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A kind of dendritic polymer and preparation method and its application as catalyst in photocatalytic hydrogen production

A kind of polymer and dendritic technology, applied in the field of energy science and catalysis science, to achieve the effect of increasing light energy utilization, simple process and good stability

Active Publication Date: 2017-04-12
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

However, it has not been reported to construct a visible light-catalyzed hydrogen production system by simultaneously utilizing the light-harvesting and site-segregation effects of dendrimers.

Method used

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  • A kind of dendritic polymer and preparation method and its application as catalyst in photocatalytic hydrogen production
  • A kind of dendritic polymer and preparation method and its application as catalyst in photocatalytic hydrogen production
  • A kind of dendritic polymer and preparation method and its application as catalyst in photocatalytic hydrogen production

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0045] Preparation of Dendrimer Modified Hydrogenase G4-Hy

[0046]

[0047] 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 2.2mmolLiBHEt under nitrogen protection and -78℃ cooling bath 3of THF solution. After the dropwise addition, keep stirring at -78°C for 0.5h. 2.1 mmol of benzyl bromide-core aryl ether dendrimers (G4-Br) were dissolved in 2.0 mL of dry tetrahydrofuran solution, and added 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 4h. After the reaction, the solvent was removed under reduced pressure, and the crude product was separated by column chromatography (dichloromethane as the eluent) to obtain a dark red solid with a yield of 43%. IR(KBr)ν(cm -1 ):3282,2929,2069(CO),2032(CO),1991(CO),1595,14...

Embodiment 2

[0049] Preparation of Dendrimer Catalyst G4-32Ir-Hy

[0050]

[0051] 1.0mmol of compound G4-Hy, 35.2mmol of compound Ir(N 3 -bpy)(ppy) 2 PF 6 , 0.2mmol of copper sulfate pentahydrate and 0.4mmol of sodium ascorbate were dissolved in tetrahydrofuran / water (volume ratio 4 / 1), and stirred for 48 hours at room temperature under nitrogen protection and light-proof conditions; the mixed solution was decompressed to remove the solvent, and the remaining The solid was dispersed in a mixture of water and dichloromethane, the organic layer was washed with saturated brine, dried, and the solvent was removed under reduced pressure, and the crude product was separated by column chromatography (the eluent was dichloromethane / dichloromethane with a volume ratio of 10 / 1 tetrahydrofuran) to obtain brown-yellow solid G4-32Ir-Hy with a yield of 25%. The H NMR spectrum and mass spectrum of compound G4-32Ir-Hy are as follows figure 1 and figure 2 shown. Infrared, NMR and mass spectromet...

Embodiment 3

[0055] In Example 3, two groups of experiments I and II were conducted simultaneously, and solvents with different concentrations were configured for photocatalytic hydrogen production.

[0056] Configure two 10mL mixed solvents of I and II respectively, V 乙腈 :V 水 = 9 / 1 and V 丙酮 :V 水 =9 / 1, 0.4M triethylamine (TEA) was added thereto to adjust the pH to 10. After 10 hours of light irradiation, the amount of photocatalytic hydrogen production is shown in Table 1:

[0057] Table 1

[0058] Hydrogen volume / microliter Solvent ratio I 439 V 乙腈 :V 水 =9 / 1

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Abstract

The invention discloses a dendritic polymer, wherein photosensitizers and hydrogenase mimics are respectively linked at periphery and core of the dendritic polymer through covalent linkage, thus, light capturing capacity of compound is improved, electron transfer processes from the photosensitizers to the hydrogenase mimics is facilitated, meanwhile, the core hydrogenase is stabilized and efficiency of catalytic hydrogen production is improved. Moreover, the photosensitizers at periphery of the polymer are distributed closely, the captured optical energy can migrate among the photosensitizers, and thus, utilization rate of optical energy is improved. The invention further discloses a preparation method of the dendritic polymer, the method has simple process and is easy for large-scale preparation, the polymer prepared by the method has very good stability and is convenient to store. In the invention, the dendritic polymer catalyst is used in hydrogen production by visible light catalytic decomposition of water for the first time, during the hydrogen production process, the catalyst has stable properties and efficient performance.

Description

technical field [0001] The present invention relates to the technical fields of energy science and catalysis science. More specifically, it relates to a dendritic polymer and its preparation method and application. Background technique [0002] Since the second industrial revolution, the large-scale use of fossil fuels (non-renewable resources such as coal, oil, and natural gas) has accelerated the industrialization process of mankind, but it has also brought serious energy crises and environmental pollution problems. People are eager to find A renewable, clean new energy to replace traditional fossil fuels. Solar energy is an inexhaustible clean energy, which can fully meet the long-term energy needs of human beings. 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 fuel wit...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C08G83/00B01J31/22C01B3/04
CPCY02E60/36
Inventor 李嫕寻知庆于天君张小辉曾毅陈金平
Owner TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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