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Molybdenum carbide supported monatomic hydrogenation catalyst, preparation method thereof and application thereof in alkyne semi-hydrogenation

A hydrogenation catalyst and atomic chemistry technology, applied in the field of hydrogenation, can solve problems such as selectivity reduction, and achieve the effects of increased selectivity, high activity and strong stability

Active Publication Date: 2020-07-10
TIANJIN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Common, supported amorphous nickel catalysts have high activity in the hydrogenation reaction of acetylene, but as the use time increases, the selectivity to ethylene will decrease sharply and only maintain about 50%

Method used

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  • Molybdenum carbide supported monatomic hydrogenation catalyst, preparation method thereof and application thereof in alkyne semi-hydrogenation
  • Molybdenum carbide supported monatomic hydrogenation catalyst, preparation method thereof and application thereof in alkyne semi-hydrogenation

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preparation example Construction

[0044] In another aspect of the present invention, the present invention provides a kind of preparation method of aforementioned hydrogenation catalyst, comprising:

[0045] Loading a metal single atom on a carrier, wherein the carrier includes MoC, and the metal single atom is chemically bonded to the molybdenum atom in the MoC;

[0046] Wherein, the metal single atom includes at least one of single-atom nickel, single-atom cobalt and single-atom copper.

[0047] In some embodiments of the present invention, the preparation method includes:

[0048] Mix citric acid with metal salt to obtain chelate;

[0049] The solid obtained after mixing the chelate compound with the carrier is calcined in a reducing atmosphere to obtain the hydrogenation catalyst.

[0050] Under the action of the organic molecule citric acid, the metal single atom will form a bond with the Mo atom exposed on the surface of MoC to form a metal single atom with metal characteristics, and then the metal sin...

Embodiment 1

[0070] The preparation method of hydrogenation catalyst is as follows:

[0071] 1. The preparation of carrier α-MoC: using ammonium molybdate as the precursor, place it in the atmosphere furnace, replace it with inert gas, and then pass it into NH 3 , at a heating rate of 5°C / min to 700°C and baked for 2 hours, followed by inert gas replacement; then CH 4 , heating up to 1200°C at a heating rate of 5°C / min and roasting for 2 hours, then cooling to room temperature to obtain α-MoC;

[0072] 2. Using α-MoC as a carrier, mix it with nickel nitrate and citric acid chelate aqueous solution at room temperature, then wash and centrifuge to obtain a uniformly mixed solid, in which the molar ratio of citric acid to nickel nitrate is 2:1, nitric acid The mass ratio of nickel element to α-MoC in nickel is 0.5%:1;

[0073] 3. Calcining the solid obtained in step 2 at 300° C. for 2 hours in a hydrogen atmosphere to obtain a hydrogenation catalyst.

Embodiment 2

[0075] The preparation method of hydrogenation catalyst is as follows:

[0076] 1. The preparation of carrier α-MoC: using ammonium molybdate as the precursor, place it in the atmosphere furnace, replace it with inert gas, and then pass it into NH 3 , at a heating rate of 5°C / min to 700°C and baked for 2 hours, followed by inert gas replacement; then CH 4 , heating up to 1200°C at a heating rate of 5°C / min and roasting for 2 hours, then cooling to room temperature to obtain α-MoC;

[0077] 2. Using α-MoC as a carrier, mix it with nickel nitrate and citric acid chelate aqueous solution at room temperature, and then wash and centrifuge to obtain a uniformly mixed solid, wherein the molar ratio of citric acid to nickel nitrate is 3:1, and nitric acid The mass ratio of nickel element to α-MoC in nickel is 0.5%:1;

[0078] 3. Calcining the solid obtained in step 2 at 300° C. for 2 hours in a hydrogen atmosphere to obtain a hydrogenation catalyst.

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Abstract

The invention provides a molybdenum carbide supported monatomic hydrogenation catalyst, a preparation method thereof and an application of the molybdenum carbide supported monatomic hydrogenation catalyst in alkyne semi-hydrogenation, which relates to the technical field of hydrogenation, the hydrogenation catalyst comprises: a carrier comprising MoC; and a metal single atom, the metal single atomis loaded on the carrier, and the metal single atom is chemically bonded with a molybdenum atom in the MoC, wherein the metal single atoms comprise at least one of single-atom nickel, single-atom cobalt and single-atom copper. The hydrogenation catalyst shows extremely high activity and 100% selectivity in semi-hydrogenation of acetylene.

Description

technical field [0001] The invention relates to the technical field of hydrogenation, in particular to a molybdenum carbide supported single-atom hydrogenation catalyst, its preparation method and its application in alkyne semi-hydrogenation. Background technique [0002] The selective hydrogenation of acetylene has great economic significance in production. For example, ethylene gas produced by petroleum cracking usually contains 0.1% to 1.0% of acetylene impurities, and the presence of acetylene poisons the catalyst in the ethylene polymerization process and affects polyethylene. The quality, so to remove trace acetylene in ethylene gas. At present, palladium catalysts can be used to selectively hydrogenate acetylene to produce ethylene. However, considering the limited palladium resources and high cost, some transitional non-noble metals (such as nickel and copper) are commonly used as alternative components of noble metal catalysts. Commonly, the supported amorphous nic...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/22B01J37/08B01J37/18C07C5/09C07C11/04C07C15/46
CPCB01J27/22B01J37/0018B01J37/18C07C5/09C07C2527/22C07C11/04C07C15/46Y02P20/52
Inventor 邹吉军高睿杰潘伦张香文
Owner TIANJIN UNIV