A Joule-heated porous foam-filled membrane reactor for ammonia decomposition

By combining Joule heating technology with porous foam-filled membrane reactor for ammonia decomposition, the problems of low thermal efficiency and insufficient gas purity of existing devices are solved, and efficient ammonia decomposition and high-purity hydrogen generation are achieved.

CN119455881BActive Publication Date: 2025-09-30ZHEJIANG UNIV OF TECH
View PDF 2 Cites 0 Cited by

Patent Information

Application Number
CN202411613944.6
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2024-11-13
Publication Date
2025-09-30
Estimated Expiration
2044-11-13

AI Technical Summary

Technical Problem

Existing Joule-heated ammonia decomposition devices have problems with low thermal efficiency and insufficient gas purity. The integration of porous foam in the ammonia decomposition membrane reactor makes it difficult to achieve optimal thermal management and gas diffusion control.

Method used

By combining Joule heating technology with a porous foam filling structure, the design cleverly couples ammonia decomposition reaction, hydrogen separation, and heating in the same reactor by integrating Joule heating technology and a porous foam-filled membrane reactor. Silicon carbide porous foam is used as a Joule heating substrate, combined with a palladium membrane and a cobalt-molybdenum nitride catalyst to achieve rapid and uniform heating and efficient hydrogen separation.

Benefits of technology

The efficiency of hydrogen production from ammonia decomposition has been significantly improved, achieving a more efficient and economical ammonia decomposition process, generating high-purity hydrogen, reducing reaction temperature and energy consumption, and improving heat transfer efficiency and gas purity.

✦ Generated by Eureka AI based on patent content.

Smart Images

  • Figure CN119455881B_ABST
    Figure CN119455881B_ABST
Patent Text Reader

Abstract

The present invention discloses a Joule-heated ammonia decomposition porous foam-filled membrane reactor, comprising an explosion-proof chamber. The present invention employs a metal palladium membrane as a hydrogen-permeable membrane and selects cobalt-molybdenum nitride as a high-efficiency catalyst. The catalyst is evenly distributed within a silicon carbide foam, which also serves as a Joule-heated substrate. The two ends of the silicon carbide foam are connected to positive and negative electrodes, respectively, and a voltage is applied to rapidly heat the catalyst bed. During operation, ammonia is first preheated by a heat exchanger before entering the membrane reactor for decomposition, generating a mixed gas of hydrogen, nitrogen, and unreacted ammonia. These gases are separated by a palladium membrane to produce high-purity hydrogen with a purity of up to 99.999%. The device of the present invention integrates the three steps of heating, hydrogen production, and purification, effectively reducing heat loss during the transfer process. Furthermore, the palladium membrane promotes the shift of the chemical reaction equilibrium toward hydrogen production, thereby improving the conversion rate of ammonia decomposition.
Need to check novelty before this filing date? Find Prior Art

Description

Technical Field

[0001] The present 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, with its high energy density and clean properties, is considered a key secondary energy source for achieving a clean, low-carbon, safe, and efficient energy system. Its high calorific value (142 MJ / kg) and zero COx and NOx emissions when used in fuel cells make it an ideal energy carrier. However, hydrogen's volatility and low volumetric energy density require demanding storage and transportation conditions. Storing hydrogen in the form of ammonia and achieving safe and efficient storage and release through ammonia synthesis and decomposition is a promising solution.

[0003] Ammonia, as a hydrogen carrier, offers advantages such as high hydrogen content, high volumetric energy density, low storage and transportation costs, and zero-carbon emission conversion. To improve the conversion rate and lower the reaction temperature for ammonia decomposition, researchers have developed a variety of catalysts and membrane reactor technologies. Ru-based catalysts, in particular, have attracted attention due to their excellent development potential, but they are expensive. While catalyst research has improved the kinetics, thermodynamic limitations and the high-purity hydrogen requirements (above 99.97%) for most applications remain key issues. In addition to catalysts, numerous hydrogen-permeable membrane reactors have been developed for ammonia decomposition. By simultaneously separating hydrogen, they shift the reaction equilibrium toward hydrogen production. In situ hydrogen removal using H2-selective membrane reactors not only shifts the chemical equilibrium toward hydrogen production but also enables high-purity hydrogen separation. However, the high conversion rate of H2-selective membrane reactors does not necessarily translate to high efficiency. For example, even with 100% conversion, energy efficiency can be low. Therefore, to achieve efficient thermochemical conversion, enhanced heat and mass transfer within the membrane reactor is necessary.

[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 electric current passes through the material to heat the material, which can achieve rapid 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 ammonia decomposition reactors can improve the uniformity of catalyst distribution, enhance heat transfer efficiency, and thus improve the efficiency of ammonia decomposition. However, how to effectively integrate porous foam into the 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:

[0008] A Joule-heated ammonia decomposition porous foam-filled membrane reactor comprises an explosion-proof chamber with openings on both left and right ends, a first flange and a second flange being respectively provided on the left and right sides of the explosion-proof chamber, a second sleeve being provided at the end of the second flange, the second sleeve extending into a heating and catalytic chamber through the second flange, the left open end of the second sleeve being located within the heating and catalytic chamber, and the right open end being provided with two openings, one for an air inlet pipe and the other for an insertion port for a second thermocouple, a membrane assembly being provided inside the explosion-proof chamber, the membrane assembly dividing the explosion-proof chamber into two mutually unconnected chambers, the inner chamber being a hydrogen separation chamber and the outer chamber being a heating and catalytic chamber, a hydrogen outlet pipe being provided on the tail wall of the hydrogen separation chamber, a porous foam with a central hole being provided within the heating and catalytic chamber, an ammonia decomposition catalyst being filled in the porous foam, a first sleeve being provided on the upper side of the heating and catalytic chamber to communicate with the outside, the upper side of the first sleeve having two openings, the left opening being a tail pipe and the upper side being an insertion port for a first thermocouple, the first sleeve being connected to the explosion-proof chamber by welding.

[0009] Furthermore, a hydrogen permeable membrane is provided on the outer wall 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 has 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.

[0010] 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.

[0011] 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.

[0012] Furthermore, a first perforated graphite wound gasket is provided between the first flange and the explosion-proof chamber, and is fastened by a first bolt; a second perforated graphite wound gasket is provided between the second flange and the explosion-proof chamber, and is fastened by a second bolt.

[0013] 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 sealing sleeve, the first thermocouple passes through the first sleeve and the porous air plug to the upper side of the heating and catalytic chamber, the porous air plug is made of 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 sealing sleeve, the second thermocouple passes through the second sleeve to the right side of the heating and catalytic chamber.

[0014] 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 on porous alumina, a palladium-silver alloy membrane supported on porous alumina, a palladium-copper alloy membrane supported on porous alumina, a palladium-gold alloy membrane supported on porous alumina, or a palladium-ruthenium alloy membrane supported on porous stainless steel.

[0015] 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.

[0016] Furthermore, it includes a current controller, the first heating wire is connected to the negative pole 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 pole of the DC power supply through an electric wire.

[0017] Furthermore, it includes a vacuum pump, a hydrogen heat exchanger, a tail gas heat exchanger, a combustion chamber and a hydrogen storage tank. 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.

[0018] Compared with the prior art, the beneficial effects of the present invention are as follows:

[0019] 1) This invention uses Joule heating and catalyst-coupled porous foam to couple the ammonia decomposition reaction, hydrogen separation, and heating within the same reactor. This ingenious structural design significantly improves the efficiency of ammonia decomposition and hydrogen production, achieving a more efficient and economical ammonia decomposition process. It is also safe, efficient, and easy to maintain.

[0020] 2) The present invention incorporates Joule heating technology into the ammonia decomposition membrane reactor. Joule heating technology can directly convert electrical energy into thermal energy, achieving rapid and uniform heating inside the reactor;

[0021] 3) The present invention uses porous silicon carbide foam as the Joule heating substrate. It has high thermal conductivity, which means it can conduct heat quickly, thereby achieving more uniform heating and faster response time during the Joule heating process. Its high resistivity means that under the same current, silicon carbide foam can generate more heat. In addition, the disorder of its porous medium greatly enhances the turbulence of the fluid when passing through the heat exchange surface, thereby generating more disturbances and vortices. These fluid dynamic phenomena effectively reduce the thickness of the heat exchange boundary layer, thereby significantly improving the heat transfer coefficient and enhancing the heat transfer efficiency.

[0022] 4) The hydrogen permeable membrane used in the present invention is a palladium membrane, which has excellent thermal stability and pressure resistance, and has extremely high hydrogen selectivity. It can efficiently extract high-purity hydrogen from the gas mixture produced by ammonia decomposition and quickly remove the hydrogen generated by the reaction, promoting the forward progress of the ammonia decomposition reaction, thereby breaking the original thermodynamic equilibrium state, improving the ammonia conversion rate, and reducing the temperature required for the reaction;

[0023] 5) The membrane reactor of this invention uses a metallic palladium membrane as the hydrogen permeable membrane and a cobalt-molybdenum nitride catalyst. The catalyst is evenly distributed within a silicon carbide foam, which also serves as a Joule heating substrate. The two ends of the silicon carbide foam are connected to positive and negative electrodes, respectively. Applying a voltage rapidly heats the catalyst bed. During operation, ammonia is preheated in a heat exchanger before entering the membrane reactor for decomposition, producing a mixture of hydrogen, nitrogen, and unreacted ammonia. These gases are separated by the palladium membrane to produce high-purity hydrogen with a purity of up to 99.99%. BRIEF DESCRIPTION OF THE DRAWINGS

[0024] Figure 1 A schematic structural diagram of a Joule-heated ammonia decomposition porous foam-filled membrane reactor provided by an embodiment of the present invention;

[0025] Figure 2 A diagram of an experimental system of a Joule-heated ammonia decomposition porous foam-filled membrane reactor provided by an embodiment of the present invention;

[0026] Figure: 1, hydrogen outlet pipe; 2, first perforated graphite spiral wound gasket; 3, first flange; 4, tail pipe; 5, first thermocouple; 6, porous vent 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 spiral wound gasket; 16, second conductive copper electrode; 17, membrane module Components; 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. Exhaust gas heat exchanger; 204. Decombustion chamber; 205. Hydrogen storage tank; 206. DC power supply; 207. Current controller; 208. Temperature data collector. DETAILED DESCRIPTION

[0027] The present invention will be further described below with reference to the accompanying drawings, but the scope of protection of the present invention is not limited to the described scope.

[0028] Please refer to Figure 1-2 A Joule-heated ammonia decomposition porous foam-filled membrane reactor includes an explosion-proof chamber 7 with openings on both ends. A first flange 3 and a second flange 10 are respectively provided on the left and right sides of the explosion-proof chamber 7. Furthermore, a first perforated graphite wound gasket 2 is provided between the first flange 3 and the explosion-proof chamber 7, and is fastened by a first bolt 22; a second perforated graphite wound gasket 15 is provided between the second flange 10 and the explosion-proof chamber 7, and is fastened by a second bolt 9.

[0029] 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 its right open end is provided with two openings, one opening is the air inlet pipe 14, and the other opening is the second thermocouple insertion port. 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 the hydrogen separation chamber 20, and the outer side is the 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 a hole in the middle is provided in the heating and catalytic chamber 8. The porous foam 18 is filled with an ammonia decomposition catalyst. The upper side of the heating and catalytic chamber 8 is provided with a first sleeve connected to the outside. The upper side of the first sleeve has two openings, the left opening is the tail pipe 4, and the upper side is the first thermocouple insertion port. The first sleeve is connected to the explosion-proof chamber 7 by welding.

[0030] A hydrogen permeable membrane 19 is provided 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 has a sleeve structure and is connected to the membrane assembly bottom plate 25 by welding. The membrane assembly bottom plate 25 is connected to the first flange 3 by welding.

[0031] A first heating wiring tube 23 is provided on the first flange 3, and 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 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.

[0032] A heating wiring tube 11 is provided on the second flange 10, and 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.

[0033] 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 insertion port is sealed and fixed with a ferrule. The first thermocouple 5 passes through a first sleeve and a porous air plug 6 to the upper side of a 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 exhaust pipe 4.

[0034] 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.

[0035] 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 on porous alumina, a palladium-silver alloy membrane supported on porous alumina, a palladium-copper alloy membrane supported on porous alumina, a palladium-gold alloy membrane supported on porous alumina, or a palladium-ruthenium alloy membrane supported on porous stainless steel.

[0036] 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 an insulating coating.

[0037] 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 via 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 via an electric wire.

[0038] A Joule-heated ammonia decomposition porous foam-filled membrane reactor also includes a vacuum pump 201, a hydrogen heat exchanger 202, an exhaust 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.

[0039] The air outlet at the top of the exhaust 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 heat exchanger 203, the air outlet on the side of the exhaust heat exchanger 203 and the combustion chamber 204 through pipelines.

[0040] The specific operating steps of a Joule-heated ammonia decomposition porous foam-filled membrane reactor for use in ammonia decomposition to produce hydrogen are as follows:

[0041] Start the vacuum pump 201. 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.

[0042] The current controller 207 controls the current of the DC power supply 206 passing through the silicon carbide foam so that the temperature of the gas at the outlet of the heating and catalytic chamber 8 reaches the set temperature (500°C);

[0043] After reaching the set temperature, the nitrogen valve is closed, the hydrogen valve is opened, and hydrogen at 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;

[0044] Close the hydrogen valve and open the ammonia valve. After passing through the exhaust heat exchanger 203 at a flow rate of 400 ml / min, ammonia is exchanged with the exhaust gas, and then passed through the hydrogen heat exchanger 202 to exchange heat with the hydrogen. The preheated ammonia enters the heating and catalytic chamber 8 through the intake pipe, is heated to a suitable operating temperature for ammonia decomposition by the silicon carbide foam, and is completely decomposed into hydrogen and nitrogen under the action of the catalyst.

[0045] Under the action of the pressure difference, hydrogen moves to the surface of the palladium alloy membrane and is adsorbed and dissociated. It then passes through the palladium membrane through the dissolution-diffusion mechanism and 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.

[0046] The remaining gas in the heating and catalytic chamber 8 is discharged from the tail gas pipe 4 to the combustion chamber 204.

[0047] In this embodiment, the porous foam 18 is made of silicon carbide, serving as a Joule heating substrate. It has an outer diameter of 27 mm, an inner diameter of 14 mm, and a thickness of 15 mm. The DC power supply 206 has a rated voltage of 24 V. The porous foam 18 is uniformly filled with Co₃Mo₃N₄g. The membrane assembly is equipped with a single porous alumina-supported pure palladium membrane with a diameter of 12 mm, an average thickness of 18 microns, and an effective length of 25 mm. After ammonia was introduced, the first thermocouple indicated an outlet temperature of 500°C at the heated catalytic chamber. Gas chromatography analysis of the outlet exhaust revealed no ammonia, indicating complete conversion and decomposition of the ammonia. Gas chromatography analysis of the hydrogen obtained after separation via the palladium membrane revealed a purity of 99.999%.

[0048] Heat transfer performance of pure catalyst and silicon carbide porous foam filled catalyst under the same conditions;

[0049] At a furnace temperature of 600°C, using the same tubular heating furnace, quartz tube, gas flow rate (400 ml / min), and catalyst loading (4 g Co3Mo3N), the outlet gas temperature of the porous silicon carbide foam-filled catalyst reached 578.3°C, while that of the pure catalyst was only 533.5°C, a difference of 44.8°C. This significant temperature difference demonstrates that the porous silicon carbide foam, due to its high thermal conductivity and porous structure, provides a larger heat exchange area, enhancing the fluid dynamics effect, thereby achieving more efficient heat transfer and shortening the thermal response time. This not only improves hydrogen production efficiency, but also helps reduce energy consumption and carbon emissions, which is of great significance for 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 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 an insertion port for a second thermocouple, characterized in that The explosion-proof chamber (7) is provided with a membrane assembly (17) inside, and the membrane assembly (17) divides the explosion-proof chamber (7) into two chambers that are not connected to each other, the inner chamber is a hydrogen separation chamber (20), and the outer chamber 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 a hole in the middle is provided in the heating and catalytic chamber (8). 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). The upper side of the first sleeve has two openings, the left opening is a tail pipe (4), and the upper side is a hot first electric couple insertion port. The first sleeve is connected to the explosion-proof chamber (7) by welding. The outer wall 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), 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. The membrane assembly bottom plate (25) is connected to the first flange (3) by welding. 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 tightly connected, and the first conductive copper electrode (21) and the first flange (3) are connected by welding; A second 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); The porous foam (18) is made of silicon carbide, has a porosity of 85% and a pore density of 40 ppi; 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 are all provided with an insulating coating.

2. 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 provided between the first flange (3) and the explosion-proof chamber (7), and is fastened by a first bolt (22); a second perforated graphite wound gasket (15) is provided between the second flange (10) and the explosion-proof chamber (7), and is fastened by a second bolt (9).

3. The Joule-heated ammonia decomposition porous foam-filled membrane reactor according to claim 1, characterized in that The invention comprises a first thermocouple (5) and a second thermocouple (13), wherein the first thermocouple insertion port is sealed and fixed with the first thermocouple (5) by a ferrule, and 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), wherein 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; and the second thermocouple insertion port is sealed and fixed with the second thermocouple (13) by a ferrule, and the second thermocouple (13) passes through a second sleeve to the right side of the heating and catalytic chamber (8).

4. The Joule-heated ammonia decomposition porous foam-filled membrane reactor according to claim 1, 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.

5. The Joule-heating ammonia decomposition porous foam-filled membrane reactor according to claim 1, characterized in that The device comprises a current controller (207), wherein the first heating wire (24) is connected to the negative electrode of the DC power supply (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 supply (206) via an electric wire.

6. The Joule-heating ammonia decomposition porous foam-filled membrane reactor according to claim 5, 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), wherein 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 at 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; and 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

  • A method and device for treating formaldehyde in air through catalytic oxidation

    CN107096380A

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

    CN108854928A