A nitrogen-hetero-condensed aromatic hydrocarbon porous framework with a two-dimensional lamellar structure and its preparation method and application
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A technology of heterocondensed aromatic hydrocarbons and porous skeletons, applied in the field of porous immobilized catalysts and their preparation, can solve problems such as limited prospects, and achieve high reaction efficiency, low cost, and high-efficiency catalytic effects
Active Publication Date: 2019-04-05
FUDAN UNIV
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[0004] Most of the heterogeneous catalysts studied at present cannot meet the following conditions at the same time: high catalytic activity, mild reaction conditions, no need to add additional solvents or / and co-catalysts, good stability, and recyclable use, etc., which limits their industrial application. application prospects
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Embodiment 1
[0027] Embodiment 1: Brunner-Emmet-Teller (BET) specific surface area is at 600m 2 Preparation of about / g aza-PAF:
[0028] 1. Preparation of monomeric HAT;
[0029] Dissolve 3 mmol of o-phenylenediamine and 1 mmol of cyclohexanone in 50 mL of methanol, and react under reflux at 80° C. for 1 h under the action of magnetic stirring. It was then lowered to and maintained at room temperature and stirring was continued overnight. After the reaction, the yellow solid was obtained by filtration and dried, which was the monomer HAT, which was set aside;
[0030] 2. Preparation of catalyst aza-PAF
[0031] Take about 0.05mmol HAT and 1mmol anhydrous AlCl 3 , into a thick-walled glass tube. Use an oil pump to pump out the air in the tube, and at the same time seal the glass tube under the blowtorch, so that the inside is in a vacuum condition. The system was put into a muffle furnace at 400° C. for 15 h. After the reaction was completed, it was lowered to room temperature to ob...
Embodiment 2
[0032] Embodiment 2: BET specific surface area is at 900 m 2 Preparation of aza-PAF around / g:
[0033] 1. The preparation of monomer HAT is as described in Example 1-1;
[0034] 2. Preparation of catalyst aza-PAF;
[0035] The preparation process is similar to Example 1-2, the difference is that 0.05mmol HAT is added with 2mmol anhydrous AlCl 3 .
Embodiment 3
[0036] Embodiment 3: BET specific surface area is at 1300 m 2 Preparation of aza-PAF around / g:
[0037] 1, the preparation of monomer HAT is described in example 1-1;
[0038] 2. Preparation of catalyst aza-PAF;
[0039] The preparation process is similar to Example 1-2, the difference is that 0.05mmolHAT is added with 3mmol anhydrous AlCl 3 .
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Abstract
The invention specifically relates to a fused aza-heterocyclic aromatic hydrocarbon porous framework of a two-dimensional lamellar structure, and a preparation method and application thereof, belonging to the technical field of functional materials. According to the invention, aza-heteropolycyclic aromatic hydrocarbon is synthesized on the basiss of cyclization of a diamino group and a diketo group for formation of phenazine and is used as a monomer; and then aza-heteropolycyclic aromatic hydrocarbon is subjected to the Scholl reaction under the catalysis of a Lewis acid salt so as to allow aza-heteropolycyclic aromatic hydrocarbon to undergo homopolymerization at high temperature and low pressure, so a conjugated polymer material of a microporous structure and with two-dimensional lamellar layers for complex catalysis of metal is produced. The two-dimensional material has the characteristics of a high specific surface area, a full conjugate plane structure, heat stability, resistance to acid and alkali, excellent catalytic activity, high recovery rate, etc. The method provided by the invention is simple to operate and controllable in process; and the prepared material can be used for catalyzing a cycloaddition reaction of CO2 with epoxypropane compounds so as to immobilize CO2 and has good application prospects.
Description
technical field [0001] The invention belongs to the technical field of functional materials, and in particular relates to a porous immobilized catalyst with a two-dimensional sheet structure and a preparation method and application thereof. Background technique [0002] carbon dioxide (CO 2 ) is currently the most important greenhouse gas on the earth and one of the main causes of global warming, but at the same time CO 2 It is also the cheapest and most abundant resource in the C1 family. Globally, CO 2 The carbon content is ten times that of oil, coal and natural gas. In today's society, energy and the environment have become topics of urgent concern to various countries and organizations, considering CO 2 characteristics, seek positive methods to incorporate CO 2 Transformation and utilization is the best way to make overall plans. In the past ten years, about CO 2 There are a lot of researches on the utilization of resources, but there are not many ways that can b...
Claims
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