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Simple method for preparing Co-Nx/C efficient selective photocatalyst

A photocatalyst and selective technology, applied in physical/chemical process catalysts, chemical instruments and methods, preparation of quinone oxides, etc., can solve the problems of low singlet oxygen quantum yield, low quantum yield, poor selectivity, etc. Achieve the effect of improving selective photocatalytic oxidation ability, enhancing singlet oxygen generation, and low cost

Inactive Publication Date: 2017-12-01
CHINA UNIV OF PETROLEUM (EAST CHINA)
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the quantum yield of singlet oxygen is not high. Only with the help of efficient photosensitizers can molecular oxygen obtain energy and convert into singlet oxygen.
[0003] Over the past few decades, a series of photosensitizers have been used to generate 1 o 2 : heavy atom (bromine, iodine) doped organic dyes, porphyrin and its derivatives, noble metal nanoparticles, semiconductor quantum dots and fullerene derivatives, etc., but due to the low quantum yield and poor selectivity of such photosensitizers , high cost and high toxicity, which greatly limit their application

Method used

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  • Simple method for preparing Co-Nx/C efficient selective photocatalyst
  • Simple method for preparing Co-Nx/C efficient selective photocatalyst
  • Simple method for preparing Co-Nx/C efficient selective photocatalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0016] Weigh 2.75g of dimethylglyoxime and 2.5g of cobalt chloride, dissolve them in 80ml of acetone, then slowly add the cobalt chloride solution into the solution of dimethylglyoxime, and keep stirring. After stirring for 5min, the mixed solution Stand still at room temperature for 24h. Finally, the mixture was filtered to obtain a green precipitate, which was washed three times with acetone, and then vacuum-dried at 60°C to obtain the metal-organic complex precursor; weigh 2g of the metal-organic complex precursor, and evenly spread it on Quartz boat, and then put the quartz boat into the tube furnace, N 2 Replace for 30 minutes, remove the oxygen in the tube, start the heating device, and heat up at a heating rate of 5°C / min. After raising the temperature to 300°C, keep the constant temperature for 2 hours, then lower the temperature naturally, take it out after cooling down to room temperature, wash the obtained solid three times with water and ethanol, and finally put i...

Embodiment 2

[0018] According to the main process method in Example 1, the thermal polymerization temperature was changed, and the temperature was raised to 250 ° C. The prepared photocatalyst was used to catalyze 1,5-dihydroxynaphthalene. The reaction time was 100 minutes, and the yield of juglone was 18.86%. .

Embodiment 3

[0020] According to the main flow method in Example 1, the thermal polymerization temperature was changed, and the temperature was raised to 350 ° C. The prepared photocatalyst was used to catalyze 1,5-dihydroxynaphthalene. The reaction time was 100 minutes, and the yield of juglone was 24.00%. .

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Abstract

Depletion of energy resources and environmental pollution are two problems needing to be resolved immediately at present, and rich solar energy provides an efficient path for solving the two problems. Effective conversion of luminous energy and chemical energy cannot be performed without a photosensitive nano-material with excellent photocatalytic activity. A metal-organic complex serves as a precursor, and the Co-Nx / C efficient selective photocatalyst is prepared through a simple one-step heat polymerization method. The invention belongs to the field of carbon material science. The organic ligand is selected from dimethylglyoxime with low price and high coordination ability, a low-price transition metal salt (cobalt chloride) is selected in the metal center, and after high-temperature calcinations, the catalytic active site (Co-Nx) is successfully introduced into the catalyst. The Co-Nx / C catalyst is capable of selectively sensitizing oxygen so as to produce high-activity singlet oxygen. The Co-Nx / C active center is formed, the energy difference (Delta EST) between a singlet state and a triplet state is reduced, the intersystem crossing (ISC) process is promoted, production of the singlet oxygen is enhanced, and the selective photocatalytic oxidation ability is improved.

Description

technical field [0001] The invention uses a metal-organic complex as a precursor to prepare a Co-Nx / C high-efficiency and selective photocatalyst through a simple one-step thermal polymerization method, and belongs to the field of carbon material science. Diacetyl oxime, which is cheap and has strong coordination ability, is selected as the organic ligand, and the transition metal salt (cobalt chloride) is selected as the metal center. After high-temperature calcination, the catalytic active center (Co-Nx) is successfully introduced into the catalyst middle. The Co-Nx / C catalyst can selectively sensitize molecular oxygen to generate highly active singlet oxygen. The present invention forms the Co-Nx active center through the coordination of metal center cobalt and pyridine nitrogen, which is beneficial to reduce the energy difference between the singlet state and the triplet state (△E ST ), to promote the intersystem crossing (ISC) process, which is conducive to enhancing th...

Claims

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Application Information

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IPC IPC(8): B01J27/24C07C46/08C07C50/32
CPCC07C46/08B01J27/24B01J35/33B01J35/39C07C50/32
Inventor 吴文婷张庆刚王小凯韩聪聪吴明铂李忠涛
Owner CHINA UNIV OF PETROLEUM (EAST CHINA)
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