Preparation method for porous biomimetic catalytic material and application thereof

A biomimetic catalysis and pore-shaped technology, applied in the field of chemical engineering, can solve the problems of low single-pass conversion rate, low selectivity, and large pollution.

Inactive Publication Date: 2013-04-24
GUANGXI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] The purpose of the present invention is to provide a porous biomimetic catalytic material in order to overcome the shortcomings of low single-pass conversion rate, low selectivity, large polluti

Method used

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  • Preparation method for porous biomimetic catalytic material and application thereof
  • Preparation method for porous biomimetic catalytic material and application thereof
  • Preparation method for porous biomimetic catalytic material and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0036] 1. Preparation of porous biomimetic catalytic material-tetrakis(p-carboxyphenyl)metal cobalt porphyrin

[0037] Weigh 34g of chitosan and dissolve it in 600ml of 2% acetic acid solution, and mechanically stir until colloidal. Add 200ml of 4% ammonia water drop by drop under stirring until the pH of the solution is 7 to form a viscous colloid. Slowly add 100ml 0.28g / L tetrakis(p-carboxyphenyl)cobalt porphyrin ethanol solution through the dropping funnel, after stirring for 24h, obtain red colloid by suction filtration, add 80g NH 4 HCO 3 , stirred until uniform, dried under an infrared lamp at 56°C, and then vacuum-dried at a controlled temperature of 56°C, a vacuum degree of 0.007MPa, and a time of 6h to prepare a porous biomimetic catalytic material - tetrakis (p-carboxyphenyl) metal cobalt porphyrin . Its real state diagram is shown in Fig.

[0038] 2. Application of porous biomimetic catalytic material - tetrakis (p-carboxyphenyl) metal cobalt porphyrin

[0039]...

Embodiment 2

[0049] Porous Biomimetic Catalytic Material-Recycling of Tetra(p-Carboxyphenyl)Metal Cobalt Porphyrin

[0050] Put the porous biomimetic catalytic material loaded with 1.0mg tetrakis(p-carboxyphenyl)cobalt porphyrin equivalent into a 500ml reaction kettle, add 200ml cyclohexane, the reaction temperature is 160°C, the air pressure is 0.9MPa, and the stirring speed is 150 revolutions per minute, when the reaction time is 3.5h, the air flow rate is 0.03m 3 / h, the conversion rate of cyclohexane is 16.29%, the selectivity of ketone alcohol is 72.09%, and the catalyst conversion number is 2.45×10 5 , The yield of ketone alcohol is 11.74%. After stopping the catalytic reaction each time, wait for the catalytic material to separate from the reaction mixture through natural sedimentation, filter, wash with ethanol, and then dry naturally to recover the catalytic material, and then use it to catalyze the air oxidation of cyclohexane under the same reaction conditions. Such reutilizat...

Embodiment 3

[0052] 1. Preparation of porous biomimetic catalytic material-tetrakis(p-carboxyphenyl)metallomanganese porphyrin

[0053] The chitosan that takes by weighing 34g is dissolved in the acetic acid solution of 600ml 2%, obtains colloid with mechanical stirring. Under high-speed stirring, add 200ml of 4% ammonia water drop by drop to pH = 6.5 to form a viscous colloid. Slowly add 100ml of 0.28g / L ethanol solution of tetrakis(p-carboxyphenyl)manganese porphyrin through the dropping funnel, stir vigorously for 24h, obtain bright yellow colloid by suction filtration, add 80g of NH 4 HCO 3 , stirred until uniform, dried under an infrared lamp (60°C), then vacuum-dried at a temperature of 60°C, a vacuum degree of 0.010MPa, and a time of 7h to prepare a porous biomimetic catalytic material - tetrakis (p-carboxyphenyl) metal manganese porphyrin.

[0054] 2. Application of porous biomimetic catalytic material - tetrakis(p-carboxyphenyl) manganese metal porphyrin

[0055] (1) Put the p...

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Abstract

The invention discloses a preparation method for a porous biomimetic catalytic material and application thereof. The preparation method comprises the following steps of dissolving chitosan into acetic acid solution, stirring and dropwise adding ammonia water until the pH value is between 6.5 and 7; adding 4-(p-carboxy phenyl) metalloporphyrin ethanol solution, stirring for 24 h, and then adding NH4HCO3 solution, and uniformly stirring; drying by an infrared lamp, and performing vacuum drying to obtain the porous biomimetic catalytic material. The porous biomimetic catalytic material comprises the following components in part by weight 17.6 parts of chitosan, 8.78 parts of glacial acetic acid, 0.0878 part of ammonia water, 0.0176 part of metalloporphyrin, 43.9 parts of ammonium bicarbonate, 500 parts of distilled water and 100 parts of ethanol. Compared with the metalloporphyrin homogeneous catalytic material, the porous biomimetic catalytic material has the advantages that the metalloporphyrin is less in using amount and lower in cost and is easier to separate. The porous biomimetic catalytic material can obviously improve the one-way conversion rate of cyclohexane and the yield of main products and can be reused at least seven times, the average conversion rate of the cyclohexane is between 15.2 and 17.0 percent, and the average conversion rate of ketone alcohol is between 10.9 and 12.7 percent.

Description

technical field [0001] The invention belongs to the technical field of chemical engineering, and relates to a preparation method and application of a porous biomimetic catalytic material, specifically, tetrakis(p-carboxyphenyl) metalloporphyrin is bonded to a porous porous material through acid-base reaction and coordination. Porous biomimetic catalytic materials prepared on biopolymer chitosan (CTS). And this kind of material is applied to the selective catalytic air oxidation of cyclohexane to produce cyclohexanone and cyclohexanol. Background technique [0002] The mixture of cyclohexanone and cyclohexanol is commonly known as KA oil, which can be used to prepare caprolactam and adipic acid, and then synthesize nylon-6 and nylon-66. Catalytic oxidation of cyclohexane in petroleum refining hydrocarbons to prepare cyclohexanone and cyclohexanol is an important industrial organic synthesis method. There are many ways to catalyze the oxidation of cyclohexane, and some are v...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J35/10C07C27/12
Inventor 黄冠沈莉蔡景莉郭勇安危素娟
Owner GUANGXI UNIV
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