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Preparation method of substitute natural gas

A technology for replacing natural gas and raw gas, applied in chemical instruments and methods, gas fuels, metal/metal oxide/metal hydroxide catalysts, etc., can solve the problem of reduced catalyst service life, high nickel loading, and low reaction space velocity and other problems, to achieve the effects of reducing one-time investment and operating costs, high methane space-time yield, and good thermal stability

Active Publication Date: 2012-05-16
江苏华昌新材料技术研究有限公司
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

For example, Chinese patent CN101733104A provides a catalyst for methanation of synthesis gas containing carbon dioxide, which consists of metal active components, additives and carriers, and the synthesis gas H 2 / CO (molar ratio)=3~8, CO conversion rate is the highest 90.5%, methane selectivity is the highest 92.2%, the disadvantage is that the reaction space velocity is low (1000-8000h -1 )
Chinese patent CN101716513A discloses a catalyst for complete methanation of coal gasification through synthesis gas, which uses rare earth oxides as the carrier, the active component is Ni, and the additive is La, which improves the high temperature resistance of the catalyst. The disadvantage is the Ni content High (>20wt%)
European patent EP1173277 discloses Ni catalysts loaded with rare earth oxides and rare earth perovskite oxides to catalyze the methanation of carbon oxides. The disadvantage is that the space velocity is low (10000h -1 ), the activity is not high enough
However, these catalysts still have some defects, such as: (1) the methanation activity still needs to be improved; (2) the reaction space velocity is still low; (3) the nickel loading is high; (4) the high temperature stability of the catalyst is still improved room for waiting
A single oxide support tends to interact strongly with active components at high temperatures, and even forms low-activity species, resulting in reduced catalyst service life

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0013] With the lanthanum-cobalt perovskite with a specific surface area of ​​70 square meters per gram as the carrier, the weight percentage of nickel oxide on the final catalyst is 10%, and the weight percentage of magnesium oxide as an auxiliary agent is 1.5%, using nickel nitrate and magnesium nitrate aqueous solution impregnation method Preparation of Ni-Mg / LaCoO 3 Catalyst (Catalyst A). Fill 5 grams of 20-40 mesh catalyst A in a quartz glass reaction tube with an inner diameter of 14 mm and a length of 250 mm, use a flow rate of 500 ml / min to contain 10% hydrogen / nitrogen mixed gas at 380 ° C for 6 hours, and then cool to room temperature , transferred to a stainless steel reactor with an inner diameter of 18 mm and a length of 300 mm. Raise the temperature of the reactor to 350°C, use the thermocouple inserted in the catalyst bed as the reaction temperature, and use syngas as the raw material to carry out the methanation reaction, where H 2 / CO (mol) = 3, CO 2 The co...

Embodiment 2

[0015] With the lanthanum-iron perovskite with a specific surface area of ​​30 square meters per gram as the carrier, the weight percent of nickel oxide on the final catalyst is 10%, and the weight percent of potassium oxide as an auxiliary agent is 1.0%, and the aqueous solution precipitation method of nickel nitrate and potassium nitrate is used Preparation of Ni-K / LaFeO 3 Catalyst (Catalyst B). According to the method described in Example 1, methanation is used to produce natural gas for replacement. The gas composition and catalyst performance after the reaction are listed in Table 1.

[0016] Table 1 Catalyst Evaluation Results*

[0017]

[0018] *GHSV=20000L / kg·h

Embodiment 3

[0020] Using lanthanum-aluminum perovskite with a specific surface area of ​​20 square meters per gram as the carrier, the weight percent of nickel oxide on the final catalyst is 5%, and the weight percent of calcium oxide as an auxiliary agent is 2.0%, using nickel nitrate and calcium nitrate aqueous solution precipitation method Preparation of Ni-Ca / LaAlO 3 Catalyst (Catalyst C). H in mole percent 2 60%, CO 20%, CO 2 5%, CH 4 15% of the gas was used as a raw material for the synthesis of substituted natural gas. The catalyst loading was 30 g. After the reaction, the gas was subjected to pressure swing adsorption to obtain 95% methane mole percent of the substituted natural gas. The performance of the catalyst was listed in Table 2.

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Abstract

The invention discloses a method for preparing a substitute natural gas from synthesis gas or coke oven gas by methanation reaction. In the method, the substitute natural gas in which the molar percentage of methane is more than 93% is obtained by the methanation reaction in a fixed bed reactor containing a methanation catalyst on the conditions that the reaction temperature is 250-750 DEG C, the reaction pressure is 0.1-6.0 Mpa and the total airspeed of feed gas is 500-50000h<-1>, wherein the feed gas can be synthesis gas or coke oven gas. Compared with the existing process, the method disclosed by the invention can be carried out at a higher airspeed, thus a higher methane space-time yield can be obtained.

Description

technical field [0001] The invention belongs to the field of synthesis gas and coke oven gas utilization, in particular to a method for preparing substitute natural gas through methanation reaction using synthesis gas or coke oven gas as raw material. Background technique [0002] Substitute natural gas (SNG) refers to the gas produced by CO, H 2 or with CO 2 The synthesis gas and coke oven gas can be methanated to obtain a gas with a methane mole percentage of more than 90%, which can be used to replace natural gas, such as compressed natural gas (CNG) vehicle fuel and civil gas. my country's energy structure is characterized by rich coal, lack of oil, and little gas. Vigorously developing clean coal technology is an important part of the energy development strategy. Therefore, using synthetic gas and coke oven gas to produce substitute natural gas is one of the effective ways to supplement the shortage of natural gas resources. one. The key reactions in the SNG process a...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/755B01J23/83B01J23/835C10L3/08C10L3/10
Inventor 宋焕玲丑凌军杨建赵军
Owner 江苏华昌新材料技术研究有限公司
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