The method of producing catalyst to obtain a vinyl acetate comprising palladium and gold on a copper-containing medium, and method for producing vinyl acetate using the obtained catalyst (options)

 

(57) Abstract:

The described method of preparation of the catalyst to obtain a vinyl acetate by the interaction of ethylene, oxygen and acetic acid, including porous media, porous surface which metallic copper precipitated in an area surrounded by sediments of catalytically effective amounts of metallic palladium and gold, which essentially is not mixed with the specified copper. According to the invention the catalyst was prepared by impregnation of the support with an aqueous solution of water-soluble salts of copper; the fixing of the specified copper in the form of a water-soluble compound by interaction with an appropriate alkaline compound, and then impregnation of the catalyst with one or more solutions of water-soluble salts of palladium and/or gold, and a quantity of elemental palladium and gold in all the last impregnating solutions of equal predetermined amounts of metallic palladium and gold required in the catalyst; fixing the catalyst of palladium and/or gold present in the catalyst in solution after each impregnation, the interaction between dissolved in this solution a water-soluble salt with an appropriate alkaline compound for oetoriya in water copper compounds, palladium and/or gold present in the catalyst after each fixation is not water-soluble compounds of palladium and/or gold or after fixing the catalyst for all the latest water-insoluble compounds. Also described methods for producing vinyl acetate by the interaction of ethylene, oxygen and acetic acid comprising contacting the latter reagents with the obtained catalyst (options). Effect: increase primary productivity vinyl acetate due to lower CO2the selectivity. 4 C. and 5 C.p. f-crystals, 1 table.

This invention relates to a new and improved catalyst for obtaining vinyl acetate by the interaction of ethylene, oxygen and acetic acid.

Description of prior and related technical field

As is known, to obtain a vinyl acetate by the interaction of ethylene, oxygen and acetic acid is used a catalyst which contains palladium, gold and copper supported on a carrier. Despite the fact that the way in which the use of such a catalyst, it is possible to obtain vinyl acetate with relatively high levels of performance, any way, leading to greater proizv be considered as publications, related to the claimed invention.

In U.S. Patent 5332710, issued July 26, 1994 (Nicolau et al.), describes a method of producing a catalyst useful in the production of vinyl acetate by the interaction of ethylene, oxygen and acetic acid, comprising the impregnation of porous media, water-soluble salts of palladium and gold, the recording media of palladium and gold in the form of insoluble compounds by dipping and turning (tumbling) impregnated carrier in the reaction solution for the deposition of such compounds and subsequent recovery of the compounds to the free metals.

In U.S. Patent 5347046, issued September 13, 1994 (White et al.), describes catalysts for production of vinyl acetate by reaction of ethylene, oxygen and acetic acid comprising the metal of palladium and/or its connection, gold and/or its connection and copper, Nickel, cobalt, iron, manganese, lead or silver, or their connection, preferably deposited on a material carrier.

Brief description of the invention

In accordance with this invention, is provided a catalyst useful for obtaining vinyl acetate by reaction of ethylene, oxygen and oxynopterinae which precipitated metallic copper in the area, surrounded by catalytically effective amounts of metallic palladium and gold, which is essentially not mixed with copper. The catalyst of the invention lose less copper as a result of evaporation during prolonged use, which leads to a smaller increase in the selectivity to carbon dioxide and, therefore, thanks to this application, the lower the loss performance of vinyl acetate, than when using the equivalent of the catalyst on the carrier containing palladium, gold, copper, but wherein the copper is present on the media, on being mixed with palladium or gold, or both of these metals due to co-deposition of copper on the carrier with one of the two or both precious metals.

Detailed description of the invention

The invention relates to the discovery, before this time is appreciated that in the preparation of vinyl acetate using supported on a carrier catalyst containing palladium, gold and copper in which copper is essentially mixed with palladium or gold or both of these metals, the copper content in the catalyst during the lifetime of the catalyst tends essentially to decrease, that is, you RDA. This loss of copper, obviously, due to the fact that in terms of the interaction of copper, which is on the surface or near the surface of the catalyst particles, interacts with one or more reagents to form compounds capable of vothonas. However, in the catalyst of this invention, the copper is fixed on the surfaces of the carrier before palladium and gold, which substantially surround the copper, and this leads to the fact that it is less exposed to the ambient conditions in the reactor. Therefore, any educated compound of copper, which is able to vothonas, has less opportunity to dispergirujutsja in the reactor, and therefore, the vapor pressure of such copper compounds close to the partial pressure sublimirovannogo copper compounds in its environment. This leads to a smaller loss of copper by means of sublimation, than when copper is mixed with one or both of noble metals on the surface or near the surface of the catalyst particles. In this regard, it is noted that while the selectivity for carbon dioxide of the process of obtaining vinyl acetate using any catalyst on the carrier containing palladium and gold, analizator into the reactor until the shutdown of the reactor for the purpose of replacement or regeneration of the catalyst, selectivity for carbon dioxide is usually lower than at any point in the lifetime of the catalyst when the catalyst contains a small amount of copper in addition to palladium and gold, than when copper is absent or present in smaller quantities. Therefore, the loss of a smaller amount of copper during the lifetime of the catalyst of this invention leads to a higher overall performance vinyl acetate than using a catalyst containing platinum, gold and copper in which the copper is mixed with one or both of noble metals on the surface or near the surface of the catalyst particles.

In the method of producing the catalyst of the present invention suitable porous carrier is first impregnated with an aqueous solution of water-soluble copper salt such as copper nitrate of three-hydrate, copper chloride anhydrous or dihydrate, copper acetate, copper sulfate or copper bromide, etc. For impregnation of copper salts can be used in methods known in the art. Preferably, the impregnation can be performed using the method of incipient moisture, in which the quantity of a solution of copper compounds used for impregnation is from about 95 to about 100 nternal copper in the solution for impregnation is equal to a predefined number in the interval for example, from about 0.3 to about 5.0 and preferably from about 0.5 to about 3.0 g/l of catalyst.

The material of the catalyst carrier consists of particles having any of various right or wrong forms, such as spheres, tablets, cylinders, rings, stars or other shapes, and may have dimensions such as diameter, length or width from approximately 1 to approximately 10 mm, preferably, from about 3 to 9 mm Sphere with a diameter of from about 4 to about 8 mm are preferred. The material of the carrier may consist of any suitable porous material, for example silicon dioxide, alumina, silica-alumina, titanium dioxide, zirconium dioxide, silicates, aluminosilicates, titanates, spinel, silicon carbide or carbon, etc.

The material of the carrier may have a surface area in the range of, for example, from about 10 to about 350 m2/g, preferably from approximately 100 to approximately 200 m2/g, the average pore size in the range of, for example, from about 50 to about 2000 angstroms and a pore volume in the range of, for example, from about 0.1 to 2 ml/g, predpochtitelney copper, copper "fix" that is precipitated in the form of a water-soluble compound such as the hydroxide, interaction with an appropriate alkaline compound, for example, hydroxide, silicate, borate, carbonate or bicarbonate of an alkali metal in an aqueous solution. The hydroxides of sodium and potassium are the preferred alkali compounds to fix. Alkali metal alkaline compound should be present in amounts of, for example, from about 1 to about 2, preferably from about 1.1 to about 1,6 mole per mole of the anion of the soluble salts of copper. Fixing of copper may be known in the art methods. However, preferably the fixation of copper is performed using the method of incipient moisture, in which the impregnated carrier is dried, for example at a temperature of 150oC for one hour in contact with the aqueous solution of alkaline compounds, constituting approximately 95-100% of the pore volume of the carrier, and leave for a period of from about 1/2 hour to about 16 hours; or by Roto-immersion (roto-immersion), in which the impregnated carrier without drying is immersed in a solution of alkaline compounds and rotate and/or perivor the th compounds of copper was formed on the surface or near the surface of the particle carrier. Rotate or flip can be performed, for example, with a speed of from about 1 to about 10 rpm during the period of time from about 0.5 to about 4 hours the way Roto-immersion described in U.S. Patent 5332710, the content of which is introduced in the form of links (the patent is U.S. only).

Media containing a fixed copper, optional can be washed to the absence of essentially the catalyst traces of anions, such as halides, dried, e.g. in a fluidized bed dryer at 100oWith or within one hour, and calcined, for example, by heating in air up to 200oWith or within 18 h, and recovered, for example, in the vapor phase by contacting a copper-containing media with gaseous hydrocarbon, such as ethylene (5% in nitrogen), for example, if 150oC for 5 h, or in the liquid phase by contacting the media prior to washing and drying with an aqueous solution of hydrazine hydrate is added, including excess molar ratio of hydrazine and copper, for example, from about 8:1 to 12:1, at room temperature for from about 0.5 to about 3 hours, after which the carrier is washed and dried as described. Although any desired purpose, these stages often are not necessary because the washing, drying and recovering copper compounds can adequately be performed through similar stages, carried out with compounds of palladium and gold, which are copper-containing material of the carrier sequentially impregnated, as more precisely described below.

Then the material of the carrier, containing an area of fixed-insoluble copper compounds such as copper hydroxide or copper in the form of free metal with some possible content of the oxide, process for the deposition of catalytic amounts of palladium and gold on the surfaces of copper-containing particles of the medium. For this purpose you can use any of various methods, which include simultaneous or separate impregnation of the carrier with one or more aqueous solutions of water-soluble compounds of palladium and/or gold. The palladium (II) chloride, notreally (II) chloride, sodium palladium (II) chloride), kallepalli (II) chloride (potassium palladium (II) chloride), nitrate, palladium (II) or sulfate, palladium (II) are examples of suitable water-soluble palladium compounds, while the alkali metal salts, for example sodium or potassium salts, chloride zastarelih gold compounds. Salt of an alkali metal solitarycharlotte acid and notreally (II) chloride are the preferred compounds because of their good solubility in water. The applied amount of these compounds is therefore to provide, for example, from about 1 to about 10 g of palladium and, for example, from about 0.5 to about 10 grams of gold per liter of the target catalyst, and the amount of gold is from about 10 to about 125 wt.% based on the weight of palladium. Palladium and gold then fixed on the copper containing material media by treatment with an aqueous solution of a suitable alkali compounds for the deposition of palladium and gold in the form of water insoluble compounds, such as hydroxides, as described previously for preliminary fixation of copper on the carrier. And again the hydroxides of sodium and potassium are preferred as fixing alkali compounds, and fixing or deposition of water insoluble compounds of palladium and gold on the surface of the material media containing copper or compound of copper, can be performed by the method of incipient moisture or by Roto-immersion, as described previously in connection with the fixation on niteline not restored) can then be subjected to recovery for example, ethylene, for example, 5% in nitrogen at 150oC for 5 h after the first washing of the catalyst containing the fixed metal compounds, to complete absence of anions, such as halogenide, and drying, for example, if 150oC for approximately 1 hour, or such recovery may be carried out before washing and drying an aqueous solution of hydrazine hydrate is added, where the excess of hydrazine relative to the amount necessary to restore all of the metal compounds present on the carrier is in the range of, for example, from about 8:1 to about 15:1, followed by rinsing and drying. Other reducing agents and the means to restore the fixed metal compounds present on the media, can be used in traditional ways. The recovery of the fixed connection of the metal leads mainly to the formation of the free metal, although very small amounts of metal oxide may also be present.

Alternative to the above methods may be used a method of "separate record" to record palladium and gold on copper-containing medium and recovering the water-insoluble compounds metallomesogens carrier is first impregnated with an aqueous solution of water-soluble compounds of palladium and any other catalytically active metal, which is used in the catalyst, with the exception of gold, by the method of incipient moisture, and palladium, and other metals present then fixed by the fixing processing with an alkaline solution by the method of incipient moisture or Roto-immersion, preferably Roto-immersion. The catalyst was then dried and separately impregnated with a solution of water-soluble gold compounds containing the number of elementary gold required for the catalyst, and the gold is fixed by the fixing processing with an alkaline solution by the method of incipient moisture or Roto-immersion, preferably Roto-immersion. If gold is to be fixed by the method of incipient moisture, such fixing may be combined with the stage of impregnation through the use of a single aqueous solution of a soluble gold compounds and fixing alkali compounds in number, taken with an excess relative to the amount required to convert all the gold in solution in a fixed insoluble compound, such as gold hydroxide, gold. If in the vapor phase as a reducing agent should be used hydrocarbons such as ethylene or hydrogen, the catalyst containing fixed by sedimentologos, as explained above. If in the liquid phase as a reducing agent should be used hydrazine, a catalyst containing a fixed connection of metal, treated with an aqueous solution containing an excess of hydrazine hydrate is added, before washing and drying to recover the metal compounds to the free metals, and then the catalyst was washed and dried as described.

Another method of producing catalyst method is modified Roto-immersion, in which only part of the gold impregnorium with palladium and other metals, if used first impregnation, the metal is fixed engagement with the locking alkaline compound by Roto-immersion, fixed metal compounds reduced to the free metals, for example, ethyl or hydrazinehydrate with washing and drying before recovering ethylene or after reduction with hydrazine. Then the catalyst is impregnated with the rest of the gold in the form of a solution of water-soluble gold compounds and the catalyst was again restored, for example, ethylene or hydrazine, after or before washing and drying, as described above.

After the catalyst containing palladium and gold in the form of free the public is additionally impregnated with a solution of acetate of an alkali metal, preferably the acetate of potassium or sodium, and most preferably potassium acetate. The catalyst is then dried so that the target catalyst contains, for example, from about 10 to about 70 g/l of catalyst, preferably from about 20 to about 60 g of the acetate of alkali metal per liter of the target catalyst.

When vinyl acetate is obtained using catalysts in accordance with this invention, the gas stream, which contains ethylene, oxygen or air, acetic acid and, preferably, alkali metal acetate, passed over the catalyst. The composition of the gas stream can vary widely with regard to explosive concentrations. For example, the molar ratio of ethylene and oxygen may range from about 80:20 to about 98:2, the molar ratio of acetic acid and ethylene may be from about 100:1 to about 1:100, and the content of gaseous alkali metal acetate may be approximately 2-200 ppm relative to the applied acetic acid. The gas stream may also contain inert gases such as nitrogen, carbon dioxide and/or saturated hydrocarbons. The reaction temperature is but 150-220oC. is Used, the pressure may be somewhat reduced pressure, normal pressure or increased pressure, preferably a pressure of up to approximately 20 excess atmospheres (2030 kPa).

The following non-limiting examples additionally illustrate the invention.

EXAMPLE 1

Material carrier comprising particles of silica spherical shape brand Sud Chewie KA-160with the normal diameter of 7 mm, a surface area of approximately 165-170 m2/g and pore volume approx 0.68 ml/g, impregnated by the method of incipient moisture aqueous solution of nitrate of copper for three-hydrate, sufficient to provide the catalyst with a content of elemental copper approximately 1.9 grams/liter Copper without drying is fixed on the carrier by the handling carrier by Roto-immersion in an aqueous solution of sodium hydroxide containing 120% of the amount of sodium hydroxide required for the conversion of copper hydroxide copper. Media containing a fixed copper hydroxide, then washed with water until the absence of anions and dried at a temperature of 100oOr 1 h in a fluidized bed dryer.

Then in media containing copper hydroxide, add the Pallady the ode rudimentary humidity aqueous solution notreally (II) chloride, sufficient for approximately 7 grams of elemental palladium per liter of catalyst. Palladium is then fixed on the carrier in the form of hydroxide, palladium (II) by treatment of the catalyst by the method of Roto-immersion in an aqueous solution of sodium hydroxide so that the molar ratio of Na/Cl was approximately 1.2:1. The catalyst was then dried at 100oOr 1 h in a fluidized bed dryer, and then by the method of incipient moisture impregnated with an aqueous solution of tetrachloroaurate sodium in sufficient quantity to obtain a catalyst containing 4 g/l of elemental gold, and sodium hydroxide so that the molar ratio of Na/Cl was approximately 1.8:1, to capture gold on the media in the form of a hydroxide of gold. The catalyst was then washed until no chloride (approximately 5 h) and dried for one hour in a stream of nitrogen. Hydroxides of copper, palladium and gold then reduced to the free metals, the contacting of the catalyst with ethylene (5% in nitrogen) in the vapor phase at 150oWith or within 5 hours, And finally the catalyst by the method of incipient moisture impregnated with an aqueous solution of potassium acetate in a quantity sufficient to provide 40 g azet the ASS="ptx2">

EXAMPLE 2

Repeat the procedure of example 1 with the difference that the media containing a fixed copper hydroxide, after drying and before impregnation with a solution of palladium salt, calicivirus by heating in a stream of air at 200oWith or within 18 PM

EXAMPLE 3

Repeat the procedure of example 2 with the difference that after calcination the media containing the hydroxide of copper, and before impregnation with a solution of salts of palladium hydroxide copper reduced to metallic copper in the vapor phase by contacting with ethylene (5% in nitrogen) at 150oWith or within 5 hours

EXAMPLE 4

Repeat the procedure of example 3 with the difference that the impregnation of the catalyst with an aqueous solution of tetrachloroaurate sodium sufficient solution used for the 7 instead of 4 g of elemental gold per liter of catalyst.

EXAMPLE 5

Repeat the procedure of example 1 with the difference that sufficient aqueous solution of nitrate of copper for three-hydrate used in the initial impregnation of the carrier to ensure 1,39, not 1.9 grams of elemental copper per liter of catalyst.

EXAMPLE 6

Repeat the procedure of example 4 with the difference that after the recovery of copper hydroxide to metallic copper impregnation and f is - MRI). In this method, the copper-containing media first method rudimentary moisture impregnated with a solution of salts of palladium and gold, sufficient to provide 7 grams of elemental palladium and 4 g of elemental gold, and metals capture method Roto-immersion in an aqueous solution of sodium hydroxide. The catalyst was then washed until no chloride solution, dried at 150oC for 5 h in a stream of nitrogen and restore in the vapor phase of 5% ethylene in nitrogen at 150oWith or 5 hours and Then the catalyst was impregnated by the method of incipient moisture aqueous solution of salt of gold, sufficient to provide the catalyst with 3 extra grams of elemental gold per liter of catalyst (7), and sodium hydroxide so that the molar ratio of Na/Cl was approximately 1.8:1 to commit additional gold, and the catalyst was washed, dried, recover ethylene and impregnated with potassium acetate as described in example 1.

EXAMPLE 7

Repeat the procedure of example 6 with the difference that the carrier is first impregnated with an aqueous solution of salt of copper, providing the catalyst with 1.39 g, instead of 1.9 grams of elemental copper per liter of catalyst impregnation with a solution of salt fell the ka second increment gold salts provides 2, instead of 3 additional grams of elemental gold per liter of catalyst containing a total of 4, not 7 grams of gold per liter of catalyst, the recovery of palladium and the first increment of gold is carried out in liquid phase using an aqueous solution of hydrazine hydrate is added in excess with the mass ratio of hydrazine and metal, equal to 12:1, and recovering the second increment of gold is carried out in the vapor phase with ethylene (5% in nitrogen) at 150oWith or within 5 hours

The catalysts obtained as described in examples 1-7 are active in the method of producing vinyl acetate by the interaction of ethylene, oxygen and acetic acid. For this, approximately 60 ml of the catalyst of each type obtained in the examples are placed in separate chronicleby basket. The temperature of each basket is measured by thermocouples at the top and the bottom of each basket. Each reaction basket placed in a reactor Bertie recirculation type with continuous stirring and maintain the temperature, which provides approximately 45% conversion of oxygen, using shirts with electric heating. A gas mixture containing approximately 50 normal liters (at normal temperature and pressure) ethno 50 mg of acetic acid and about 40 mg of potassium acetate, pass under pressure from approximately 12 atmospheres (1220 kPa) through each basket. The reaction is complete after about 18 hours the Analysis of the products is carried out by gas chromatography method "on line" in conjunction with the analysis of the liquid product by the method of "off line" by the condensation of the product flow at approximately 10oFor optimal analysis of the final products.

The following table presents the results obtained with the catalyst of each example and expressed in percentage selectivity for CO2(CO2, % sat.) and a heavy product (TP, % sat.) and the relative activity of the reaction (Act.). In addition, the table shows the content of palladium, gold and copper in each catalyst, expressed in grams per liter of catalyst (Pd/Au/Cu, g/l) obtained if the catalyst separate commit (SF) or by the modified method of Roto-immersion (MRI) (Meth. Floor. Cat.) and restored if palladium and gold to the metallic state by ethylene (C2H4) or hydrazine (N2H4or both reagents (C2H4+ N2H4) (Reducing agent).

The results presented in the table show that the catalyst of this invention in the General case, the actuator is ti, than the catalyst, limited equivalent quantities of palladium and gold as catalytically active metals. However, because the copper in the catalyst of the present invention is present on the surfaces of the carrier below palladium and gold, the rate of loss of copper due to sublimation of the reaction conditions is lower than in the case where copper is impregnated with palladium and gold, due to joint fixation or co-deposition in the form of water insoluble compounds, such as hydroxides impregnated water-soluble salts of copper, palladium and/or gold.

1. The method of producing catalyst to obtain a vinyl acetate by the interaction of ethylene, oxygen and acetic acid, comprising impregnating a porous support with solutions of water-soluble salts of copper, palladium and/or gold, the recording media by the interaction of the salt with an appropriate alkaline compound, recovering to a metallic state, wherein the porous carrier is first impregnated with an aqueous solution of water-soluble salts of copper, then fix the specified copper in the form of a water-soluble compound by interaction with an appropriate alkaline compound, and then osushestvljali salts of palladium and/or gold, while the number of elemental palladium and gold in the last impregnating solutions of equal predetermined amounts of metallic palladium and gold required in the catalyst, and then perform the recording on the catalyst of palladium and/or gold in solution, present in the catalyst after each impregnation, the interaction of the dissolved water-soluble salt in this solution with a suitable alkaline compound to precipitate the water-insoluble compounds of palladium and/or gold and restoration to the formation of water insoluble compounds of copper, palladium and/or gold present in the catalyst after each fixation is not water-soluble compounds of palladium and/or gold, or after fixing all the latest water-insoluble compounds on the carrier with a fixed copper and palladium.

2. The method according to p. 1, characterized in that after the restoration of all things palladium and gold in the catalyst, the catalyst is impregnated with a solution of acetate of an alkali metal.

3. The method according to p. 1, characterized in that the water-soluble compound of copper is a copper nitrate trihydrate or copper chloride dehydrate, the specified water-soluble compound of palladium in the palladium sulfate (II), the specified water-soluble compound of gold is a salt of an alkali metal chloride of gold (III) or solitarycharlotte (III) acid, and the specified alkaline compound to fix these copper, palladium and gold represents the sodium hydroxide.

4. The method according to p. 2, characterized in that said alkali metal acetate is the acetate of potassium.

5. The method according to p. 1, characterized in that after the specified fixation of copper in the form of a water-soluble compound carrier successively impregnated with a solution of water-soluble palladium compounds in the absence of any connection of gold, palladium fixed on the carrier in the form of water-insoluble compounds by interaction with an appropriate alkaline compound, the catalyst is impregnated with a solution of water-soluble gold compounds, gold is fixed on the carrier in the form of water-insoluble compounds by interaction with an appropriate alkaline compound, copper, palladium and gold in their fixed water-insoluble compounds reduced to the free metals, and a catalyst, optionally, impregnated with a solution of alkali metal acetate and dried.

6. Way tel sequentially impregnated with a solution of such a large number of water-soluble palladium compounds, which contains all elementary palladium required in the target catalyst, and the amount of water-soluble gold compounds, which is only part of the quantity of elemental gold required in the target catalyst, palladium and gold in the last solution is fixed on the carrier in the form of water-insoluble compounds by rotating and/or flipping impregnated carrier when immersed in a solution of the corresponding alkali compounds; fixed copper, palladium and gold reduced to the free metals; the catalyst is impregnated with a solution of such a large number of water-soluble gold compounds that the total number of elemental gold in the catalyst is equal to the number required in the target catalyst, and this last solution also contains the number of the corresponding alkali compounds, sufficient to capture the added gold in the form of a water-soluble compound, a fixed-added gold reduced to the free metal and the catalyst is optionally impregnated with a solution of alkali metal acetate and dried.

7. The method of producing vinyl acetate by the interaction of ethylene, oxygen michauxia fact, using the catalyst obtained under item 1, and the reaction is carried out at a molar ratio of ethylene and oxygen from 80:20 to 98:2, molar ratio of acetic acid and ethylene from 100:1 to 1:100 and the content of gaseous alkali metal acetate 2-200 ppm relative to acetic acid and the reaction temperature in the range of from 150 to 220oC.

8. The method of producing vinyl acetate by the interaction of ethylene, oxygen and acetic acid comprising contacting these reagents by passing them over a catalyst, characterized in that the use of the catalyst obtained under item 5, and the reaction is carried out at a molar ratio of ethylene and oxygen from 80:20 to 98:2, molar ratio of acetic acid and ethylene from 100:1 to 1:100 and content of the gaseous alkali metal acetate 2-200 ppm relative to the applied acetic acid and the reaction temperature in the range of from 150 to 220oC.

9. The method of producing vinyl acetate by the interaction of ethylene, oxygen and acetic acid comprising contacting these reagents by passing them over a catalyst, characterized in that the use of a catalyst obtained by p. 6, when the molar ratio of ethylene and oxygen from 80:20 to PR the Tata alkali metal 2-200 ppm relative to the applied acetic acid and the reaction temperature in the range of from 150 to 220oC.

 

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