Hydrogen recovery device in reforming catalyst regeneration reaction

Abstract

The utility model discloses a hydrogen recovery device in reforming catalyst regeneration reaction, which comprises a gas mixing device, an inlet of which is connected with a hydrogen pipeline, a methane pipeline and a carbon dioxide pipeline and is used for forming reaction gas; an inlet of the fixed bed reactor is connected with an outlet of the gas mixing device, and the fixed bed reactor is used for catalyst regeneration and methane dry reforming reaction under the reaction gas atmosphere; an inlet of the circulating gas pump is connected with an outlet of the fixed bed reactor, and the circulating gas pump is used for collecting carbon monoxide and hydrogen mixed gas generated by the methane dry reforming reaction; an inlet of the gas pressurizing and liquefying device is connected with an outlet of the circulating gas pump, and the gas pressurizing and liquefying device is used for pressurizing, cooling and liquefying the collected mixed gas of the carbon monoxide and the hydrogen so as to separate the carbon monoxide from the hydrogen. The device not only can integrate catalyst regeneration and methane dry reforming reaction, but also can recover and separate CO and H2 generated by reaction for recycling, so that the cost is saved, the carbon emission is reduced, and the device has a good application prospect.

Description

Technical Field

[0001] The utility model belongs to the technical field of metal element recovery and re-production devices, and in particular relates to a hydrogen recovery device suitable for a reforming catalyst regeneration reaction process. Background Art

[0002] In the context of economic growth and industrial expansion, the demand for high-octane gasoline produced by naphtha catalytic reforming process has increased rapidly, which has also promoted the application and development of reforming catalysts. Petrochemical catalysts are consumables, and a huge amount of them are scrapped every year in my country. Catalyst regeneration can extend the service life of the catalyst, reduce the generation of waste, improve the efficiency and stability of the catalyst, restore the activity and selectivity of the catalyst, make it reusable, reduce the demand for new catalysts, and thus reduce production costs and resource consumption.

[0003] my country needs to vigorously develop efficient and clean energy technologies and accelerate the construction of a green and low-carbon energy system. As a high-quality, efficient, green and clean low-carbon energy, the promotion and application of natural gas is of great significance under the current situation. The recovery of hydrogen not only reduces economic costs and saves resources, but also promotes the recycling of clean energy and reduces environmental pollution. At present, other catalytic reforming reaction devices directly discharge the carbon monoxide and hydrogen generated by the reaction to the outside without recycling or collecting them. Utility Model Content

[0004] The utility model aims to solve at least one of the technical problems existing in the prior art. To this end, the utility model provides a hydrogen recovery device in the catalyst regeneration reaction, aiming to solve the problem that the above-mentioned catalyst is not recovered after the reforming reaction, and carbon monoxide and hydrogen are often discharged outdoors. Over time, this will cause environmental pollution to a large extent, consume a lot of clean energy, and increase economic costs.

[0005] In order to achieve the above purpose, the utility model adopts the following technical solutions:

[0006] A hydrogen recovery device for a reforming catalyst regeneration reaction comprises: a gas mixing device, wherein the inlet of the gas mixing device is respectively connected to a hydrogen pipeline, a methane pipeline and a carbon dioxide pipeline for forming a reaction gas; a fixed bed reactor, wherein the inlet of the fixed bed reactor is connected to the outlet of the gas mixing device for performing catalyst regeneration and methane dry reforming reaction under a reaction gas atmosphere; a circulating gas pump, wherein the inlet of the circulating gas pump is connected to the outlet of the fixed bed reactor for collecting a mixed gas of carbon monoxide and hydrogen generated by the methane dry reforming reaction; and a gas pressurizing and liquefying device, wherein the inlet of the gas pressurizing and liquefying device is connected to the outlet of the circulating gas pump for pressurizing, cooling and liquefying the collected mixed gas of carbon monoxide and hydrogen to achieve separation of carbon monoxide and hydrogen.

[0007] Preferably, the hydrogen recovery device in the reforming catalyst regeneration reaction also includes a hydrogen recovery cylinder and a mixed gas recovery cylinder, the inlet of the hydrogen recovery cylinder is connected to the hydrogen output port at the upper end of the gas pressurization liquefaction device, and the inlet of the mixed gas recovery cylinder is connected to the mixed gas output port at the lower end of the gas pressurization liquefaction device.

[0008] Preferably, the fixed bed reactor comprises: a reaction tank, the top of which is provided with an inlet of the fixed bed reactor, and the bottom of the reaction tank is provided with a catalyst unloading port; a gas distribution pipe, which is circumferentially arranged on the inner wall of the reaction tank and is used to evenly distribute the reaction gas into the reaction tank; a central tube, which is axially arranged in the reaction tank, and the bottom end of the central tube passes through the reaction tank to form an outlet of the fixed bed reactor to discharge the carbon monoxide and hydrogen mixed gas produced by the methane dry reforming reaction; a catalyst, which is filled in the annular space between the gas distribution pipe and the central tube; and a cap, which is sealed and arranged at the top of the central tube and covers the top of the catalyst, so as to prevent the reaction gas from diffusing upward.

[0009] Preferably, the circulating air pump comprises: a pump body; an intake valve, which is arranged at the lower end of the pump body and connected to the outlet of the fixed bed reactor; an exhaust valve, which is arranged at the upper end of the pump body and connected to the inlet of the gas pressurization liquefaction device; a piston, which is slidably arranged in the pump body; and a crank-connecting rod mechanism, wherein the action end of the crank-connecting rod mechanism is connected to the piston, and is used to drive the piston to reciprocate in the pump body.

[0010] The utility model adopts the above technical solution, which has the following advantages:

[0011] 1. The hydrogen recovery device in the reforming catalyst regeneration reaction provided by the utility model can effectively solve the process problem of hydrogen recovery in the catalyst regeneration reaction. The equipment independently develops the reforming catalyst regeneration reaction process to realize the regeneration and recycling of the waste reforming catalyst. On the basis of the existing regeneration process, through process optimization and combination, a new process for hydrogen recovery in the reforming catalyst regeneration reaction is developed to realize the comprehensive utilization of the waste catalyst regeneration and recycling and hydrogen recovery cycle. The device has significant social and economic benefits.

[0012] 2. The hydrogen recovery device in the reforming catalyst regeneration reaction provided by the utility model can not only integrate the catalyst regeneration and methane dry reforming reaction, but also recover and separate the CO and H2 generated by the reaction for recycling, which saves economic costs to a great extent, protects the environment and reduces carbon emissions. It is convenient and flexible to operate and has a good prospect for use. BRIEF DESCRIPTION OF THE DRAWINGS

[0013] By reading the detailed description of the preferred embodiment below, various other advantages and benefits will become clear to those of ordinary skill in the art. The accompanying drawings are only used for the purpose of illustrating the preferred embodiment and are not considered to be limiting of the present invention. The same reference numerals are used throughout the accompanying drawings to represent the same components. In the accompanying drawings:

[0014] Figure 1 A schematic structural diagram of a hydrogen recovery device in a reforming catalyst regeneration reaction provided in one embodiment of the utility model.

[0015] The reference numerals in the figures are as follows:

[0016] 1. Hydrogen pipeline; 2. Methane pipeline; 3. Carbon dioxide pipeline; 4. Gas mixing device; 5. Fixed bed reactor; 6. Gas distribution pipe; 7. Catalyst; 8. Central pipe; 9. Cap; 10. Catalyst discharge port; 11. Reaction tank; 12. Circulating air pump; 13. Intake valve; 14. Piston; 15. Pump body; 16. Exhaust valve; 17. Crank-connecting rod mechanism; 18. Gas pressurization liquefaction device; 19. Hydrogen output port; 20. Hydrogen recovery cylinder; 21. Mixed gas output port; 22. Mixed gas recovery cylinder. DETAILED DESCRIPTION

[0017] In order to make the purpose, technical solution and advantages of the utility model clearer, the technical solution of the utility model will be clearly and completely described below in conjunction with the accompanying drawings. Obviously, the described embodiments are part of the embodiments of the utility model, not all of the embodiments. Based on the embodiments of the utility model, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the utility model.

[0018] In the description of the present invention, it should be understood that the terms "center", "longitudinal", "lateral", "length", "width", "thickness", "up", "down", "front", "back", "left", "right", "vertical", "horizontal", "top", "bottom", "inside", "outside", "clockwise", "counterclockwise", "axial", "radial", "circumferential" and the like indicate orientations or positional relationships based on the orientations or positional relationships shown in the accompanying drawings, and are only for the convenience of describing the present invention and simplifying the description, and do not indicate or imply that the referred device or element must have a specific orientation, be constructed and operated in a specific orientation, and therefore should not be understood as a limitation on the present invention.

[0019] In addition, the terms "first" and "second" are used for descriptive purposes only and should not be understood as indicating or implying relative importance or implicitly indicating the number of the indicated technical features. Therefore, the features defined as "first" and "second" may explicitly or implicitly include one or more of the features. In the description of the present utility model, the meaning of "plurality" is more than two, unless otherwise clearly and specifically defined.

[0020] In the present invention, unless otherwise clearly specified and limited, the terms "install", "connect", "connect", "fix" and the like should be understood in a broad sense, for example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection or an indirect connection through an intermediate medium, it can be the internal connection of two elements or the interaction relationship between two elements. For ordinary technicians in this field, the specific meanings of the above terms in the present invention can be understood according to specific circumstances.

[0021] In the present utility model, unless otherwise clearly specified and limited, a first feature being "above" or "below" a second feature may mean that the first and second features are in direct contact, or the first and second features are in indirect contact through an intermediate medium. Moreover, a first feature being "above", "above" or "above" a second feature may mean that the first feature is directly above or obliquely above the second feature, or simply means that the first feature is higher in level than the second feature. A first feature being "below", "below" or "below" a second feature may mean that the first feature is directly below or obliquely below the second feature, or simply means that the first feature is lower in level than the second feature.

[0022] In the description of this specification, the description with reference to the terms "one embodiment", "some embodiments", "example", "specific example", or "some examples" etc. means that the specific features, structures, materials or characteristics described in conjunction with the embodiment or example are included in at least one embodiment or example of the utility model. In this specification, the schematic representations of the above terms do not necessarily refer to the same embodiment or example. Moreover, the specific features, structures, materials or characteristics described may be combined in any one or more embodiments or examples in a suitable manner. In addition, those skilled in the art may combine and combine the different embodiments or examples described in this specification and the features of the different embodiments or examples, without contradiction.

[0023] The hydrogen recovery device in the reforming catalyst regeneration reaction provided by the utility model includes: a gas mixing device, whose inlet is connected to a hydrogen pipeline, a methane pipeline and a carbon dioxide pipeline, for forming a reaction gas; a fixed bed reactor, whose inlet is connected to the outlet of the gas mixing device, for performing catalyst regeneration and methane dry reforming reaction under a reaction gas atmosphere; a circulating gas pump, whose inlet is connected to the outlet of the fixed bed reactor, for collecting the carbon monoxide and hydrogen mixed gas generated by the methane dry reforming reaction; a gas pressurized liquefaction device, whose inlet is connected to the outlet of the circulating gas pump, for pressurizing, cooling and liquefying the collected carbon monoxide and hydrogen mixed gas to achieve separation of carbon monoxide and hydrogen. The utility model can not only integrate the catalyst regeneration and methane dry reforming reaction, but also recover and separate the CO and H2 generated by the reaction for recycling, saving costs, reducing carbon emissions, and having a good prospect of use.

[0024] The hydrogen recovery device for the reforming catalyst regeneration reaction provided by the embodiment of the utility model is described in detail below in conjunction with the accompanying drawings.

[0025] Embodiment 1

[0026] See also Figure 1 The utility model provides a hydrogen recovery device for a reforming catalyst regeneration reaction, comprising: a gas mixing device 4, the inlet of the gas mixing device 4 is respectively connected to a hydrogen pipeline 1, a methane pipeline 2 and a carbon dioxide pipeline 3, for forming a reaction gas; a fixed bed reactor 5, the inlet of the fixed bed reactor 5 is connected to the outlet of the gas mixing device 4, for performing catalyst regeneration and methane dry reforming reaction under a reaction gas atmosphere; a circulating gas pump 12, the inlet of the circulating gas pump 12 is connected to the outlet of the fixed bed reactor, for collecting carbon monoxide produced by the methane dry reforming reaction and a hydrogen mixed gas; a gas pressurizing and liquefying device 18, the inlet of the gas pressurizing and liquefying device 18 is connected to the outlet of the circulating gas pump 12, and the gas pressurizing and liquefying device 18 is used to pressurize, cool and liquefy the collected carbon monoxide and hydrogen mixed gas to achieve the separation of carbon monoxide and hydrogen; a hydrogen recovery gas cylinder 20 and a mixed gas recovery gas cylinder 22, the inlet of the hydrogen recovery gas cylinder 20 is connected to the hydrogen output port 19 at the upper end of the gas pressurizing and liquefying device 18, and the inlet of the mixed gas recovery gas cylinder 22 is connected to the mixed gas output port 21 at the lower end of the gas pressurizing and liquefying device 18.

[0027] In the above embodiment, preferably, the fixed bed reactor 5 includes: a reaction tank 11, a fixed bed reactor 5 inlet is formed at the top of the reaction tank 11, and a catalyst unloading port 10 is provided at the bottom of the reaction tank 11; a gas distribution pipe 6 is circumferentially arranged on the inner wall of the reaction tank 11, and is used to evenly distribute the reaction gas into the reaction tank 11; a central tube 8 is axially arranged in the reaction tank 11, and the bottom end of the central tube 8 passes through the reaction tank 11 to form an outlet of the fixed bed reactor 5 to discharge the carbon monoxide and hydrogen mixed gas produced by the methane dry reforming reaction; a catalyst 7 is filled in the annular space between the gas distribution pipe 6 and the central tube 8; a cap 9 is sealed and arranged at the top of the central tube 8 and covers the top of the catalyst 7, so as to prevent the reaction gas from diffusing upward.

[0028] In the above embodiment, preferably, the circulating gas pump 12 comprises: a pump body 15; an air intake valve 13, which is arranged at the lower end of the pump body 15 and connected to the outlet of the fixed bed reactor 5; an air exhaust valve 16, which is arranged at the upper end of the pump body 15 and connected to the inlet of the gas pressurizing and liquefying device 18; a piston 14, which is slidably arranged in the pump body 15; a crank connecting rod mechanism 17, the action end of which is connected to the piston 14, and is used to drive the piston 14 to reciprocate in the pump body 15. Thus, when the piston 14 moves backward, the pressure in the pump chamber decreases, and the carbon monoxide and hydrogen mixed gas is sucked into the pump chamber through the air intake valve 13; when the piston 14 moves forward, the pressure in the pump chamber increases, and the carbon monoxide and hydrogen mixed gas is discharged from the pump chamber through the air exhaust valve 16.

[0029] Embodiment 2

[0030] During use, the hydrogen recovery device for the reforming catalyst regeneration reaction provided by the utility model comprises the following specific steps: firstly, the catalyst is synthesized by an impregnation method, the catalyst 7 is loaded into a fixed bed reactor 5, and hydrogen is introduced into a gas distribution pipe 6 from the inlet of the fixed bed reactor 5 and dispersed in the catalyst 7, the temperature of the fixed bed reactor 5 is controlled at 400° C., so that the catalyst 7 is regenerated and reduced in a hydrogen atmosphere; then, methane and carbon dioxide gas are introduced into a gas distribution pipe 6 from the inlet of the fixed bed reactor 5 and dispersed in the catalyst 7, so that the catalyst 7 undergoes a methane dry reforming reaction at different temperatures under a methane and carbon dioxide atmosphere, and the carbon monoxide and hydrogen mixed gas generated after the reaction is discharged from the outlet of the fixed bed reactor 5; the carbon monoxide and hydrogen mixed gas discharged from the outlet of the solid bed reactor 5 is collected by a circulating air pump 12, and the mixed gas is first sucked into a pump body 15 from an air intake valve 13 at the lower end of the circulating air pump 12 by the reciprocating motion of a piston 14, and then the carbon monoxide and hydrogen mixed gas is discharged into a gas pressurization liquefaction device 18 from an exhaust valve 16 at the upper end of the circulating air pump 12. In the gas pressure liquefaction device 18, since the liquefaction temperature of CO is -190°C, the liquefaction temperature of H2 is -253°C, and the density of CO is 8.9 g / cm 3, the density of H2 is 0.089g / L. Therefore, based on this difference, pressurized cooling treatment is carried out in the gas pressurized liquefaction device 18 to cool the temperature to -200°C. At this time, CO is liquefied, while H2 is still a gas, and H2 is very light and is above the gas pressurized liquefaction device 18. Therefore, H2 is discharged from the hydrogen output port 19 at the upper end of the gas pressurized liquefaction device 18 and loaded into the hydrogen recovery gas cylinder 20 for recovery and recycling. The liquefied CO and H2 mixed gas is discharged from the mixed gas output port 21 at the lower end of the gas pressurized liquefaction device 18 and then further processed.

[0031] In summary, the hydrogen recovery device in the reforming catalyst regeneration reaction can effectively solve the process problem of hydrogen recovery in the catalyst regeneration reaction. The device independently develops a reforming catalyst regeneration reaction process to realize the regeneration and recycling of waste reforming catalysts. On the basis of the existing regeneration process, through process optimization and combination, a new process for hydrogen recovery in the reforming catalyst regeneration reaction is developed to realize the comprehensive utilization of waste catalyst regeneration cycle and hydrogen recovery cycle, which has significant social and economic benefits.

[0032] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, rather than to limit it. Although the present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art should understand that they can still modify the technical solutions described in the aforementioned embodiments, or make equivalent replacements for some of the technical features therein. However, these modifications or replacements do not deviate the essence of the corresponding technical solutions from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A hydrogen recovery device for a reforming catalyst regeneration reaction, characterized in that: include: A gas mixing device, wherein the inlets of the gas mixing device are respectively connected to a hydrogen pipeline, a methane pipeline and a carbon dioxide pipeline to form a reaction gas; A fixed bed reactor, wherein the inlet of the fixed bed reactor is connected to the outlet of the gas mixing device, and is used for performing catalyst regeneration and methane dry reforming reaction under a reaction gas atmosphere; A circulating air pump, the inlet of which is connected to the outlet of the fixed bed reactor, and is used to collect the carbon monoxide and hydrogen mixed gas produced by the methane dry reforming reaction; A gas pressurizing and liquefying device, wherein the inlet of the gas pressurizing and liquefying device is connected to the outlet of the circulating gas pump, and is used for pressurizing, cooling and liquefying the collected carbon monoxide and hydrogen mixed gas to achieve separation of carbon monoxide and hydrogen.

2. The hydrogen recovery device in the reforming catalyst regeneration reaction according to claim 1, characterized in that: It also includes a hydrogen recovery cylinder and a mixed gas recovery cylinder, wherein the inlet of the hydrogen recovery cylinder is connected to the hydrogen output port at the upper end of the gas pressurization and liquefaction device, and the inlet of the mixed gas recovery cylinder is connected to the mixed gas output port at the lower end of the gas pressurization and liquefaction device.

3. The hydrogen recovery device in the reforming catalyst regeneration reaction according to claim 1, characterized in that: The fixed bed reactor comprises: A reaction tank, wherein the fixed bed reactor inlet is formed at the top of the reaction tank, and a catalyst discharge port is provided at the bottom of the reaction tank; A gas distribution pipe is circumferentially arranged on the inner wall of the reaction tank and is used to evenly distribute the reaction gas into the reaction tank; A central tube is axially arranged in the reaction tank, and the bottom end of the central tube passes through the reaction tank to form an outlet of the fixed bed reactor to discharge a mixed gas of carbon monoxide and hydrogen produced by a methane dry reforming reaction; A catalyst is filled in the annular space between the gas distribution pipe and the central pipe; A cap is provided at the top of the central tube to cover the top of the catalyst and prevent the reaction gas from diffusing upward.

4. The hydrogen recovery device in the reforming catalyst regeneration reaction according to claim 1, characterized in that: The circulating air pump comprises: Pump body; An air intake valve is arranged at the lower end of the pump body and connected to the outlet of the fixed bed reactor; An exhaust valve is arranged at the upper end of the pump body, and the exhaust valve is connected to the inlet of the gas pressurizing and liquefying device; A piston, slidably disposed in the pump body; A crank-connecting rod mechanism, wherein the action end of the crank-connecting rod mechanism is connected to the piston and is used to drive the piston to reciprocate in the pump body.

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