The method of converting hydrocarbon steam reforming and installation for its implementation

 

(57) Abstract:

Use: during the processing of hydrocarbons. The inventive purified hydrocarbon gas-vapor mixture is divided into two parallel streams. One stream is fed to the first apparatus primary catalytic reforming units, and the second to the second apparatus primary catalytic reforming. Combine streams from the first and second devices. The resulting stream is mixed with the oxidant and serves on stage adiabatic secondary reforming. The resulting product is passed through a second device of the primary reformer for indirect heat exchange with steam and gas mixture flowed forward and away. Source purified gas-vapor mixture before separation of the two streams is subjected to sequential indirect heating and partial catalytic reforming countercurrent to the product from stage adiabatic reforming, and later advance via a second device of the primary reformer. The installation includes a line for supplying purified mixture of hydrocarbons and steam, means for separating vapor-gas mixture into two flow lines, one of which is connected with the first device to the primary reformer, the other line is connected to the second device per the VA of the second apparatus of the primary reformer, the outlet side of which is made with a line connected to a line between the first device to the primary reformer and apparatus adiabatic secondary reforming. The installation is equipped with an additional heater, the apparatus of the partial catalytic reforming, additional line and output line of the product. 2 S. and 4 C. p. F.-ly, 3 ill., 3 table.

The invention relates to the processing of hydrocarbons, in particular to a method and installation for the conversion of hydrocarbon steam reforming.

A known method of converting hydrocarbons steam reforming, which is that the purified mixture of hydrocarbons and steam is divided into first and second flows with a volume ratio of 40:6085:15, the first stream is subjected to indirect heat exchange with the use of heat radiation with further in the first device primary catalytic reforming units, and the second stream is subjected to indirect heat exchange with the use of heat radiation with subsequent feeding it to the second apparatus primary catalytic reforming, the output from the first and second apparatuses streams unite, the combined stream is mixed with the oxidant gas and the resulting stream serves npart primary reformer for countercurrent indirect heat exchange with the gas-vapor mixture and the resulting product divert known techniques.

Installation for the implementation of this method contains a line for supplying purified mixture of hydrocarbons and steam, provided with means to separate the gas mixture into two streams, with separate lines placed in them by the heat exchanger, the first device primary reformer connected to a line for feeding the first stream and executed with means for heat radiation and inner tubes filled with catalyst, the device is adiabatic secondary reforming placed in it a layer of catalyst, provided with a means for supplying oxidant gas and coupled with the first production unit of the primary reformer, and a second device of the primary reformer with internal pipes, filled with catalyst and the inlet of the second unit of the primary reformer is connected to the line for supplying the second thread, and the release of the second apparatus of the primary reformer is connected to the connecting line between the first device to the primary reformer and apparatus adiabatic secondary reforming unit, which is connected with the annular space of the second device primary reforming near its outlet end, with the second device nogo end.

A disadvantage of the known technical solution is its susceptibility to damage due to the following reasons.

It is well known that the reformed hydrocarbon gas with a high content of carbon monoxide causes a reaction carburizing the metal parts of the installation with which the gas is in contact. The result places the formation of cracks in the surface layers of the material with subsequent destruction or separation of the protective layers, for example, in the form of fibers or fine dust. This phenomenon, called metal dusting occurs at different metals at different temperatures. Thus, to prevent metal dusting, leading to the subsequent suspension of the reforming process, it is necessary to prevent the critical temperature of the metal at the stages of reforming, which is an indirect heat exchange.

The aim of the invention is to overcome this drawback, i.e., improving the reliability of the conversion of hydrocarbon steam reforming.

This goal is achieved in the proposed method of converting hydrocarbons steam reforming, involving separation of the purified gas mixture in the far East, what about the second apparatus primary catalytic reforming, combining flows from the first and second devices, mixing the latter with an oxidizing agent and filing of the received stream to the stage adiabatic secondary reforming, followed by passing the resulting product through a second device of the primary reformer for indirect heat exchange with steam and gas mixture, extraction of the resulting product due to the fact that the indirect heat exchange of the product with adiabatic secondary reforming with steam and gas mixture in the second apparatus of the primary reformer are parallel, the original purified gas-vapor mixture before separation into two streams sequentially subjected to indirect heating and partial catalytic reforming countercurrent to the product from stage adiabatic reforming, and later advance via a second device of the primary reformer.

Before the conclusion of the process, the product obtained from stage adiabatic secondary reforming, taken from the stage partial reforming, can be used for heating the purified mixture of hydrocarbons by indirect heat exchange.

This goal is achieved also offer installation for the conversion of hydrocarbon steam reforming, including Liwa flow with the lines, one of which is connected with the first device to the primary reformer, made with means for heat radiation and inner tubes filled with catalyst, and the other line connected to the second apparatus the primary reformer, made from inner tubes filled with catalyst, the device is adiabatic secondary reforming with a line for supplying oxidant gas is connected by a line with the first device to the primary reformer, and a line for the output of the finished product linking apparatus adiabatic secondary reforming with the side of the tube space of the second device to the primary reformer, the outlet side of which is made with the line connected to the line between the first device to the primary reformer and apparatus adiabatic secondary reforming, due to the fact that it is equipped with an additional heater, the apparatus of the partial catalytic reforming, made with tubes filled with catalyst, additional connecting line and the output line of the product, while the output of the second unit of the primary reformer is connected to the additional line from the outlet of the partial reforming unit, and the side pipe space anago reforming placed between a line for supplying purified mixture of hydrocarbons and steam, and means for separating a mixture, and the heater is placed on the line of feed of the mixture of feedstock and steam.

According to a preferred form of the proposed installation inner tube of the apparatus of the partial reforming have narrowed the input ends. In addition, the input end of the inner tube of the apparatus of the partial reforming unit and the second unit of the primary reformer can be telescopically mounted in the support. Furthermore, the said inner tube can be provided with a bellows concentrically placed around their input ends and fixed to the input ends and the pole, and an additional line for the output product can be filtered through a heater.

Hydrocarbon may be any hydrocarbon, a hydrocarbon fraction, or a mixture of hydrocarbons, usually used as raw materials steam reforming of hydrocarbons. Common raw materials are natural gas, exhaust gas refining, liquefied petroleum gases and various petroleum fractions, for example, light gasoline distillate. For hydrocarbon raw materials were suitable for use as raw material steam reforming, it is usually subjected to preliminary desulfurization to reduce it to the raw materials in the amount providing gas with a ratio of steam and carbon that is high enough to prevent the deposition of carbon on the catalyst particles. In this case, the ratio of steam and carbon is indicated in mol of steam per atom of carbon.

The reaction of the primary steam reforming begins when coming in contact of the feedstock with the catalyst placed in the apparatus of the partial reforming. The temperature of the source gas inlet catalyst layer is typically 400-700aboutAnd the reforming is carried out at a ratio of steam and carbon equal to 1.1 to 7.0, preferably of 2.0 to 4.5. For reasons of economy reforming and partial first stage of the primary reforming is carried out at elevated pressures of about 2-60 bar. Within these limits, the pressure of the process can be coordinated with the pressure at which the stream withdrawn from the process target product use or serves to further processing, for example 30-40 bar. As the catalyst used in stage a partial reforming unit, the first and second stages of the primary reformer can take any commercially available catalyst designed for steam reforming. The catalytically active component of this catalyst is I secondary reformer are Nickel and a mixture of Nickel oxide and oxides of the metal, for example, the oxide of Nickel in combination with oxides of iron, cobalt or magnesium as a promoter.

The first stage of the primary reforming stage and adiabatic secondary reforming is carried out in known conditions. The temperature of the joint, held primary reforming of the gas stream at the inlet of the apparatus adiabatic secondary reformer can range between 700aboutC and 900aboutWith, depending on conditions at the primary stages of reforming, and by reaction with the oxidant gas rises to 800-1100aboutWith the release of the device adiabatic secondary reforming. As the oxidant gas, you can use the air to obtain the desired product, suitable for the production of ammonia, or oxygen, or oxygen-enriched air (for example, when receiving the synthesis gas for the production of oxygen-containing hydrocarbons such as alcohols, ethers or carboxylic compounds). Hot product which is withdrawn from the apparatus adiabatic secondary reformer at a temperature of 900-1100aboutWith that served in the second apparatus primary reforming with continuous flow through the annulus in the indirect heat exchange with prosesi this hot gas is cooled to a moderate temperature, and the enthalpy of the cooled product is used in the apparatus of the partial reforming unit for the implementation of the response partial reforming of the original mixture by countercurrent indirect heat exchange.

Through a combination of once-through heat exchange in the second stage of primary reformer and counterflow heat exchange at the stage of partial reforming and regulating the ratio of the number of the last partial reforming gas supplied to the first and second stage of primary reformer, it is possible to avoid the temperature of the tubes in the apparatus for implementing data stages, which would be in the critical range, i.e. within, which usually occurs dusting of metal pipe.

In Fig.1 presents the proposed installation in a simplified schematic form in Fig.2 a longitudinal section through the apparatus of the partial reforming unit and the second unit of the primary reformer installation of Fig.1; Fig.3 the inlet end of the apparatus of Fig.2 in an enlarged scale.

The proposed system includes a line 1 for supplying purified mixture of hydrocarbons and steam, connected to the apparatus 2 partial catalytic reforming, made with internal t the mixture relating to the first thread, supplied through line 7 in the first device 8 of the primary reformer, made from inner tubes 9, filled with a catalyst, and means 10 for heat radiation by combustion of fuel and the second stream supplied through line 11 to the second apparatus 12 of the primary reformer, made from the inner tubes 13, is filled with catalyst. In addition, the proposed system includes apparatus 14 adiabatic secondary reforming, is supplied by line 15 for supplying oxidant gas and a layer 16 of a catalyst. The first device 8 of the primary reformer and the apparatus 14 adiabatic secondary reformer are connected by a line 17, which is connected to line 18, is placed on the discharge end 19 of the second apparatus 12 of the primary reformer. According Fig.1 proposed facility also contains a line for outputting the finished product from the apparatus 14 adiabatic secondary reforming, consisting of the first line 20 connecting the discharge side 21 of the apparatus 14 adiabatic secondary reforming with the side of the tube space 22 of the second apparatus 12 of the primary reformer, the connecting line 23 connecting the output 19 of the second apparatus 12 of the primary reformer exit 4 of the apparatus 2 partial riformista through the heater 26.

In Fig. 2 shows that the head sections 27, 28 of the apparatus 2 and 12 provided with a connecting element 29 with the hatch 30 and the shutter 31.

The inlet end 32 of the tube 3 and 13, placed in the apparatus 2 and 12, respectively, passed through a bearing 33, and installed it using the steps described below with reference to Fig.3 the fastening means 34, allowing movement of the pipe. The inlet end 32 of the tube 3, 13 have the shape of the necks of bottles, i.e., is made tapering, which ensures optimal distribution of gas into the space between the tubes 3, 13 or coming out of it. On the rounded end 35 of the pipe 3, 13 are connected with the pipes 36 to release gas passed through the bottom 37 of the apparatus 2 and 12, respectively. In places of passage of pipes 36 and bottom 37 is equipped with a cylindrical tube 38 that serve to align the temperature surrounding the pipes 36 and secured to the outer surface of the bottom 37. Pipe 36 to the gas outlet connected to the reservoir 39 and 40, respectively, is positioned outside the apparatus 2 and 12. The manifold 39 is connected to the line 5 and the collector 40 with line 18. The means 6 for separation of gas mixture supplied by the throttle valve 41 serving to regulate the amount of partially reformed gas fed via line 1 is in question 42 for distributing the incoming gas through pipes 3 and 13, respectively. Devices 2 and 12, and the connector 23 has an internal refractory lining 43. Configuration and installation of the pipes 3, 13 shown in more detail in Fig.3, represents a partial view of the tube space 25 of the apparatus 2 in an enlarged scale. Similarly executed and tube space 22 of the second apparatus 12 of the primary reformer.

Essential for installation passed through a bearing 33, and is made in the form of the neck of the bottle inlet end 32 of each tube 3 mounting means 34 in the form of metal bellows, concentrically placed around the upper ends of the tubes 3, passed through the bearing 33. The upper ends 44 of the fastening means 34 is fixed at the inlets 45 of the pipe 3, and their lower ends 46 on the support 33. Thus, the mounting means 34 allow telescopic movement of the tubes 3 in the support 33 by thermal expansion of the latter. As already mentioned, the inlet ends 32 of the tubes 3 have the shape of the necks of the bottles that on the one hand facilitates the installation of the pipe 3 in the support 33 by saving space, and on the other hand provides the optimum performance of the gas flow in the space between the tubes 3, as the differential pressure decreases due to the expansion of this space BC is adicheskogo secondary reformer are of known construction, and therefore they are not explicitly represented in the drawing.

The proposed method is as follows. Supplied through the line 1 of the source gas containing hydrocarbons and steam is preheated to a temperature of about 500-600aboutWith the path of the heat exchange target gas output by an additional line 24 from the apparatus 2 and having a temperature of about 550-650aboutC. Pre-heated source gas is distributed through the elongated tube 3 placed in the apparatus 2. Tube 3 filled with suitable known catalyst. Hot target gas exhaust line 20 from the apparatus 14 adiabatic secondary reformer at a temperature of about 950-1050aboutWith the second apparatus 12 of the primary reformer is cooled to a temperature of about 810-900aboutWith in which the gas-side pipe space served in the apparatus 2 in order to provide the necessary for the implementation of the partial reforming heat by countercurrent indirect heat exchange. The temperature of the walls of the tube 3 is maintained at about 500-600aboutWith the inlet end and 650-770aboutWith the outlet end of the pipe 3.

During passage through the apparatus 2, the source gas is subjected to partial reforming unit,divided into two streams. The tool 6 may be provided with a regulating valve, allowing the gas distribution on both stream into different fractions. About 20-60% by volume of the partially reformed gas through line 11 serves in the second apparatus 12 of the primary reformer, and the rest of the gas is fed through line 7 to the first device 8 primary reforming, representing a furnace of known construction, containing filled suitable catalyst pipe 9 with the heated walls to complete the primary reformer supplied through line 7, partially reformed gas.

Supplied through the line 11, the gas is subjected to a primary reforming in the bandwidth through a host in the second apparatus 12 primary reforming extra long, filled with a suitable catalyst pipe 13. Needed for this endothermic reaction heat is provided by indirect heat exchange with hot target gas discharged from the apparatus 14 adiabatic secondary reformer through line 20 and fed into the tube space 22 of the second device 12 primary reforming parallel with the gas discharged through the pipe 13. When this hot target gas is cooled to a temperature of about 950-1100aboutWith the intake end of the second apparaat through the connecting line 23 to the apparatus 2. The temperature of the tube wall 13 is 860-910aboutWith on the intake end and 780-890aboutOn the exhaust end. The actual temperature depends on the amount of gas supplied through the line 11. Thus, by regulating the number of partially reformed gas supplied through the line 11 to the second apparatus 12 of the primary reformer, and by heat exchange countercurrent and co-current in devices 2 and 12, respectively, can be adjusted and the temperature of the metal material used to perform the devices 2 and 12. You can avoid those temperatures at which there is a dusting of metal on the walls of the pipes in these devices, through which passes the gas with a high content of carbon monoxide.

Withdrawn from the apparatus 12 and 8 flows past the primary reforming gas are combined and fed into the apparatus 14 adiabatic secondary reforming with a layer 16 of suitable known catalyst. For secondary reforming in the apparatus 14 also serves oxidant gas. Due to the heat released by the partial oxidation contained in gas of hydrogen and hydrocarbons, the temperature of the gas increases from approximately 800-900aboutWith the intake end to the example. the similar gas of the following composition, mol. ABOUT20,00; N21,01; N2ABOUT 70,45; N20,35; 0,00; CO20,04; AG 0,00; CH428,14, pre-heated to a temperature of 510aboutWith and served in apparatus 2 (see Fig.1). When passing through the device 2, the source gas is subjected to partial reforming by indirect heat exchange target gas is passed in indirect heat exchange in the second stage of the primary reformer. Then partially reformed gas is divided into two streams in the proportion supplied through line 7 flow supplied through line 11 to flow, equal to 3.4 (experiment 1), and 1.8 (experiment 2) and 0.7 (experiment 3). Then supplied through the line 11, the partially reformed gas is then subjected to a primary reforming apparatus 12 through once-through indirect heat exchange with hot target gas and combined with the gas obtained in the apparatus 8 of known construction by primary reforming gas supplied through line 7. The combined streams then the device 14 of known construction is subjected to secondary reforming by reaction with supplied through line 19 air. Hot target gas which is withdrawn from the apparatus 14, is fed into the tube space 22 of the second apparatus 12 of the primary reformer and once-through heat exchange part of the Ref is ransta 25 of the apparatus 2 in countercurrent indirect heat exchange source gas, and after passing through this apparatus is removed from the process. The resulting gas can be used for ammonia synthesis. These and other reaction conditions are given in table.1-3, which show the results of experiments 1-3, respectively.

Are given in table. 1-3 the results of the experiments show that the temperature of the pipe walls in the apparatus 2 and the second apparatus 12 of the primary reformer, which contacts the carbon monoxide gas can be maintained within certain ranges without negative influence on the composition of the produced gas which is withdrawn from the apparatus 14 adiabatic secondary reforming, through a combination of straight-through indirect heat exchange with counter-current indirect heat exchange and regulation of quantitative flow ratio partially reformed gas fed to the first 8 and the second apparatus 12 of the primary reformer. It is possible to avoid such a temperature at which the metal dusting.

1. A method of converting hydrocarbons steam reforming, involving separation of the purified gas mixture into two parallel flow, the flow of one stream into the first device primary catalytic reforming units, and the second - second catalytic apparatus is m and the flow of the received stream to the stage adiabatic secondary reforming, followed by passing the resulting product through a second device of the primary reformer for indirect heat exchange with steam and gas mixture, removal of the resulting product, wherein the indirect heat exchange of the product with adiabatic secondary reforming with steam and gas mixture in the second apparatus of the primary reformer are parallel, the original purified gas-vapor mixture before separation into two streams sequentially subjected to indirect heating and partial catalytic reforming countercurrent to the product from stage adiabatic reforming, and later advance via a second device of the primary reformer.

2. Installation for the conversion of hydrocarbon steam reforming, comprising a line for supplying purified mixture of hydrocarbons and steam, means for separating vapor-gas mixture into two flow lines, one of which is connected with the first device to the primary reformer, made with means for heat radiation and inner tubes filled with catalyst, and the other line connected to the second apparatus the primary reformer, made from inner tubes filled with catalyst, the device is adiabatic secondary reforming with a line for supplying oxidant gas is connected by a line with the first device to the primary reformer, and the line for Vivadent second aparate primary reforming, the outlet side of which is made with a line connected to a line between the first device to the primary reformer and apparatus adiabatic secondary reformer, wherein it is further provided with a heater, the apparatus of the partial catalytic reforming, made with tubes filled with catalyst, additional connecting line and the output line of the product, while the output of the second unit of the primary reformer is connected to the additional line from the outlet of the partial reforming unit, and the side tube space of the apparatus of the partial reforming unit is connected to the additional line for the output product, when this apparatus is a partial reforming unit placed between a line for supplying purified mixture of hydrocarbons and steam, and means for separating the mixture, and the heater is placed on the line of feed of the mixture of feedstock and steam.

3. Installation under item 2, characterized in that the inner tube of the apparatus of the partial reforming have narrowed the input ends.

4. Installation on PP. 2 or 3, characterized in that the inner tube of the apparatus of the partial reforming unit and the second unit of the primary reformer at the input end telescopically mounted in the support.

6. Installation under item 2, characterized in that an additional line to output the product has been passed through the heater.

 

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