SU1479414A1 - Method of producing metal-complex composition of coal - Google Patents

Abstract

The invention relates to the technology of metal complex compounds of coal (MKSU), which can be used in catalysis and electrocatalysis. The purpose of the invention is to simplify the process of obtaining the metal complex of coal and the expansion of its raw material base. The method of obtaining the metal complex of coal includes the preparation of a mixture of a nitrogen-containing polymer and an inorganic metal salt, whose chlorides, nitrides, carbonates or acetates have a melting point above 250 ° C at a mass ratio of polymer and salt (0.5-100): 1. The mixture is subjected to carbonization by heating from 250 to 350 ° C at a rate of 0.4-0.6 ° C / min and further to 850 ° C at a speed of 6.6-8.0 ° C / min. The obtained MSCB is catalytically active. For example, by passing a current through a single molar solution of sulfuric acid at 60 ° C using an MKSU electrode, the maximum current density is 44 mA / cm ₂ . The temperature resistance of the MKSU as a catalyst is 850 ° C. The method of obtaining MCS is simplified due to the possibility of using the metal salt in the form of a powder, since this eliminates the need to pre-dissolve the polymer in concentrated metal salts, which is inherent in the prototype, and the range of MKSUs is also expanded due to a greater choice of starting metal salts. 2 hp f-ly.

Description

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The invention relates to the technology of materials of inorganic chemistry, namely to the synthesis of complex compounds of coal, which can be used in catalysis and electrocatalysis.

The purpose of the invention is to simplify the process of obtaining the metal complex of coal and the expansion of its raw material base.

Example 1 The amount of 20 g of cryonitrile polymeta-i powder is mixed with cobalt carbonate СоС03 in the amount of 0.82 g. The mixture is thoroughly mixed in a mortar and subjected to carbonization in a quartz reactor under argon in the following temperature mode: from 250 to 350 ° C, heating rate 0, 4 ° С / min, from 350 to 850 ° С - 8.0 ° С / min.

X-ray diffraction analysis revealed that the crystal lattice of the salt is completely destroyed. Chemical analysis installed

duet compound composition, wt%: C - base; N 17.1; Co 12.0; H 2.1.

Example 2 Under the conditions of Example 1, a mixture of 20 g of polyethylnitrile and 0.82 g of CoCO3 is carbonized.

The composition of the obtained product, wt.%: With - the basis; K7 19.5; From 12.1; H 2.2.

Example 3. Under the conditions of example 1, a mixture of 16 g of polyacrylonitrile and 0.65 g of MpSC salt is carbonized.

The composition of the obtained product, wt.%: With - the basis; N 17.4; Mp 8.7, - H 2.23.

Example 4. Under the conditions of Example 1, a mixture of 20 g of acrylonitrile and 0.82 g of calcium nitrate Ca (NO j) .j is carbonized.

The composition of the obtained product, wt.%: With the basis; N 21.1; Ca 7.7; H 1.8.

Example 5. Under conditions of example 1, a mixture of carbonated mixture of 20 g of acrylonitrile and 0.61 g of sodium acetate NaCCH COO is carbonized.

The composition of the obtained product, wt.%: C - basis j N 17,3; Ka 4,2; H 2.1.

Example 6. The mixture is carbonized with 16 g of polyacrylonitrile with 0.65 g of MnCl salt. Under the following temperature conditions: from 250 to 35 ° C, the heating rate is 0.6 C / min, from 350 to 850 ° C - 6.6 C / min

The composition of the resulting product is the same as in example 3.

Example 7. Carbonization of a mixture of 16 g of polyacrylonitrile with 0.65 g of salt is carried out in the following temperature conditions: from 250 to 350 C, the loading rate is 0.6 C / min, from 350 to 850 ° C, 7.2 ° C / min.

The composition of the product is the same as in example 2.

Example 8. Carbonization of a mixture of 16 g of polyacrylonitrile with 0.65 g of MnCl salt is carried out under the following conditions: from 250 to 350 ° C. The heating rate is 0.5 ° C / min, from 350 to 850 ° C - 6.6 ° C / min

The composition of the obtained product is the same as in example 3.

Example 9. Carbonization of a mixture of 16 g of polyacrylonitrile with 0.65 g of MnCl-j salt is carried out under the following conditions: from 250 to 350 ° C speed

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heating 0.5 ° C / min, from 350 to 850 ° C - 7.2 ° C / min.

X-ray phase analysis data similar to example 1.

The composition of the obtained product, wt.%: With - the basis; N 17.4; MP 8.7, H 2.2.

Example 10. Carbonization of a mixture of 20 g of polyacrylonitrile with 0.2 g of MnCl2 (acrylonitrile: salt ratio 100: 1) is carried out under the conditions of example 1

The composition of the obtained product; wt.%: C - basis; N 18.76; MP 2.3, H 2.4.

Example 11. A mixture of 5 g of polyacrylonitrile and 10 g of MnCl2 (polymer: salt ratio 0.5: 1) is carbonized under the conditions of example 1.

X-ray phase analysis data similar to example 1.

The composition of the product, wt.%: C 26,24; N 5.4; MP 66.56, H 0.8.

Example 12. Under the conditions of Example 1, a mixture of 20 g of acrylononthril and 0.82 g of iron carbonate is carbonized.

The composition of the obtained product, wt.%: With - the basis; N $ 17.9 Fe 11.5; H 1.7.

Example 13. Under conditions of example 1, a mixture of 20 g of acrylonitrile and 0.82 g of sodium nitrate was carbonized.

The composition of the product, wt.%: C - basis; N 21.0; Na 8,1, - H 1, 8.

Example 14. Under the conditions of Example 1, a mixture of 10 g of polyacrylonitrile and 0.8 g of CoCl 1 was carbonized.

Composition of the product, wt.%: C - base, N 18.0-, Co 12.1; H 1, 6.

The metal complex carbon (MKSU) has catalytic properties.

For example, when a current is passed through a single molar solution of sulfuric acid at 60 ° C using a ZnCl-j based electrode and the polymer of the prototype, the maximum current density is 37 mA / cm2, and using electrodes made from MKSU according to the invention, 44 mA / cm2.

In addition, oxygen is adsorbed on the surface of the product obtained by the proposed method.

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heat of adsorption is 15-60 kcal / mol and forms active states of oxygen, for example, and 0. This indicates the activity of these compounds in heterogeneous catalytic oxidation reactions of organic compounds.

The temperature resistance of the MKSU as a catalyst is 850 ° C.

A deterioration in the catalytic activity is observed during the heat treatment of the MKSU in an argon atmosphere, since with increasing temperature above 850 ° C, the nitrogen content in coal decreases.

The invention makes it possible to simplify the process of obtaining MKSU by using a metal salt in the form of a powder, since this eliminates the need to pre-dissolve the polymer in concentrated metal salts, while expanding the range of MKSUs due to a wider range of starting metal salts.

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the invention

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Claims (3)

1. A method for the preparation of a metal-complex coal compound, which includes the preparation of a mixture of a nitrogen-containing polymer and an inorganic metal salt and the subsequent carbonization of the mixture by heating from 250 to, and from 350 to 850CC at a rate of 6.6-8.00 C / min, about t l and in order to simplify the process and expand the raw material base, a mixture of polymer powders and a metal salt is fed to carbonization, and heating from 25 ° C to 350 ° C is conducted at a rate of 0.4-0.6 ° C / min. 2. Method as claimed in claim 1, characterized in that the salts used are chlorides, nitrides, carbonates or acetates of metals, the melting point of which is higher than 250 ° C, 3. Method according to paragraphs. 1 and 2, that is, that the nitrogen-containing polymer and the salt are taken in a weight ratio of 0.5-100: 1.