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LaCeNiO perovskite catalyst with ultra-wide Ni (111) crystal face as well as preparation method and application of LaCeNiO perovskite catalyst

A catalyst and perovskite technology, which is applied in the field of methanation catalyst and its preparation and application, can solve the problems of easy deactivation, and achieve the effects of convenient operation, low preparation temperature and simple process

Pending Publication Date: 2022-07-08
任杰
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Conventional support such as Al 2 o 3 , CeO 2 、TiO 2 and SiO 2 etc. have been proven to have a certain CO 2 methanation activity, however, commercially available commercial catalysts such as Ni / γ-Al 2 o 3 , are very susceptible to deactivation due to carbon deposition, catalyst sintering, pore plugging, and metallic Ni oxidation

Method used

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  • LaCeNiO perovskite catalyst with ultra-wide Ni (111) crystal face as well as preparation method and application of LaCeNiO perovskite catalyst
  • LaCeNiO perovskite catalyst with ultra-wide Ni (111) crystal face as well as preparation method and application of LaCeNiO perovskite catalyst
  • LaCeNiO perovskite catalyst with ultra-wide Ni (111) crystal face as well as preparation method and application of LaCeNiO perovskite catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0040] Preparation of La with La:Ce=2:0 2 NiO 4 perovskite catalyst

[0041] Weigh 2.9863g La (NO 3 ) 3 ·6H 2 O, 0g Ce (NO 3 ) 3 6H 2 O, 1.0027g Ni (NO 3 ) 3 ·6H 2 O, 2.9815g citric acid, add 80mL water to fully dissolve, add ammonia water to adjust the pH of the mixed solution to 4, stir at 80°C, evaporate and concentrate to 20mL gel, take out, fully dry in a blast drying oven at 100°C for 12h to obtain the precursor body. After the precursor was crushed and sieved to 70 mesh, it was put into a muffle furnace, heated to 350°C for 4 hours at a heating rate of 3°C / min, and then calcined at a heating rate of 5°C / min to 600°C for 5 hours. After cooling, take it out, put it into a tube furnace, and pass 50mL / min H 2 Reduced for 1 h to obtain highly dispersed metallic Ni, ultra-wide Ni(111) crystal planes, and La rich in oxygen vacancies 2 NiO 4 perovskite catalysts. Ce 2 NiO 4 STEM and high-resolution transmission images of catalysts such as figure 2 As shown, ...

Embodiment 2

[0043] Preparation of La with La:Ce=1.5:0.5 1.5 Ce 0.5 NiO 4 perovskite catalyst

[0044] Weigh 2.2397g La (NO 3 ) 3 ·6H 2 O, 0.7487g Ce (NO 3 ) 3 ·6H 2 O, 1.0027g Ni (NO 3 ) 3 ·6H 2 O, 2.9815g citric acid, add 80mL water to fully dissolve, add ammonia water to adjust the pH of the mixed solution to 4, stir at 80°C, evaporate and concentrate to 20mL gel, take out, fully dry in a blast drying oven at 100°C for 12h to obtain the precursor body. After the precursor was crushed and sieved to 70 mesh, it was put into a muffle furnace, heated to 350°C for 4 hours at a heating rate of 3°C / min, and then calcined at a heating rate of 5°C / min to 600°C for 5 hours. After cooling, take it out, put it into a tube furnace, and pass 50mL / min H 2 Reduced for 1 h to obtain highly dispersed metallic Ni, ultra-wide Ni(111) crystal planes, and La rich in oxygen vacancies 1.5 Ce 0.5 NiO 4 perovskite catalysts.

Embodiment 3

[0046] Preparation of LaCeNiO with La:Ce=1:1 4 perovskite catalyst

[0047] Weigh 1.4931g La (NO 3 ) 3 ·6H 2 O, 1.4973g Ce (NO 3 ) 3 ·6H 2 O, 1.0027g Ni (NO 3 ) 3 ·6H 2 O, 2.9815g citric acid, add 80mL water to fully dissolve, add ammonia water to adjust the pH of the mixed solution to 4, stir at 80°C, evaporate and concentrate to 20mL gel, take out, fully dry in a blast drying oven at 100°C for 12h to obtain the precursor body. After the precursor was crushed and sieved to 70 mesh, it was put into a muffle furnace, heated to 350°C for 4 hours at a heating rate of 3°C / min, and then calcined at a heating rate of 5°C / min to 600°C for 5 hours. After cooling, take it out, put it into a tube furnace, and pass 50mL / min H 2 Reduction for 1 h to obtain LaCeNiO with highly dispersed metallic Ni, ultra-wide Ni(111) crystal face, and abundant oxygen vacancies 4 perovskite catalysts.

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Abstract

The invention discloses a LaCeNiO perovskite catalyst with an ultra-wide Ni (111) crystal face as well as a preparation method and application of the LaCeNiO perovskite catalyst. The preparation method comprises the following steps: by taking water as a solvent, citric acid as a chelating agent, La and Ce as carrier metals and metal Ni as an active metal, drying, screening, calcining and reducing by adopting a sol-gel method to obtain the LaCeNiO perovskite catalyst. The LaCeNiO perovskite catalyst is characterized in that the size of Ni particles reaches 10-25 nm, the crystal face of Ni (111) reaches 10 nm, the proportion of oxygen vacancies reaches 20-30%, the specific surface area of the catalyst is 12-38 m < 2 > / g, the average pore size is 5-13 nm, and the total pore volume is 0.03-0.08 cm < 3 > / g. The catalyst is low in Ni loading capacity and simple to prepare, and when the catalyst is applied to a CO2 methanation reaction, the highest CO2 conversion rate can reach 57.4 mmol CO2 / mol Ni / s, and the methane selectivity reaches 99.8%. Compared with a conventional commercial Ni / gamma-Al2O3 catalyst, the catalyst has excellent catalyst activity, stability and regeneration performance for dynamic gas supply and high water vapor atmosphere.

Description

technical field [0001] The invention relates to a methanation catalyst and the field of preparation and application thereof, in particular to a LaCeNiO perovskite catalyst with an ultra-wide Ni(111) crystal plane, a preparation method thereof, and an ultra-wide Ni(111) crystal plane LaCeNiO perovskite catalyst 2 Applications in methanation Background technique [0002] As of now, traditional energy sources such as coal, oil and natural gas still account for most of the world's energy consumption. However, the excessive consumption of traditional energy will lead to problems such as environmental pollution, ecological imbalance and huge carbon dioxide emissions. Therefore, countries around the world have gradually shifted their energy research goals to the efficient use and development of renewable energy. To address energy shortages and meet growing energy demands, both reliable renewable energy utilization and energy storage must be developed. Among the known developed s...

Claims

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Application Information

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IPC IPC(8): B01J23/83C07C1/12C07C9/04
CPCB01J23/002B01J23/83C07C1/12B01J2523/00C07C2523/83B01J2523/3706B01J2523/3712B01J2523/847C07C9/04Y02P20/133Y02P20/52
Inventor 任杰刘忆玲
Owner 任杰
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