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Conjugated polymer loaded high-concentration monatomic metal site heterogeneous catalyst and preparation method thereof

A technology of conjugated polymers and heterogeneous catalysts, applied in organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, chemical instruments and methods, etc. Construct high-loaded single-atom sites, shape and crystal phase changes, etc., to achieve the effect of simple preparation methods

Pending Publication Date: 2022-07-08
BEIJING UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, on the one hand, high-temperature treatment will change the carrier itself (such as morphology, defects, and crystal phase); on the other hand, metal species are easy to cluster and form particles at high temperature, which makes it impossible to construct high-loaded single-atom sites.
For conjugated polymer semiconductors, most materials may undergo pyrolysis or carbonization to varying degrees above 400 °C, so it is very important to construct high-loaded single-atom metal sites on conjugated polymer semiconductors by general high-temperature treatment. difficult

Method used

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  • Conjugated polymer loaded high-concentration monatomic metal site heterogeneous catalyst and preparation method thereof
  • Conjugated polymer loaded high-concentration monatomic metal site heterogeneous catalyst and preparation method thereof
  • Conjugated polymer loaded high-concentration monatomic metal site heterogeneous catalyst and preparation method thereof

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Effect test

Embodiment 1

[0050] The present embodiment provides a heterogeneous catalyst with a conjugated polymer (carbon nitride) loaded with a high concentration of single-atom metal (platinum) sites, and the preparation method is as follows:

[0051] 100 mg of carbon nitride was dispersed in 20 mL of toluene, and 8 mg of platinum dibenzylideneacetone was added, followed by mixing and stirring for 3 hours.

[0052] Toluene was removed by rotary evaporation and dried in an oven at 100°C for 5 hours.

[0053] The obtained dry solid was dispersed in 200 mL of water, replaced with argon gas, and illuminated under an LED lamp for 1 hour.

[0054] The light-treated solid was centrifuged and dried in an oven at 100°C for 5 hours.

[0055] After the temperature dropped to room temperature, the solid powder was repeatedly washed with toluene, and then dried in an oven at 100° C. for 5 hours to obtain the target platinum carbon nitride single-atom heterogeneous photocatalyst.

[0056] The platinum loading ...

Embodiment 2

[0059] The present embodiment provides a conjugated polymer (modified carbon nitride) loaded heterogeneous catalyst with high concentration of single-atom metal (palladium) sites, and its preparation method is as follows:

[0060] 1 g of modified carbon nitride (phosphorus-doped carbon nitride) was dispersed in 100 mL of cyclohexane, then 300 mg of bis(tri-tert-butylphosphine)palladium was added, and the mixture was mixed and stirred for 24 hours.

[0061] Cyclohexane was removed by rotary evaporation and dried in an oven at 70°C for 15 hours.

[0062] The obtained dry solid was dispersed in 1 L of water, nitrogen was replaced, and the mixture was exposed to sunlight for 10 hours.

[0063] The light-treated solids were centrifuged and dried in an oven at 120°C for 3 hours.

[0064] After the temperature dropped to room temperature, the solid powder was repeatedly washed with cyclohexane, and then dried in an oven at 70° C. for 15 hours to obtain the target palladium-modified ...

Embodiment 3

[0068] The present embodiment provides a heterogeneous catalyst with a conjugated polymer (covalent organic framework) loaded with a high concentration of single-atom metal (copper) sites, and the preparation method is as follows:

[0069] 100 mg of the covalent organic framework (COF-LZU-1) was dispersed in 20 mL of dichloromethane, then 15 mg of copper bis(acetylacetonate) was added, and the mixture was mixed and stirred for 8 hours.

[0070] The dichloromethane was removed by evaporation in a fume hood and dried in an oven at 50°C for 8 hours.

[0071] The resulting dry solid was dispersed in 150 mL of water and illuminated under a xenon lamp for 6 hours under air.

[0072] The light-treated solid was centrifuged and dried in an oven at 150°C for 2 hours.

[0073] After the temperature dropped to room temperature, the solid powder was repeatedly washed with dichloromethane, and then dried in an oven at 50° C. for 8 hours to obtain the target copper covalent organic framewo...

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Abstract

The invention provides a conjugated polymer loaded high-concentration monatomic metal site heterogeneous catalyst and a preparation method thereof. The preparation method comprises the following steps: by taking a conjugated polymer and a metal-complex precursor as raw materials, inducing ligand exchange through illumination radiation; the conjugated polymer is carbon nitride, a carbon nitride derivative, a covalent organic framework, a linear organic conjugated polymer or a composite material formed by one or more of carbon nitride, a carbon nitride derivative, a covalent organic framework and a linear organic conjugated polymer; the general formula of the metal-complex precursor is MLnXm, and the transition metal M is one or more of platinum, rhodium, palladium, gold, silver, ruthenium, iridium, copper, iron, cobalt and nickel; the organic ligand L is one or more of triphenylphosphine, tri-tert-butylphosphine, bipyridine, dibenzylideneacetone, acetylacetone, hexafluoroacetylacetone, trifluoroacetylacetone, dibenzoylacetone, benzoylacetone, octyl-1, 5-diene, methyl and carbonyl, and n is equal to 1 to 4; halogen X is Cl or Br, and m is 0-3.

Description

technical field [0001] The invention relates to the technical field of catalyst preparation, in particular to a heterogeneous catalyst with a high concentration of single-atom metal sites supported on a conjugated polymer semiconductor and a preparation method thereof. Background technique [0002] Compared with traditional inorganic oxide supports and carbon black supports, the structure of conjugated polymer semiconductors is flexible and can be synthesized from synthetic Structural regulation at the molecular level is easy and inexpensive. Conjugated polymer semiconductors generally have a certain degree of amphiphilicity, including a hydrophobic organic conjugated framework structure, as well as hydrophilic end groups and defect sites. Selective regulation in heterogeneous catalysis. In addition, conjugated polymer semiconductors generally have good light absorption properties, and even most of them respond to visible light. Therefore, catalysts supported by them can b...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J31/28B01J31/06
CPCB01J27/24B01J31/28B01J31/06B01J35/39Y02P20/584
Inventor 宗绪鹏孙再成
Owner BEIJING UNIV OF TECH
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