A kind of synthetic gas oxygen carrier produced by chemical chain partial oxidation of methane and its preparation method and application

Abstract

A chemical chain partial oxidation of methane to synthesize gas oxygen carrier and its preparation method and application, using LaFeO 3 The carrier is added to the nickel nitrate solution, immersed and stirred evenly, then dried, and then roasted at 400 to 800°C for 1 to 12 hours to obtain the oxygen carrier. When the oxygen carrier is used in the partial oxidation of methane in the chemical chain to produce synthesis gas, a connected fuel reactor and a regeneration reactor are used, and the oxygen carrier circulates between the fuel reactor and the regeneration reactor; the preparation method of the oxygen carrier of the present invention is simple and With good reproducibility, it can use its own lattice oxygen to partially oxidize methane to produce synthesis gas with high selectivity (>90%) in a wide temperature range, and can be used in air, water vapor, carbon dioxide, water / carbon dioxide mixed gas It is regenerated in a variety of oxidizing atmospheres and simultaneously produces high value-added products such as high-purity hydrogen, carbon monoxide or synthesis gas. After multiple cycle reactions, the oxygen carrier has high reactivity 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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