Method for regulating and controlling surface plasmon photocatalysis and application

A plasmonic and photocatalytic technology applied in the field of photocatalysis to achieve the effect of promoting efficiency

Active Publication Date: 2020-09-08
NANJING UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, this literature only proposed a molecule that promotes the water oxidation reaction and did not involve the purpose of regulating the reaction by changing the energy level structure of the modified molecule.

Method used

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  • Method for regulating and controlling surface plasmon photocatalysis and application
  • Method for regulating and controlling surface plasmon photocatalysis and application
  • Method for regulating and controlling surface plasmon photocatalysis and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0027] Example 1: Method principle of different thiol or thiophenol molecules regulating the hot carrier-driven photocatalytic reaction generated by surface plasmons

[0028] figure 1 It is a schematic diagram of the separation behavior of hot carriers in the process of photocatalytic reaction driven by hot carriers generated by different thiol or thiophenol molecules. In the figure, the transfer behavior of hot electrons is taken as an example;

[0029] Table 1 shows the LUMO and HOMO energy levels of some common thiols and thiophenols;

[0030]

[0031] Organic molecules contain the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO), which can be compared to the valence and conduction bands in semiconductors. Similar to metal-semiconductor heterostructures, when molecules are adsorbed on the surface of plasmonic metals, if the energy of excited hot electrons (or hot holes) can be matched with the energy level of LUMO (or HOMO), t...

Embodiment 2

[0032] Embodiment 2: Modification method of thiol or thiophenol molecules

[0033] Under the strong chemical bond between thiol and metal, thiol and thiophenol molecules can be chemisorbed on the surface of plasmonic metal. The specific operation process is as follows:

[0034] Dissolve an appropriate amount of thiol or thiophenol molecules in ethanol, add them to the prepared plasmonic metal nanostructure solution or substrate, mix for about one hour, and a uniform and densely distributed self-assembled molecular layer can be formed on the metal surface . Afterwards, the sample can be washed with ethanol. Such as figure 2 as shown, figure 2 is the Raman signal map of thiophenol molecules adsorbed on silver nanowires, indicating that the molecules are successfully adsorbed on the surface of plasmonic metals; the signals of thiophenol molecules adsorbed on silver nanowires are detected by Raman spectroscopy, indicating successful adsorption of the molecule.

Embodiment 3

[0035] Example 3: Thiol and thiophenol molecules regulate the oxidation reaction of p-aminothiophenol mediated by plasmons

[0036] Silver nanoparticles were used as surface plasmon photocatalysts to catalyze the oxidation of p-aminothiophenol (PATP) to p-mercaptoazobenzene (DMAB). Taking no molecular modification on silver nanoparticles as a blank group, the effects of different thiol and thiophenol molecules on the oxidation process of PATP were quantitatively studied. Among them, the PATP oxidation rate of the blank group was set as 1, and the oxidation rate diagram of PATP after adsorbing different thiol and thiophenol molecules was drawn, image 3 It is the result that different thiols and thiophenols regulate the plasmon-mediated oxidation of p-aminothiophenol. Changing the type of substituents of thiophenol molecules and changing the type of modified molecules can significantly affect the oxidation reaction process of p-aminothiophenol.

[0037] The result is as ima...

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Abstract

The invention provides a method for modifying different mercaptan or thiophenol molecules on the surface of plasmon metal to regulate and control a hot carrier-driven photocatalytic reaction generatedby plasmon. In the method, mercaptan and thiophenol molecules can be chemically adsorbed on the surface of the surface plasmon metal, and the operation process is simple, convenient and rapid. Meanwhile, it has been proved that the method can regulate plasmon-driven oxidation reaction of p-aminothiophenol, reduction reaction of p-nitrothiophenol, silver corrosion reaction, decarboxylation reaction of p-mercaptobenzoic acid and the like.

Description

technical field [0001] The invention relates to a method for regulating a photocatalytic reaction, in particular to a method and application for regulating a photocatalytic reaction driven by hot carriers generated by surface plasmons, and belongs to the technical field of photocatalysis. Background technique [0002] Harvesting solar energy is one of the important methods to solve the global energy crisis and environmental pollution problems, among which photochemical conversion is an effective way to collect solar energy. Initially, semiconductor photocatalysts were designed and used for photochemical conversion, but they suffer from the disadvantages of large optical bandgap and poor photochemical stability. In order to further utilize visible light, the use of plasmonic metal photocatalysts (commonly used materials include: nanostructures of gold, silver, copper, and aluminum) has become an effective method to solve this problem. Exciting plasmons can generate hot carri...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/50B01J21/02B01J23/52B01J23/72B01J31/02B01J35/00C07B61/00C07C319/12C07C323/48C07C321/26
CPCB01J35/004B01J31/0217B01J23/50B01J23/52B01J23/72B01J21/02B01J31/0238B01J31/0271B01J31/0244B01J31/0229B01J31/0235B01J31/0232C07B61/00C07C319/12B01J2231/60B01J2231/70C07C321/26C07C323/48Y02P20/133
Inventor 吕刚张成玉陈钰琴
Owner NANJING UNIV OF TECH
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