Nitrogen-doped tungsten carbide catalyst, and preparation method and application thereof

A tungsten carbide catalyst and nitrogen doping technology, applied in the field of catalysis, can solve the problems of low selectivity and low conversion rate, and achieve the effects of reducing selectivity, improving conversion rate, high activity and stability

Active Publication Date: 2020-05-15
ZHEJIANG NORMAL UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0007] Therefore, the technical problem to be solved in the present invention is to overcome the low efficiency of CO2 catalytic hydrogenation to ethanol and propanol technology in the prior art Conversion rate, low selectivity, reasonable matching of C-C bond formation rate and C-OH bond cleavage rate in CO2 hydrogenation process, thus providing a supported tungsten carbide catalyst as CO 2 Catalysts for the preparation of ethanol and propanol products with high activity and high selectivity

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  • Nitrogen-doped tungsten carbide catalyst, and preparation method and application thereof
  • Nitrogen-doped tungsten carbide catalyst, and preparation method and application thereof
  • Nitrogen-doped tungsten carbide catalyst, and preparation method and application thereof

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Embodiment 1

[0040] This embodiment discloses a nitrogen-doped tungsten carbide catalyst (N-W 2 The specific implementation of C / B) comprises the following steps:

[0041] Add 10mmol ammonium metatungstate and 8mmol hexamethylenediamine into water to mix the solution, impregnate the mixed solution with an equal volume on 5g of HZSM-5 molecular sieve containing B acid sites, let it stand at room temperature for 12h, and then put it in the oven After drying at 100°C for 24 hours, the precursor of nitrogen-doped tungsten carbide catalyst was obtained. The mass fraction of tungsten element in the precursor was measured to be 27%, and the mass fraction of nitrogen element was 0.5%;

[0042] The precursor was heated to 600°C for carbonization in a mixed gas of hydrogen and nitrogen for 4h, wherein the volume fraction of hydrogen in the mixed gas was 10%, and the rate of temperature increase was 1.5°C / min to obtain a nitrogen-doped tungsten carbide catalyst (N-W 2 C / B), such as figure 1 As show...

Embodiment 2

[0044] This embodiment discloses a nitrogen-doped tungsten carbide catalyst (N-W 2 The specific implementation of C / B) comprises the following steps:

[0045] Add 6.8mmol of ammonium metatungstate and 20.4mmol of hexamethylenediamine into water to mix the solution, impregnate the mixed solution on 5g of H-β molecular sieve containing B acid sites, let it stand at room temperature for 12h, and then put it in the oven After drying at 80°C for 18 hours, the precursor of the nitrogen-doped tungsten carbide catalyst was obtained, and the mass fraction of tungsten element in the precursor was measured to be 20%, and the mass fraction of nitrogen element was 1%;

[0046] The precursor was heated to 800°C for carbonization in a mixed gas of hydrogen and helium for 4h, wherein the volume fraction of hydrogen in the mixed gas was 30%, and the rate of temperature increase was 2.0°C / min to obtain a nitrogen-doped tungsten carbide catalyst ( N-W 2 C / B), such as figure 2 As shown, the p...

Embodiment 3

[0048] This embodiment discloses a nitrogen-doped tungsten carbide catalyst (N-W 2 The specific implementation of C / B) comprises the following steps:

[0049] Add 15.3mmol of ammonium metatungstate and 19.2mmol of hexamethylenediamine into water to mix the solution, impregnate the mixed solution on 5g of H-Y molecular sieve containing B acid sites, let it stand at room temperature for 12h, and then place it in an oven at 120°C After drying for 24 hours, the precursor of nitrogen-doped tungsten carbide catalyst was obtained, and the mass fraction of tungsten element in the precursor was measured to be 36%, and the mass fraction of nitrogen element was 0.8%;

[0050] The precursor was heated to 700°C for carbonization in a mixed gas of hydrogen and nitrogen for 2h, wherein the volume fraction of hydrogen in the mixed gas was 40%, and the rate of temperature increase was 1.0°C / min, to obtain a nitrogen-doped tungsten carbide catalyst (N-W 2 C / B), such as image 3 As shown, the ...

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Abstract

The invention relates to the technical field of catalysis, and concretely relates to a nitrogen-doped tungsten carbide catalyst, and a preparation method and an application thereof. The nitrogen-dopedtungsten carbide catalyst comprises a nitrogen-doped tungsten carbide active center and a carrier containing a B acid site, the nitrogen-doped tungsten carbide active center is nitrogen-doped tungsten carbide nanoparticles, the particle size of the nitrogen-doped tungsten carbide nanoparticles is less than or equal to 10 nm, CO2 can be converted into ethanol and propanol products with high addedvalues, and the conversion rate and the selectivity of ethanol and propanol are remarkably improved. The co-impregnation preparation method is adopted, and the method is simple and convenient, the concentration of a metal salt solution does not need to be strictly controlled, and the content of C and N in the prepared catalyst active center is reasonably matched, so that the catalyst has high activity and stability; and a W2C electron structure is regulated, so that the C-C bond generation rate and the C-O bond breaking rate during the CO2 hydrogenation process are effectively regulated, theselectivity of the C1 product is substantially reduced, the selectivity of the ethanol and propanol products is improved, and the wide application prospect is provided.

Description

technical field [0001] The invention relates to the technical field of catalysis, in particular to a nitrogen-doped tungsten carbide catalyst and its preparation and application. Background technique [0002] Ethanol and propanol are very important organic solvents and basic chemical raw materials, and their uses are very extensive. Ethanol can be used to manufacture chemical raw materials such as acetaldehyde, ether, ethyl acetate, ethylamine, etc., and can also be transferred into gasoline as a vehicle fuel; Alcohol can be used to synthesize bulk chemicals such as propyl acetate, glycol ether, and propylamine, as well as pharmaceutical and pesticide supplies such as propylparaben, perfluoropropionic acid, and trifluralin; ethanol and propanol are used in the defense industry , Medical and health, organic synthesis, food industry, industrial and agricultural production have a wide range of uses. [0003] The existing ethanol preparation methods mainly include fermentation ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/48B01J29/78B01J29/16B01J29/26B01J27/24C07C31/08C07C31/10C07C29/156C07C29/153
CPCB01J29/48B01J29/7815B01J29/166B01J29/26B01J27/24B01J35/023C07C29/156C07C29/153B01J2229/186B01J2229/40C07C2529/16C07C2529/26C07C2529/48C07C2529/78C07C31/08C07C31/10Y02P20/52
Inventor 马睿李亚云杨冠恒张瑜珑刘瑞新卢信清王宁伟王雪彭安娜许春慧涂高美朱伟东
Owner ZHEJIANG NORMAL UNIVERSITY
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