Method for production of gas enriched with hydrogen and/or carbon oxide

FIELD: autothermal catalytic reforming of hydrocarbon feed stream.

SUBSTANCE: method relates to method for reforming of hydrocarbon feed stream with water steam at elevated temperature to produce gas enriched with hydrogen and/or carbon oxide. Hydrocarbon stream is passed through water steam reforming catalyst bed wherein oxygen is fed through oxygen-permeable membrane followed by removing of finished product from this bed. Said catalyst bed contains in input region catalyst with reduced or without water steam reforming activity, but having hydrocarbon feed oxidation activity.

EFFECT: process with improved characteristics due to temperature controlling in reactor.

3 cl, 1 dwg

 

The present invention relates to an autothermal catalytic reforming with water vapor hydrocarbons. In particular, the invention is directed to a method of obtaining a gas enriched in hydrogen and/or carbon monoxide.

A method of obtaining a gas enriched in hydrogen and/or carbon monoxide, which is that of the hydrocarbon feedstock is subjected to reforming with water vapor at elevated temperatures by passing through a layer of catalyst reforming with water vapor, which serves oxygen through the membrane, permeable to oxygen, with subsequent removal of the final product from this layer (see international patent application WO 98/48921, 01 D 53/22, 01 3/34, 09.04.1998).

Getting gas enriched in hydrogen and/or carbon monoxide, for example, synthesis gas may be represented by the following three reactions:

CH4+H2About⇔ CO+3H2

CH4+1/2O2CO+2H2

CO+H2About⇔ CO2+H2

At the entrance of the above process, the gas temperature usually lies between 500 and 800° C. the Pressure of the membrane from the synthesis gas range from atmospheric up to 90 bar, and the pressure of the gas containing oxygen from atmospheric up to 26 bar.

The reaction of reforming with water vapor and methane conversion is usually close to equilibrium at the output R of the actor.

The aim of the present invention is to improve the characteristics of the process by controlling the temperature gradient in the reactor.

This goal is achieved by the proposed method of obtaining a gas enriched in hydrogen and/or carbon monoxide, which is that of the hydrocarbon feedstock is subjected to reforming with water vapor at elevated temperatures by passing through a layer of catalyst reforming with water vapor, which serves oxygen through the membrane, permeable to oxygen, with subsequent removal of the final product from this layer, the method characterized by the fact that hydrocarbons are passed through the catalyst bed in the input field which contains a catalyst having reduced activity or absolutely no activity in reforming with water vapor and with activity in the oxidation of hydrocarbon of raw materials.

As the catalyst layer can be used a fixed layer or the layer deposited on the membrane.

The method according to the present invention is further explained with reference to the drawing showing schematically a reactor for autothermal catalytic reforming with water vapor of hydrocarbons with the use of the membrane.

Raw material 1 containing hydrocarbons, for example methane, is introduced into the reactor 2 by penetration of 3 membranes is 4. Branch on this side of the membrane 4 download catalyst reforming with water vapor and/or a catalyst for partial oxidation 5. At the entrance of raw materials the activity of the catalyst in the upper part of layer 6 is reduced in comparison with the activity of the catalyst in the rest of the catalyst layer. Instead of being fixed, the catalyst can also be directly applied on the side of the permeation 3 membrane 4 (not shown).

The stream containing oxygen, 7, such as air, enters the reactor from the opposite side of the membrane 4. Suitable materials for the membranes with the ability to transport oxygen. When oxygen ions are movable particles, electrons move through the membrane in the opposite direction, thus ensuring electroneutrality. The oxygen flow depends mainly on the difference of partial pressures of oxygen.

When the catalyst has no activity in reforming with water vapor in the upper part of layer 6, the catalyst serves as an oxidation catalyst.

The method according to the present invention has the following advantages:

- mechanical design of the reactor becomes less complicated;

operate at low inlet temperature of the feedstock and oxidant becomes feasible, which leads to reduced the horses of the heat exchanger and lower fuel consumption;

- the desired size of the membrane becomes less.

Catalysts for the oxidation of hydrogen or hydrocarbons known in the art. Catalytic reforming with water vapor with low activity in the reforming process can be obtained by the application of the material medium low amounts of catalytic material and/or adding the promoting compounds, which lower the activity of the catalytically active material. Such methods of producing catalysts and catalysts with low activity in reforming with water vapor is also known to experts.

As a further advantage of the catalyst with low activity allows operation without the formation of soot at low ratio of water vapor to the carbon by the addition of promoters to the catalyst to increase the resistance to soot, and the decrease of activity of this catalyst in the reforming with water vapor.

During operation of the catalytic autothermal reforming with water vapor with oxygen through the membrane, the equilibrium temperature of the reforming with steam injected gas is lower than the temperature at the inlet of the injected gas in a conventional reactor. The reaction of reforming with water vapor takes place at this immediately, as soon as the feed gas comes into contact with the catalyst. As the reaction re the orminge with water vapor much endothermic, there will be a lowering of the gas temperature and the catalyst compared to the inlet temperature of the gas.

The flow of oxygen through the membrane increases with increasing temperature, and below a certain temperature (T0) the oxygen flow is practically zero.

Therefore, you will benefit from a reduced flow of oxygen through the membrane per unit area in the reactor with catalysts having a high activity in reforming with water vapor. It has one of two effects:

a) the Temperature in the reactor drops to the level below which a stream of oxygen through the membrane becomes negligible. The only way to avoid this is to increase the temperature at the gas inlet.

b) the oxygen Flow is reduced in comparison with a stream of oxygen at a temperature of the intake gas.

Through the proposed method works on the catalyst with low or zero activity part of the catalyst at the entrance of the reactor in the reforming with water vapor, the temperature decreases eliminate or make much less pronounced. Therefore, the temperature can either be reduced to levels close to T0or size of the membrane can be reduced, because the oxygen is transferred through the membrane at a higher (average) temperature.

1. A method of obtaining a gas enriched in hydrogen and/or oxide, in which laroda, by reforming with water vapor of hydrocarbons at elevated temperatures by passing through a layer of catalyst reforming with water vapor, which serves oxygen through permeable to oxygen membrane, with subsequent removal of the final product from this layer, characterized in that the hydrocarbons are passed through the catalyst bed in the input field which contains a catalyst having reduced activity or absolutely no activity in reforming with water vapor and with activity in the oxidation of hydrocarbons.

2. The method according to claim 1, characterized in that as a layer of catalyst using a fixed layer.

3. The method according to claim 1, wherein the used catalyst layer deposited on the membrane.



 

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FIELD: autothermal catalytic reforming of hydrocarbon feed stream.

SUBSTANCE: method relates to method for reforming of hydrocarbon feed stream with water steam at elevated temperature to produce gas enriched with hydrogen and/or carbon oxide. Hydrocarbon stream is passed through water steam reforming catalyst bed wherein oxygen is fed through oxygen-permeable membrane followed by removing of finished product from this bed. Said catalyst bed contains in input region catalyst with reduced or without water steam reforming activity, but having hydrocarbon feed oxidation activity.

EFFECT: process with improved characteristics due to temperature controlling in reactor.

3 cl, 1 dwg

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