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Th-MOF loaded Cu-based single-site catalytic material as well as preparation method and application thereof

A catalytic material and single-site technology, applied in electrolytic components, electrodes, electrolytic processes, etc., can solve the problem of low catalytic activity of catalysts

Active Publication Date: 2021-09-14
EAST CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] The present invention is to solve the technical problem of low catalytic activity of existing catalysts, and provides a Th-MOF supported Cu-based single-site catalytic material and its preparation method and application

Method used

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  • Th-MOF loaded Cu-based single-site catalytic material as well as preparation method and application thereof
  • Th-MOF loaded Cu-based single-site catalytic material as well as preparation method and application thereof
  • Th-MOF loaded Cu-based single-site catalytic material as well as preparation method and application thereof

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Experimental program
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Embodiment 1

[0029] Embodiment 1: The preparation method of a Th-MOF supported Cu-based single-site catalytic material of this embodiment is carried out according to the following steps:

[0030] Step 1. Preparation of Th-MOF material: Dissolve 1 mmol of thorium nitrate hexahydrate and 1 mmol of 2,2'-bipyridine-5,5'-dicarboxylic acid in 3 mL of N,N'-dimethylformamide solution, then add 1mmol of nitric acid, stir evenly, transfer to a polytetrafluoroethylene lining, seal it and put it into a high-pressure reactor, heat it to 110°C at a heating rate of 1°C / min in a muffle furnace and keep the temperature constant Reacted for 3 days, centrifuged after the reaction, washed with methanol, and vacuum-dried at a temperature of 70 ° C to obtain a colorless octahedral crystal Th-BPYDC (see figure 1 ), namely Th-MOF material;

[0031] Step 2, preparing a precursor solution containing copper ions: dissolving 0.5 g of copper chloride in 5 mL of acetonitrile solution to prepare a precursor solution co...

Embodiment 2

[0035] Example 2: The Th-MOF-loaded Cu-based single-site catalytic material (Cu@Th-BPYDC) prepared in Example 1 was used in the electroreduction of NO 3 - Application in synthetic ammonia.

[0036]Electroreduction of NO with Cu@Th-BPYDC prepared in Example 1 3 - Synthetic ammonia, the result is as Figure 4-Figure 8 shown.

[0037] Depend on Figure 4 It can be seen that the Cu@Th-BPYDC of Example 1 has excellent electroreduction of NO 3 - Ammonia performance with current density up to 80.7mA cm at -0.1Vvs RHE potential -2 , much better than Cu-free Th-BPYDC. With the increase of cathode potential, the rate of ammonia formation gradually increased ( Figure 5 ), but the Faradaic efficiency presents a volcanic trend of first increasing and then decreasing ( Figure 6 ), the ammonia formation rate and Faradaic efficiency are as high as 225.3 μmol h at the optimal voltage -0.1 V vs RHE -1 cm -2 and 92.5%. The Cu@Th-BPYDC single-site catalyst has excellent stability, ...

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Abstract

The invention discloses a Th-MOF loaded Cu-based single-site catalytic material as well as a preparation method and application thereof. The invention belongs to the field of catalytic materials. The invention aims to solve the technical problem that an existing catalyst is low in catalytic activity. The catalytic material is composed of a single-site Cu and a Th-MOF material, the Th-MOF material is Th-BPYDC, the Th-MOF material is of a regular octahedron structure, and the space site group is Fm3m. The method comprises the steps of 1, preparing a Th-MOF material; 2, preparing a precursor solution containing copper ions; and 3, preparing the Th-MOF loaded Cu-based single-site catalytic material. The invention also relates to application of the Th-MOF loaded Cu-based single-site catalytic material in an electro-reduction NO3-ammonia synthesis reaction. The obtained catalytic material can achieve an ammonia generation rate up to 225.3 [mu] mol.h<-1 >.cm <-2 > and a Faraday efficiency of 92.5%.

Description

technical field [0001] The invention belongs to the field of catalytic materials, and in particular relates to a Th-MOF loaded Cu-based single-site catalytic material and a preparation method and application thereof. Background technique [0002] As one of the most common industrial chemicals, ammonia plays an important role in the national economy. It not only plays an important role in agriculture, textile industry, pharmaceutical industry and other fields, but also can be used by humans as a new generation of high energy density green carrier (4.3kWh / kg). At present, the industry mainly uses the traditional Haber-Bosch method to synthesize ammonia. This process uses nitrogen and hydrogen as raw materials, and the reaction conditions are harsh. It is a synthetic route that consumes a lot of energy. The current electroreduction ammonia synthesis technology using NO3- as raw material and water as hydrogen source has attracted widespread attention because of its greenness, h...

Claims

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Application Information

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IPC IPC(8): C25B11/095C25B1/27
CPCC25B11/095C25B1/27
Inventor 高志赖玉莲陶源王悦
Owner EAST CHINA UNIV OF TECH
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