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Method for synthesizing ultrathin ZSM-5 molecular sieve nanosheets under low temperature and normal pressure

A technology of ZSM-5 and molecular sieve, which is applied in the direction of nanotechnology, crystalline aluminosilicate zeolite, borocarbane silicone crystalline aluminosilicate zeolite, etc., to achieve good catalytic activity, simplify hydrothermal synthesis steps, and controllable size Effect

Active Publication Date: 2020-06-23
NANKAI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0008] In addition, the low-temperature synthesis of ZSM-5 molecular sieve membranes is also involved in the published patent (CN201010220350.0), but the focus of this method is to synthesize molecular sieve membranes containing carbon tubes. The synthesis temperature is 90-180 ° C, but the The synthesis conditions in the examples are all at 150°C, and no examples below 100°C or even 100°C have been seen

Method used

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  • Method for synthesizing ultrathin ZSM-5 molecular sieve nanosheets under low temperature and normal pressure
  • Method for synthesizing ultrathin ZSM-5 molecular sieve nanosheets under low temperature and normal pressure
  • Method for synthesizing ultrathin ZSM-5 molecular sieve nanosheets under low temperature and normal pressure

Examples

Experimental program
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Effect test

Embodiment 1

[0044] Synthesis method: Dissolve 14.45g tetrapropylammonium hydroxide (25%) and 33.3g silica sol (40%) in 10ml water, mix and stir for 12h, then add 0.92g aluminum sol, 6.58g ammonium fluoride, 80°C Stir evenly for pre-crystallization for 12 hours, then put it into a polytetrafluoroethylene-lined stainless steel reactor for medium crystallization at 80°C for 36 hours, then cool to room temperature, wash with deionized water, and dry at 80°C to obtain the final product.

[0045] figure 1 It is the XRD spectrogram of the product obtained in Example 1, it can be seen that the product has the characteristic diffraction peak of the MFI structure, and has a higher crystallinity. figure 2 It is the SEM spectrogram of the product obtained in Example 1. It can be seen that the sample presents a sheet-like morphology with a thickness of about 15 nm.

Embodiment 2

[0047] Using the same conditions as in Example 1, change the template agent to ethylenediamine, the dosage is 3.9g, stir evenly at 80°C for pre-crystallization for 12h, and then put it into a stainless steel reactor lined with polytetrafluoroethylene at 80°C Mesocrystallization for 36 hours, cooled to room temperature, washed with deionized water, and dried at 80°C to obtain the final product. The SEM spectrum shows that the sample presents a sheet-like morphology, and the thickness of the nanosheet is about 80nm.

Embodiment 3

[0049] Using the same conditions as in Example 1, change the fluorine source to ammonium hexafluorosilicate, the dosage is 3.9g, stir evenly at 80°C for pre-crystallization for 12h, and then put it into a stainless steel reactor lined with polytetrafluoroethylene at 80°C Crystallize for 36 hours, then cool to room temperature, wash with deionized water, and dry at 80°C to obtain the final product. to get the final product. The SEM image shows that the sample presents a sheet-like morphology, and the thickness of the nanosheet is about 60nm.

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Abstract

The invention discloses a method for synthesizing an ultrathin ZSM-5 molecular sieve according to a low-temperature and normal-pressure hydrothermal method. Trace ammonium salt, silicon sol, a fluorine source and an aluminum source which serve as raw materials are subjected to hydrothermal synthesis. The method is characterized by comprising the following steps: stirring a template agent (ammoniumsalt), a silicon source and a certain amount of water uniformly at room temperature, sequentially adding the aluminum source and the fluorine source, and stirring and performing pre-crystallization at 50 to 100 DEG C for 1 to 50 hours; performing crystallization at 50 to 100 DEG C for 12 to 240 hours; after the reaction ends, cooling a reaction kettle to room temperature and then centrifuging, washing and drying the products. According to the method, the synthesis temperature is low, the synthesis pressure is low or normal pressure, the use amount of the template agent is small, skeleton heteroatoms can be regulated and controlled, and the thickness of a nanometer sheet can be regulated and controlled effectively. The crystallinity degree of the ultrathin nanometer sheet-like ZSM-5 molecular sieve is high, the synthesis cost is greatly saved due to a trace amount of template agent, the use of a high-pressure reaction kettle can be avoided due to low temperature and normal pressure, and the method is favorable for industrial amplification production and has strong industrial promotion prospect.

Description

technical field [0001] The invention belongs to the technical field of synthesis of zeolite molecular sieves, in particular to a method for synthesizing ultrathin nanosheet ZSM-5 molecular sieves under low temperature and normal pressure conditions. Background technique [0002] It is well known that ZSM-5 molecular sieves exhibit different catalytic effects due to different axial orientations. Among them, the nanosheet ZSM-5 molecular sieve (grows relatively fast along the a-axis direction, that is, the (010) crystal plane is large, but grows very slowly along the b-axis direction, and the (100) crystal plane and (X0Z) crystal plane are small. , with a hexagonal flake-like cross-section) compared with other shapes of MFI zeolites, it shows good separation and permeability performance and excellent anti-carbon deposition ability. [0003] At present, the commonly used methods for synthesizing sheet-like ZSM-5 sieves include layered silicate exfoliation method and hydrotherm...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C01B39/40B82Y40/00
CPCB82Y40/00C01B39/40C01P2002/72C01P2004/03C01P2004/22
Inventor 戴卫理代卫炯李兰冬武光军曹戈关乃佳
Owner NANKAI UNIV
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