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Metal@BN core-shell structure nanometer catalyst for synthesis gas methanation reaction, and preparation method thereof

A nano-catalyst and metal nano-particle technology, applied in physical/chemical process catalysts, chemical instruments and methods, and hydrocarbon production from carbon oxides, etc., can solve complex catalyst preparation methods, unsuitable for large-scale preparation, catalyst deactivation, etc. problems, to achieve the effects of avoiding catalyst deactivation, preventing sintering and loss, high and low temperature activity and high temperature stability

Active Publication Date: 2016-12-07
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Second, metal sintering leads to catalyst deactivation
Third, metal loss leads to catalyst deactivation
However, the preparation method of the catalyst is complicated, and the raw materials used involve toxic ammonium metavanadate, which is not suitable for large-scale preparation

Method used

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  • Metal@BN core-shell structure nanometer catalyst for synthesis gas methanation reaction, and preparation method thereof
  • Metal@BN core-shell structure nanometer catalyst for synthesis gas methanation reaction, and preparation method thereof
  • Metal@BN core-shell structure nanometer catalyst for synthesis gas methanation reaction, and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0023] 1. Preparation of 20wt.% Ni / SiO by impregnation method 2 Catalyst: Dissolve 0.805g of nickel chloride hexahydrate in 4ml of deionized water, then add 2ml of absolute ethanol and stir evenly, then add 0.806g of silica carrier, stir and evaporate to dryness at room temperature; the sample is heated in hydrogen at 450°C Reduction treatment for 2h to obtain 20wt.%Ni / SiO 2 -H 2 Nano catalyst;

[0024] 2. Impregnate 20wt.% Ni / SiO with a boric acid aqueous solution with a concentration of 0.374mol / L 2 -H 2 Catalyst, wherein the B / Ni atomic ratio is 3:1, stirred and volatilized to dryness, and dried at 60°C for 12h; further in NH 3 Nitriding treatment at 850°C for 1 hour in the atmosphere to obtain 20wt.% Ni 1 @(BN) 3 / SiO 2 Core-shell structured nanocatalytic materials.

[0025] High-resolution electron microscopy (see figure 1 ) shows that SiO 2 The surface of the loaded Ni nanoparticles is covered by boron nitride to form a core-shell structure. X-ray diffraction ...

Embodiment 2

[0027] 1. Dissolve 0.248g of nickel nitrate hexahydrate in 4ml of deionized water, then add 2ml of absolute ethanol and stir evenly, then add 0.95g of silica carrier, stir and volatilize at room temperature until dry; further put the sample in hydrogen at 650°C Reduction treatment for 2h to obtain 5wt.%Ni / SiO 2 -H 2 Nano catalyst;

[0028] 2. Immerse 5wt.% Ni / SiO with a boron trioxide aqueous solution with a concentration of 0.374mol / L 2 -H 2 Catalyst, wherein the B / Ni atomic ratio is 1:10, stirred and volatilized to dryness, and dried at 60°C for 12h; 2 Nitriding treatment at 750°C for 1 hour in the atmosphere to obtain 5wt.% Ni 10 @(BN) 1 / SiO 2 Core-shell structured nanocatalytic materials.

Embodiment 3

[0030] 1. Dissolve 0.805g of nickel chloride hexahydrate with 4ml of deionized water, then add 2ml of absolute ethanol and stir evenly, then add 0.806g of silica carrier, stir and volatilize to dryness at room temperature, and further place the sample in hydrogen for 500 ℃ reduction treatment for 2h to get 20wt.%Ni / SiO 2 -H 2 Nano catalyst;

[0031] 2. Impregnate 20wt.% Ni / SiO with a boric acid aqueous solution with a concentration of 0.374mol / L 2 -H 2 Catalyst, wherein the B / Ni atomic ratio is 1:1, stirred and volatilized to dryness, dried at 60°C for 12h, and further put the sample in NH 3 Nitriding treatment at 850°C for 1 hour in the atmosphere to obtain 20wt.% Ni 1 @(BN) 1 / SiO 2 Core-shell structured nanocatalytic materials.

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Abstract

The invention discloses a metal@BN core-shell structure nanometer catalyst for a synthesis gas methanation reaction, and a preparation method thereof. According to the present invention, the composition of the catalyst is 5-30wt.%Mx@(BN)y / SiO2, wherein metal M nanoparticles are loaded on a SiO2 support, the loading mass percentage is 5-30%, an ultrathin boron nitride (BN) layer is covered on the surface, the catalyst has a core-shell structure, and a molar ratio y / x of the BN to the metal nanoparticles is 0.1-10; with the application of the catalyst in the methane preparation reaction through the hydrogenation of the catalytic synthesis gas, the sintering and the loss of the metal nanoparticles can be prevented, and the catalyst deactivation caused by the carbon deposition on the catalyst active site surface can be prevented with the core-shell structure; and the catalyst has high low-temperature activity and high high-temperature stability.

Description

technical field [0001] The invention relates to a metal@BN core-shell structure nano-catalyst used for synthesis gas methanation reaction and a preparation method thereof. Background technique [0002] With the increasingly tense world energy supply and people's urgent demand for clean energy, coal-to-natural gas technology has attracted widespread attention. Synthetic natural gas can not only enrich the composition of energy, but also reduce the import of natural gas. Combined with the specific national conditions of our country, which is relatively "rich in coal and low in oil", it is possible to pressure-gasify and methanize scattered coal and transport it through pipelines for centralized supply, thereby improving people's quality of life and improving the ecological environment. [0003] For the methanation reaction of syngas, noble metal catalysts have quite high catalytic activity at low temperature. However, due to the limited natural reserves of precious metals in...

Claims

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Application Information

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IPC IPC(8): B01J27/24B01J35/02C07C9/04C07C1/04
Inventor 傅强高丽君包信和
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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