Artificial simulation hydrogenase of aromatic ether dendritic polymer and application of artificial simulation hydrogenase

An artificial analog, dendritic technology, applied in the field of energy science and catalysis science, can solve the problem of hydrogen production activity gap

Active Publication Date: 2013-01-16
TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although the stability of artificial simulated hydrogenase has been improved, there is still a huge gap in its hydrogen production activity compared with natural hydrogenase. Improving the catalytic activity of artificial simulated hydrogenase is of great significance for reducing the cost of hydrogen production.

Method used

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  • Artificial simulation hydrogenase of aromatic ether dendritic polymer and application of artificial simulation hydrogenase
  • Artificial simulation hydrogenase of aromatic ether dendritic polymer and application of artificial simulation hydrogenase
  • Artificial simulation hydrogenase of aromatic ether dendritic polymer and application of artificial simulation hydrogenase

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0083] Synthesis of a first-generation bibranched aryl ether dendrimer artificially mimicking hydrogenase (Hy-G1):

[0084]

[0085] Add 1.0 mmol of [(μ-S 2 )Fe(CO) 6 ] and 10.0 mL of dry tetrahydrofuran, liquid nitrogen freezing-vacuumizing-nitrogen, repeat three times. Slowly drop 2.0mL containing 2.0mmol LiBHEt under nitrogen protection and -78℃ cooling bath 3 THF solution, flow rate 1ml / 5min. After the dropwise addition, keep stirring at -78°C for 10 minutes. Dissolve 2.0 mmol of first-generation benzyl bromide core aryl ether dendrimers (G1-Br) in 2.0 mL of dry tetrahydrofuran solution, and add to the above reaction solution after purging with nitrogen to remove oxygen. After the addition was completed, it was raised to room temperature, and the stirring reaction was continued for 5h. After the reaction, the solvent was removed under reduced pressure, and the crude product was separated by column chromatography (eluent: 5 / 2 dichloromethane / petroleum ether) to obta...

Embodiment 2

[0087] Synthesis of second-generation bibranched aryl ether dendrimers artificially mimicking hydrogenase (Hy-G2):

[0088]

[0089] Add 1.0 mmol of [(μ-S 2 )Fe(CO) 6 ] and 10.0 mL of dry tetrahydrofuran, liquid nitrogen freezing-vacuumizing-nitrogen, repeat three times. Slowly add 10.0mL of LiBHEt containing 2.0mmol LiBHEt 3 THF solution, flow rate 1ml / 5min. After the dropwise addition, keep stirring at -78°C for 10 minutes. Dissolve 2.0 mmol of aryl ether dendrimers (G2-Br) with a digeneration benzyl bromide core in 2.0 mL of dry tetrahydrofuran solution, and add to the above reaction solution after purging with nitrogen to remove oxygen. After the addition was completed, it was raised to room temperature, and the stirring reaction was continued for 5h. After the reaction, the solvent was removed under reduced pressure, and the crude product was separated by column chromatography (eluent: 5 / 2 dichloromethane / petroleum ether) to obtain a red glassy solid with a yield ...

Embodiment 3

[0091] Synthesis of three-generation bis-branched aryl ether dendrimers artificially mimicking hydrogenase (Hy-G3):

[0092]

[0093] Add 1.0 mmol of [(μ-S 2 )Fe(CO) 6 ] and 10.0 mL of dry tetrahydrofuran, liquid nitrogen freezing-vacuumizing-nitrogen, repeat three times. Slowly add 10.0mL of LiBHEt containing 2.0mmol LiBHEt 3 THF solution, flow rate 1ml / 5min. After the dropwise addition, keep stirring at -78°C for 10 minutes. Dissolve 2.0 mmol of three-generation benzyl bromide-core aryl ether dendrimers (G3-Br) in 2.0 mL of dry tetrahydrofuran solution, and add to the above reaction solution after purging with nitrogen to remove oxygen. After the addition was completed, it was raised to room temperature, and the stirring reaction was continued for 5h. After the reaction, the solvent was removed under reduced pressure, and the crude product was separated by column chromatography (eluent: 5 / 2 dichloromethane / petroleum ether) to obtain a red glassy solid with a yield of...

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Abstract

The invention discloses an artificial simulation hydrogenase of an aromatic ether dendritic polymer. The artificial simulation hydrogenase has the following two molecular structures of a molecular structure (I) and a molecular structure (II), wherein X is the aromatic ether dendritic polymer and has a structural formula shown in the description, R1, R2, R3 and R4 are carbonyl, isocyano, triphenylphosphino, trimethylphosphino, triethylphosphino, tributylphosphino or tripyzzolephosphino. Compared with natural hydrogenase, the artificial simulation hydrogenase of the aromatic ether dendritic polymer disclosed by the invention has good stability and is convenient to store; the artificial simulation hydrogenase is firstly used as a proton reduction catalyst for hydrogen production by water decomposed under catalysis of visible light; during hydrogen production, the catalyst has a stable property and a rather high hydrogen production catalytic activity; so far, the artificial simulation hydrogenase is an artificially synthesized artificial simulation hydrogenase with a highest catalytic activity.

Description

technical field [0001] The invention belongs to the fields of energy science and catalysis science, and in particular relates to an artificial simulated hydrogenase of aromatic ether dendrimers and its synthesis and application. Background technique [0002] The large-scale use of fossil fuels has greatly accelerated the process of human industrialization, but it has also brought about serious energy crises and environmental pollution while creating huge wealth. Therefore, people urgently need to find a clean and renewable energy to solve the current problems. The problem. Solar energy is an inexhaustible clean energy, and the total amount is very large, which can fully meet the needs of human beings for energy. However, solar energy cannot be directly stored and transported, and needs to be converted into other forms of energy. Therefore, research on solar energy conversion has become a hot spot in the field of energy research. [0003] Hydrogen is a clean energy with a h...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C08G83/00B01J31/22C01B3/02
Inventor 李嫕于天君曾毅陈金平李迎迎
Owner TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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