Samarium manganese mullite type nickel-based catalyst for hydrogen production by autothermal reforming of acetic acid

A nickel-based catalyst, autothermal reforming technology, applied in the direction of metal/metal oxide/metal hydroxide catalyst, physical/chemical process catalyst, hydrogen, etc., can solve the problem of reducing active site exposure, reducing catalyst activity, catalyst Problems such as agglomeration and sintering can achieve the effect of improving anti-coke ability, excellent thermal stability, and improving transfer ability

Active Publication Date: 2022-04-12
CHENGDU UNIVERSITY OF TECHNOLOGY
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, although the Ni-based catalyst has high activity, when the acetic acid molecule CH3COOH is adsorbed and activated on the Ni-based catalyst, the formed CH3COOH undergoes a series of dehydrogenation, dehydroxylation, decarboxylation, etc. sub>3COO*, CH3CO*, CH3* and other intermediate species further break bonds to form C* species, and a large number of C* Agglomerated to form carbon deposits, covering the surface of Ni-based catalysts, reducing the exposure of active sites, which in turn reduces the activity of the catalyst and leads to deactivation
In addition, in the process of autothermal reforming hydrogen production of acetic acid, due to the existence of the front end region of the catalyst bed as high as 1000 °C, the catalyst is prone to agglomeration and sintering. At the same time, in the oxidizing atmosphere, the active metal Ni is more easily oxidized, thereby reducing the catalyst activity, and even deactivation of the catalyst

Method used

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  • Samarium manganese mullite type nickel-based catalyst for hydrogen production by autothermal reforming of acetic acid
  • Samarium manganese mullite type nickel-based catalyst for hydrogen production by autothermal reforming of acetic acid

Examples

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Effect test

example 1

[0024] Weigh 2.000g of γ-Al 2 o 3 Pour it into a beaker while weighing 0.866g of Ni(NO 3 ) 2 ·6H 2 O, add a certain amount of deionized water to dissolve, and then add dropwise to γ-Al 2 o 3 middle; placed at room temperature for 12h, dried, and then calcined in a tube furnace at 700°C for 4h to obtain the CDUT-NA catalyst, which formed a catalyst supported on γ-Al 2 o 3 The Ni-based catalyst on the catalyst; the weight percentage of the catalyst in terms of oxides consists of: nickel oxide (NiO) is 10.0%, γ-Al 2 o 3 was 90.0%.

[0025] The reactivity evaluation of autothermal reforming of acetic acid was carried out in a continuous flow fixed bed reactor. Grind and tablet the catalyst, then sieve it into 20-40 mesh particles, weigh 0.1-0.2g and put it into the reactor, and put it under H at a temperature of 500-800°C 2 The mixture solution of acetic acid and water was then injected into the vaporizer with a constant flow pump and vaporized, mixed with oxygen, and ni...

Embodiment 1

[0028] Weigh 7.203g of Sm(NO 3 ) 3 ·6H 2 O and 6.532g of Mn(CH 3 COO) 2 4H 2 O, dissolved in 30ml of ethylene glycol and 20ml of ethanol solution, stirred for 24h, placed in an oven at 80°C for 8h, then placed in a muffle furnace and roasted at 500°C for 8h, and finally roasted in a tube furnace at 800°C for 8h , to obtain samarium manganese mullite oxide SmMn 2 o 5 Carrier, add 20ml of water, stir to form a suspension; prepare a nickel nitrate solution, add it to the suspension of samarium manganese mullite, add ammonia water, adjust the pH value to 11±0.5, keep it in a water bath at 60°C for 3 hours, put it in 80 ℃ oven for 10 hours, and then baked in a tube furnace at 750 ℃ ​​for 5 hours to obtain the CDUT-NSM-18 catalyst, forming a catalyst supported on SmMn 2 o 5 spinel NiMn on 2 o 4 Oxide and a small amount of NiO, after reduction, a mesoporous structure with Ni-Mn-Sm-O active centers is obtained, and the pore size is concentrated at 4nm. Its typical crystal st...

Embodiment 2

[0031] Weigh 7.203g of Sm(NO 3 ) 3 ·6H 2 O and 6.532g of Mn(CH 3 COO) 2 4H 2 O, dissolved in 30ml of ethylene glycol and 20ml of ethanol solution, stirred for 24h, placed in an oven at 80°C for 8h, then placed in a muffle furnace and roasted at 500°C for 8h, and finally roasted in a tube furnace at 800°C for 8h , to obtain samarium manganese mullite oxide SmMn 2 o 5 Carrier, add 20ml of water, stir to form a suspension; prepare a nickel nitrate solution, add it to the suspension of samarium manganese mullite, add ammonia water, adjust the pH value to 11±0.5, keep it in a water bath at 60°C for 3 hours, put it in 80 ℃ in an oven for 10 h, and then baked in a tube furnace at 750 °C for 5 h to obtain 2 o 5 spinel-containing NiMn 2 o 4 A CDUT-NSM-15 catalyst with a mesoporous structure of oxide and Ni-Mn-Sm-O active center; the catalyst is composed of 15.0% nickel oxide NiO, mullite oxide SmMn 2 o 5 was 85.0%.

[0032] Catalyst CDUT-NSM-15 was investigated by autother...

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Abstract

The invention relates to a samarium manganese mullite type nickel-based catalyst for hydrogen production by autothermal reforming of acetic acid. The invention provides a novel catalyst which is high in activity, resistant to carbon deposition and resistant to oxidation aiming at the inactivation problem of an existing catalyst in the autothermal reforming process of acetic acid. The chemical component of the catalyst is (NiO) a (SmMn2O5) b, a ranges from 0.107 to 0.281, and b ranges from 0.232 to 0.270. According to the preparation method, Ni species are loaded on a SmMn2O5 carrier by adopting an impregnation-precipitation method, and a novel catalyst which contains a stable NiMn2O4 spinel structure and has a Ni-Mn-Sm-O active center is formed through roasting. The catalyst provided by the invention effectively promotes the conversion of acetic acid, inhibits the generation of by-products such as acetone, and improves the yield and reaction stability of hydrogen.

Description

technical field [0001] The present invention relates to a specific samarium manganese mullite type oxide SmMn 2 o 5 The preparation method of the supported Ni-based catalyst and its application in the process of producing hydrogen by autothermal reforming of acetic acid belong to the technical field of producing hydrogen by autothermal reforming of acetic acid. Background technique [0002] The sustainable use of energy is an eternal problem. At present, social and economic development mainly depends on fossil energy, and the massive consumption of fossil energy not only causes environmental pollution, but also affects the sustainable development of economy. Therefore, the development of renewable energy has become particularly important, among which clean hydrogen energy has attracted great attention. In the traditional chemical industry production process, hydrogen energy is often obtained through the processing of fossil resources such as natural gas and coal, but the ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/889B01J35/10C01B3/22
Inventor 黄利宏徐映春陈慧
Owner CHENGDU UNIVERSITY OF TECHNOLOGY
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