Pure silicon S-1 molecular sieve catalyst for packaging metal nanoparticles and preparing method and application of catalyst

A technology of metal nanoparticles and metal particles, applied in molecular sieve catalysts, catalyst activation/preparation, chemical instruments and methods, etc., can solve the problems of catalyst activity, aromatic hydrocarbon selectivity and poor stability, long crystallization time, agglomeration, etc. It has both economic and market competitive advantages, good phenol conversion rate, low hydrogen consumption and energy consumption.

Active Publication Date: 2019-04-19
INST OF PROCESS ENG CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0009] CN 107020147A (2017) discloses a MFI structure sheet molecular sieve catalyst, preparation method and application of encapsulating metal oxide or metal nanoparticles. Its technical feature is that the sheet MFI structure molecular sieve is first synthesized, and then the silicon support column is used to support the sheet Molecular sieve with MFI structure and metal oxide or metal nanoparticles are encapsulated between the sheets, which is equivalent to the method of post-treatment modification to realize MFI structure molecular sieve encapsulation of metal oxide or metal nanoparticles, metal oxide in the whole catalyst The content is 0.1~5wt%; In addition, this method needs many steps, crystallization time is long
[0010] The currently reported patents and documents focus more on molecular sieve-encapsulated noble metal catalysts, but as future industrial catalysts, non-noble metals such as Ni, Co, and Fe will have more competitive advantages, but the current reports on non-noble metals Ni, Co, and Fe are still limited
In addition, when the metal catalyst prepared by the traditional wet impregnation method is applied to the catalytic conversion of phenolic compounds, low selectivity of aromatics, uneven distribution of metal particles on the catalyst, uneven particle size, easy migration, agglomeration and loss, which directly lead to catalyst Poor activity, aromatics selectivity, and stability, needs improvement

Method used

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  • Pure silicon S-1 molecular sieve catalyst for packaging metal nanoparticles and preparing method and application of catalyst

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Embodiment 1

[0095] This embodiment illustrates the pure silicon S-1 molecular sieve catalyst and preparation method of the encapsulated metal Ni nanoparticles provided by the present invention:

[0096] (1) Mix ethyl orthosilicate, tetrapropylammonium hydroxide, and deionized water uniformly to obtain mixture A, wherein SiO 2 , TPAOH and H 2 The molar ratio of O is 1:0.15:30; the mixture A is hydrothermally treated at 80°C for 4h;

[0097] (2) Dissolve nickel nitrate in deionized water, then add ethylenediamine for complexation to obtain a purple transparent solution of nickel and ethylenediamine complexation; then, add this transparent complexed purple solution to step (1) hydrothermal treatment Among the obtained products, a mixture B was obtained, and the mixture B was hydrothermally treated at 60°C for 6h; wherein, the SiO in the mixture B 2 , TPAOH, H 2 The molar ratio of O and Ni is: 1:0.15:30:0.02, and the theoretical content of metal Ni is 2wt% Ni;

[0098] (3) Transfer the pr...

Embodiment 2

[0101] This example illustrates the pure silicon S-1 molecular sieve catalyst encapsulated with metal Ni nanoparticles provided by the present invention, its preparation method and its application in the catalyzed reaction of phenol.

[0102] 1. Synthesis of pure silicon S-1 molecular sieves encapsulated with metal Ni nanoparticles:

[0103] (1) Mix ethyl orthosilicate, tetrapropylammonium hydroxide, and deionized water uniformly to obtain mixture A, wherein SiO 2 , TPAOH and H 2 The molar ratio of O is 1:0.15:30; the mixture A is treated at 80° C. for 4 hours;

[0104] (2) Dissolve nickel nitrate in deionized water, then add ethylenediamine for complexation to obtain a purple transparent solution of nickel and ethylenediamine complexation; then, add this transparent complexed purple solution to step (1) hydrothermal treatment Among the obtained products, a mixture B was obtained, and the mixture B was hydrothermally treated at 60°C for 6h; wherein, the SiO in the mixture B ...

Embodiment 3

[0110] This embodiment illustrates the pure silicon S-1 molecular sieve catalyst and preparation method of the encapsulated metal Ni nanoparticles provided by the present invention:

[0111] (1) Mix ethyl orthosilicate, tetrapropylammonium hydroxide, and deionized water uniformly to obtain mixture A, wherein SiO 2 , TPAOH and H 2 The molar ratio of O is 1:0.15:30; the mixture A is hydrothermally treated at 80°C for 4h;

[0112] (2) Dissolve nickel nitrate in deionized water, and then add it dropwise to the product obtained in step (1) hydrothermal treatment to obtain mixture B, which is hydrothermally treated at 60°C for 6h; wherein, SiO in mixture B 2 , TPAOH, H 2 The molar ratio of O and Ni is: 1:0.15:30:0.02, and the theoretical content of metal Ni is 2wt% Ni;

[0113] (3) Transfer the product obtained in step (2) into a closed crystallization kettle, crystallize at 170.5°C for 12 hours, take it out, filter, dry, roast, and reduce to obtain pure silicon S encapsulated wi...

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Abstract

The invention relates to a pure silicon S-1 molecular sieve catalyst for packaging metal nanoparticles and a preparing method and application of the catalyst. By means of the catalyst, a metal precursor is added in the pure silicon S-1 molecular sieve in-situ synthesis process, and the metal nanoparticles are packaged by a pure silicon S-1 molecular sieve through a one-step method. The packaging catalyst is neat in morphology, and the metal nanoparticles are uniform in distribution and particle size and have the size of 1-10 nm. The metal content in the pure silicon S-1 molecular sieve for packaging the metal nanoparticles is 0.1-20 wt%. The packaging catalyst is applied in the phenol catalysis reaction; compared with a metal catalyst synthesized through a traditional wet impregnation method, the phenol conversion rate, the phenol selectivity and the catalysis stability are remarkably improved.

Description

technical field [0001] The present invention relates to the field of catalysts, in particular to a pure silicon S-1 molecular sieve catalyst encapsulated with metal nanoparticles, its preparation method and its application. Catalyst, preparation method and application of pure silicon S-1 molecular sieve of at least one kind of nanoparticle in catalytic reaction of oxygen-containing compounds. Background technique [0002] Benzene (B), toluene (T) and xylene (X) (BTX for short) among aromatic hydrocarbons are very important basic chemical raw materials. Because they are mainly derived from petroleum, their prices are closely related to petroleum prices; the current domestic market is in short supply. At present, most of the medium and low temperature coal tar are burned directly, which wastes resources and pollutes the environment again; the preparation of gasoline and diesel by hydrogenation has temporarily become a mainstream processing method. However, due to the impact o...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/03C07C1/20C07C15/04B01J37/10B01J37/18
CPCB01J29/03B01J35/0013B01J35/008B01J37/10B01J37/18B01J2229/18C07C1/20C07C15/04Y02P20/52
Inventor 石艳春曹宏斌谢勇冰
Owner INST OF PROCESS ENG CHINESE ACAD OF SCI
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