Catalyst for methane dry gas reforming reaction and preparation method thereof

A dry gas reforming and catalyst technology, which can be used in catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc., and can solve the problems of increasing the thermal conductivity of oxide carriers, easy collapse of packaging materials, and limited stabilization. , to achieve the effects of improving heat transfer efficiency, improving carbon deposition resistance, and simple preparation method

Active Publication Date: 2021-08-06
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 catalyst for methane dry gas reforming reaction and a preparation method thereof. According to the catalyst, an oxide with the surface wrapped by ultra-thin boron nitride (h-BN, 1-2 layers) is adopted as a carrier, the size of an active component Ni nano particle supported on the oxide ranges from 2 nm to 5 nm, and the oxide is any one of SiO2, Al2O3, MgAl2O4, MgO and ZrO2. The prepared catalyst can be used for a reaction of reforming methane and carbon dioxide to prepare synthesis gas, the h-BN ultra-thin wrapping layer can greatly enhance the heat-conducting property of the oxide carrier, and the transfer efficiency of heat around Ni particles is improved; and in the reaction atmosphere, CO2 and CH4 can interact with the h-BN layer rich in defects, Ni particles can be partially wrapped and prevented from being sintered, the Ni particles can be modified by the element B in real time, and the carbon deposition resistance of the Ni particles is greatly improved. The catalyst simultaneously solves the problems of carbon deposition and sintering of metal nano particles in the reaction, the preparation method is simple, and the catalyst has a wide application prospect.

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 Applications(China)
IPC IPC(8): B01J27/24B01J37/02B01J37/08B01J37/18C01B3/40
CPCB01J27/24B01J23/002B01J35/0013B01J35/006B01J35/0086B01J37/0207B01J37/08B01J37/18C01B3/40C01B2203/0238C01B2203/1058C01B2203/1082Y02P20/52
Inventor 傅强白云星包信和
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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