Oxygen carrier applied to chemical looping partial oxidation process for preparing synthesis gas by using methane, and preparation method and application of oxygen carrier

An oxygen carrier and chemical chain technology, which is applied in the field of chemical chain partial oxidation of methane to synthesis gas oxygen carrier and its preparation, can solve the problems of reduced oxygen carrier performance, low methane conversion rate, and poor cycle stability, so as to maintain cycle stability , high reactivity, strong interaction effect

Active Publication Date: 2018-11-23
NORTHWEST UNIV(CN)
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, pure iron oxide has poor cycle stability due to its rapid agglomeration and sintering due to the phase transition during the redox process.
Although the sintering of iron can be suppressed to a certain extent by selecting a suitable support, the deactivation of iron-based oxygen carriers cannot be completely avoided, mainly because the high-temperature redox conditions lead to phase separation of iron oxides from the support or interaction to form spinels. Stone, the...

Method used

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  • Oxygen carrier applied to chemical looping partial oxidation process for preparing synthesis gas by using methane, and preparation method and application of oxygen carrier
  • Oxygen carrier applied to chemical looping partial oxidation process for preparing synthesis gas by using methane, and preparation method and application of oxygen carrier
  • Oxygen carrier applied to chemical looping partial oxidation process for preparing synthesis gas by using methane, and preparation method and application of oxygen carrier

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preparation example Construction

[0037] The preparation method of the above-mentioned chemical chain partial oxidation methane synthesis gas oxygen carrier comprises the following steps:

[0038] 1) Preparation of LaFeO 3 Carrier:

[0039] Prepared by sol-gel method: add lanthanum nitrate and iron nitrate precursors to the citric acid solution according to the molar ratio of 1:1, the amount of citric acid and the ratio of the total amount of matter between La and Fe cations are (2.0~ 3.0): 1. After completely dissolving, use ammonia water with a mass concentration of 5% to 28% to adjust the pH value to 5 to 8, then evaporate to dryness in a water bath at 60 to 100°C to a gel state, and dry at 60 to 180°C 2~24h, and finally roasted at 700~1400℃ for 1~12h to get LaFeO 3 carrier;

[0040] When the sol-gel method is used to prepare, preferably, the ratio of the amount of citric acid to the total amount of La and Fe cations is 2.5:1, and after being completely dissolved, ammonia water with a mass concentration ...

Embodiment 1

[0050] Dissolve lanthanum nitrate and ferric nitrate in deionized water at 60°C, the total concentration of La and Fe cations is 0.2mol / L, then quickly add ammonium carbonate solution with a concentration of 1mol / L to the solution, and adjust the pH to 8, Then stir rapidly at 60°C for 4h, stand and age for 2h, filter, wash, dry at 80°C for 12h, and then bake at 900°C for 4h to obtain LaFeO 3 carrier.

Embodiment 2

[0056] Dissolve lanthanum nitrate and ferric nitrate in deionized water at 60°C, the total concentration of La and Fe cations is 0.2mol / L, then quickly add ammonium carbonate solution with a concentration of 1mol / L to the solution, and adjust the pH to 8, Then stir rapidly (250-625r / min) at 60°C for 4h, let it stand for aging for 2h, filter, wash, dry at 80°C for 12h, and then roast at 900°C for 4h to obtain LaFeO 3 Carrier, weigh 2gLaFeO 3 Carrier, and then slowly pour it into the pre-prepared 0.344mol / L nickel nitrate solution, stir rapidly for 1 hour, dry at 60°C for 12h, and roast at 400°C for 4h to obtain the composite oxide oxygen carrier.

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Abstract

The invention relates to an oxygen carrier applied to a chemical looping partial oxidation process for preparing synthesis gas by using methane, and a preparation method and application of the oxygencarrier. The preparation method comprises the steps of adding a LaFeO3 carrier into a nickel nitrate solution, soaking, evenly stirring and then drying; after that, calcining for 1-12h at 400-800 DEGC so as to obtain the oxygen carrier. When the oxygen carrier is applied to the chemical looping partial oxidation process for preparing the synthesis gas by using the methane, a fuel reactor and theregeneration reactor which are communicated with each other are adopted, and the oxygen carrier is circulated between the fuel reactor and the regeneration reactor; the oxygen carrier is simple in preparation method and good in repeatability, can utilize the high selectivity (greater than 90%) of self lattice oxygen in a wider temperature to perform partial oxidation on the methane for producing the synthesis gas, and can be regenerated in various oxidizing atmospheres such as air, water vapor, carbon dioxide, water/carbon dioxide gas mixture; meanwhile, high value-added products such as highpurity hydrogen, carbon monoxide or synthesis gas can be produced. After being subjected to a circular reaction for a plurality of times, the oxygen carrier is higher in reaction activity and synthesis gas selectivity.

Description

technical field [0001] The invention belongs to the field of chemical chain partial oxidation of methane to synthesis gas, in particular to an oxygen carrier of chemical chain partial oxidation of methane to synthesis gas and its preparation method and application. Background technique [0002] Methane is the main component of natural gas, unconventional natural gas (shale gas, tight sand gas, coal bed methane and combustible ice), and converting it into liquid fuel can not only increase added value, but also facilitate product transportation. At present, the main means of producing liquid fuels from methane in industry is to first convert methane into synthesis gas, and then convert it into liquid chemicals through methods such as Fischer-Tropsch synthesis. At present, there are three main methods for producing syngas from methane, including steam reforming, carbon dioxide dry reforming and partial oxidation. Since steam reforming and carbon dioxide dry reforming are stron...

Claims

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Application Information

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IPC IPC(8): B01J23/83C01B3/38C01B3/02
CPCB01J23/002B01J23/83B01J2523/00C01B3/02C01B3/38B01J2523/3706B01J2523/847B01J2523/842Y02P20/52
Inventor 朱燕燕吴坚刘瑞林申倩倩黄传德王晓东
Owner NORTHWEST UNIV(CN)
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