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Catalyst for methane dry gas reforming reaction and preparation method thereof

A technology of dry gas reforming and catalyst, which is applied in the direction of catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc. It can solve the problems of increasing the thermal conductivity of oxide carriers, easy collapse of wrapping materials, and limited stabilization effect , to achieve the effects of improving heat transfer efficiency, improving anti-carbon performance, and simple preparation method

Active Publication Date: 2022-04-15
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the former can stabilize nanoparticles, but at the cost of sacrificing catalyst activity, and the encapsulation material is easy to collapse under high-temperature reaction conditions and loses its protective effect; while the latter has limited stabilizing effect under high-temperature conditions, and cannot be used in actual DRM reactions. Avoid Ni particle sintering
In addition, due to the strong endothermic characteristics of the DRM reaction, the temperature of the catalyst bed often appears "cold spot" (the actual temperature is even lower than the set temperature by 100-200 ° C), which easily leads to the generation of carbon deposits, so it is necessary to increase the current temperature. Thermal conductivity of oxide support

Method used

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  • Catalyst for methane dry gas reforming reaction and preparation method thereof
  • Catalyst for methane dry gas reforming reaction and preparation method thereof
  • Catalyst for methane dry gas reforming reaction and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0037] (1) Dissolve 0.05g boric acid in 3ml water, then add 1g MgAl 2 o 4 Spinel, mixed and stirred until it became a paste and then dried for 12 hours to obtain MgAl modified with boron species 2 o 4 Prebody;

[0038] (2) the boron-containing species modified MgAl obtained in step (1) 2 o 4 Precursor, in NH 3 Under the atmosphere, the flow rate is 100ml / min, the temperature is raised to 800°C at 8°C / min and kept for 1h, and the temperature is raised to 1000°C at 2°C / min and kept for 1h to obtain MgAl 2 o 4 @h-BN;

[0039] (3) Dissolve 0.127g of nickel acetate in 2.5ml of water, add the MgAl obtained in step (2) 2 o 4 In @h-BN, stir and impregnate to a paste and then dry for 12 hours to obtain a catalyst precursor;

[0040] (4) Preform obtained in step (3) in H 2 Under atmosphere, heat up to 800°C at 1°C / min for 1h, H 2 Flow rate is 100ml / min, then lowers the temperature, obtains described methane dry reforming catalyst 3%Ni / MgAl 2 o 4 @h-BN.

[0041] For the ca...

Embodiment 2

[0047] (1) Dissolve 0.05g boric acid in 3ml water, then add 1g MgAl 2 o 4 Spinel, mixed and stirred until it became a paste and then dried for 12 hours to obtain MgAl modified with boron species 2 o 4 Prebody;

[0048] (2) the boron-containing species modified MgAl obtained in step (1) 2 o 4 Precursor, in NH 3 Under the atmosphere, the flow rate is 100ml / min, the temperature is raised to 800°C at 8°C / min and kept for 1h, and the temperature is raised to 1000°C at 2°C / min and kept for 1h to obtain MgAl 2 o 4 @h-BN;

[0049] (3) 0.424g of nickel acetate is dissolved in 3ml of water, and the MgAl obtained in step (2) is added 2 o 4 In @h-BN, stir and impregnate to a paste and then dry for 12 hours to obtain a catalyst precursor;

[0050] (4) Preform obtained in step (3) in H 2 Under atmosphere, heat up to 800°C at 1°C / min for 1h, H 2 Flow rate is 100ml / min, then lowers the temperature, obtains described methane dry reforming catalyst 10%Ni / MgAl 2 o 4 @h-BN. The res...

Embodiment 3

[0052] (1) Dissolve 0.2g boric acid in 3ml water, then add 1g SiO 2 , mixed and stirred to paste and then dried for 12h to obtain SiO modified with boron species 2 Prebody;

[0053] (2) SiO modified with boron-containing species obtained in step (1) 2 Precursor, in NH 3 Under the atmosphere, the flow rate is 100ml / min, the temperature is raised to 800°C at 8°C / min and kept for 1h, and the temperature is raised to 1000°C at 2°C / min and kept for 1h to obtain SiO 2 @h-BN;

[0054] (3) Dissolve 0.424g nickel acetate in 3ml water, add SiO obtained in step (2) 2 In @h-BN, stir and impregnate to a paste and then dry for 12 hours to obtain a catalyst precursor;

[0055] (4) Preform obtained in step (3) in H 2 Under atmosphere, heat up to 800°C at 1°C / min for 1h, H 2 Flow rate is 100ml / min, then lowers the temperature, obtains described methane dry reforming catalyst 10%Ni / SiO 2 @h-BN. The resulting Ni particle size is around 2nm.

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Abstract

The invention discloses a novel methane dry gas reforming reaction catalyst as well as its preparation and application. The catalyst of the present invention uses an oxide whose surface is covered by ultrathin boron nitride (h-BN, 1-2 layers) as a carrier, and the size of the active component Ni nanoparticles carried thereon is between 2nm and 5nm, wherein : The oxide is SiO 2 、Al 2 o 3 , MgAl 2 o 4 , MgO, ZrO 2 any of the. The catalyst prepared by the present invention can be used for the reaction of methane and carbon dioxide reforming to produce synthesis gas. The h-BN ultra-thin coating can greatly enhance the thermal conductivity of the oxide carrier and improve the heat transfer efficiency around the Ni particles; the CO in the reaction atmosphere 2 and CH 4 It can interact with the defect-rich h-BN layer, which can partially wrap Ni particles and prevent them from sintering, and the B element can also modify Ni particles in real time, greatly improving its anti-carbon deposition performance. The catalyst simultaneously solves the problems of carbon deposition and sintering of metal nanoparticles during the reaction, has a simple preparation method and has wide application prospects.

Description

technical field [0001] The invention belongs to the field of methane dry gas reforming, and in particular relates to a catalyst for methane dry gas reforming reaction and a preparation method thereof. Background technique [0002] Methane dry reforming reaction (CH 4 +CO 2 =2CO+2H 2 , Dry Reforming of Methane / DRM) is one of the effective ways to convert and utilize natural gas resources and greenhouse gas carbon dioxide. The synthesis gas produced by the reaction is an important platform molecule for the production of oil products and high value-added chemicals. It is recognized as green and sustainable. Many practitioners are committed to the industrial application of methane dry gas reforming related processes. [0003] Transition metals and noble metals including Rh, Ru, Pt, Ir, and Ni all have good catalytic activity for DRM reactions, among which Ni-based catalysts have attracted the most attention due to their high activity and low cost. The methane dry reforming p...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/24B01J37/02B01J37/08B01J37/18C01B3/40
CPCB01J27/24B01J23/002B01J37/0207B01J37/08B01J37/18C01B3/40C01B2203/0238C01B2203/1058C01B2203/1082B01J35/398B01J35/393B01J35/23Y02P20/52
Inventor 傅强白云星包信和
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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