Cyclic application method of Pd/mpg-C3N4 catalyst in HBIW hydrogenolysis reaction

A technology of mpg-c3n4 and hydrogenolysis reaction, applied in the direction of metal/metal oxide/metal hydroxide catalyst, physical/chemical process catalyst, chemical instrument and method, etc., can solve the problem of catalyst deactivation and achieve the realization of cycle application, good application prospects, and the effect of increasing security

Active Publication Date: 2020-09-11
BEIJING INSTITUTE OF TECHNOLOGYGY
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] The purpose of the present invention is to solve the problem of deactivation after use of catalysts in the prior art, and to provide a method for recycling Pd / mpg-C3N4 catalysts in HBIW hydrogenolysis reactions

Method used

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  • Cyclic application method of Pd/mpg-C3N4 catalyst in HBIW hydrogenolysis reaction
  • Cyclic application method of Pd/mpg-C3N4 catalyst in HBIW hydrogenolysis reaction
  • Cyclic application method of Pd/mpg-C3N4 catalyst in HBIW hydrogenolysis reaction

Examples

Experimental program
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Effect test

Embodiment 1

[0029] Pd / mpg-C 3 N 4 Catalyst preparation

[0030] 1g mpg-C 3 N 4 Disperse in 100ml deionized water, stir for 15min, add 3.4ml PdCl 2 Aqueous solution (50mg / ml), stirred for 3h, then added 4.2ml NaBH 4 solution (2mg / ml), stirred for 1h, filtered, washed with water until neutral, and vacuum dried at 70°C for 10h to obtain Pd / mpg-C with a palladium content of 4.91%. 3 N 4 catalyst.

[0031] Hydrogenolysis of Hexabenzylhexaazaisowurtzitane

[0032] 3.4g HBIW, 346mg 4.91% Pd / mpg-C 3 N 4 Add the catalyst and 6ml DMF into the reaction flask, keep the temperature <10°C in a cold water bath, replace the gas in the reaction flask with nitrogen three times, then replace the gas in the reaction flask with hydrogen three times, add 0.06ml of bromobenzene and 6ml of acetic anhydride, and start the stirring reaction. Hydrogen is supplied continuously with a hydrogen balloon. Raise the temperature to 18°C ​​for 1 hour, and then raise the temperature to 45°C for 8 hours. After the...

Embodiment 2

[0034] 1g mpg-C 3 N 4 Disperse in 100ml deionized water, stir for 15min, add 5ml PdCl 2 Aqueous solution (50mg / ml), stirred for 3h, then added 6.2ml NaBH 4 solution (2mg / ml), stirred for 1h, filtered, washed with water until neutral, and vacuum dried at 70°C for 10h to obtain Pd / mpg-C with a palladium content of 7.44%. 3 N 4 catalyst.

[0035] Hydrogenolysis of Hexabenzylhexaazaisowurtzitane

[0036] 3.4g HBIW, 228mg 7.44% Pd / mpg-C 3 N 4 Add the catalyst and 6ml DMF into the reaction flask, keep the temperature <10°C in a cold water bath, replace the gas in the reaction flask with nitrogen three times, then replace the gas in the reaction flask with hydrogen three times, add 0.06ml of bromobenzene and 6ml of acetic anhydride, and start the stirring reaction. Hydrogen is supplied continuously with a hydrogen balloon. Raise the temperature to 18°C ​​for 1 hour, and then raise the temperature to 45°C for 8 hours. After the reaction, cool down to room temperature, filter, ...

Embodiment 3

[0038] 1g mpg-C 3 N 4 Disperse in 100ml deionized water, stir for 15min, add 6.7ml PdCl 2 Aqueous solution (50mg / ml), stirred for 3h, then added 8.3ml NaBH 4 solution (2mg / ml), stirred for 1h, filtered, washed with water until neutral, and vacuum dried at 70°C for 10h to obtain Pd / mpg-C with a palladium content of 11.13%. 3 N 4 catalyst.

[0039] Hydrogenolysis of Hexabenzylhexaazaisowurtzitane

[0040] 3.4g HBIW, 153mg 11.13% Pd / mpg-C 3 N 4 Add the catalyst and 6ml DMF into the reaction flask, keep the temperature <10°C in a cold water bath, replace the gas in the reaction flask with nitrogen three times, then replace the gas in the reaction flask with hydrogen three times, add 0.06ml of bromobenzene and 6ml of acetic anhydride, and start the stirring reaction. Continuous supply of hydrogen with a hydrogen balloon,. Raise the temperature to 18°C ​​for 1 hour, and then raise the temperature to 45°C for 8 hours. After the reaction, cool down to room temperature, filter, e...

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Abstract

The invention relates to a cyclic application method of a Pd / mpg-C3N4 catalyst in an HBIW hydrogenolysis reaction, and belongs to the technical field of noble metal catalysis. According to the preparation method, common palladium metal is loaded on a novel carrier mpg-C3N4; the metal palladium in the catalyst has relatively high dispersity and stability; the catalyst has a graphite phase mesoporous structure and unsaturated -NH and -NH2 groups, so that the adsorbability of the catalyst to the HBIW is improved; the transmission efficiency of the HBIW in the catalyst is improved. According to the method disclosed by the invention, high-efficiency hydrogenation of HBIW under a low-pressure condition is realized and the catalyst can be recycled, so that the problem that the catalyst is inactivated after being used in HBIW hydrogenolysis in the industry at present is solved, the production cost of CL-20 is greatly reduced, and the method has a very high application prospect.

Description

technical field [0001] The present invention relates to a kind of palladium (Pd / mpg-C) supported by mesoporous graphite phase carbon nitride 3 N 4 ) The cyclic application of catalyst in the hydrogenolysis reaction of hexabenzylhexaazaisowurtzitane (HBIW) belongs to the technical field of noble metal catalysis. Background technique [0002] Hexanitrohexaazaisowurtzitane (CL-20), as a cage-like high-energy and high-density material, is the fourth-generation explosive widely used in the world. At present, the production of CL-20 is mainly synthesized by hydrogenolysis and nitration of hexabenzylhexaazaisowurtzitane (HBIW). However, since the cage structure of HBIW is unstable after debenzyl grouping, its hydrogenolysis often occurs at It is carried out at normal temperature, and at the same time, acetyl reagent is used to protect the cage structure in the process of hydrogenolysis, so the catalyst is required to have higher catalytic activity. The currently widely used cata...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J23/44B01J37/16C07D487/22
CPCB01J23/44B01J27/24B01J37/16C07D487/22Y02P20/584
Inventor 陈锟刘伟黎胜富陈树森金韶华李丽洁束庆海陈煜
Owner BEIJING INSTITUTE OF TECHNOLOGYGY
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