Fused aza-heterocyclic aromatic hydrocarbon porous framework of two-dimensional lamellar structure, and preparation method and application thereof
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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 limiting prospects, and achieve high reaction efficiency, no by-products, and high reusability
Active Publication Date: 2016-09-21
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 condition
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[0027] Example 1: Brunner-Emmet-Teller (BET) specific surface area at 600m 2 / g About the preparation of aza-PAF:
[0028] 1. Preparation of monomer HAT;
[0029] 3mmol o-phenylenediamine and 1mmol cyclohexanone were dissolved in 50mL methanol, and the reaction was refluxed at 80°C for 1h under the action of magnetic stirring. After that, it was lowered to and maintained at room temperature and stirring continued overnight. After the reaction is over, filter to obtain a yellow solid and dry, which is the monomer HAT, ready for use;
[0030] 2. Preparation of aza-PAF catalyst
[0031] Take about 0.05mmol HAT and 1mmol anhydrous AlCl 3 , Added to the 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 torch to make the inside a vacuum condition. The system was placed in a muffle furnace at 400°C for 15 hours. After the reaction, the temperature was lowered to room temperature to obtain a black solid, which was ...
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[0032] Example 2: BET specific surface area is 900 m 2 Preparation of aza-PAF around / g:
[0033] 1. The preparation of monomer HAT is the same as that described in Example 1-1;
[0034] 2. Preparation of catalyst aza-PAF;
[0035] The preparation process is similar to Example 1-2, except that 0.05mmol HAT is added with 2mmol anhydrous AlCl 3 .
Example Embodiment
[0036] Example 3: BET specific surface area at 1300 m 2 Preparation of aza-PAF around / g:
[0037] 1. The preparation of monomer HAT is the same as that described in Example 1-1;
[0038] 2. Preparation of catalyst aza-PAF;
[0039] The preparation process is similar to Example 1-2, except 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 specifically relates to a porous solid-supported 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 the three major energy sources of oil, coal and natural gas. In today’s society, energy and the environment have become a topic of urgent concern to all countries and organizations. Considering the CO 2 Characteristics, seek a positive way to CO 2 Conversion and utilization are 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...
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