Joule heating type ammonia decomposition porous foam filled membrane reactor

By integrating Joule heating technology and porous foam filling structure in the ammonia decomposition membrane reactor, the problems of low thermal efficiency and insufficient gas purity of the existing ammonia decomposition device are solved, and efficient and economical ammonia decomposition hydrogen production process is achieved, and high Purity of hydrogen.

CN119455881AActive Publication Date: 2025-02-18ZHEJIANG UNIV OF TECH
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Patent Information

Application Number
CN202411613944.6
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2024-11-13
Publication Date
2025-02-18
Estimated Expiration
2044-11-13

AI Technical Summary

Technical Problem

The existing Joule heating ammonia decomposition device has problems such as low thermal efficiency and insufficient gas purity, and the integration of porous foam in the ammonia decomposition membrane reactor is difficult, resulting in poor thermal management and gas diffusion control effects.

Method used

A Joule-heated ammonia-decomposed porous foam-filled membrane reactor was designed. Through the integrated Joule heating technology and porous foam filling structure, silicon carbide porous foam is used as the Joule heating substrate, and palladium film is used as the hydrogen permeable film in the membrane reactor. , realize the coupling of ammonia decomposition reaction, hydrogen separation and heating.

Benefits of technology

The hydrogen production efficiency of ammonia decomposition is significantly improved, and a more efficient and economical ammonia decomposition process is achieved. Through efficient thermal management and gas separation, high-purity hydrogen is obtained.

✦ Generated by Eureka AI based on patent content.

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Abstract

The invention discloses a Joule heating type ammonia decomposition porous foam filled membrane reactor which comprises an explosion-proof cavity, a metal palladium membrane is adopted as a hydrogen permeation membrane, cobalt molybdenum nitride is selected as an efficient catalyst, the catalyst is uniformly distributed in silicon carbide foam, and the silicon carbide foam plays a role of a Joule heating substrate at the same time; the two ends of the silicon carbide foam are connected to a positive electrode and a negative electrode respectively, rapid heating of the catalyst bed layer is achieved by applying voltage, in the operation process of the reactor, ammonia gas is preheated through the heat exchanger firstly and then enters the membrane reactor to be decomposed, and hydrogen, nitrogen and unreacted ammonia gas mixed gas are generated; after the gases are separated through a palladium membrane, high-purity hydrogen with the purity reaching up to 99.999% can be obtained. According to the device disclosed by the invention, three steps of heating, hydrogen production and purification are integrated, so that the loss of heat in the transfer process is effectively reduced, and the palladium membrane also promotes the movement of chemical reaction equilibrium towards the hydrogen production direction, so that the conversion rate of ammonia decomposition is improved.
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Description

Technical Field

[0001] The invention belongs to the field of new energy hydrogen production, and in particular relates to a Joule-heating ammonia decomposition porous foam-filled membrane reactor. Background Art

[0002] Hydrogen energy, with its high energy density and clean characteristics, is regarded as a key secondary energy source for achieving a clean, low-carbon, safe and efficient energy system. The high calorific value of hydrogen (142MJ / kg) and zero COx and NOx emissions when generating electricity in fuel cells make it an ideal energy carrier. However, the volatility and low volumetric energy density of hydrogen require demanding storage and transportation conditions. Storing hydrogen in the form of ammonia and achieving safe and efficient storage and release of hydrogen through the synthesis and decomposition of ammonia is a promising solution.

[0003] As a hydrogen carrier, ammonia has the advantages of high hydrogen content, high volumetric energy density, low storage and transportation costs, and zero carbon emission conversion. In order to improve the conversion rate of ammonia decomposition and reduce the reaction temperature, researchers have developed a variety of catalysts and membrane reactor technologies. In particular, Ru-based catalysts have attracted attention due to their excellent development potential, but they are expensive. Although the research on catalysts has improved the kinetics, the main problems of thermodynamic limitations and high-purity H2 requirements (greater than 99.97%) for most applications have not been solved. In addition to catalysts, many hydrogen permeable membrane reactors have been developed for ammonia decomposition. By separating hydrogen at the same time, the reaction equilibrium is developed in a direction that is favorable to hydrogen production. The use of H2-selective membrane reactors for in-situ hydrogen removal can not only promote the chemical equilibrium in favor of hydrogen production, but also achieve high-purity hydrogen separation. However, the high conversion rate of H2-selective membrane reactors does not mean high efficiency. For example, even if the conversion rate is 100%, the energy efficiency may be low. Therefore, in order to achieve efficient thermochemical conversion, it is necessary to strengthen the heat and mass transfer processes in the membrane reactor.

[0004] In order to solve the above problems, researchers have been exploring more efficient and economical ammonia decomposition methods. In recent years, Joule heating technology has attracted attention due to its fast and uniform heating characteristics. Joule heating uses the Joule heat generated when an electric current passes through a material to heat the material, which can achieve fast and uniform heating, thereby improving the reaction rate and efficiency. However, existing Joule heating ammonia decomposition devices generally lack effective thermal management and gas diffusion control, resulting in low thermal efficiency and insufficient gas purity. In addition, porous foam, as a porous material, has been widely studied due to its high specific surface area and good thermal conductivity. The use of porous foam in an ammonia decomposition reactor can improve the uniformity of catalyst distribution and enhance heat transfer efficiency, thereby improving the efficiency of ammonia decomposition. However, how to effectively integrate porous foam into an ammonia decomposition membrane reactor to achieve optimal thermal management and gas diffusion control remains a technical challenge.

[0005] The present invention aims to provide a Joule-heated ammonia decomposition porous foam-filled membrane reactor, which solves the problems of low thermal efficiency and insufficient gas purity in the prior art by integrating Joule heating technology and a porous foam filling structure. Summary of the invention

[0006] In view of the problems existing in the prior art, the purpose of the present invention is to provide a Joule-heated ammonia decomposition porous foam-filled membrane reactor to overcome the shortcomings of low thermal efficiency, low purity and low hydrogen production efficiency in the existing ammonia decomposition hydrogen production process.

[0007] To achieve the above purpose, the protection scheme of the present invention is as follows: A Joule-heated ammonia decomposition porous foam filled membrane reactor comprises an explosion-proof chamber with openings at both left and right ends, a first flange and a second flange are respectively provided on the left and right sides of the explosion-proof chamber, a second sleeve is provided at the end of the second flange, the second sleeve extends into a heating and catalytic chamber through the second flange, the left open end of the second sleeve is in the heating and catalytic chamber, and the right open end thereof is provided with two openings, one opening is an air inlet pipe, and the other opening is a second thermocouple insertion port, a membrane assembly is provided inside the explosion-proof chamber, the membrane assembly divides the explosion-proof chamber into two chambers that are not connected to each other, the inner side is a hydrogen separation chamber, and the outer side is a heating and catalytic chamber, a hydrogen outlet pipe is provided on the tail wall of the hydrogen separation chamber, a porous foam with a hole in the middle is provided in the heating and catalytic chamber, an ammonia decomposition catalyst is filled in the porous foam, a first sleeve connected to the outside is provided on the upper side of the heating and catalytic chamber, the upper side of the first sleeve has two openings, the left opening is a tail gas pipe, and the upper side is a first thermocouple insertion port, and the first sleeve is connected to the explosion-proof chamber by welding.

[0008] Furthermore, a hydrogen permeable membrane is provided on the outer wall surface of the membrane assembly, and the hydrogen permeable membrane is a tubular palladium membrane or a palladium alloy composite membrane. One end of the membrane assembly is closed and the other end is open, wherein the open end is a hydrogen outlet pipe, which passes through the bottom plate of the membrane assembly and the first flange in sequence. The membrane assembly is a sleeve-type structure and is connected to the bottom plate of the membrane assembly by welding, and the bottom plate of the membrane assembly is connected to the first flange by welding.

[0009] Furthermore, a first heating wiring tube is provided on the first flange, a first conductive copper electrode is provided on the inner wall surface between the first flange and the explosion-proof cavity, a first heating wire is provided in the first heating wiring tube, the first conductive copper electrode is tightly connected to the first heating wire, and the first conductive copper electrode is connected to the first flange by welding.

[0010] Furthermore, a heating wiring tube is provided on the second flange, a second conductive copper electrode is provided on the inner wall surface between the second flange and the explosion-proof cavity, a second heating wire is provided inside the second heating wiring tube, and the second conductive copper electrode is tightly connected to the second heating wire.

[0011] Furthermore, a first perforated graphite wound gasket is arranged between the first flange and the explosion-proof cavity, and is fastened and connected by a first bolt; a second perforated graphite wound gasket is arranged between the second flange and the explosion-proof cavity, and is fastened and connected by a second bolt.

[0012] Furthermore, it includes a first thermocouple and a second thermocouple, the first thermocouple is fixed to the insertion port of the first thermocouple by a sleeve seal, the first thermocouple passes through a first sleeve and a porous air plug to the upper side of the heating and catalytic chamber, the porous air plug is PM-35 material, its pore size is 35μm, and is connected to the heating and catalytic chamber by welding; the second thermocouple is fixed to the insertion port of the second thermocouple by a sleeve seal, and the second thermocouple passes through the second sleeve to the right side of the heating and catalytic chamber.

[0013] Furthermore, the ammonia decomposition catalyst is cobalt-molybdenum nitride, and the active components are cobalt and molybdenum; the hydrogen permeable membrane is a pure palladium membrane supported by porous alumina, a palladium-silver alloy membrane supported by porous alumina, a palladium-copper alloy membrane supported by porous alumina, a palladium-gold alloy membrane supported by porous alumina, or a palladium-ruthenium alloy membrane supported by porous stainless steel.

[0014] Furthermore, the porous foam material is silicon carbide, with a porosity of 85% and a pore density of 40ppi; the explosion-proof cavity, the first flange, the second flange, the first heating wiring pipe, the hydrogen outlet pipe, the second heating wiring pipe, the air inlet pipe and the sleeve surface are all coated with an insulating coating.

[0015] Furthermore, it includes a current controller, the first heating wire is connected to the negative electrode of the DC power supply through a wire, the second heating wire is connected to the current controller, and the current controller is connected to the positive electrode of the DC power supply through an electric wire.

[0016] Furthermore, it includes a vacuum pump, a hydrogen heat exchanger, a tail gas heat exchanger, a combustion chamber and a hydrogen storage tank, wherein the hydrogen outlet pipe is connected to the vacuum pump, the air inlet on the side of the hydrogen heat exchanger, the air outlet on the side of the hydrogen heat exchanger and the hydrogen storage tank through a pipeline; the air outlet at the top of the tail gas heat exchanger, the air inlet at the bottom of the hydrogen heat exchanger, the air outlet at the top of the hydrogen heat exchanger and the air inlet pipe are connected through a pipeline; the tail gas pipe is connected to the air inlet on the side of the tail gas heat exchanger, the air outlet on the side of the tail gas heat exchanger and the combustion chamber through a pipeline.

[0017] Compared with the prior art, the beneficial effects of the present invention are as follows: 1) The present invention uses Joule heating and catalyst-coupled porous foam to couple ammonia decomposition reaction, hydrogen separation and heating in the same reactor. The structural design is ingenious, which greatly improves the efficiency of ammonia decomposition and hydrogen production, realizes a more efficient and economical ammonia decomposition process, and is safe, efficient and easy to maintain; 2) The present invention incorporates Joule heating technology into the ammonia decomposition membrane reactor. The Joule heating technology can directly convert electrical energy into thermal energy, thereby achieving rapid and uniform heating inside the reactor; 3) The present invention uses silicon carbide porous foam as a Joule heating substrate, which has high thermal conductivity, which means that it can conduct heat quickly, thereby achieving more uniform heating and faster response time during Joule heating; its resistivity is high, and under the same current, silicon carbide foam can generate more heat; and the disorder of its porous medium greatly enhances the disturbance of the fluid when passing through the heat exchange surface, thereby generating more disturbances and vortices. These fluid dynamics phenomena effectively reduce the thickness of the heat exchange boundary layer, thereby significantly improving the heat transfer coefficient and enhancing the heat transfer efficiency; 4) The hydrogen permeable membrane used in the present invention is a palladium membrane, which has good thermal stability and pressure resistance, and has extremely high hydrogen selectivity. It can efficiently extract high-purity hydrogen from the gas mixture produced by the decomposition of ammonia, and quickly remove the hydrogen generated by the reaction, so as to promote the forward decomposition reaction of ammonia, thereby breaking the original thermodynamic equilibrium state, so that the conversion rate of ammonia is improved and the temperature required for the reaction is reduced; 5) The membrane reactor of the present invention uses a metal palladium membrane as a hydrogen permeable membrane, and selects cobalt molybdenum nitride as a high-efficiency catalyst. The catalyst is evenly distributed in the silicon carbide foam, which also acts as a Joule heating substrate. The two ends of the silicon carbide foam are respectively connected to the positive and negative electrodes. The catalyst bed is quickly heated by applying voltage. During the operation of the reactor, ammonia is first preheated by a heat exchanger, and then enters the membrane reactor for decomposition to generate hydrogen, nitrogen and unreacted ammonia mixed gas. After these gases are separated by the palladium membrane, high-purity hydrogen with a purity of up to 99.99% can be obtained. BRIEF DESCRIPTION OF THE DRAWINGS

[0018] Figure 1 A schematic diagram of the structure of a Joule-heated ammonia decomposition porous foam-filled membrane reactor provided in an embodiment of the present invention; Figure 2 A diagram of an experimental system of a Joule-heating ammonia decomposition porous foam-filled membrane reactor provided in an embodiment of the present invention; In the figure: 1, hydrogen outlet pipe; 2, first perforated graphite wound gasket; 3, first flange; 4, tail pipe; 5, first thermocouple; 6, porous air plug; 7, explosion-proof chamber; 8, heating and catalytic chamber; 9, second bolt; 10, second flange; 11, second heating wiring pipe; 12, second heating wire; 13, second thermocouple; 14, intake pipe; 15, second perforated graphite wound gasket; 16, second conductive copper electrode; 17, membrane group 1. Parts; 18. porous foam; 19. hydrogen permeable membrane; 20. hydrogen separation chamber; 21. first conductive copper electrode; 22. first bolt; 23. first heating wiring pipe; 24. first heating wire; 25. membrane assembly bottom plate; 201. vacuum pump; 202. hydrogen heat exchanger; 203. tail gas heat exchanger; 204. decombustion chamber; 205. hydrogen storage tank; 206. DC power supply; 207. current controller; 208. temperature data collector. DETAILED DESCRIPTION

[0019] The present invention will be further described below in conjunction with the accompanying drawings, but the scope of protection of the present invention is not limited to the described scope.

[0020] Please refer to Figure 1-2 A Joule-heated ammonia decomposition porous foam-filled membrane reactor comprises an explosion-proof chamber 7 with openings at both ends, a first flange 3 and a second flange 10 are respectively arranged on the left and right sides of the explosion-proof chamber 7, further, a first perforated graphite wound gasket 2 is arranged between the first flange 3 and the explosion-proof chamber 7, and is fastened and connected by a first bolt 22; a second perforated graphite wound gasket 15 is arranged between the second flange 10 and the explosion-proof chamber 7, and is fastened and connected by a second bolt 9.

[0021] A second sleeve is provided at the end of the second flange 10, and the second sleeve extends into the heating and catalytic chamber 8 through the second flange 10. The left open end of the second sleeve is in the heating and catalytic chamber 8, and the right open end thereof is provided with two openings, one opening is an air inlet pipe 14, and the other opening is an insertion port for a second thermocouple. A membrane assembly 17 is provided inside the explosion-proof chamber 7, and the membrane assembly 17 divides the explosion-proof chamber 7 into two chambers that are not connected to each other, the inner side is a hydrogen separation chamber 20, and the outer side is a heating and catalytic chamber 8. A hydrogen outlet pipe 1 is provided on the tail wall of the hydrogen separation chamber 20, and a porous foam 18 with holes in the middle is provided in the heating and catalytic chamber 8, and an ammonia decomposition catalyst is filled in the porous foam 18. A first sleeve connected to the outside is provided on the upper side of the heating and catalytic chamber 8, and the upper side of the first sleeve has two openings, the left opening is a tail pipe 4, and the upper side is an insertion port for a first thermocouple, and the first sleeve is connected to the explosion-proof chamber 7 by welding.

[0022] A hydrogen permeable membrane 19 is arranged on the outer wall of the membrane assembly 17. One end of the membrane assembly 17 is closed and the other end is open, wherein the open end is a hydrogen outlet pipe 1, which passes through the membrane assembly bottom plate 25 and the first flange 3 in sequence. The membrane assembly 17 is a sleeve-type structure and is connected to the membrane assembly bottom plate 25 by welding, and the membrane assembly bottom plate 25 is connected to the first flange 3 by welding.

[0023] A first heating wiring tube 23 is provided on the first flange 3, a first conductive copper electrode 21 is provided on the inner wall surface between the first flange 3 and the explosion-proof cavity 7, a first heating wire 24 is provided in the first heating wiring tube 23, the first conductive copper electrode 21 is tightly connected to the first heating wire 24, and the first conductive copper electrode 21 is connected to the first flange 3 by welding.

[0024] A heating wiring tube 11 is provided on the second flange 10 , a second conductive copper electrode 16 is provided on the inner wall surface between the second flange 10 and the explosion-proof chamber 7 , a second heating wire 12 is provided inside the second heating wiring tube 11 , and the second conductive copper electrode 16 is tightly connected to the second heating wire 12 .

[0025] The present invention provides a Joule-heated ammonia decomposition porous foam-filled membrane reactor, which also includes a first thermocouple 5 and a second thermocouple 13. The first thermocouple 5 is fixed to the first thermocouple insertion port by a sleeve seal. The first thermocouple 5 passes through the first sleeve and the porous air plug 6 to the upper side of the heating and catalytic chamber 8. The porous air plug 6 is made of PM-35 material with a pore size of 35 μm. It is connected to the heating and catalytic chamber 8 by welding to prevent the catalyst from blowing into the tail pipe 4.

[0026] The second thermocouple 13 is fixed to the second thermocouple insertion port by a sleeve seal to measure the inlet gas temperature. The second thermocouple 13 passes through the second sleeve to the right side of the heating and catalytic chamber 8.

[0027] The ammonia decomposition catalyst is cobalt-molybdenum nitride, and the active components are cobalt and molybdenum; the hydrogen permeable membrane 19 is a pure palladium membrane supported by porous alumina, a palladium-silver alloy membrane supported by porous alumina, a palladium-copper alloy membrane supported by porous alumina, a palladium-gold alloy membrane supported by porous alumina, or a palladium-ruthenium alloy membrane supported by porous stainless steel.

[0028] The porous foam 18 is made of silicon carbide, with a porosity of 85% and a pore density of 40ppi; the explosion-proof cavity 7, the first flange 3, the second flange 10), the first heating wiring pipe 23, the hydrogen outlet pipe 1, the second heating wiring pipe 11, the air inlet pipe 14 and the sleeve surface are all coated with insulation.

[0029] A Joule-heated ammonia decomposition porous foam-filled membrane reactor also includes a current controller 207, a first heating wire 23 is connected to the negative electrode of a DC power supply 206 through a wire, a second heating wire 12 is connected to the current controller 207, and the current controller 207 is connected to the positive electrode of the DC power supply 206 through an electric wire.

[0030] A Joule-heated ammonia decomposition porous foam-filled membrane reactor also includes a vacuum pump 201, a hydrogen heat exchanger 202, a tail gas heat exchanger 203, a combustion chamber 204 and a hydrogen storage tank 205. The hydrogen outlet pipe 1 is connected to the vacuum pump 201, the air inlet on the side of the hydrogen heat exchanger 202, the air outlet on the side of the hydrogen heat exchanger 202 and the hydrogen storage tank 205 through pipelines.

[0031] The air outlet at the top of the exhaust gas heat exchanger 203, the air inlet at the bottom of the hydrogen heat exchanger 202, the air outlet at the top of the hydrogen heat exchanger 202 and the air inlet pipe 14 are connected by pipelines; the exhaust pipe 4 is connected to the air inlet on the side of the exhaust gas heat exchanger 203, the air outlet on the side of the exhaust gas heat exchanger 203 and the combustion chamber 204 by pipelines.

[0032] The specific operation steps of a Joule-heated ammonia decomposition porous foam filled membrane reactor for use in ammonia decomposition and hydrogen production are as follows: Start the vacuum pump 201, and under the condition of vacuum in the hydrogen separation chamber, nitrogen at a flow rate of 400 ml / min enters the heating and catalytic chamber 8 through the air inlet pipe, so that the heating and catalytic chamber 8 and the membrane assembly 17 are in a nitrogen protective atmosphere; The current controller 207 controls the current size of the DC power supply 206 passing through the silicon carbide foam, so that the gas temperature at the outlet of the heating and catalytic chamber 8 reaches the set temperature (500° C.); After reaching the set temperature, the nitrogen valve is closed, the hydrogen valve is opened, and hydrogen with a flow rate of 400 ml / min enters the heating and catalytic chamber 8 through the inlet pipe to pretreat the catalyst for 1 hour to remove oxides on the catalyst surface; The hydrogen valve is closed, and the ammonia valve is opened. The ammonia with a flow rate of 400 ml / min is heat-exchanged with the tail gas through the tail gas heat exchanger 203, and then heat-exchanged with the hydrogen through the hydrogen heat exchanger 202. The preheated ammonia enters the heating and catalytic chamber 8 through the air inlet pipe, and is heated to a working temperature suitable for ammonia decomposition by the silicon carbide foam, and is completely decomposed into hydrogen and nitrogen under the action of the catalyst; Under the action of pressure difference, hydrogen moves to the surface of the palladium alloy membrane and is adsorbed and dissociated, then passes through the palladium membrane through the dissolution-diffusion mechanism, recombines into hydrogen molecules on the other side and enters the hydrogen separation chamber. The separated hydrogen enters the hydrogen storage tank 205 through the hydrogen outlet pipe; The remaining gas in the heating and catalytic chamber 8 is discharged from the tail gas pipe 4 to the combustion chamber 204.

[0033] In this embodiment, the porous foam 18 is made of silicon carbide as a Joule heating substrate, with an outer diameter of 27 mm, an inner diameter of 14 mm, and a thickness of 15 mm. The rated voltage of the DC power supply 206 is 24 V, and the porous foam 18 is uniformly filled with Co3Mo3N4g. The membrane assembly is installed with a single porous alumina-loaded pure palladium membrane, with a diameter of 12 mm, an average thickness of 18 microns, and an effective length of 25 mm. After the ammonia is introduced, the first thermocouple shows that the outlet temperature of the heated catalytic chamber is 500°C. The outlet tail gas is analyzed by gas chromatograph, and no ammonia components are detected, indicating that the ammonia is completely converted and decomposed. The purity of the hydrogen obtained after separation by palladium membrane is 99.999% by gas chromatograph analysis.

[0034] Heat transfer performance of pure catalyst and silicon carbide porous foam filled catalyst under the same conditions; At a furnace temperature of 600°C, using the same tubular heating furnace, quartz tube, gas flow rate (400ml / min) and catalyst loading (4gCo3Mo3N), it was found that the outlet gas temperature of the silicon carbide porous foam filled catalyst reached 578.3°C, while the pure catalyst was only 533.5°C, a difference of 44.8°C. This significant temperature difference proves that the silicon carbide porous foam, due to its high thermal conductivity and porous structure, provides a larger heat exchange area and enhances the fluid dynamics effect, thereby achieving more efficient heat transfer and shortening the thermal response time, which not only improves the hydrogen production efficiency, but also helps to reduce energy consumption and carbon emissions, which is of great significance to improving the economic benefits and environmental friendliness of hydrogen production technology.

Claims

1. A Joule-heated ammonia decomposition porous foam-filled membrane reactor, comprising an explosion-proof chamber (7) with openings at both left and right ends, a first flange (3) and a second flange (10) being respectively provided on the left and right sides of the explosion-proof chamber (7), a second sleeve being provided at the end of the second flange (10), the second sleeve extending into the heating and catalytic chamber (8) through the second flange (10), the left open end of the second sleeve being located in the heating and catalytic chamber (8), the right open end of the second sleeve being provided with two openings, one opening being an air inlet pipe (14), and the other opening being a second thermocouple insertion port, characterized in that A membrane assembly (17) is provided inside the explosion-proof chamber (7), and the membrane assembly (17) divides the explosion-proof chamber (7) into two chambers that are not connected to each other, the inner chamber being a hydrogen separation chamber (20), and the outer chamber being a heating and catalytic chamber (8). A hydrogen outlet pipe (1) is provided on the rear wall of the hydrogen separation chamber (20), a porous foam (18) with a hole in the middle is provided inside the heating and catalytic chamber (8), and an ammonia decomposition catalyst is filled in the porous foam (18). A first sleeve connected to the outside is provided on the upper side of the heating and catalytic chamber (8), and the upper side of the first sleeve has two openings, the left opening being a tail pipe (4), and the upper side being a first thermocouple insertion port, and the first sleeve is connected to the explosion-proof chamber (7) by welding.

2. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 1, characterized in that The outer wall surface of the membrane assembly (17) is provided with a hydrogen permeable membrane (19), and the hydrogen permeable membrane (19) is a tubular palladium membrane or a palladium alloy composite membrane. The membrane assembly (17) is sealed at one end and open at the other end, wherein the open end is a hydrogen outlet pipe (1) that passes through the membrane assembly bottom plate (25) and the first flange (3) in sequence. The membrane assembly (17) is a sleeve-type structure and is connected to the membrane assembly bottom plate (25) by welding, and the membrane assembly bottom plate (25) is connected to the first flange (3) by welding.

3. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 1, characterized in that A first heating wiring tube (23) is provided on the first flange (3), a first conductive copper electrode (21) is provided on the inner wall surface between the first flange (3) and the explosion-proof chamber (7), a first heating wire (24) is provided in the first heating wiring tube (23), the first conductive copper electrode (21) and the first heating wire (24) are hermetically connected, and the first conductive copper electrode (21) and the first flange (3) are connected by welding.

4. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 3, characterized in that A heating wiring tube (11) is provided on the second flange (10), a second conductive copper electrode (16) is provided on the inner wall surface between the second flange (10) and the explosion-proof chamber (7), a second heating wire (12) is provided inside the second heating wiring tube (11), and the second conductive copper electrode (16) is tightly connected to the second heating wire (12).

5. The Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 1, characterized in that A first perforated graphite wound gasket (2) is arranged between the first flange (3) and the explosion-proof chamber (7), and is fastened and connected by a first bolt (22); a second perforated graphite wound gasket (15) is arranged between the second flange (10) and the explosion-proof chamber (7), and is fastened and connected by a second bolt (9).

6. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 4, characterized in that The invention comprises a first thermocouple (5) and a second thermocouple (13); the first thermocouple insertion port is sealed and fixed with a ferrule; the first thermocouple (5) passes through a first sleeve and a porous air-permeable plug (6) to the upper side of a heating and catalytic chamber (8); the porous air-permeable plug (6) is made of PM-35 material and has a pore size of 35 μm, and is connected to the heating and catalytic chamber (8) by welding; the second thermocouple insertion port is sealed and fixed with a second thermocouple (13) by a ferrule; the second thermocouple (13) passes through a second sleeve to the right side of the heating and catalytic chamber (8).

7. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 2, characterized in that The ammonia decomposition catalyst is cobalt-molybdenum nitride, and the active components are cobalt and molybdenum; the hydrogen permeable membrane (19) is a pure palladium membrane supported by porous alumina, a palladium-silver alloy membrane supported by porous alumina, a palladium-copper alloy membrane supported by porous alumina, a palladium-gold alloy membrane supported by porous alumina, or a palladium-ruthenium alloy membrane supported by porous stainless steel.

8. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 4, characterized in that The porous foam (18) is made of silicon carbide, has a porosity of 85% and a pore density of 40 ppi; the explosion-proof chamber (7), the first flange (3), the second flange (10), the first heating wiring pipe (23), the hydrogen outlet pipe (1), the second heating wiring pipe (11), the air inlet pipe (14) and the sleeve are all provided with an insulating coating.

9. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 4 or 8, characterized in that It comprises a current controller (207), wherein the first heating wire (23) is connected to the negative electrode of a DC power source (206) via a wire, the second heating wire (12) is connected to the current controller (207), and the current controller (207) is connected to the positive electrode of the DC power source (206) via an electric wire.

10. A Joule-heated ammonia decomposition porous foam filled membrane reactor according to claim 9, characterized in that The invention comprises a vacuum pump (201), a hydrogen heat exchanger (202), a tail gas heat exchanger (203), a combustion chamber (204) and a hydrogen storage tank (205); the hydrogen outlet pipe (1) is connected to the vacuum pump (201), the air inlet on the side of the hydrogen heat exchanger (202), the air outlet on the side of the hydrogen heat exchanger (202) and the hydrogen storage tank (205) through a pipeline; the air outlet on the top of the tail gas heat exchanger (203), the air inlet on the bottom of the hydrogen heat exchanger (202), the air outlet on the top of the hydrogen heat exchanger (202) and the air inlet pipe (14) are connected through a pipeline; the tail gas pipe (4) is connected to the air inlet on the side of the tail gas heat exchanger (203), the air outlet on the side of the tail gas heat exchanger (203) and the combustion chamber (204) through a pipeline.

Citation Information

Patent Citations

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  • Preparation method for reaction and separation double-effect dense ceramic membrane reactor for ammonia decomposition hydrogen production

    CN108854928A

  • Ammonia decomposition membrane reactor and application

    CN112919407A

  • High temperature impact heating for thermochemical reactions

    CN115485257A