The catalyst for the oxidation of carbon monoxide and hydrocarbons (options)

 

(57) Abstract:

The invention relates to catalysts for deep oxidation of CO, hydrocarbons, soot, purification of vehicle exhaust and waste gases of industrial enterprises. The proposed catalyst contains aluminum metal and oxide composite consisting of aluminum oxide, oxides of transition metals and, optionally, oxides of rare earth elements or their compounds and/or phosphorus oxide and/or silicon oxide and/or mixtures of oxides of transition metals. The catalyst may also contain platinum metals or their mixtures. The catalyst has high activity and stability in relation to the above processes. 2 C. and 23 C.p. f-crystals, 1 table.

The invention relates to the field of technical chemistry, catalysts for deep oxidation of CO, hydrocarbons, soot, purification of vehicle exhaust and waste gases of industrial plants.

It is known that the oxidation processes are usually accompanied by heat, cause overheating to the deactivation of the catalysts. The afterburning processes of pollutants in the exhaust and flue gases are characterized by large pressure drops during operation, splicecom layer and to increase the mechanical strength of the catalysts is the use as catalysts of "ceramometal", combining thermal stability of oxide ceramics, mechanical strength and thermal conductivity of metals [1]. Among ceramometal become more and more widespread catalysts based on oxides of aluminum and aluminum metal [2-4].

Thus, in [2] described the method of preparation of oxidation catalyst comprising an agglomeration of powders TiO2and aluminum, followed by the introduction compounds containing Mo, V, K2SO4.

There is also known a method of preparation of the catalyst based on aluminum foil, in which copper or Nickel is applied onto the foil from the solution by galvanic method, then oxidizes when anodizing, and 0.05 wt.% Pd introduced by impregnation [3]. Obtained from the foil cell catalyst is not only high strength and conductivity, and low hydraulic resistance, which is important for reducing the cost of gas treating processes.

In [4] , selected as a prototype, patented not only the way of cooking, but also the composition of the catalyst. The catalyst of the prototype is a porous monolith, in which the active ingredient is evenly distributed between the surface and the volume of pellets. Get seceretariat on the air. The catalyst of the prototype contains metallic aluminum (Al0) 27,4 - or 39.3 wt.%, when the content weight. % of aluminum oxide - 41,1 - 58,7, cobalt oxide - 2,1 - 31,5. Thus, presented in patent literature catalysts based on aluminum metal and oxide composite material include oxide or composite composition of Al1,20-1,88Co0.05-0.50 toOythe number of 60.5 - to 72.6 wt.%, aluminum metal - rest; or catalysts include platinum metal in the amount of 0.05 wt.% without specifying the concentration of the other catalyst components.

The most important disadvantage of the catalysts based on aluminum metal, including the prototype, is the formation of aluminum at temperatures above 660oC through the cracks in the oxide ceramic layer, which leads to the destruction and decontamination of catalysts [5].

The challenge which seeks the invention is to improve thermostability and activity of catalysts based on aluminum metal and oxide composite while maintaining high mechanical strength and thermal conductivity of the catalyst. The problem is solved by reducing the concentration of oxide composite catalyst to 5.0 to 34.4 wt.% and IZMENENIY, of silicon oxide, phosphorus oxide in various combinations, increasing the density and thermal stability of the ceramic coating on the surface of aluminum metal and not letting it flow out of the ceramic shell at temperatures above the melting temperature of aluminum. The active ingredient in the proposed catalyst is concentrated in the surface of the ceramic layer of a thickness of not more than several tens of microns. However, the overall composition of the modified oxide composite corresponds to the formula: Al0,52-1,95Ln0-0,06P0-0,16Si0-0,26Me0,003-0,73Oywhere Ln is a rare earth elements, or mixtures thereof, Me - transitional elements or mixtures thereof. Moreover, the additional incorporation in the catalyst of the platinum metals or their mixtures in large than is noted in the patent literature, quantities - 0.06 to 1.20 weight. % in combination with a modified oxide composite also allows you to increase thermostability and activity of the catalyst. The composition of the oxide of the composite corresponds to the formula:

Al0,64-2,0Ln0-0,06P0-0,42Si0-0,47Me0-0,82Oy.

Thus, the proposed catalyst in addition to aluminum metal, oxide and the IDA rare earth elements (Ln) or their mixtures - 0,06-2,00; or a phosphorus oxide - 0,2-3,1; or a silicon oxide - 0,1-5,0; or various combinations of these oxides. In addition, the catalyst in addition to aluminum metal, aluminum oxide (0,9-21,8% wt.) additionally contains (wt.%): platinum metals (M), or a mixture thereof is 0.06-1,20; oxides of transition metals or mixtures thereof, and 0.1-8,4; or oxides of rare earth elements, or mixtures thereof is 0.06 to 2.0; or a phosphorus oxide, and 0.1 - 5,1; or a silicon oxide - 0,2-4,6; or various combinations of these oxides.

The term "platinum group metals" (M) refers to the transition metals 5 and 6 periods VII group of the periodic table platinum collection [6]. The term "rare earth elements (Ln) is used in a broad sense, including the elements of the periodic table group IIIb, and 4f elements or the lanthanides [7]. The term "transition elements" (Me) refers to the 3d elements of the 4th period of the periodic system.

The proposed catalyst was prepared by electrochemical oxidation of smooth or corrugated aluminum foil or other products of aluminum metal. The thickness of the oxide coating will vary with the change of time, current and voltage of the electrochemical process. Ceramometal containing aluminum oxide and aluminum metal, silicon receive anode-spark method similar to [8]. The composition of the oxide layer varies, changing the composition of the electrolyte. After stage electrochemical oxidation ceramometal washed of impurities of sodium, dried and calcined at 400-600oC. Then, in the case of using aluminum foil, alternating layers of smooth and corrugated foil or put in a spiral of Archimedes [5], or in parallel layers with subsequent consolidation perimeter in a steel shell. After that enter the oxides of rare earth and transition elements together or separately by impregnation of ceramometal in solutions of nitrate salts of the corresponding composition, followed by drying and calcination at 400 to 600oC. Platinum metals introduced by impregnation of ceramometal in or ammonium chloride solutions of the corresponding PGE, followed by drying and calcination at 400 to 600oC.

Example 1. On an aluminum foil of a thickness of 0.5 mm put a layer of aluminum oxide of a thickness of 4 μm by anodic oxidation similarly to [5], then put the cerium oxide and palladium. The catalyst composition, wt.%: Al0- 98,0; oxide composite (Al1,94Ce0,04Oy) - 1,94; Pd - 0,06.

Example 2. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide of a thickness of 6 μm anode which meets the composite (Al1,84Ce0,01Mn0,07Oy) - 5,0.

Example 3. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide of a thickness of 22 μm anodic oxidation similarly to [5], then applied palladium. The composition of the catalyst weight. %: Al0- 82,1; oxide composite (Al2,0O3) - 17,8; Pd is 0.1.

Example 4. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide with a thickness of 30 μm by anodic oxidation similarly to [5], then put the oxides of cerium, lanthanum and manganese. The catalyst composition, wt.%: Al0- 65,9; oxide composite (Al1,42Ce0,01La0,01Mn0,28Oy) to 34.4.

Example 5. On an aluminum foil of a thickness of 0.5 mm put a layer of aluminum oxide of a thickness of 4 μm by anodic oxidation similarly to [5], then applied manganese oxide and palladium. The catalyst composition, wt.%: Al0- 96,6; oxide composite (Al1,84Mn0,08Oy) - 3,2; Pd - 0,2.

Example 6. On an aluminum foil of a thickness of 0.5 mm put a layer of aluminum oxide with a thickness of 5 μm similarly to [5], then put the oxides of lanthanum, manganese, and palladium. The catalyst composition, wt.%: Al0- 85,8; oxide composite (Al1,62La0,05Mn0,13Oy) - 4,0; Pd - 0,2.

Example 7. On the aluminum foil with the thickness of 0.3 mm nanos is utilizator, weight. %: Al0- 74,4; oxide composite (Al1,77Ce0,05Mn0,02Oy) - 24,4; Pd - 1,2.

Example 8. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and phosphorus from solution sodium hexametaphosphate thickness of 22 μm anodic spark oxidation similarly to [8], then applied manganese oxide. The catalyst composition, wt.%: Al0- 82,1; oxide composite (Al1,95P0,002Mn0,003) and 17.9.

Example 9. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and phosphorus with a thickness of 4 μm anodic spark oxidation similarly to [8], then put the cerium oxide and palladium. The catalyst composition, wt.%: Al0- 73,04; oxide composite (Al1,56Ce0,06P0,16Oy) and 26.9; Pd - 0,06.

Example 10. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and phosphorus with a thickness of 15 μm similarly to [8], then put the oxides of lanthanum, manganese, and palladium. The catalyst composition, wt.%: Al0- 89,8; oxide composite (Al1,84La0,02P0,03Mn0,01Oy) - 10,1; Pd is 0.1.

Example 11. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and phosphorus with a thickness of 20 μm similarly to [8], then put the oxides of cerium, cobalt and Nickel. The composition of the catalyst,ptx2">

Example 12. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and silicon from the solution of sodium silicate with a thickness of 5 μm anodic spark oxidation similarly to [8] , then put the cobalt oxide. The catalyst composition, wt.%: Al0- 67,7; oxide composite (Al0,98Si0,26Co0,45Oy) is 32.3.

Example 13. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and silicon thickness of 10 μm similarly to [8], then put the oxides of cerium, manganese, and palladium. The catalyst composition, wt.%: Al0- 87,4; oxide composite (Al0,64Si0,02Mn0,82Oy) - 12,5; Pd is 0.1.

Example 14. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and silicon thickness of 22 μm similarly to [8], then applied palladium. The catalyst composition, wt.%: Al0- 96,5; oxide composite (Al1,87Si0,08Oy) - 4,3; Pd - 0,2.

Example 15. On the aluminum foil with the thickness of 0.3 mm is applied a layer of oxides of aluminum, phosphorus and silicon thickness of 20 μm anodic spark oxidation similarly to [8], then put the oxides of lanthanum, manganese and platinum. The catalyst composition, wt.%: Al0- 82,5; oxide composite (Al1,34La0,03P0,003Siof 0.47Mn0,01Oy) - 16,3; Pt - 1,2.

P what about the [8], then put the oxides of cerium, chromium, and palladium. The catalyst composition, wt.%: Al0- 78,3; oxide composite (Al1,69Ce0,01Si0,19Cr0,01Oy) - 21,5; Pd - 0,2.

Example 17. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and silicon thickness of 20 μm similarly to [8], then put the cerium oxide and palladium. The composition of the catalyst weight. %: Al0- 78,1; oxide composite (Al1,66Ce0,01Si0,19Oy) - 21,7; Pd - 0,2.

Example 18. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide and silicon thickness of 15 μm similarly to [8], then put the oxides of lanthanum, chromium and manganese. The catalyst composition, wt.%: Al0- 78,5; oxide composite (Al1,66La0,01Si0,19Mn0,005Cr0,005Oy) - 21,5.

Example 19. On an aluminum foil of a thickness of 0.5 mm put a layer of aluminum oxide and phosphorus with a thickness of 5 μm similarly to [8], then applied manganese oxide and palladium. The catalyst composition, wt.%: Al0- 84,0; oxide composite (Al1,61P0,14Mna 0.1Oy) - 15,8; Pd - 0,2.

Example 20. On an aluminum foil of a thickness of 0.5 mm put a layer of aluminum oxide and phosphorus with a thickness of 5 μm similarly to [8], then applied palladium. The catalyst composition, wt.%: Al00- 98,5; oxide composite (Al1,26P0,10Mn0,39Oy) - 1,4; Pd is 0.1.

Example 22. On the aluminum foil with the thickness of 0.3 mm is applied a layer of oxides of aluminum, phosphorus and silicon thickness of 10 μm similarly to [8], then put the oxides of cerium and manganese. The catalyst composition, wt.%: Al0- 94,0; oxide composite (Al0,52P0,06Si0,03Ce0,06Mn0,73Oy) - 6,0.

Example 23. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide. phosphorus and silicon thickness of 10 μm similarly to [8], then put a cerium oxide, platinum and palladium. The catalyst composition, wt.%: Al0- 86,0; oxide composite (Al1,79Ce0,01P0,04Si0,07Oy) - 13,8; Pt - 0,1; Pd Is 0.1.

Example 24. On the aluminum foil with the thickness of 0.3 mm is applied a layer of oxides of aluminum, phosphorus and silicon thickness of 8 μm similarly to [8], then applied palladium. The composition of the catalyst weight. %: Al0- 88,4; oxide composite (Al1,33P0,42Si0,02Oy) - 11,5; Pd is 0.1.

Example 25. On the aluminum foil with the thickness of 0.3 mm is applied a layer of oxides of aluminum, phosphorus and silicon thickness of 10 μm similarly to [8], then put the chrome oxide and palladium. DC1,5; Pd is 0.1.

Example 26. On the aluminum foil with the thickness of 0.3 mm put a layer of aluminum oxide of silicon and phosphorus from solutions of sodium hexametaphosphate and sodium silicate thickness of 9 μm similarly to [8], then applied manganese oxide. The catalyst composition, wt.%: Al0- 88, 2; oxide composite (Al1,74P0,06Si0,03Mn0,06Oy) 11.8 in.

The stoichiometry of elements in oxide composite is determined by the mole fractions of oxides, stable in this temperature region: Al2O3La2O3CeO2, MnO2, Cr2O3, Co3O4, NiO, P2O5, SiO2. The catalytic activity of samples of the catalyst determine bigradient methods: in the oxidation of butane in the oxidation rate at an initial concentration of 0.5 vol.% and stationary -0,2 about. % in air, a temperature of 400oC; in the oxidation of CO at temperatures reach 50% degree of reaction is about 1.% CO in air for 1 g of catalyst. The results are given in the table.

As can be seen from the table, the proposed activity of catalysts containing oxides of transition metals, high enough for catalysts based on metallic media not containing the platinum metal is the stability of the catalysts. It must be emphasized that the catalysts with platinum metals, calcined at 700oC showed high stability both in terms of activity (table) and save the mechanical strength of the structure.

Sources of information taken into account:

1. The Ananyin Century. And. , Belyaev Centuries, Parmon C. N., Sadykov C. A., S. Tikhov F., Starostina, So New materials based on aluminum tracks for problems of ecology and alternative energy. XY Mendeleev Congress on General and applied chemistry, Minsk: Nauka i techno (Belarus), 1993, T. 1, S. 35-36.

2. A patent. Holland N 144497, class B 01 J 21/00, 1968.

3. USSR author's certificate N 923588, class B 01 J 37/02, B. I. N 16, 1982.

4. Application copyright certificates of the USSR N 92001114, class B 01 J 37/00, B. I. N 27, 1995.

5. USSR author's certificate N 1034762, class B 01 J 37/02; B 01 J 35/04, B. I. N 30, 1983.

6. Nekrasov B. C. fundamentals of General chemistry I. 3, M.: Chemistry, 1970, S. 380.

7. Cotton F., D. Wilkinson D. Modern inorganic chemistry., so 3 Chemistry of transition elements, M.: Mir, 1969, S. 500.

8. Chernenko Century. And., Snezhko L. A., Papanov And. And. coatings anodic spark electrolysis, L.: Chemistry, 1991, S. 150.

1. The oxidation catalyst oxide coal is xed transition metal (Me), characterized in that the oxide composite further comprises an oxide of rare earth element (Zn), or a mixture of oxides of rare earth elements, and/or phosphorus oxide and/or silicon oxide, or a mixture of oxides of transition metals (Me), and the catalyst contains, by weight.

Oxide composite 5,0 34,4

Metal aluminum Else

2. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

y is determined by the valence of the cations and the values a, b.

3. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < c < 0,06;

y is determined by the valence of the cations and the values a, b, c.

4. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebPdOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < d < 0,16;

y is determined by the valence of the cations and the values a, b, d.

5. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

Alais entoto cations and the values of a, b, e.

6. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncPdOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < c < 0,06;

0 < d < 0,16;

y is determined by the valence of the cations and the values a, b, c, d.

7. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebPdSieOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < d < 0,16;

0 < e < 0,26;

y is determined by the valence of the cations and the values a, b, d, c.

8. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncSicSieOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < c < 0,06;

0 < e < 0,26;

y is determined by the valence of the cations and the values a, b, c, e.

9. The catalyst p. 1, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncPdSieOy,

where 0,52 < a < 1,95;

0,003 < b < 0,73;

0 < c < 0,06;

0 < d < 0,16;

0 < e < 0,26;

y is determined by the valence of the cations and the values a, b, c, d, e.

M 0,06 1,20

Oxide composite 1,0 26,9

Metal aluminum Else

11. The catalyst according to p. 10, characterized in that the oxide composite catalyst contains composite, optionally containing an oxide of rare earth element (Zn), or a mixture of oxides of rare earth elements, and/or phosphorus oxide and/or silicon oxide and/or oxide of the transition metal (Me), or a mixture of oxides of transition metals.

12. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

y is determined by the valence of the cations and the values a, b.

13. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaZncOy,

where 0,64 < a < 2,0;

0 < c < 0,06;

y is determined by the valence of the cations and the values of a, c.

14. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaPa, d.

15. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaSieOy,

where 0,64 < a < 2,0;

0 < e < 0,47;

y is determined by the valence of the cations and the values of a, e.

16. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < c < 0,06;

y is determined by the valence of the cations and the values a, b, c.

17. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebPdOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < d < 0,42;

y is determined by the valence of the cations and the values a, b, d.

18. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebSieOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < e < 0,47;

y is determined by the valence of the cations and the values a, b, e.

19. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaPdZncOy,

where 0,64 < a < 2,0;

0 < d < 0,42;

0 < the clinical topics the composition of the oxide of the composite corresponds to the formula

AlaPdSieOy,

where 0,64 < a < 2,0;

0 < d < 0,42;

0 < e < 0,47;

y is determined by the valence of the cations and the values of a, d, e.

21. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaZncSieOy,

where 0,64 < a < 2,0;

0 < c < 0,06;

0 < e < 0,47;

y is determined by the valence of the cations and the values of a, c, e.

22. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncPdOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < c < 0,06;

0 < d < 0,42;

y is determined by the valence of the cations and the values a, b, c, d.

23. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncSieOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < c < 0,06;

0 < e < 0,47;

y is determined by the valence of the cations and the values a, b, c, e.

24. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaZncPdSieOy,

where 0,6 what uchinami a, c, d, e.

25. The catalyst according to p. 11, characterized in that the composition of the oxide of the composite corresponds to the formula

AlaMebZncPdSieOy,

where 0,64 < a < 2,0;

0 < b < 0,82;

0 < c < 0,06;

0 < d < 0,42;

0 < e < 0,47;

y is determined by the valence of the cations and the values a, b, c, d, e.

 

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