Method for oxidation of liquid hydrocarbons in barrier discharge

FIELD: organic chemistry, chemical technology.

SUBSTANCE: invention relates to a method for oxidizing liquid hydrocarbons in barrier discharge carried out in the bubble reactor with mixtures of oxygen with helium, argon or nitrogen. Method involves using helium, argon and nitrogen taken in the amount 20-80%. The oxidation process is carried out in the presence of solid additives wherein aluminum, nickel, molybdenum, copper oxides or zeolite catalyst ZSM-5 comprising 1.2% of Fe is used. Method provides reducing energy consumptions for oxidation of the parent hydrocarbon in the barrier discharge.

EFFECT: improved oxidizing method.

3 cl, 2 tbl, 10 ex

 

The invention relates to the oxidation of liquid hydrocarbons in the barrier electric discharge in hydroxyl and carbonyl compounds without destroying the carbon skeleton of the original molecule. The resulting products can be used as intermediate products for organic and petrochemical synthesis.

There is a method of carrying out chemical reactions using barrier discharge (patent No. 2118912, publ. 20.09.1998 g), however, obtained by liquid hydrocarbons fails.

Closest to the proposed method is the oxidation of hydrocarbons with oxygen in a flowing gas discharge reactor with barrier discharge (patent of Russia №2127248, publ. 10.03.99 year). Oxidation of hydrocarbons leads to the formation of hydroxyl and carbonyl compounds with the same number of carbon atoms, as in the original connection.

The main disadvantage of this method is the high energy cost of the transformation of the original hydrocarbon.

The objective of the invention is to reduce energy costs for oxidation of hydrocarbon source in the barrier discharge.

The technical result is achieved in that the hydrocarbons are oxidized in the bubble plasma-chemical reactor with a barrier discharge in oxygen, air, mixtures of oxygen with helium, argon, nitrogen without and in the presence of TV is rdih additives Al 2About3, Ni2O3, MoO3, CuCl2, zeolite catalyst (ZSM-5+1.2% Fe).

As a source of hydrocarbons using n-hexane and cyclohexane.

In all examples, the temperature of the walls of the reactor 10°C, pressure of 1.2 ATM, the amplitude of the pulse voltage of 28 kV, repetition rate 50 Hz. Specific discharge energy - 2.8·10-2W·h·l-1.

The method is illustrated by the following examples.

Example 1. The oxidation of n-hexane and cyclohexane hold oxygen. The energy consumption for the conversion of n-hexane and cyclohexane are 21.9 and 8.2 kW·h·kg-1respectively. Anagnostaras and data on the composition of the products in table 1.

Example 2. The oxidation of n-hexane and cyclohexane spend oxygen of the prototype. The energy consumption for the conversion of n-hexane and cyclohexane are and 29.2 16.6 kW·h·kg-1respectively. The composition of the products and the energy consumption for the transformation of the original hydrocarbons are given in table 1.

Example 3. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%). The energy consumption for the conversion of cyclohexane are 4.0 kW·h·kg-1.

Example 4. The oxidation of cyclohexane is carried out with a mixture of Ar(50%)-02(50%). The energy consumption for the conversion of cyclohexane are 4.7 kW·h·kg-1.

Example 5. The oxidation of cyclohexane spend N 2(80%)-O2(20%). The energy consumption for the conversion of cyclohexane are 8.0 kW·h·kg-1.

Example 6. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%) in the presence of 0.7 wt.% MoO3. The energy consumption for the conversion of cyclohexane up to 3.2 kW·h·kg-1.

Further, in all examples, the weight of the solid additive is 0.7 wt.% by weight of the hydrocarbon.

Example 7. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%) in the presence of Ni2O3. The energy consumption for the conversion of cyclohexane are 3.1 kW·h·kg-1.

Example 8. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%) in the presence of Al2About3. The energy consumption for the conversion of cyclohexane are 3.6 kW·h·kg-1.

Example 9. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%) in the presence of CuCl2. The energy consumption for the conversion of cyclohexane up to 3.2 kW·h·kg-1.

Example 10. The oxidation of cyclohexane is carried out with a mixture of No(20%)-O2(80%) in the presence of zeolite catalyst ZSM-5+1.2% Fe. The energy consumption for the conversion of cyclohexane are 3.6 kW·h·kg-1.

The composition of the reaction products and the selectivity of their education in examples 3-10, as in example 1.

Thus, the present invention allows to oxidize the hydrocarbon liquid in p is outstay additives or without them in bubble plasma-chemical reactor with a barrier discharge in oxygen or mixtures of air with inert gases with low energy costs.

Table 1.
The composition of the oxidation products of hexane and cyclohexane and the energy consumption for the transformation of the original hydrocarbon.
HydrocarbonProductsContent, wt.%Power consumption, kW·h·kg-1
Bubble reactorThe placeholderBubble reactor, the airThe prototype, oxygen
Example 1Example 2Example 1Example 2
HexaneHexanal20.0022.06
Hexane-3,24.2121.45
Hexanon-2
Hexanol-329.4727.4921.929.2
Hexanol-218.6419.90&x0200A;
Hexanol-17.667.74
CyclohexaneCyclohexanoneAt 42.5347.66
The cyclohexanolAt 56.4452.118.216.6

Table 2.
The energy consumption for the conversion of cyclohexane in examples 3-10.
Example345678910
Power consumption, kW·h·kg-14.04.78.03.23.13.63.23.6

1. The method of oxidation of liquid hydrocarbons in plasma-chemical reactor mixtures of oxygen with helium, argon or nitrogen, wherein the oxidation is carried out in a barrier discharge in a bubble reactor.

2. The method according to claim 1, characterized in that use helium, argon, nitrogen in an amount of from 20 to 80%.

3. The method according to claim 1, characterized in that the oxidation is carried out in the presence of solid additives, as to the which use oxides of aluminum, Nickel, molybdenum, copper or the zeolite catalyst ZSM-5, containing 1.2% Fe.



 

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