The method of producing catalyst for conversion of carbon monoxide with water vapor

 

(57) Abstract:

The invention relates to methods of producing catalysts based on copper and zinc for the process of low-temperature steam reforming of carbon monoxide. The method consists in mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon, the formation of granules of the catalyst with subsequent heat treatment. By mixing the catalyst components in addition enter at least one connection alkaline earth metal and/or at least one compound of rare earth metals, and the total content of the additional additives is not more than 2.0 wt.%. The technical result consists in increasing thermal stability of the catalyst while maintaining high activity and durability. 1 C.p. f-crystals, 2 tab.

The present invention relates to methods of producing catalysts based on copper and zinc for the process of low-temperature steam reforming of carbon monoxide.

There is a method of preparation of the catalyst for steam reforming of carbon monoxide, comprising mixing and processing of copper-and zinc-containing components, manganese oxide and calcium aluminate complexing attaliates, prepared according to this technology, does not meet the requirements for mechanical strength and thermal stability. The term "thermal stability" is established and characterizes the stability of the active component of the catalyst to sintering when the temperature rises above the temperature of operation (Catalyst Handbook, edited by Martyn V. Twigg, Manson publishing, 1989, England).

Closest to the invention to the technical essence and the achieved results is the method of producing catalyst for conversion of carbon monoxide with water vapor, comprising mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon, forming granules of the catalyst followed by heat treatment (SU 1732537).

In the known method, the heat treatment is carried out by wilting in the air or drying, which is carried out at 70-130oC for 2 to 6 hours.

The disadvantage of the catalyst obtained by this technology is the low thermal stability.

The invention

The problem solved by the present invention is the development and creation method of producing catalyst for conversion of carbon monoxide with water vapor at which the catalyst becomes improved parameters PU.

The solution of this task is implementing a new technical result, namely, that increases thermal stability of the catalyst.

This technical result is achieved in that in the method of producing catalyst for conversion of carbon monoxide with water vapor, comprising mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon, forming granules of the catalyst with subsequent heat treatment, mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon, optionally introducing at least one connection alkaline earth metal and/or at least one compound of rare earth metals in a total content not more than 2.0 wt.%.

As compounds of alkaline earth metals are used, a substance selected from the group of oxides, hydroxides, carbonates of calcium, oxides, hydroxides, carbonates of magnesium, as well as compounds of rare earth metals used substance selected from the group of oxides, hydroxides, carbonates of lanthanum; oxides, hydroxides, cerium carbonate; oxides, hydroxides, carbonates neodymium.

The main distinguishing feature of this is the alkaline earth metals and/or at least one compound of rare earth metals in a total content not more than 2.0 wt.%.

An additional distinctive feature is that as compounds of alkaline earth metals use a substance selected from the group of oxides, hydroxides, carbonates of calcium, oxides, hydroxides, carbonates of magnesium, as well as compounds of rare earth metals used substance selected from the group of oxides, hydroxides, carbonates of lanthanum; oxides, hydroxides, cerium carbonate; oxides, hydroxides, carbonates neodymium.

The proposed set of features for a method of preparation of the catalyst the conversion of carbon monoxide with water vapor meets the conditions of patentability of "novelty" and "inventive step" for the following reasons. Source information is not known that the proposed set of features leads to the solution of the above problem to obtain a new technical result, namely: the introduction of additional compounds of alkaline earth metals and/or compounds of rare earth metals in a total content not more than 2.0 wt.% by mixing the catalyst components provides increased thermal stability of the catalyst for Discoteca fact, that the addition of compounds of alkaline earth metals by mixing the catalyst components increases the degree of hydration of calcium aluminates and accordingly the degree of interaction between the active components hydrocalumite calcium, which leads to the development of the specific surface of the catalyst, to improve formemost catalyst mass and, ultimately, to obtain a catalyst with high thermal stability. Adding to the components of the catalyst of rare earth compounds prevents the sintering of the active component is copper, that is, increases thermal stability of the catalyst, its resistance to possible overheating during operation.

The above additives are compounds of alkaline earth and rare earth metals is impractical to enter more than 2.0 wt.%, as with increased content of compounds of alkaline earth metals in the hydration of aluminates of calcium increases the content of compounds of the type of calcite, dramatically reducing the strength of the catalyst, and the high content of rare-earth metal compounds significantly reduces the activity of the catalyst in the conversion of carbon monoxide with water vapor.

Information, podvergayuschimsya load 250 g zinkernagel connection with the content of Zn0 - 43 wt.% and CuO - 57 wt.% (on calcined basis) and promoters - 0.8 g ground activated carbon, 0.6 g of a basic carbonate of manganese, 70 g of technical calcium aluminate. After mixing these substances add 45 ml of water, stir and bring a lot to the state of formemost. After molding granules them dried and subjected to heat treatment in the presence of water vapor. Tests of the obtained catalyst is conducted under the following conditions:

Temperature 180oC, space velocity of 5000 h-1the steam:gas ratio=0,7. Activity is defined as the degree of conversion of carbon monoxide, thermostability as (-1)/, where the degree of conversion of carbon monoxide,1the degree of conversion of carbon monoxide after overheating of the catalyst at 350oC for 2 h in the conditions of the reaction medium. The decrease in the value of this index means an increase in thermal stability of the catalyst, i.e. the improvement of its operational characteristics.

The results of tests of strength, activity and thermal stability of the sample catalyst in low-temperature steam reforming of carbon monoxide are shown in table. 1.

Below are examples of (2 - 6) for the described method palluconi examples (2 - 6), were carried out as in example 1. The results are given in table. 1.

Example 2.

The catalyst prepare and test as in example 4, but further added to 1.00 g of calcium oxide.

Example 3.

The catalyst prepare and test as in example 1, but further added 0.84 g of lanthanum carbonate, 0.27 g of cerium carbonate and 0.10 g of neodymium hydroxide.

Example 4.

The catalyst prepare and test as in example 1, but further added 1.06 g of calcium hydroxide and 0.2 g of magnesium oxide.

Example 5.

The catalyst prepare and test as in example 1, but additionally introduce 1.07 calcium carbonate and 0.4 g of cerium oxide.

Example 6 (with a maximum content of compounds of alkaline earth and rare earth metals).

The catalyst prepare and test as in example 1, but further added 0.5 g of calcium oxide, of 1.16 g of magnesium hydroxide, 1.20 g of lanthanum oxide, 0.10 g of cerium hydroxide and 0.9 g of neodymium oxide.

From the comparison of example 1 (method - the closest equivalent) with examples (2 - 6) for the described method of preparation of the catalyst shows that the additional introduction of compounds of alkaline earth and/or rare earth metals in ivesti and strength of the catalyst, obtained by the method closest analogue.

Example 7 (with the beyond the content of compounds of alkaline earth and rare earth metals).

The catalyst prepare and test as in example 1, but further added to 1.00 g of calcium oxide, and 1.00 g of magnesium oxide, 0.84 g of lanthanum carbonate, 1.0 g of cerium oxide and 0.49 g of neodymium hydroxide.

As can be seen from the test results, when beyond the content of the alkaline earth and rare earth metals sharply decreases the strength of the catalyst and reduces its activity.

In table. 2 shows the data content in the samples of catalyst compounds of alkaline earth and rare earth metals.

1. The method of producing catalyst for conversion of carbon monoxide with water vapor, comprising mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon, forming granules of the catalyst with subsequent heat treatment, characterized in that the mixing zinkernagel connection with the aluminates of calcium, manganese carbonate and activated carbon addition to impose at least one connection alkaline earth metal and/or at least one compound of rare earth metalla water vapor by p. 1, characterized in that compounds of alkaline earth metals use a substance selected from the group of oxides, hydroxides, carbonates of calcium, oxides, hydroxides, carbonates of magnesium, as well as compounds of rare earth metals used substance selected from the group of oxides, hydroxides, carbonates of lanthanum; oxides, hydroxides, cerium carbonate; oxides, hydroxides, carbonates neodymium.

 

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