mixed with 3.0% FI27 ethanol solution, and stirred continuously at 40°C for 6 hours to obtain mixture A. According to P to total metal molar ratio n P / (n Zr +n Al )=0.75, F127 and P+Zr+Al molar ratio n F127 / (n P +n Zr +n Al )=0.016 ratio, 63.0g (5.0mmol) of F127 was dissolved in 600mL of absolute ethanol, stirred at 30°C for 60min to obtain F127 ethanol solution; 43.5g (135.0mmol) of zirconium oxychloride was dissolved in 300mL of absolute ethanol , stirred at a temperature of 30°C for 60min to obtain an ethanol solution of zirconium oxychloride; dissolved 6.0g (45.0mmol) of anhydrous aluminum chloride in 150mL of absolute et...

Embodiment 3

[0055] Example 3: Ca 0.05 Zr 0.95 Preparation of PO / HY core-shell structure composite molecular sieve catalyst

[0056] (1)Ca 0.05 Zr 0.95 Synthesis of PO / HY core-shell composite molecular sieves

[0057] According to the solid-to-liquid mass ratio of 1:50, 10.0 g of inner microporous HY molecular sieve powder and 5.0% mass concentration of FI27 ethanol solution were stirred and mixed, and stirred continuously at 50° C. for 2 hours to obtain mixture A. According to P to metal molar ratio n P / (n Zr +n Ca )=0.95, F127 and P+Zr+Ca molar ratio n F127 / (n P +n Zr +n Ca )=0.036 ratio, 126.0g (10.0mmol) of F127 was dissolved in 800mL of absolute ethanol, stirred at 40°C for 30min to obtain F127 ethanol solution; 43.5g (135.0mmol) of zirconium oxychloride was dissolved in 300mL of absolute ethanol , stirred at a temperature of 40°C for 30min to obtain an ethanol solution of zirconium oxychloride; dissolved 0.79g (7.1mmol) of anhydrous calcium chloride in 100mL of absolute ...

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Abstract

The invention discloses a method for refining aromatic hydrocarbons by using a microporous-mesoporous core-shell structure composite molecular sieve. Liquid-phase aromatic hydrocarbons contact and react with a solid acid catalyst at a temperature of 100-300 DEG C under a pressure of 0.2-10 MPa and at a feeding mass space velocity of 0.2-15 h<-1> to carry out alkylation and superposition reactionson a tiny amount of olefins in the aromatic hydrocarbons in order to remove the tiny amount of olefins in the aromatic hydrocarbons, refine the aromatic hydrocarbons and obtain olefin-removed aromatichydrocarbons; the solid acid catalyst is the core-shell structure composite molecular sieve catalyst or a modified mesoporous zirconium phosphate molecular sieve catalyst loaded with a modifying compound; the solid acid catalyst prepared in the invention has a high activity, and the olefin removal rate is 98% or above; the catalyst has a good activity stability, and the activity stabilization time exceeds 3000 h; and the selectivity of the reaction for removing olefins from aromatic hydrocarbons is high, and the generation mass fraction of toluene refined by C8 aromatic hydrocarbons is less than 0.1%, and frequent switching operation of reactor reaction and regeneration can be avoided.

Description

[0001] (1) Technical field [0002] The invention relates to an aromatic hydrocarbon refining method for removing trace olefins in aromatic hydrocarbons, in particular to an aromatic hydrocarbon refining method using a composite molecular sieve with a microporous mesoporous core-shell structure. [0003] (2) Background technology [0004] The increase in demand for p-xylene has promoted the construction and expansion of catalytic reforming units in petrochemical enterprises. During the production of aromatics in the reforming unit, the dual-functional reforming catalyst will lead to the formation of a small amount of by-product olefins, and with the promotion of low-pressure reforming technology, the content of olefin impurities in aromatics will increase significantly. These olefins are active in nature, not only easy to form colloids and affect product quality, but also lead to the failure of adsorbents for adsorption and separation, and the deactivation of catalysts such as ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/84C07C7/148C07C15/04C07C15/06C07C15/08C07C15/02C10G55/06
CPCB01J29/005B01J35/0073C07C7/14833C10G55/06B01J29/84B01J29/40B01J29/7007B01J29/084B01J2229/186B01J29/7876B01J29/166C07C2529/84C10G2400/30C07C15/04C07C15/06C07C15/08C07C15/02Y02P20/584Y02P20/52
Inventor 任杰刘冰邓优金辉
Owner ZHEJIANG UNIV OF TECH
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