The catalyst for ammonia synthesis, a method of producing the catalyst and the method of synthesis of ammonia

 

(57) Abstract:

The invention relates to the chemical industry, and more particularly to a catalytically active materials, compositions, and can be used as a catalyst in producing ammonia by reacting nitrogen with hydrogen. The catalyst for ammonia synthesis contains: a) as a carrier - carbon material, which is a three-dimensional carbon matrix with the pore volume of 0.2 - 1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 and with a radius of curvature of 100-10000 having a true density of 1.80-2.10 g/cm3, x-ray density 2.112-2.236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in the range of 40-200 b) 1-15 wt.% (in terms of metal) at least one of the compounds of alkali and alkaline earth metals from a number of K, Cs, BA;) 1-8 wt.% (in terms of metal) at least one of the compounds of ruthenium; g) not more than 7 wt.% the oxygen. The method of receiving calzature ammonia synthesis includes sequential impregnation of the carbon carrier with solutions of compounds of ruthenium, impregnation promoting connect the W, as starting compounds of ruthenium use solutions of complex compounds of ruthenium with mono - and mostly polydentate nitrogen - or oxygen-containing ligands; as a carbon carrier used material, which is a three-dimensional carbon matrix with the pore volume of 0.2-1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 and with a radius of curvature of 100-10000 having a true density of 1.80-2.10 g/cm3, x-ray density 2,112-2,236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in the range of 3 40-200 stage of recovery is carried out before the oxygen content in the catalyst is not more than 7 wt.%. The method of synthesis of ammonia, based on the interaction of nitrogen and hydrogen, is carried out at elevated temperatures and pressures using a ruthenium catalyst on a carbon carrier; the catalyst contains ruthenium compounds (1-8 wt.% in terms of metal), at least one of the compounds of alkali and alkaline earth metals from a number of K, Cs, BA (1-15 wt.% in terms of metal) and not more than 7 wt.% oxygen in the carbon media, PR exercise is the RTO in obtaining catalyst ammonia, with a higher mechanical strength and catalytic activity in comparison with the known. The described catalyst is not pyrophoric under operating conditions. 3 S. and 3 C.p. f-crystals, 2 tab.

The invention relates to the chemical industry and, more specifically, to a catalytically active materials, compositions and can be used as a catalyst in producing ammonia by reacting nitrogen with hydrogen.

Among the known catalysts prepared from various materials, the most similar in chemical composition to the claimed material is ruthenium catalysts on activated carbon media, designed for the synthesis of ammonia from nitrogen and hydrogen.

A known catalyst for ammonia synthesis, representing the media based on graphite-containing carbon, the active component is ruthenium and the promoter is an alkali metal (U.S. Patent T 4 142 993, MKI3B 01 J 21/18, publ. 06.03.79 year). The disadvantage of the catalyst is low mechanical strength, the catalyst has a property of spontaneous ignition in air.

A known catalyst for ammonia synthesis, including the graphite-containing operon the major attention is paid to the selection of media with specific characteristics. The catalyst is prepared dostudio, impregnating the carrier with an aqueous solution of halides or nitrates ruthenium, dried and restore in a stream of hydrogen is then impregnated with aqueous solutions of nitrate, carbonate or acetate of potassium, or rubidium, or barium (Patent England N 1565074, MKI3B 01 J 23/58, publ. 16.04.80 year). The disadvantage of the catalyst is low specific activity of the catalyst per unit of the active component.

The closest technical solution to the claimed is an improved catalyst and method thereof (patent Application EP N 0120655, MKI4B 01 J 23/58, 01 1/04, publ. 17.12.86, prototype). Carbon carrier having certain characteristics (e.g. the specific surface not less than 100 m2/g, the ratio of the value of the specific surface according to BET to the value of the basal surface is not higher than 4:1, the ratio of the value of the basal surface to the edge surface of at least 10:1, or other specified ratio), impregnated with a halogenated compound of ruthenium, restore the connection of ruthenium to the metallic state of hydrogen, then applied from aqueous solutions promoting compounds of an alkali metal (except lithium and barium. The disadvantages of this catalyst I is s solves the problem of increasing the mechanical strength of the catalyst for ammonia synthesis, maintain a high level of catalytic activity, reduce proforest and hydrogen inhibition.

The problem is solved by using a catalyst for ammonia synthesis, containing:

a) as a carrier - carbon material, which is a three-dimensional carbon matrix with the pore volume of 0.2-1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 and with a radius of curvature of 100-10000 having a true density of 1.80-2.10 g/cm3, x-ray density 2.112-2.236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in the range of 40-200 b) 1-15 wt.% (in terms of metal, each at least one or a mixture of compounds of alkali and alkaline earth metals from a number of potassium, cesium, barium; C) 1 to 8 wt.% (in terms of metal) at least one of the compounds of ruthenium; g) not more than 7 wt.% the oxygen.

The active component of the catalyst is a phase of interaction, including both atoms EN0, EN+nMe+m(where Me - K, Cs, Ba; 0, n, m - oxidation) and O-2with the General chemical formula RuxMeyOzthe PDF of the form of crystallites with a predominantly (at least 80%) less than 25

The catalyst has the following composition, wt.%:

Ruthenium (in terms of metal) - 1-8

Potassium (in terms of metal) - 1-15

Cesium (in terms of metal) - 1-15

Barium (in terms of metal) - 1-15

Oxygen - 0.5-7

Carbon media - Rest

The method of producing catalyst for ammonia synthesis includes sequential impregnation of the carbon carrier with solutions of compounds of ruthenium, impregnation promoting compounds of alkali and alkaline earth metals from group K, Cs, Ba, recovery of the catalyst, drying, calcining, as the parent compound of ruthenium use solutions of complex compounds of ruthenium with mono - and mostly polydentate nitrogen - or oxygen-containing ligands; as a carbon carrier used material, which is a three-dimensional carbon matrix with the pore volume of 0.2-1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 and with a radius of curvature of 100-10000 having a true density of 1.80-2.10 g/cm3, x-ray density 2.112-2.236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in dipsposal synthesis of ammonia, based on the interaction of nitrogen and hydrogen is carried out at elevated temperatures and pressures using a ruthenium catalyst on a carbon carrier, the catalyst contains ruthenium compounds (1-8 wt.% in terms of metal), at least one of the compounds of alkali and alkaline earth metals from a number of K, Cs, Ba (1-15 wt.% in terms of metal) and not more than 7 wt.% oxygen on a carbon carrier, representing a three-dimensional carbon matrix with the pore volume of 0.2-1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 and with a radius of curvature of 100-10000 having a true density of 1.80-2.10 g/cm3, x-ray density 2.112-2.236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in the range of 40-200 carried out at a pressure of 0.6-30.0 MPa, a temperature of 300-500oC, space velocities of 1000-200000 h-1.

The use of carbon in the catalyst carrier with certain parameters provides the necessary operational strength properties of catalyst - P=30-500 kg/cm2required adsorption properties with respect to the components implement luccheni properties.

The use of complex compounds of ruthenium with mono - and polydentate ligands of the formula [Ru-(N-L)n]Xmand [Ru(O-L)kXi1lets get on the surface of the carrier particles of the active component with the prevailing specific particle size, allowing higher concentrations of active centers of ammonia synthesis. Recovery when doing so, so that the oxygen content in the catalyst was in the range of up to 7 wt.%. The presence of oxygen in the catalysts for ammonia synthesis is traditionally considered a negative factor. The catalysts prior to operation are recovering hydrogen or reducing gas, but the oxygen content is not monitored.

In the proposed solution the presence of chemically bound oxygen in the catalyst: (a) prevents spontaneous ignition in air at boot (in the reactor) and unloading (from reactor) catalyst; (b) prevents hydrogen inhibition of the activation of dinitrogen and as a consequence increases the activity of the catalysts at pressures of 1.0-30.0 MPa; (C) prevents the loss of strength media with the introduction of the alkali metal in the carbon material.

Kaia with mono - and mostly polydentate ligands of the formula [Ru-(N-L)n] Xmand [Ru(O-L)n]X1where N-L, O-L nitrogen-containing (e.g., 2,2-dipyridyl or 1,10-phenanthrolin or pyridyl), oxygen (for example, the remains of a polybasic organic acid, oxalates, citrates) and nitrogen-, oxygen-containing (e.g., EDTA) ligands; Xmanion (e.g., Cl-), X1- cation (FOR example,+), l, m, n - stoichiometric ratios (2 to 6), and ruthenium ion is in oxidation state +2 or +3 or +4 (mostly +2 or +3); - modifying cations TO+Cs+, Ba+2enter predominantly from solutions of hydroxides or acetic acid salts; entering after impregnation of the carrier compounds of ruthenium and its restoration (mostly) or of joint solutions of compounds of ruthenium and modifying cation. The volume of injected solution modifier contains the estimated number of input modifier relative to the ruthenium. Then the catalyst is dried, restore.

The resulting catalyst samples are characterized by high activity against the reaction of the synthesis of ammonia from nitrogen and hydrogen, have a mechanical strength that is close to the magnitude of the strength of the original matrix, remain within dlitelnij in achieving consistently high activity is the size of the ligand and the absence of halogen ions in the initial compound of ruthenium or their absence in the inner sphere of the ruthenium ion in the initial compound. Tests showed that the highest activity have samples made from halogen-free complexes of ruthenium with large ligands.

The synthesis process is carried out at pressures of 0.6-30.0 MPa, temperatures of 300-500oC and space velocities of from 1000 to 200,000 h-1. For testing use of stoichiometric and non-stoichiometric nitrogen-hydrogen mixture (N2: H2= O. 33-1.0). Analysis of N2H2and NH3spend the detector. Estimate the strength of the obtained catalysts was performed on the instrument MP-9S. The chemical composition of the catalyst, the composition of the active component define the known methods of analysis: x-ray, XRF, rentgenofotoelektronnoj spectroscopy. To determine the crystallite size of ruthenium using scanning electron microscope SEM-U. To illustrate the claimed material the following are specific examples. Data on the composition, preparation, activity and properties of the catalysts are given in table. 1 and 2.

Example 1. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared as follows. An aliquot 76 ml of impregnating solution of ruthenium dipyridamolee [Ru(dip)3] Cl2with the concentration of the element of a three-dimensional carbon matrix with the pore volume of 0.2-1.7 cm3/g formed by the belt layers of carbon with a thickness 100-10000 with a radius of curvature of 100-10000 having a true density equal to 1.80 to 2.10 g/cm3, x-ray density 2.112-2.236 g/cm3and porous structure with a pore distribution with a maximum in the range 200-2000 or biporous structure with pore distribution with an additional maximum in the range of 40-200 ), dried (120oC, 2 h), recover hydrogen (400oC, 5 h), controlling the content into hydrogen and formed water. The resulting product is subjected to repeated impregnation, using the second part of the solution, identically reproducing all of the above-mentioned sequence of operations. The resulting product, containing 4 wt.% EN, impregnated, using an aliquot of 13.2 ml of a solution of potassium hydroxide KOH concentration of 47.6 g/l (0.85 M), dried (120oC, 2 h), recover hydrogen (400oC) controlling the content into hydrogen and formed water. The catalyst composition defined according to x-ray, x-ray and chemical analysis gives the following molecular formula: 4%Ru/4%K/1.4%O/C.

The resulting catalyst was investigated in the reaction of ammonia synthesis in conditions close to those described in the source information is isometrically (N2: H2= 1:3) of a gas mixture is equal to 30000 h-1, a pressure of 7.1 MPa and a temperature of 370oC. the Concentration of ammonia in the reaction mixture at the outlet of the reactor is 11.8%. The measurement result values of crushing strength for the sample was $ 123.1 kg/cm2.

Example 2. The catalyst composition of 4%Ru/15%K/3.7%O/C prepare and test as in example 1, using an aliquot of the solution dipyridamolee ruthenium 106,9 ml and an aliquot of 15.6 ml of a solution of potassium hydroxide KOH concentration 178.5 g/l (3.19 M).

Example 3. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared by the joint application of the ruthenium and the promoter. To the aliquot 22 ml of impregnating solution of ruthenium dipyridophenazine [Ru (dip)3] (OH)3with a concentration of 5.0 g EN/l add an aliquot 1.65 ml of a solution of potassium hydroxide KOH concentration 95.2 g/l (1.7 M) and used for impregnation of 5 g of granules of carbon carrier, and then dried (120oC, 2 h), recover hydrogen (400oC) controlling the content into hydrogen and formed water. The resulting product subjected to the same operations, receiving the specified catalyst composition.

Example 4 (example for comparison). The catalyst composition of 4%Ru/15.5%K/3.7%O/C is prepared analogously to example 1, with ISOE is repicci 3 g carbon media and with the introduction of promoter - potassium - uses 6.3 ml aliquot of a solution of potassium hydroxide KOH concentration 95.2 g/l (1.7 M).

Example 5. The catalyst composition of 4%EN/1%K/0.8%O/C prepare and test as in example 1, using an aliquot of the solution dipyridamolee ruthenium 36,6 ml and an aliquot of 4 ml of a solution of potassium hydroxide KOH concentration of 35.7 g/l (0.64 M).

Example 6. The catalyst composition of 8%Ru/4%K/2.1%O/C prepare and test as in example 3, using an aliquot 46.6 ml of impregnating solution of ruthenium dipyridophenazine [Ru (dip)3](OH)3with a concentration of 10.0 g EN/l and an aliquot of 3.5 ml of KOH solution with a concentration of 95,2 g/L.

Example 7. The catalyst composition of 1%Ru/4%K/0.8%O/C prepare and test as in example 3, using an aliquot of 10.6 ml of impregnating solution of ruthenium dipyridophenazine [Ru (dip)3](OH)3with a concentration of 5.0 g EN/l and an aliquot of 1.6 ml of KOH solution with a concentration of 95,2 g/L.

Example 8. The catalyst composition of 4%Ru/15%Cs/1.5%O/C prepare and test as in example 1, using the introduction of ruthenium aliquot 86,2 ml and then, with the introduction of a promoter, an aliquot of 3.2 ml of a solution of cesium hydroxide CsOH concentration of 66.7 g/l (0.44 M).

Example 9. The catalyst composition of 4%EN/1%Cs/0.7%O/C prepare and test anal the ora of cesium hydroxide CsOH concentration of 8.9 g/l (0.06 M).

Example 10. The catalyst composition of 1%Ru/1%K/1%Cs/1%Ba/0.5%O/C prepare and test as in example 1, using an aliquot of 36.6 ml of impregnating solution of ruthenium dipyridamolee [Ru(dip)3]Cl2with a concentration of 2.9 g Ru/l, the promoters applied sequentially, beginning potassium, using an aliquot of 25.7 ml of a solution of potassium hydroxide KOH concentration of 11.9 g/l (0.21 M), then cesium, using 18 ml aliquot of a solution of cesium hydroxide CsOH concentration of 13.3 g/l (0.088 M), and then barium, using an aliquot 10.4 ml of a solution of barium nitrate, Ba(NO3)2the concentration of 18.3 g/l (0.07 M).

Example 11. The catalyst composition of 4%Ru/15%Ba/2.4%O/C prepare and test as in example 1, using the introduction of ruthenium aliquot 87,9 ml and, with the introduction of a promoter, an aliquot 66,2 ml of a solution of barium nitrate, Ba(NO3)2the concentration of 54.9 g/l (0.21 M).

Example 12. The catalyst composition of 4%EN/1%Ba/0.7%O/C prepare and test as in example 1, using the introduction of ruthenium aliquot 73,1 ml and, with the introduction of a promoter, an aliquot of 13.6 ml of a solution of barium hydroxide Ba(OH)2the concentration of 9.6 g/l (0.056 M).

Example 13. The catalyst composition of 4%Ru/4%oBa/1.1%O/C prepare and test as in example 1, using the introduction of ruthenium aliquot of 76 ml, with an introd the emer 14. The catalyst composition of 4%Ru/4%Cs/4%Ba/1.3%O/C prepare and test as in example 1, using the introduction of ruthenium aliquot of 79.6 ml and, with the introduction of the promoter of the mixture formed by the aliquot of 14.4 ml of a solution of cesium hydroxide CsOH concentration of 36.0 g/l (0.24 M) and an aliquot of 30 ml of a solution of barium hydroxide Ba(OH)2the concentration of 18.9 g/l (0.11 M).

Example 15. The catalyst composition of 4%Ru/4%Cs/15%Ba/2.6%O/C prepare and test as in example 1 by introducing ruthenium from aliquots 93,2 ml; promoters were applied sequentially, first cesium, using an aliquot of 16.7 ml of a solution of cesium hydroxide CsOH concentration of 36.0 g/l (0.24 M) and then, after drying, put the second promoting component, using an aliquot 69,8 ml of a solution of barium hydroxide Ba(OH)2the concentration of 35.8 g/l (0.21 M).

Example 16. The catalyst composition of 4%Ru/8%Cs/8%Ba/2.1%O/C prepare and test as in example 1 by introducing ruthenium from aliquots to 88.4 ml; promoters applied sequentially, first cesium, using an aliquot 32,3 ml solution of cesium hydroxide CsOH concentration of 36.0 g/l (0.24 M) and then, after drying, put the second promoting component, using an aliquot of 36.3 ml of a solution of barium hydroxide Ba(OH)2the concentration of 35.8 g/l (0.21 M).

Example 17. The catalyst composition of 8%PT/15%K/15%Cs/15%Ba/7.0%dipyridamolee [Ru(dip)3]Cl2with a concentration of 11.6 g Ru/l, the promoters applied sequentially, beginning potassium, using an aliquot of 25.7 ml of a solution of potassium hydroxide KOH concentration 178.5 g/l (3.19 M), then cesium, using an aliquot of 54.1 ml solution of cesium hydroxide CsOH concentration of 66.7 g/l (0.44 M), and then barium, using an aliquot 52 ml of a solution of barium nitrate, Ba(NO)3)2the concentration of 54.9 g/l (0.21 M).

Example 18 (an example of the prototype). The catalyst composition of 4%Ru/20%K/39%Ba/C prepare and test as in example 8 prototype (Application EP N 0120655, MKI4B 01 J 23/58, SS 1/4, publ. 17.12.86 year). Granulated activated carbon media brand AG in an amount of 10 g, a specific surface area of 700 m2/g, the ratio of the specific surface value to the magnitude of the basal surface of 2.5: 1, the ratio of the value of the basal surface to the edge surface 150: 1, but not having the tape layers of carbon, impregnated with ruthenium chloride, using an aliquot 39 ml of impregnating solution of ruthenium chloride with a concentration of RuCl356.9 g/l, water is removed in a rotary vacuum evaporator; a sample dried at 100oC (2 h), restore the connection of ruthenium to the metallic state of hydrogen at 200oC (2 h), cooled to 20oC, after h brezec catalyst after impregnation is crushed to a fraction of 16-30 mesh, thus determining the magnitude of the tensile crushed, placed in a tubular reactor, which is activated in a stream of hydrogen, increasing the temperature to 450oC with a speed of 5oC/min, then maintained at a temperature of 450oC (1 1/4 hours). After cooling, the catalyst was tested in the reaction of ammonia synthesis at a fixed flow rate stoichiometric N2:H2= 1: 1) gas mixture equal to 30000 h-1, a pressure of 7.1 MPa and a temperature of 370 C. the Concentration of ammonia in the reaction mixture at the outlet of the reactor is 11.8%. The measurement result values of crushing strength for the sample was 2.1 kg/cm2.

Example 19 (an example of comparison). The catalyst composition of 4%Ru/4%K/1.4%O/C prepared according to example 1, with the ruthenium make of the impregnating solution chloralhydrate ruthenium RuCl3xH2O. the catalyst was investigated in the reaction of ammonia synthesis in the conditions described in the information source (application EP N 0120655, MKI B 01 J 23/58, C 01 C 1/04, publ. 17.12.86, prototype), i.e., at a fixed flow rate stoichiometric N2:H2= 0.33) of a gas mixture is equal to 1300 h-1, at a pressure of 3.0 MPa and a temperature of the si, 2,700 h-1at a pressure of 0.6 MPa and a temperature of 350oC. concentrations of ammonia in the reaction mixture at the outlet of the reactor are given in table. 2. The measurement result of the prevailing crystallite size of ruthenium for the sample was 80 .

Example 20. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared according to example 1, with the ruthenium make of the impregnating solution of ruthenium dipyridamolee [Ru(dip)3] Cl2. The resulting catalyst was investigated in the reaction of ammonia synthesis according to example 19.

Example 21. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared according to example 1, with the ruthenium make of the impregnating solution of ruthenium nitrosylated Ru(NO) (NO3)3. The resulting catalyst was investigated in the reaction of ammonia synthesis according to example 19.

Example 22. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared according to example 1, with the ruthenium make of the impregnating solution of ruthenium dipyridophenazine [Ru(dip)3] (OH)3. The resulting catalyst was investigated in the reaction of ammonia synthesis according to example 19.

Example 23. The catalyst composition of 4%Ru/4%/1.4%O/S is prepared according to example 1, with the ruthenium make of the impregnating solution based on potassium-Tris-acculturational (III) ERU 19.

Example 24. The catalyst composition of 4%Ru/4%K/1.4%O/C prepared according to example 1, with the ruthenium make of the impregnating solution on the basis of potassium-bis-nitrotoluene (III) K3[Ru(citrate)2]. The resulting catalyst was investigated in the reaction of ammonia synthesis according to example 19.

Thus, the presented examples show that the proposed catalyst has high mechanical strength and catalytic activity in the synthesis of ammonia; the resulting catalyst is not pyrophoric under operating conditions.

1. The catalyst for ammonia synthesis carbon media, including in terms of metal 1 to 8 wt.% compounds of ruthenium, 1 to 15 wt.% at least one of the compounds of alkali and alkaline earth metals from a number of potassium, cesium, barium, characterized in that as the carbon carrier used material, which is a three-dimensional carbon matrix with the pore volume of 0.2 - 1.7 cm3/g formed by the belt layers of carbon with a thickness of 100 to 10,000 and with a radius of curvature of 100 - 10000 having a true density of 1.80 - 2.10 g/cm3, x-ray density 2,112 - 2,236 g/cm3and porous structure with a pore distribution with a maximum in the range of 200 to 2000 or biporous straw, wt.%:

Ruthenium (in terms of metal) - 1 - 8

At least one or a mixture of compounds of alkali and alkaline earth metals from a number of potassium, cesium, barium (in terms of metal, each) - 1 - 15

Oxygen is Not more than 7

Media - Rest

2. The catalyst p. 1, characterized in that the active component of the catalyst is a phase of interaction, including both atoms ENabout, EN+nMe+m(where Me - K, Cs, Ba, o, n, m - oxidation) and O-2with the General chemical formula RuxMeyOzwhen x = 1, y = 1 to 10, z = 0.2 to 8,0 (where x, y and z are stoichiometric coefficients), dispergirovannoyj in the carbon matrix of the media in the form of crystallites with a predominantly (at least 80%) less than 25

3. The catalyst p. 1, characterized in that it has the following composition, wt.%:

Ruthenium (in terms of metal) - 1 - 8

Potassium (in terms of metal) - 1 - 15

Cesium (in terms of metal) - 1 - 15

Barium (in terms of metal) - 1 - 15

Oxygen - 0.5 to 7

Media - Rest

4. The method of producing catalyst for ammonia synthesis, including sequential impregnation of the carbon carrier with solutions of compounds of ruthenium, impregnation promoting compounds, molocnica fact, as source compounds of ruthenium use solutions of complex compounds of ruthenium with mono - and mostly polydentate nitrogen - or oxygen-containing ligands; as a carbon carrier used material, which is a three-dimensional carbon matrix with the pore volume of 0.2 - 1.7 cm3/g formed by the belt layers of carbon with a thickness of 100 to 10,000 and with a radius of curvature of 100 - 10000 having a true density of 1.80 - 2.10 g/cm3, x-ray density 2,112 - 2,236 g/cm3and porous structure with a pore distribution with a maximum in the range of 200 to 2000 or biporous structure with pore distribution with an additional maximum in the range 40 - 200 stage of recovery is carried out before the oxygen content in the catalyst is not more than 7 wt.%.

5. The method of synthesis of ammonia, based on the interaction of nitrogen and hydrogen is carried out at elevated temperatures and pressures using a ruthenium catalyst on a carbon carrier, wherein the catalyst contains (in terms of metal), 1 to 8 wt.% compounds of ruthenium, 1 to 15 wt.% at least one of the compounds of alkali and alkaline earth metals from a number of K, Cs, Ba, and not more than 7 wt.% oxygen operon tape layers of carbon with a thickness of 100 10000 and with a radius of curvature of 100 - 10000 having a true density of 1.80 - 2.10 g/cm3, x-ray density 2,112 - 2,236 g/cm3and porous structure with a pore distribution with a maximum in the range of 200 to 2000 or biporous structure with pore distribution with an additional maximum in the range 40 - 200 and the ammonia synthesis is carried out at a pressure of 0.6 - 30,0 MPa, a temperature of 300 - 500oC, space velocities of 1000 to 200000 h-1.

6. The method according to p. 5, characterized in that the synthesis of ammonia is carried out at a pressure of 3 to 11 MPa, a temperature of 340 - 415oC, space velocities of 10000 - 100000 h-1.

 

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6 cl, 6 ex

FIELD: inorganic synthesis catalysts.

SUBSTANCE: ammonia synthesis catalyst is based on ruthenium on carrier of inoxidizable pure polycrystalline graphite having specific BET surface above 10 m2/g, said graphite being characterized by diffraction pattern comprising only diffraction lines typical of crystalline graphite in absence of corresponding bands of amorphous carbon and which graphite being activated with at least one element selected from barium, cesium, and potassium and formed as pellets with minimal dimensions 2x2 mm (diameter x height). Catalyst is prepared by impregnating above-defined catalyst with aqueous potassium ruthenate solution, removing water, drying, reduction to ruthenium metal in hydrogen flow, cooling in nitrogen flow, water flushing-mediated removal of potassium, impregnation with aqueous solution of BaNO3 and/or CsOH, and/or KOH followed by removal of water and pelletizing of catalyst.

EFFECT: increased activity of catalyst even when charging ruthenium in amount considerably below known amounts and increased resistance of catalyst to methane formation.

12 cl, 1 tbl

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