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Cobalt-based catalyst having core-shell structure, and preparation method thereof

A cobalt-based catalyst, core-shell structure technology, applied in chemical instruments and methods, preparation of liquid hydrocarbon mixtures, catalysts for physical/chemical processes, etc. and other problems, to achieve the effect of high oil-wax selectivity, easy industrial scale-up, and lower production costs

Active Publication Date: 2016-05-25
SHANGHAI ADVANCED RES INST CHINESE ACADEMY OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, due to the large size of the prepared catalyst particles, the synthesis gas is prone to diffusion limitation during the reaction process, which makes it difficult for the cobalt active center at the core of the catalyst particles to fully contact with the synthesis gas, and the H 2 The difference in the diffusion rate of CO leads to the surface H of the Co active site at the core position 2 / CO ratio increases, leading to CH 4 increased selectivity
In addition, the larger catalyst particle size also makes it difficult for the formed hydrocarbon products to diffuse out in time, and adsorbed on the active sites of metal cobalt to reduce the number of active sites actually participating in the catalytic reaction, thereby reducing the catalytic activity.
In addition, if the heat of reaction generated by Fischer-Tropsch synthesis cannot be effectively removed, it will easily lead to the generation of local hot spots, which will cause the sintering of the catalyst and cause the deactivation of the catalyst.

Method used

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  • Cobalt-based catalyst having core-shell structure, and preparation method thereof

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Experimental program
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Effect test

Embodiment 1

[0024] By mass percentage Co:MnO 2 :ZrO 2 / Al 2 o 3 Composite oxide carrier=10:1:89 ratio to synthesize cobalt-based catalyst. Specific steps are as follows:

[0025] Step 1, according to the above-mentioned mass percentage of 10:1:89, first weigh out 5g microspherical ZrO 2 / Al 2 o 3 Composite oxide carrier (prepared by spray drying molding technology, particle size is 500μm, specific surface area is 230m 2 / g, the pore volume is 1.1cm 3 / g, the average pore size distribution is 15nm).

[0026] Step 2, take by weighing 2.77g cobalt nitrate and 0.16g manganese nitrate, be dissolved in 5mL alcoholic water (V 乙醇 :V 水 =1:1), it is prepared as an impregnating solution.

[0027] Step 3, 5g microspherical ZrO 2 / Al 2 o 3 The composite oxide carrier was placed in a rotary evaporator, and under the condition of rapid stirring, every 1g of ZrO 2 / Al 2 o 3 At a drop rate of 1mL / s for the composite oxide carrier, the impregnation solution prepared in step 2 was quickly p...

Embodiment 2

[0029] By mass percentage Co:La 2 o 3 :SiO2 2 / Al 2 o 3 Composite oxide carrier=15:0.5:84.5 ratio to synthesize cobalt-based catalyst. Specific steps are as follows:

[0030] Step 1, according to the above mass percentage of 15:0.5:84.5, first weigh out 5g of clover-type SiO 2 / Al 2 o 3 Composite oxide carrier (prepared by extrusion molding technology, the particle size length is in the range of 10mm, the diameter is 5mm, and the specific surface area is 260m 2 / g, the pore volume is 1.0cm 3 / g, the average pore size distribution is 14nm).

[0031] Step 2, weigh 4.38g cobalt nitrate and 0.08g lanthanum nitrate, dissolve in 5mL alcohol water (V 乙醇 :V 水 =2:1), prepared as impregnation solution.

[0032] Step 3, 5g clover-type SiO 2 / Al 2 o 3 The composite oxide carrier was put into a rotary evaporator, and under the condition of rapid stirring, every 1g SiO 2 / Al 2 o 3 At a dropping rate of 1.5mL / s for the composite oxide carrier, the impregnation solution prep...

Embodiment 3

[0034] By mass percentage Co:NiO:TiO 2 / Al 2 o 3 Composite oxide carrier=20:0.5:79.5 ratio to synthesize cobalt-based catalyst. Specific steps are as follows:

[0035] Step 1, according to the above mass percentage of 20:0.5:79.5, first weigh out 5g cylindrical TiO 2 / Al 2 o 3 Composite oxide carrier (prepared by extrusion molding technology, the particle size length is in the range of 8mm, the diameter is 4mm, and the specific surface area is 250m 2 / g, the pore volume is 0.9cm 3 / g, the average pore size distribution is 12nm).

[0036] Step 2, weigh 6.21g cobalt nitrate and 0.12g nickel nitrate, dissolve in 4.5mL alcohol water (V 乙醇 :V 水 =5:1), prepared as impregnation solution.

[0037] Step 3, 5g cylindrical TiO 2 / Al 2 o 3 The composite oxide carrier was placed in a rotary evaporator, and under rapid stirring conditions, every 1g TiO 2 / Al 2 o 3 At the drop rate of the composite oxide carrier 2mL / s, the impregnation solution prepared in step 2 was quickly ...

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Abstract

The present invention discloses a preparation method of a cobalt-based catalyst having a core-shell structure. The preparation method comprises: 1) selecting an industrially molded composite oxide as a carrier; 2) dissolving a soluble cobalt salt and a metal auxiliary agent salt in an alcohol and water mixing solvent to prepare an impregnating solution; 3) at the high speed flipping state of the composite oxide carrier, rapidly and uniformly mixing the impregnating solution and the composite oxide carrier to prepare a solid catalyst precursor; and 4) drying, and calcining to obtain the cobalt-based catalyst having the core-shell structure. The present invention further discloses the cobalt-based catalyst having the core-shell structure and prepared through the method. According to the present invention, the industrially molded composite oxide is selected as the carrier, and the cobalt salt and the metal auxiliary agent salt adopted as the active components are uniformly impregnated on the outer surface of the carrier by using the rapid rolling of the carrier, such that the defect that the traditional impregnating method cannot accurately control the active species distribution appearance is broken through, the efficient utilization of the cobalt metal is achieved, the catalyst preparation cost is reduced, and the activity and the operation stability of the catalyst are improved.

Description

technical field [0001] The invention relates to a supported heterogeneous catalyst, in particular to a cobalt-based catalyst for Fischer-Tropsch synthesis and a preparation method thereof. Background technique [0002] Facing the looming energy crisis and the characteristics of my country's energy consumption structure, using Fischer-Tropsch synthesis to convert coal, natural gas or biomass into liquid fuels through syngas has become a feasible way to solve the energy crisis in our country. Fischer-Tropsch synthesis is synthesis gas (CO and H 2 Mixed gas) reacts on transition metal catalysts (such as iron-based, cobalt-based) to generate hydrocarbons and a small amount of oxygen-containing compounds. High-quality liquid fuels (such as gasoline, diesel, aviation kerosene, etc.) can be obtained through deep processing. These fuels do not contain sulfides and nitrogen compounds, and are very clean motor fuels. At present, iron-based and cobalt-based catalysts are commonly use...

Claims

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Application Information

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IPC IPC(8): B01J23/889B01J23/83B01J23/755B01J35/02C10G2/00
Inventor 孙予罕解荣永王春玲王慧赵铁均
Owner SHANGHAI ADVANCED RES INST CHINESE ACADEMY OF SCI
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