Mullite-loaded W-promoted Co-based catalyst for hydrogen production by auto-thermal reforming of acetic acid

An autothermal reforming and catalyst technology, applied in metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, heterogeneous catalyst chemical elements, etc., can solve the problem of easy oxidation and easy sintering of active metals. And other issues

Active Publication Date: 2021-05-04
CHENGDU UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0011] The problem to be solved by the present invention is that in the process of hydrogen production by autothermal reforming of acetic acid in the existing catalysts, there are a large number of C* species formed by acetic acid molecules through a series of dehydrogenation and deoxygenation transformations, and too many C* species Carbon is deposited on the surface of the catalyst. At the same time, in the process of autothermal reforming, the active metal Co is easy to sinter and oxidize. It provides a new catalyst with good thermal stability, sintering resistance, oxidation resistance and carbon deposition resistance.

Method used

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  • Mullite-loaded W-promoted Co-based catalyst for hydrogen production by auto-thermal reforming of acetic acid
  • Mullite-loaded W-promoted Co-based catalyst for hydrogen production by auto-thermal reforming of acetic acid

Examples

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Effect test

example 1

[0029] Take by weighing 18.753g aluminum nitrate nonahydrate (Al(NO 3 ) 3 9H 2 (O) and 2.322g tetraethyl orthosilicate (TEOS) were added into 80mL ethanol to obtain a white solution, and 36.701g ammonium carbonate ((NH 4 ) 2 CO 3 ) into the white solution, heated in a water bath at 60°C and vigorously stirred for 5 hours, dried in an oven at 120°C for 64 hours, and then calcined in a muffle furnace at 1200°C for 4 hours to obtain the carrier Mullite; 1.166g cobalt nitrate and 1.314g Dissolve ammonium tungstate in deionized water, stir thoroughly for 3 hours, then add 1.60g Mullite carrier, continue stirring for 2 hours, put it in an oven at 105°C for 16 hours, and then bake it in a tube furnace at 700°C for 4 hours to obtain CWM-V Catalyst, the weight percentage of this catalyst is composed of: cobalt oxide (CoO) is 15.0%, tungsten oxide (WO 3 ) is 5.0%, Mullite (3Al 2 o 3 -2SiO2 2 ) is 80.0%.

[0030] The reactivity evaluation of autothermal reforming of acetic acid ...

Embodiment 1

[0033] Take by weighing 18.753g aluminum nitrate nonahydrate (Al(NO 3 ) 3 9H 2 O) and 2.322g tetraethyl orthosilicate (TEOS) were added into 80mL ethanol to obtain a white solution, and 36.701g ammonium carbonate ((NH 4 ) 2 CO 3 ) into the white solution, heated in a water bath at 60°C and stirred vigorously for 5 hours, dried in an oven at 120°C for 64 hours, and then calcined in a muffle furnace at 1200°C for 4 hours to obtain the carrier Mullite; mix 1.166g of cobalt nitrate and 0.263g of tungsten Dissolve ammonium acid in deionized water, stir thoroughly for 3 hours, then add 1.680g Mullite carrier, continue stirring for 2 hours, put the drug in an oven at 105°C for 16 hours, put the dried drug in a tube furnace at 700°C for 4 hours , the CWM-I catalyst was obtained, and the spinel-containing CoAl supported on Mullite was formed 2 o 4 and composite oxide CoWO 4 The mesoporous composite oxide catalyst with Co-W-Al-O active center, its typical crystal structure is sho...

Embodiment 2

[0036] Take by weighing 18.753g aluminum nitrate nonahydrate (Al(NO 3 ) 3 9H 2 O) and 2.322g tetraethyl orthosilicate (TEOS) were added into 80mL ethanol to obtain a white solution, and 36.701g ammonium carbonate ((NH 4 ) 2 CO 3 ) was added to the above white solution, heated in a water bath at 60°C and vigorously stirred for 5h, dried in an oven at 120°C for 64h, and then calcined in a muffle furnace at 1200°C for 4h to obtain the carrier Mullite; 1.166g of cobalt nitrate and 0.536g Dissolve ammonium tungstate in deionized water, stir thoroughly for 3 hours, then add 1.659g Mullite carrier, continue stirring for 2 hours, put the drug in an oven at 105°C for 16 hours, put the dried drug in a tube furnace at 700°C for roasting 4h, the CWM-II catalyst was obtained, and spinel-containing CoAl supported on Mullite was formed 2 o 4 and composite oxide CoWO 4 The mesoporous composite oxide catalyst with Co-W-Al-O active center, its typical crystal structure is shown in the at...

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Abstract

The invention relates to a Mullite carrier-loaded W-promoted Co-based catalyst for hydrogen production by auto-thermal reforming of acetic acid. The invention provides a novel catalyst which is high in activity, resistant to carbon deposition, resistant to sintering and resistant to oxidation, aiming at the problem of catalytic inactivation of an existing catalyst in the auto-thermal reforming process of acetic acid. The molar composition of the catalyst provided by the invention is (CoO)a(WO3)b(3Al2O3-2SiO2)c, a is in a range of 0.469 to 0.517, b is in a range of 0.010 to 0.054, and c is in a range of 0.449 to 0.502. According to the preparation method, Co and W components are impregnated on a Mullite carrier by adopting an impregnation method, a mesoporous composite oxide Co-W / Mullite catalyst containing spinel CoAl2O4 and a composite oxide CoWO4 is formed after calcination, and a Co-W-Al-O active center loaded on Mullite is obtained. The catalyst provided by the invention efficiently promotes the adsorption activation of acetic acid molecules and the conversion of intermediate products, inhibits the generation of by-products, and further improves the hydrogen yield and the stability of the catalyst.

Description

technical field [0001] The invention relates to a stable Mullite loaded W to promote the application of a Co-based catalyst in the autothermal reforming of acetic acid to produce hydrogen, and belongs to the field of producing hydrogen from the autothermal reforming of acetic acid. Background technique [0002] Hydrogen is a renewable green and clean energy, which is usually produced by water electrolysis, petroleum catalytic cracking and natural gas catalytic reforming. The cost of electrolyzing water to produce hydrogen is relatively high, and the large-scale use of fossil resources such as oil and natural gas to produce hydrogen will lead to greenhouse gas emissions. Therefore, finding low-cost renewable energy sources to produce hydrogen is an attractive and sustainable solution. [0003] Biomass is one of the four energy sources after crude oil, coal and natural gas. Biomass can be converted into biomass oil through rapid pyrolysis, and the composition of biomass oil ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/888C01B3/32
CPCB01J23/005B01J23/888B01J23/002C01B3/326C01B2203/0227C01B2203/1052C01B2203/1082B01J2523/00B01J2523/31B01J2523/41B01J2523/69B01J2523/845Y02P20/52
Inventor 黄利宏陈慧宋玉鑫
Owner CHENGDU UNIVERSITY OF TECHNOLOGY
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