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

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...

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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, thereby reducing the performance of the oxygen carrier (Appl.Catal.,B,2015,164,371-379)

In addition, pure phase or supported Fe 2 o 3 Oxidation is too strong, making CH 4 Oxidation to produce CO 2 and H 2 O (Int. J. Hydrogen Energy, 2009, 34, 1301-1309)

Mihai et al. (Ind. Eng. Chem. Res., 2011, 50, 2613-2621) found that LaFeO with perovskite structure 3 Highly selective partial oxidation of methane to produce syngas, but low methane conversion limits access to higher syngas yields

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