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Method for producing hydrogen by photocatalysis of nitrogen-containing heterocyclic compound

A nitrogen heterocyclic compound, photocatalysis technology, applied in chemical instruments and methods, organic compound/hydride/coordination complex catalysts, chemical/physical processes, etc. Difficulty recycling and other problems, to achieve the effect of reducing process cost, excellent hydrogen production performance and simple operation

Active Publication Date: 2020-04-24
WUHAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0002] The dehydrogenation reaction of nitrogen heterocyclic compounds usually needs to be carried out under the conditions of high temperature (>100 ℃) and the participation of noble metal catalysts (such as, R.Yamaguchi, C.Ikeda, Y.Takahashi, K.I.Fujita, J.Am.Chem .Soc.2009,131,8410-8412; etc.), even under photocatalytic conditions, also need the participation of noble metal catalysts (K.H.He, F.F.Tan, C.Z.Zhou, G.J.Zhou, X.L.Yang, Y.Li, Angew. Chem.Int.Ed.2017,56,3080-3084.); In addition, the photocatalysts used in the existing nitrogen heterocyclic compound dehydrogenation process are usually metal-organic compounds, which are difficult to recycle and reuse, which is not conducive to reducing process costs and energy consumption

Method used

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  • Method for producing hydrogen by photocatalysis of nitrogen-containing heterocyclic compound

Examples

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Embodiment 1

[0031] A method for producing hydrogen from photocatalytic nitrogen-containing heterocyclic compounds, the schematic diagram of the photocatalytic hydrogen desorption equipment used is shown in figure 1 ; Concretely include the following steps:

[0032] 1) Porphyrin-based MOF; 20mg ZrOCl 2 ·8H 2 O, 20mg TCPP, 500μl formic acid and 300mg p-chlorobenzoic acid were added to the N,N-dimethylformamide solution, ultrasonically dispersed and mixed evenly, heated at 120°C for 8 hours, cooled to room temperature, and powdered after centrifugation Solid, namely porphyrin-based MOF;

[0033] 2) Activate the porphyrin-based MOF obtained in step 1) to remove unreacted raw materials and solvent molecules. The specific steps are as follows: immerse the porphyrin-based MOF in N,N-dimethylformamide for solvent exchange, repeat every day Repeat three times for three days; then immerse in acetone, pour out the acetone after about 8 hours, add new acetone, repeat three times a day, repeat for ...

Embodiment 2~3

[0040] A method for producing hydrogen from photocatalyzed nitrogen-containing heterocyclic compounds. The specific steps are roughly the same as in Example 1, except that the small molecule regulating acids used are benzoic acid and p-chlorobenzoic acid respectively; and the corresponding dosages are 325mg respectively. , 500 mg.

[0041] After testing, the porphyrin-based MOFs obtained in Examples 2 to 3 can also exhibit better photocatalytic hydrogen production performance from tetrahydroquinoline.

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Abstract

The invention discloses a method for producing hydrogen by photocatalysis of a nitrogen-containing heterocyclic compound, which realizes the hydrogen production effect of the nitrogen-containing heterocyclic compound under the condition of visible light by adding a porphyrin-based catalyst into a nitrogen-containing heterocyclic compound solution. According to the invention, the porphyrin-based catalyst is applied to a process for producing hydrogen by photocatalysis of the nitrogen-containing heterocyclic compound for the first time; the method has the advantages of mild reaction conditions,simple operation, excellent hydrogen production performance, effective avoiding of the use of precious metals, realization of recycling, provision of a brand new idea for the efficient dehydrogenationtechnology of nitrogen-containing heterocyclic compounds, and wide application in the field of energy sources.

Description

technical field [0001] The invention belongs to the technical field of photocatalytic hydrogen production, and relates to a method for photocatalytic hydrogen production of nitrogen-containing heterocyclic compounds. Background technique [0002] The dehydrogenation reaction of nitrogen heterocyclic compounds usually needs to be carried out under the conditions of high temperature (>100 ℃) and the participation of noble metal catalysts (such as, R.Yamaguchi, C.Ikeda, Y.Takahashi, K.I.Fujita, J.Am.Chem .Soc.2009,131,8410-8412; etc.), even under photocatalytic conditions, also need the participation of noble metal catalysts (K.H.He, F.F.Tan, C.Z.Zhou, G.J.Zhou, X.L.Yang, Y.Li, Angew. Chem.Int.Ed.2017,56,3080-3084.); In addition, the photocatalysts used in the existing nitrogen heterocyclic compound dehydrogenation process are usually metal organic compounds, which are difficult to recycle and reuse, which is not conducive to reducing process costs and energy consumption. ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C01B3/22B01J31/22
CPCC01B3/22B01J31/1691B01J31/183B01J2531/48C01B2203/0277B01J35/39
Inventor 邓鹤翔宫煊舒于飞
Owner WUHAN UNIV
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