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A kind of graphene/molecular sieve composite catalyst and preparation method thereof

A composite catalyst and graphene technology, applied in molecular sieve catalysts, including molecular sieve catalysts, carbon compound catalysts, etc., can solve the problems of HZSM-5 and graphene acid catalytic activity and catalytic performance that have not been reported, and achieve enhanced The effect of catalytic activity and good application prospect

Active Publication Date: 2019-01-11
SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003] However, so far, only 3 papers have reported the composite of graphene and molecular sieves, in which graphene with fewer layers is formed by direct charge and discharge of graphite, and then composited with titanium-silicon molecular sieves. Phenol has good photocatalytic activity; graphene oxide induces the formation of large-grained silica with MFI structure and 2.0~2.5nm mesoporous, but its catalytic performance has not been reported
In addition, existing reports mainly focus on 3D bulk ZSM-5 crystals, and the composites of HZSM-5 and graphene and their acid catalytic activity have not been reported so far.

Method used

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  • A kind of graphene/molecular sieve composite catalyst and preparation method thereof
  • A kind of graphene/molecular sieve composite catalyst and preparation method thereof
  • A kind of graphene/molecular sieve composite catalyst and preparation method thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0059] In this example, mesoporous ZSM-5 / graphene composites were prepared in the following manner, and the steps are as follows.

[0060] Weigh 120 mg of graphene, add 6 ml of deionized water, ultrasonically disperse evenly, weigh 1 g of tetrapropylammonium hydroxide and add it to the graphene aqueous solution, stir for 30 min to mix evenly, and record it as A solution; Add 60 mg of aluminum isopropoxide and 2 ml of tetraethyl orthosilicate in sequence and stir evenly, and record it as solution B; firstly stir solution B at 30 °C for 1 h, then raise the temperature to 90 °C and stir for 24 h; then use this solution B with After repeated washing with ethanol and deionized water for 2 to 3 times, it was transferred to a polytetrafluoroethylene-lined autoclave for crystallization at 180 °C for 3 days to obtain ZSM-a / graphene composites. After the product was washed with ethanol and deionized water for 3–5 times, it was vacuum-dried at 100 °C for 12 h, calcined at 600 °C for 5 h,...

Embodiment 2

[0064] Weigh 120 mg of graphene, add 8 ml of deionized water, ultrasonically disperse evenly, weigh 2 g of tetrapropylammonium hydroxide and add it to the graphene aqueous solution, stir for 30 min to mix evenly, and record it as A solution; Add 13.4 mg of sodium metaaluminate and 2 ml of tetraethyl orthosilicate in sequence and stir evenly, and record it as solution B; first stir solution B at 30 °C for 1 h, then at 60 °C for 2 h, then raise the temperature to 80 °C and stir for 6 h, then The B solution was repeatedly washed with ethanol and deionized water for 2 to 3 times, and then transferred to a polytetrafluoroethylene-lined autoclave for crystallization at 170 °C for 2 days to obtain the ZSM-b / graphene composite. After the product was washed with ethanol and deionized water for 3–5 times, it was vacuum-dried at 100 °C for 12 h, calcined at 600 °C for 5 h, and then treated with 0.2 mol / L NH 4 NO 3 The solution was exchanged at 80 °C for 6 h, and then washed, dried, and ...

Embodiment 3

[0069]Weigh 120 mg of graphene, add 6 ml of deionized water, ultrasonically disperse evenly, weigh 3.7 g of tetrapropylammonium hydroxide and add it to the graphene aqueous solution, stir for 30 min to mix evenly, and record it as A solution; Add 222 mg of aluminum isopropoxide and 7.4 ml of tetraethyl orthosilicate in sequence and stir evenly, and record it as solution B; firstly stir solution B at 30 °C for 1 h, then raise the temperature to 90 °C and stir for 24 h; then use this solution B with After repeated washing with ethanol and deionized water for 2 to 3 times, it was transferred to a polytetrafluoroethylene-lined autoclave for crystallization at 180 °C for 3 days to obtain ZSM-a / graphene composites. After the product was washed with ethanol and deionized water for 3–5 times, it was vacuum-dried at 100 °C for 12 h, calcined at 600 °C for 5 h, and then treated with 0.2 mol / L NH 4 NO 3 The solution was exchanged at 80°C for 6 h, and then washed, dried, and calcined to ...

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Abstract

The invention discloses a graphene / molecular sieve composite catalyst and a preparation method thereof. The composite catalyst comprises, by weight, 5-40% of graphene and 60-95% of molecular sieve. The composite material has a quasi-two-dimensional lamellar structure, the ratio of the area of a single lamella to the thickness of the single lamella is more than 100 micrometers, the molecular sieve is evenly loaded on the surface of the graphene, and mesopore diameter is 2-30 nanometers. The preparation method includes: mixing the graphene, a silicon source, an aluminum source and a surfactant, separating out a graphene-containing part, crystalizing, purifying, and removing the surfactant. The graphene / molecular sieve composite catalyst has the advantages that the composite catalyst serving as a solid acid catalyst has enhanced catalytic activity, product yield and reusability can be evidently increased while the catalytic activity is not lowered when the catalyst is used in CBG and EHB reaction, and accordingly the catalyst is promising in application prospect.

Description

technical field [0001] The invention relates to a graphene / molecular sieve composite catalyst and a preparation method thereof, belonging to the technical field of catalysts and preparation thereof. Background technique [0002] Molecular sieve catalysts are widely used in many fields such as industrial petroleum refining, catalysis and separation. ZSM-5 has a three-dimensional network microporous structure. It has become an indispensable solid acid catalyst with its unique pore structure, good catalytic performance, excellent hydrothermal stability and thermal stability, and has good shape selectivity. However, traditional molecular sieves are all microporous, and 90% of the pores are smaller than 2nm. The pore size of conventional ZSM-5 is only 0.5 nm. Molecular sieves are disadvantageous in catalytic applications due to the limited transport pathways for molecules due to their microporous structure. In addition, the traditional ZSM-5 only has a microporous structure, w...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/40C07C41/56C07C43/305C07D317/20C07D319/06C07C2/86C07C15/16C07C67/08C07C69/24C07C45/74C07C49/835C07D311/32
CPCB01J29/40B01J2229/18C07C2/861C07C41/56C07C45/74C07C67/08C07C2521/18C07C2529/40C07D311/32C07D317/20C07D319/06C07C43/305C07C15/16C07C69/24C07C49/835
Inventor 王俊中张会念王俊英
Owner SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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