A kind of oxygen carrier for producing high-quality syngas and its preparation method and application

An oxygen carrier and synthesis gas technology, which is applied in the chemical method of reacting gas medium with gas medium, gas and gas reaction under catalytic active body, gas fuel, etc., can solve the problem of low cycle reaction activity, investment and operating costs It can improve the conversion rate of CH4, increase the conversion rate of methane, and improve the selectivity of synthesis gas.

Active Publication Date: 2019-11-05
NORTHWEST UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, due to the disadvantages of high energy consumption, large and complex equipment, large floor space, and high investment and operating costs, the production cost of synthesis gas accounts for about 60% of the total investment and production costs of the entire natural gas chemical process, and the synthetic gas produced Gas H 2 / CO is too high (H 2 / CO=3), not suitable for direct use in Fischer-Tropsch synthesis
The second important way to produce synthesis gas is CH 4 -CO 2 Reforming, due to reduced investment and energy consumption, especially in mitigating the greenhouse gas CO 2 The pressure of emission reduction is of great significance in protecting the environment, so people pay more and more attention to it. However, due to the high cost of noble metal catalysts, nickel-based catalysts are prone to carbon deposition and deactivation, and the synthesis gas H 2 / CO is too low (H 2 / CO=1) and other problems, it is still far from meeting the requirements of industrialization
The currently developed oxygen carriers have shortcomings such as low oxygen loading rate, low quality of synthesis gas, low cycle reactivity, and inability to withstand high reaction temperature.

Method used

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  • A kind of oxygen carrier for producing high-quality syngas and its preparation method and application
  • A kind of oxygen carrier for producing high-quality syngas and its preparation method and application
  • A kind of oxygen carrier for producing high-quality syngas and its preparation method and application

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preparation example Construction

[0041] The preparation method of the present invention comprises the following steps:

[0042] 1) Dissolve barium nitrate / lanthanum nitrate in 60-80°C deionized water to obtain barium nitrate / lanthanum nitrate solution; dissolve ferric nitrate in 60-80°C deionized water to obtain ferric nitrate solution; dissolve aluminum nitrate in 60 Aluminum nitrate solution is obtained in deionized water at ~80°C; barium nitrate / lanthanum nitrate solution, ferric nitrate solution, and aluminum nitrate solution are all 0.9-1.2mol / L, and the concentration of cerium nitrate solution is 0.1-40.5mol / L;

[0043] 2) After uniformly mixing the barium nitrate / lanthanum nitrate solution and the ferric nitrate solution, use 0.1-2mol / L nitric acid to adjust the pH value to 1-2, then add the aluminum nitrate solution, and mix well to obtain a mixed solution; wherein the barium nitrate / The mol ratio of lanthanum nitrate and ferric nitrate is 1:n, and the mol ratio of ferric nitrate and aluminum nitrate...

Embodiment 1

[0057] Non-equilibrium plasma treatment of CeO prepared by impregnation method 2 -BF 3 (x=0.5) Complex oxygen carriers. Barium nitrate (Ba(NO 3 ) 2 ), ferric nitrate (Fe(NO 3 ) 3 9H 2 O) and aluminum nitrate (Al(NO 3 ) 3 9H 2 O) were respectively dissolved in deionized water at 70° C. to form 1.0 mol / L solutions of barium nitrate, iron nitrate and aluminum nitrate. After mixing barium nitrate solution and ferric nitrate solution evenly, use 0.1moL / L nitric acid to adjust the pH value to 1.0, then add aluminum nitrate solution, after mixing evenly, to obtain a mixed solution, quickly add the mixed solution to an excess of 1.1mol / L In L saturated ammonium carbonate solution, stir rapidly at 70°C at a speed of 625r / min for 5 hours, filter and dry at 110°C for 11 hours, then first roast at 400°C for 4 hours, then roast at 1200°C for 5 hours, grind Oxygen carrier BF 3 .

[0058] Oxygen carrier BF 3 Slowly pour into the previously prepared 4.2mol / L cerium nitrate soluti...

Embodiment 2

[0060] Preparation of CeO prepared by non-equilibrium plasma treatment impregnation method at different calcination temperatures 2 -BF 3 (x=0.5) Complex oxygen carriers. Prepare the precursor CeO before roasting with the method of embodiment 1 earlier 2 -BF 3 , and then placed in a muffle furnace, first fired at 500°C for 4 hours, and then fired at 600°C, 700°C, 900°C, and 1000°C for 5 hours.

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Abstract

The invention relates to an oxygen carrier that generates high-quality synthesis gas and its preparation method and application. The oxygen carrier is CeO 2 with AFe n Al 12‑n o 19 (A=Ba,La) composite, the general formula of this composite metal oxygen carrier is CeO 2 ‑AFe n Al 12‑n o 19 (A=Ba, La), wherein, 0<n≤12, the total molar ratio x of cerium to ferrocerium ranges from 0.1 to 0.9. The preparation process is as follows: first, use barium nitrate or lanthanum nitrate, iron nitrate, and aluminum nitrate as precursors to prepare a nitrate solution, and add ammonium carbonate as a precipitant for co-precipitation. After suction filtration, washing, drying, and roasting, the carrier AFe is obtained. n Al 12‑n o 19 , and then prepare a cerium nitrate solution, impregnate, dry in the shade, dry, non-equilibrium plasma treatment, and then roast. This oxygen carrier not only has a higher CH 4 Conversion rate, H 2 Selective to CO and able to selectively oxidize methane to H 2 / CO is very close to the theoretical value of 2 high-quality syngas.

Description

【Technical field】 [0001] The invention belongs to the field of methane conversion to produce synthesis gas, and in particular relates to an oxygen carrier for producing high-quality synthesis gas and its preparation method and application. 【Background technique】 [0002] In recent years, it has been proven that the world's unconventional natural gas reserves have reached 9 million cubic meters, which has greatly eased human demand for natural gas. Unconventional natural gas generally includes shale gas, tight sand gas, mud gas (biogas), combustible ice, and coal seams Gas or coal mine gas etc. According to the statistics of the International Energy Agency (IEA) in 2012, the proven technically recoverable reserves of unconventional natural gas in my country are about 50 trillion cubic meters, including 36 trillion cubic meters of shale gas and 3 trillion cubic meters of tight gas. meters, and coalbed methane is 9 trillion cubic meters. As my country's non-traditional natural...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J12/00B01J8/02C10L3/08B01J19/30
CPCB01J8/02B01J12/007B01J19/30C10L3/08
Inventor 朱燕燕薛鹏孙雪艳刘伟伟赵彬然马晓迅
Owner NORTHWEST UNIV
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