Silicon-based covalent organic framework photoelectrode and preparation method and application thereof

A covalent organic framework and photoelectrode technology, which is applied in chemical instruments and methods, physical/chemical process catalysts, catalyst regeneration/reactivation, etc., can solve the problem of photocatalyst and electronic mediator loss, limited improvement of regeneration efficiency, The number of electrons is small, etc., to achieve the effect of improving electron transfer efficiency, preventing corrosion, and being easy to obtain

Pending Publication Date: 2022-07-01
THE NAT CENT FOR NANOSCI & TECH NCNST OF CHINA
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the number of photogenerated electrons generated by the photocatalyst itself is relatively small, and it is easy to recombine, so the photocatalyst after the immobilized [Cp*Rh(bpy)Cl]Cl can improve the regeneration efficiency of the coenzyme NAD(P)H is relatively limited.
And the photocatalyst needs to be re-dried and dispersed after use, which will also cause the loss of photocatalyst and electronic mediator
[0006] However, relevant research results are relatively lacking in the field of photoelectrochemical coenzyme regeneration, so it is necessary to develop a new photoelectrode for photoelectrochemical coenzyme NAD(P)H regeneration to enhance the electron transfer efficiency between the electron mediator and the electrode. In this way, the efficiency of coenzyme regeneration can be effectively improved, and at the same time, the in-situ recovery and utilization of electronic mediators can be realized, and the loss of electronic mediators can be reduced to achieve large-scale applications.

Method used

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  • Silicon-based covalent organic framework photoelectrode and preparation method and application thereof
  • Silicon-based covalent organic framework photoelectrode and preparation method and application thereof
  • Silicon-based covalent organic framework photoelectrode and preparation method and application thereof

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Embodiment 1

[0075] This embodiment provides a preparation method of a silicon-based covalent organic framework photoelectrode, and the preparation method includes the following steps:

[0076] (1) Prepare the silicon substrate used in the electrode, cut the P-type silicon to a size of 1 cm×1 cm, and use acetone, isopropanol and ethanol for ultrasonic cleaning in sequence;

[0077] (2) prepare a metal foil with graphene, and spin-coat a layer of polymethyl methacrylate support layer on the graphene, then use a mixed aqueous solution of copper sulfate and hydrochloric acid as an etching solution to remove the metal foil to obtain graphene / polymethyl methacrylate film, after the graphene / polymethyl methacrylate film is washed multiple times and then transferred to a silicon substrate, after drying, soaked in remover acetone to remove polymethyl methacrylate, Finally, use isopropanol and / or water to clean, and use nitrogen to dry, form an electron conduction layer, and obtain a first compos...

Embodiment 2

[0081] This embodiment provides a method for preparing a silicon-based covalent organic framework photoelectrode, except that in step (3), 0.6 mg of 5,10,15,20-tetrakis(4-aminophenyl) is dissolved by ultrasonic waves Porphyrin and 0.3 mg of 2,2'-bipyridine-5,5'-dicarbaldehyde were subjected to a solvothermal reaction at 140°C for 2 days and stirring for 4h in step (4), other conditions and Example 1 Exactly the same.

Embodiment 3

[0083] This embodiment provides a method for preparing a silicon-based covalent organic skeleton photoelectrode. In the method, in addition to using a mixed solvent consisting of 1 mL of tetrahydrofuran, 7 mL of ethanol and 1 mL of acetic acid to dissolve 0.45 mg of 5, 10, 15 , 20-tetrakis(4-aminophenyl)porphyrin and 0.3 mg of 2,2'-bipyridine-5,5'-dicarbaldehyde in a solvothermal reaction at 160°C for 1 day and step (4) The other conditions were exactly the same as in Example 1, except that the mixture was stirred for 8 h.

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Abstract

The invention provides a silicon-based covalent organic framework photoelectrode and a preparation method and application thereof. The silicon-based covalent organic framework photoelectrode comprises a silicon substrate, and an electron conduction layer, a covalent organic framework layer and an electron mediator layer which are sequentially arranged on one side of the silicon substrate from bottom to top. According to the invention, the electron mediator is fixed on the covalent organic framework layer in a mode of forming coordinate bonds, electron transfer between the electron mediator and the covalent organic framework layer can be greatly promoted, and meanwhile, the photoelectrode is constructed into a stacked arrangement structure, so that efficient transfer of electrons between layers can be promoted; and finally, the electron transfer efficiency between the electron mediator and the silicon substrate is improved, and in-situ recovery and utilization of the electron mediator are realized. By means of the photoelectrode, the catalytic activity of photoelectrochemical coenzyme NAD (P) H regeneration can be effectively improved, meanwhile, the preparation method is simple and convenient, complex operation is not needed, and large-scale application in industrial production is facilitated.

Description

technical field [0001] The invention belongs to the technical field of photoelectrochemical coenzyme regeneration, and relates to a photoelectrode and a preparation method thereof, in particular to a silicon-based covalent organic skeleton photoelectrode and a preparation method and application thereof. Background technique [0002] In recent years, enzymatic reactions have been widely used in the chemical synthesis industry. Most enzymatic reactions require nicotinamide coenzymes (NAD(P)H / NAD(P) + ) as a direct donor of electrons or protons, and in industrial production, continuous supply of coenzymes is an important condition to ensure the continuous and efficient enzymatic reactions. However, the coenzyme itself is expensive, so how to achieve efficient regeneration and recycling of coenzymes has become an urgent problem to be solved. At present, photochemical, electrochemical and photoelectrochemical methods can be used to achieve coenzyme regeneration, in which photoe...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C08G83/00B01J38/00
CPCC08G83/008B01J38/00Y02P20/584
Inventor 贾鑫蕊宫建茹
Owner THE NAT CENT FOR NANOSCI & TECH NCNST OF CHINA
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