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Preparation method of hierarchical porous Beta molecular sieve and Ni catalyst for hydrogen production by ethanol steam reforming

A steam reforming and multi-level pore technology is applied in the preparation of catalysts and in the field of multi-level porous molecular sieves, which can solve the problems of easy sintering, agglomeration and deactivation of nickel-based catalysts, carbon deposition, and low utilization rate of pore structure.

Active Publication Date: 2019-03-29
TAIYUAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] The present invention solves the problem that molecular sieves have a single pore structure, the pore structure utilization rate is not high, the pore is not completely open, the molecular sieve skeleton can only serve as a physical adsorption reaction medium, the nickel-based catalyst is easy to sinter, agglomerate and deactivate, and it is easy to flow through the reaction medium during the catalysis process. To solve the problem of carbon deposition, provide a multi-level porous Beta molecular sieve with various pore structures and a high degree of pore opening, and use the molecular sieve as a carrier to introduce active metals into the molecular sieve surface framework in the form of chemical bonding force through the hydrothermal method. Preparation of a kind of core-shell structure catalyst to achieve high yield of ethanol steam reforming

Method used

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  • Preparation method of hierarchical porous Beta molecular sieve and Ni catalyst for hydrogen production by ethanol steam reforming
  • Preparation method of hierarchical porous Beta molecular sieve and Ni catalyst for hydrogen production by ethanol steam reforming
  • Preparation method of hierarchical porous Beta molecular sieve and Ni catalyst for hydrogen production by ethanol steam reforming

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Embodiment 1

[0033] Embodiment 1: The preparation method of multi-stage porous Beta molecular sieve for hydrogen production by steam reforming of ethanol, comprising the following steps:

[0034] 1) Dissolve 0.2mol of 1-bromododecane and 0.1mol of tetramethylhexamethylenediamine in 50mL of a mixed solution of toluene and acetonitrile with a volume ratio of 1:1, and reflux in a water bath at 70°C 48h; cooled to room temperature, the solid product was filtered and washed with cold ether solution, and the obtained white solid was vacuum-dried at 50°C for 5h, and the obtained white gemini surfactant [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - Soluble in deionized water; through anion exchange resin, transparent [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][OH] 2 - solution, the above [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12...

Embodiment 2

[0049] Embodiment 2: the preparation method of multi-stage porous Beta molecular sieve for hydrogen production by steam reforming of ethanol, comprising the following steps:

[0050] 1) Dissolve 0.2mol of 1-bromododecane and 0.1mol of tetramethylhexamethylenediamine in 50mL of a mixed solution of toluene and acetonitrile with a volume ratio of 1:1, and reflux in a water bath at 70°C 48h; cooled to room temperature, the solid product was filtered and washed with cold ether solution, and the obtained white solid was vacuum-dried at 50°C for 5h, and the obtained white gemini surfactant [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - Soluble in deionized water; through anion exchange resin, transparent [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][OH] 2 - solution, the above [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 )2 C 12 h...

Embodiment 3

[0065] Embodiment 3: the preparation method of multi-stage porous Beta molecular sieves for hydrogen production by steam reforming of ethanol, comprising the following steps:

[0066] 1) Dissolve 0.2mol of 1-bromododecane and 0.1mol of tetramethylhexamethylenediamine in 50mL of a mixed solution of toluene and acetonitrile with a volume ratio of 1:1, and reflux in a water bath at 70°C 48h; cooled to room temperature, the solid product was filtered and washed with cold ether solution, and the obtained white solid was vacuum-dried at 50°C for 5h, and the obtained white gemini surfactant [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][Br] 2 - Soluble in deionized water; through anion exchange resin, transparent [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 12 h 25 ][OH] 2 - solution, the above [C 12 h 25 (CH 3 ) 2 N + (CH 2 ) 6 N + (CH 3 ) 2 C 1...

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Abstract

The invention relates to a hierarchical porous molecular sieve and a catalyst prepared from the molecular sieve, specifically to a preparation method of a hierarchical porous Beta molecular sieve andan Ni catalyst thereof, and solves the problems of single pore structure, low utilization rate, incomplete opening, only an adsorption role, easy sintering, agglomeration and deactivation, and formation of carbon deposit. The scheme includes: stirring deionized water, sodium metaaluminate NaAlO2 and a dual template agent to obtain a clarified solution, adding fumed silica and performing stirring,then transferring the mixture into a polytetrafluoroethylene container, and conducting constant temperature heating and static crystallization in a reaction kettle, then performing cooling, and carrying out high temperature calcination, then taking nickel carbonate tetrahydrate, ammonium chloride and ammonia water, and performing stirring in deionized water, adding the molecular sieve and performing stirring, conducting hydrothermal synthesis for certain period of time, then conducting washing and pumping filtration, retaining the solid product, and conducting drying. The prepared hierarchicalporous Beta molecular sieve is rich in micro-mesoporous biphasic highly interconnected pore structure. The prepared catalyst is core-shell-like structure catalyst, and has high yield.

Description

technical field [0001] The invention relates to a multi-stage porous molecular sieve and a preparation method of a catalyst prepared by the molecular sieve, in particular to a preparation method of a multi-stage porous Beta molecular sieve and a Ni-type catalyst for hydrogen production by steam reforming of ethanol. Background technique [0002] Currently, steam reforming of non-renewable feedstocks based on fossil fuels (essentially natural gas) is the most commonly used technology, but this ignores the subsequent costs of environmental impacts. Hydrogen energy is a pollution-free and renewable "green" energy. The use of bioethanol steam reforming to produce hydrogen has the advantages of high unit energy, high hydrogen content, non-toxicity, and easy storage and transportation, and has become a hot spot in recent years. [0003] The use of non-noble metal nickel as the active metal for hydrogen production by steam reforming of ethanol has the characteristics of high activ...

Claims

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Application Information

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IPC IPC(8): B01J29/70B01J29/76B01J35/10C01B3/32
CPCC01B3/326B01J29/7007B01J29/7615C01B2203/1058C01B2203/1229C01B2203/0233B01J2229/183B01J35/61B01J35/60
Inventor 王诗瑶谢鲜梅贺博田韧代蓉
Owner TAIYUAN UNIV OF TECH
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