CN213475418U - Hydrogen purification device - Google Patents
Hydrogen purification device Download PDFInfo
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- CN213475418U CN213475418U CN202021222574.0U CN202021222574U CN213475418U CN 213475418 U CN213475418 U CN 213475418U CN 202021222574 U CN202021222574 U CN 202021222574U CN 213475418 U CN213475418 U CN 213475418U
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Abstract
The utility model provides a hydrogen purification device, which comprises a catalytic reactor, wherein the catalytic reactor comprises a combustion layer and a selective oxidation layer adjacent to the combustion layer; the combustion layer is provided with a catalytic combustion catalyst, and the selective oxidation layer is provided with a carbon monoxide selective oxidation catalyst; the combustion layer is provided with a fuel inlet and a combustion layer oxidizing gas inlet; the selective oxidation layer is provided with a hydrogen inlet, a selective oxidation layer oxidation gas inlet and a hydrogen outlet. The utility model discloses still provide the method of using above-mentioned hydrogen purification device purification hydrogen. The utility model discloses a hydrogen purification device compact structure, hydrogen purification efficiency/volume ratio is high, can regard as the hydrogen normal position purification device at the hydrogen point of application-as on-vehicle hydrogen purification device, domestic fuel cell Cogeneration of Heat and Power (CHP) hydrogen purification device or hydrogenation station hydrogen purification device, allows to use hydrogen fuel in a flexible way, can reduce the operation cost, improves fuel cell power system's reliability and efficiency to supply power in succession for a long time.
Description
Technical Field
The utility model relates to a hydrogen purification field, concretely relates to small-size low grade hydrogen normal position purification device.
Background
The hydrogen energy can utilize various primary energy sources to cleanly and efficiently generate electric energy and heat energy, and is a key solution of 21 st century energy sources. Hydrogen energy has zero emission energy conversion and power generation characteristics and is currently being designed for a range of application scenarios including automotive, stationary power supplies, aerospace, and consumer electronics. Future development goals of hydrogen energy and fuel cells include: (1) the cost is reduced; (2) flexibility in fuel supply is achieved; (3) the system is efficiently integrated; (4) has excellent reliability and durability; (5) strengthening the foundation construction; (6) understanding and complying with governmental legal regulations regarding fuel cell site selection, insurance and certification.
Hydrogen energy is not a primary energy source like coal and natural gas, but an energy carrier, which is produced by existing energy systems based on different conventional primary energy sources. In the long term, renewable energy will become the most important source of hydrogen energy production. The combination of regenerating hydrogen, producing hydrogen from nuclear energy, and producing hydrogen from fossil-powered energy conversion systems coupled with the capture and safe sequestration of carbon dioxide emissions is an almost completely carbon-free hydrogen production route. Currently, hydrogen produced in various hydrogen production modes contains impurities mainly of carbon monoxide (CO) and possibly trace amounts of sulfides (mainly H)2S), carbon dioxide, hydrocarbons, inert gases, particulates, water, and oxygen.
CO is H2One of the most prominent impurities in Proton Exchange Membrane Fuel Cell (PEMFC) applications is that it blocks the active sites in the Pt catalyst and poisons the fuel cell catalyst. Studies suggest that H for PEMFC2The CO content should be less than 10 ppm. SAE J-2719 and ISO/PDTS 14687-2 define a minimum purity of "fuel cell grade hydrogen" of 99.99% (99.97% if helium is considered), allowing less than 100ppm total impurities, including less than 5ppm (typically 1-3ppm) oxygen, less than 5ppm (typically 1-3ppm) water, and less than 100ppb CO. For producing H2The outlet CO concentration of the Water Gas Shift (WGS) reactor is 0.1-1.0%, and the Pressure Swing Adsorption (PSA) technology can reach most of H proposed by SAE/ISO2Impurities standard, but may be H2The cost is increased by 20%. Realization of H2Medium and ultra low CO concentration vs. H2Production proposes to be heavyThe great challenge, resulting in the high cost of "fuel cell grade hydrogen", has been identified as one of the obstacles in the practical application of fuel cells.
At present, the hydrogen purification technology is mainly divided into physical purification technology and chemical purification technology. The physical purification technique is to utilize H2And impurities, including: pressure Swing Adsorption (PSA) method, which removes impurities using an adsorbent; high Temperature Diffusion (HTD) method uses metal films to produce High purity H2But the cost is higher; low Temperature Diffusion (LTD) diffuses hydrogen gas through a polymer membrane to produce high purity H2(ii) a Solvent absorption processes separate CO and CO at high pressure and low temperature2Dissolving in solvent to obtain pure H2In the gas phase. These physical purification techniques are well established, require complex and cumbersome designs, and have low power to weight ratios suitable for large scale hydrogen purification, but are not suitable for small scale hydrogen purification at the point of hydrogen use. Chemical purification techniques remove impurities from low grade hydrogen by chemical oxidation reactions, including: low Temperature Shift (LTS) technology, typically used in industrial scale hydrogen production processes, must be very large in size and weight to achieve significant conversion due to the relatively slow reaction rate; selective oxidation (PROX) uses a small amount of oxygen to selectively oxidize CO while consuming a minimal amount of H2The reaction is fast, has the greatest application potential through proper reactor design and proper temperature control, and can remarkably reduce the overall weight of the system and the cost. Selective oxidation of carbon monoxide is a multistep process, generally following the Langmuir-Hinshelwood kinetics for CO and O2Single site competition mechanism between: in the first step, CO is chemisorbed on a Pt surface, while an oxygen molecule must be adsorbed in the vicinity of the Pt surface site, the O-O bond is cleaved, and the oxygen atom reacts with the surface activated CO molecule to form carbon dioxide.
The chemical composition of the hydrogen sold in the market at present has large difference, and low-grade hydrogen (CO concentration is more than 10ppm) cannot be directly used for the PEMFC. In addition, due to the vehicleThe hydrogen fuel for the fuel cell needs to be filled at the hydrogen refueling station, which means that the hydrogen fuel for the vehicle fuel cell needs to be transported from the hydrogen production/purification plant to the hydrogen refueling station, during which it is possible for H to be supplied2Causing contamination and thus even for hydrogen that has a factory purity that meets PFMFC usage requirements, the purity may no longer meet PFMFC usage requirements when the hydrogen station is filled onto a vehicle.
SUMMERY OF THE UTILITY MODEL
The utility model aims at providing a can be high carry out high-efficient purification hydrogen's compact hydrogen purification device at the application point.
The technical scheme is as follows: the utility model provides a hydrogen purification device, which comprises a catalytic reactor and a controller, wherein the catalytic reactor comprises a combustion layer and a selective oxidation layer adjacent to the combustion layer; the combustion layer is provided with a fuel inlet and a combustion layer oxidizing gas inlet; the selective oxidation layer is provided with a hydrogen inlet, a selective oxidation layer oxidation gas inlet and a hydrogen outlet; the fuel inlet and the hydrogen inlet are respectively connected with a flow regulator, and the hydrogen inlet is also connected with a hydrogen purity sensor; a temperature sensor is arranged between the combustion layer and the selective oxidation layer; the flow regulator, the hydrogen purity sensor and the temperature sensor are respectively connected with the controller. The utility model directly integrates the heat source generating part which provides heat for selective oxidation into the hydrogen purification device, but not arranged outside the purification device and then transmitted into the hydrogen purification device through the heat conducting part or the heat conducting fluid, thereby greatly improving the energy utilization rate, simultaneously reducing the volume of the hydrogen purification device to the maximum extent and improving the hydrogen purification efficiency; the combustion layer and the selective oxidation layer are arranged to be layered, and the selective oxidation layer is stacked on one side or two sides of the combustion layer, so that heat generated by catalytic combustion in the combustion layer can be efficiently transferred to the selective oxidation layer, the volume of the hydrogen purification device is further reduced, and the reaction temperature of the selective oxidation layer is efficiently controlled.
Preferably, the selective oxidation layer is arranged on two sides of the combustion layer or the combustion layer is arranged on one side or two sides of the selective oxidation layer; the combustion layer comprises a fuel distribution layer and an oxidation gas distribution layer, the oxidation gas distribution layer is arranged on two sides of the fuel distribution layer, or the fuel distribution layer is arranged on one side or two sides of the oxidation gas distribution layer; the oxidizing gas distribution layer and the fuel distribution layer are communicated through the porous plate. The structural design can promote the fuel and the oxidizing gas to be mixed in the combustion layer timely and fully, and the release of heat in the combustion layer is controlled conveniently by the mixing of the fuel and the oxidizing gas, so that the temperature control accuracy of the hydrogen purification device is improved.
The hydrogen purification device also comprises a hydrogen supply pipeline and an oxidizing gas supply pipeline; the fuel inlet and the hydrogen inlet are respectively connected with a hydrogen supply pipeline; the combustion layer oxidizing gas inlet and the selective oxidation layer oxidizing gas inlet are respectively connected with an oxidizing gas supply pipeline; the oxidizing gas supply line supplies air or oxygen.
Specifically, the combustion layer is provided with a catalytic combustion catalyst, and the selective oxidation layer is provided with a carbon monoxide selective oxidation catalyst and a sulfur-resistant catalyst; the catalytic combustion catalyst can be a catalyst which can catalyze fuel (such as hydrogen) to perform catalytic combustion, and preferably, the catalytic combustion catalyst comprises an alumina carrier and Pt/Pd supported on the alumina carrier; the carbon monoxide selective oxidation catalyst may be an existing catalyst that selectively catalyzes the oxidation of carbon monoxide, and preferably, the carbon monoxide selective oxidation catalyst comprises gamma-Al2O3Carrier and supported on gamma-Al2O3The core-shell structure nano-particle catalyst is a metal M with a platinum monolayer covered on the surface, and the metal M is one or more of Ru, Rh, Ir and Pd; existing sulfur tolerant catalysts may be used.
In order to further accurately control the reaction temperature of the selective oxidation of carbon monoxide in the selective oxidation layer, the combustion layer oxidation gas inlet and the selective oxidation layer oxidation gas inlet are respectively connected with a flow regulator, and the flow regulators are connected with a controller.
The hydrogen purity sensor can use the existing device which can detect and send a hydrogen concentration signal; preferably, the hydrogen purity sensor is a hydrogen purity sensor based on solid oxide fuel cell, surface plasmon resonance, bragg fiber, palladium-plated thin film micromirror, palladium-plated tapered fiber, or low temperature electrochemical cell technology.
The hydrogen purification device can be arranged to comprise one or more than two catalytic reactors according to the amount of hydrogen required to be purified, and the two or more than two catalytic reactors can be arranged in a stacking mode or other integrated modes.
The combustion layer and the selective oxidation layer are stacked together to form a layered structure, and specific dimensions can be specifically set according to the scale of hydrogen purification.
The utility model discloses a hydrogen purification device's theory of operation is: the carbon monoxide selective oxidation reaction is an endothermic process during the light-off phase; in addition, although the selective oxidation of carbon monoxide is an exothermic reaction in the normal reaction process, the heat released by the selective oxidation of carbon monoxide in the hydrogen purification process is not enough to support the reaction to continue, and therefore, the selective oxidation of carbon monoxide in the hydrogen purification process requires external heat supply. When the hydrogen purification device works, fuel and oxidizing gas are supplied to the combustion layer, catalytic combustion is carried out under the action of the catalytic combustion catalyst, and heat is released; the heat emitted by the combustion layer is transferred to the selective oxidation layer stacked together with the combustion layer, so that heat is provided for the selective oxidation reaction of carbon monoxide in the selective oxidation layer; a temperature sensor is arranged between the combustion layer and the selective oxidation layer, and the temperature sensor sends temperature information between the combustion layer and the selective oxidation layer to the controller; supplying hydrogen to be purified to the selective oxidation layer, detecting the purity of the hydrogen entering a hydrogen supply pipeline by a hydrogen purity sensor, and sending hydrogen purity information to a controller; the controller controls the flow of fuel and oxidizing gas into the combustion layer according to the temperature and hydrogen purity information, thereby precisely controlling the reaction temperature of the selective oxidation layer.
Has the advantages that: the utility model discloses a hydrogen purification device compact structure, hydrogen purification efficiency/volume ratio are high, can regard as the hydrogen normal position purification device at hydrogen application point-as on-vehicle hydrogen purification device, domestic fuel cell Cogeneration of Heat and Power (CHP) hydrogen purification device or hydrogen station hydrogen purification devicePurification device capable of detecting and selectively oxidizing low-grade H at the point of application of hydrogen2Of (1) is described. The utility model discloses a hydrogen purification device and method allow the nimble hydrogen fuel that uses, reduce the operation cost, improve fuel cell power system's reliability and efficiency to supply power for a long time in succession.
Drawings
Fig. 1 is a schematic structural diagram of the hydrogen purification apparatus of the present invention.
Wherein the reference numerals are as follows:
1-a catalytic reactor; 2-a controller; 3-a hydrogen supply line; 4-an oxidizing gas supply line; 5-a combustion layer; 6-a selective oxidation layer; 7-a thermocouple; 8-a fuel distribution layer; 9-an oxidizing gas distribution layer; 10-a fuel inlet; 11-combustion layer oxidizing gas inlet; 12-a hydrogen inlet; 13-a selective oxidation layer oxidation gas inlet; 14-a hydrogen outlet; 15-hydrogen output line; 16-hydrogen purity sensor; 17-a first flow regulator; 18-a second flow regulator; 19-third flow regulator.
The arrows in fig. 1 indicate the direction of fluid flow/diffusion or signal transmission.
Detailed Description
The following detailed description presents certain specific details for the purpose of understanding the invention. However, it will be understood by those skilled in the art that the present invention may be practiced without these specific details. It should be noted that, for ease of understanding, the dimensions of the various parts shown in the drawings are not drawn to scale. Techniques known to those skilled in the art may not be described in detail herein, but should be considered part of the specification.
As shown in fig. 1, a hydrogen purification apparatus includes a catalytic reactor 1, a controller 2, a hydrogen supply line 3, and an oxidizing gas supply line 4. The catalytic reactor 1 comprises a combustion layer 5 and selective oxidation layers 6 stacked on two sides of the combustion layer, wherein a thermocouple 7 is arranged between the combustion layer 5 and the selective oxidation layers 6 and used for detecting reaction temperature and sending temperature information to the controller 2. A catalytic combustion catalyst is provided in the combustion layer 5. The combustion layer 5 comprises a fuel distribution layer 8 and an oxidizing gas distribution layer 9 which are stacked together and communicated through a porous plate, the oxidizing gas distribution layer 9 is arranged on two sides of the fuel distribution layer 8, the fuel distribution layer 8 is provided with a fuel inlet 10, the fuel inlet 10 is connected with the hydrogen supply pipeline 3, the oxidizing gas distribution layer 9 is provided with a combustion layer oxidizing gas inlet 11, the combustion layer oxidizing gas inlet 11 is connected with the oxidizing gas supply pipeline 4, and air or oxygen is supplied into the oxidizing gas supply pipeline 4. A carbon monoxide selective oxidation catalyst and a sulfur-resistant catalyst are provided in the selective oxidation layer 6. The selective oxidation layer 6 is provided with a hydrogen inlet 12, a selective oxidation layer oxidation gas inlet 13 and a hydrogen outlet 14, the hydrogen inlet is connected with the hydrogen supply pipeline 3, the selective oxidation layer oxidation gas inlet 13 is connected with the oxidation gas supply pipeline 4, and the hydrogen outlet 14 is connected with the hydrogen output pipeline 15. The hydrogen supply pipeline 3 is provided with a hydrogen purity sensor 16 and a first flow regulator 17, and the hydrogen purity sensor 16 is used for detecting the purity of the hydrogen entering the hydrogen purification device and sending the purity information to the controller 2; the first flow regulator 17 is configured to receive a command from the controller to control the flow rate of hydrogen. The combustion layer oxidizing gas inlet 11 is connected to a second flow regulator 18, and the selective oxidation layer oxidizing gas inlet 13 is connected to a third flow regulator 19. The second flow regulator 18 and the third flow regulator 19 are configured to receive instructions from the controller 2 and control the flow rate of the oxidizing gas.
It should be noted that, although fig. 1 shows that the hydrogen purification apparatus includes only one catalytic reactor, when the flow rate of hydrogen to be purified is large, more than two catalytic reactors may be disposed in the hydrogen purification apparatus, and different catalytic reactors may be integrated in a layer-by-layer stacking manner to reduce the volume of the overall hydrogen purification apparatus. Although fig. 1 shows the hydrogen purification apparatus in which the combustion layer is also connected to the hydrogen supply line, the combustion layer is not necessarily connected to the hydrogen supply line, but may be connected to other fuel supply lines, since the hydrogen supplied to the combustion layer is only supplied for catalytic combustion to supply heat for the selective oxidation reaction of carbon monoxide in the selective oxidation layer. In addition, although fig. 1 shows the connection positions of the combustion layer and the hydrogen supply line and the oxidizing gas supply line and the connection positions of the selective oxidation layer and the hydrogen supply line and the oxidizing gas supply line in the hydrogen purification apparatus are located on the same side, these connection positions may not be located on the same side. Although fig. 1 shows the selective oxidation layer disposed on both sides of the combustion layer including the fuel distribution layer and the oxidation gas distribution layer disposed on both sides of the fuel distribution layer, it is also possible to dispose the combustion layer on one side or both sides of the selective oxidation layer, the combustion layer not being divided into the fuel distribution layer and the oxidation gas distribution layer, or the fuel distribution layer being disposed on one side or both sides of the oxidation gas distribution layer.
The method for purifying hydrogen using the above hydrogen purification apparatus comprises the steps of:
the fuel and the oxidizing gas enter the combustion layer 5, and the fuel and the oxidizing gas are subjected to catalytic combustion under the action of a catalytic combustion catalyst; the thermocouple 7 is enabled to detect the temperature between the combustion layer 5 and the selective oxidation layer 6 and send temperature information to the controller 2;
passing the hydrogen to be purified into the selective oxidation layer 6; the hydrogen purity sensor 16 detects the concentration of hydrogen to be purified and sends the hydrogen purity information to the controller 2;
the controller 2 judges whether the reaction in the selective oxidation layer 6 is in the optimum temperature range or not according to the temperature information and the hydrogen purity information, and when the controller 2 judges that the reaction temperature in the selective oxidation layer 6 is lower than the optimum temperature, the flow of fuel and/or oxidizing gas entering the combustion layer 5 is increased by controlling the flow regulator, or the flow of hydrogen to be purified entering the selective oxidation layer 6 is reduced;
when the controller 2 judges that the reaction temperature in the selective oxidation layer 6 is higher than the optimum temperature, the flow rate of the fuel and/or the oxidizing gas into the combustion layer 5 is reduced by controlling the flow rate regulator, or the flow rate of the hydrogen gas to be purified into the selective oxidation layer 6 is increased.
The utility model discloses a hydrogen purification device can purify CO concentration and be 5ppm ~ 5000 ppm's hydrogen, makes CO concentration reduce in the hydrogen below 5ppm, because PEMFC is 10ppm to the sensitive lower limit of CO, consequently, uses the utility model discloses a hydrogen purification device can satisfy the purity requirement of PEMFC with hydrogen completely.
Claims (6)
1. A hydrogen purification apparatus comprising a catalytic reactor and a controller, the catalytic reactor comprising a combustion layer and a selectively oxidized layer adjacent to the combustion layer; the combustion layer is provided with a fuel inlet and a combustion layer oxidizing gas inlet; the selective oxidation layer is provided with a hydrogen inlet, a selective oxidation layer oxidation gas inlet and a hydrogen outlet; the fuel inlet and the hydrogen inlet are respectively connected with a flow regulator, and the hydrogen inlet is also connected with a hydrogen purity sensor; a temperature sensor is arranged between the combustion layer and the selective oxidation layer; the flow regulator, the hydrogen purity sensor and the temperature sensor are respectively connected with the controller.
2. The hydrogen purification apparatus according to claim 1, wherein the selectively oxidizing layer is provided on both sides of the combustion layer or the combustion layer is provided on one side or both sides of the selectively oxidizing layer; the combustion layer comprises a fuel distribution layer and an oxidation gas distribution layer, the oxidation gas distribution layer being disposed on either side of the fuel distribution layer, or the fuel distribution layer being disposed on one or both sides of the oxidation gas distribution layer; the oxidizing gas distribution layer and the fuel distribution layer are communicated through a porous plate.
3. The hydrogen purification apparatus according to claim 1, further comprising a hydrogen supply line and an oxidizing gas supply line; the fuel inlet and the hydrogen inlet are respectively connected with the hydrogen supply pipeline; the combustion layer oxidizing gas inlet and the selective oxidation layer oxidizing gas inlet are respectively connected with the oxidizing gas supply pipeline; the oxidizing gas supply line is supplied with air or oxygen.
4. The hydrogen purification apparatus according to claim 1, wherein the combustion layer oxidizing gas inlet and the selective oxidation layer oxidizing gas inlet are respectively connected with a flow regulator; the flow regulator is connected with the controller.
5. The hydrogen purification apparatus according to claim 4, wherein the hydrogen purity sensor is a hydrogen purity sensor based on solid oxide fuel cell, surface plasmon resonance, Bragg fiber, palladium-plated thin film micro-mirror, palladium-plated tapered fiber, or low temperature electrochemical cell technology.
6. The hydrogen purification apparatus according to claim 1, comprising one or more catalytic reactors; the one or more catalytic reactors are stacked on top of each other.
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| CN202021222574.0U CN213475418U (en) | 2020-06-28 | 2020-06-28 | Hydrogen purification device |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113666337A (en) * | 2021-07-30 | 2021-11-19 | 清华大学 | Non-pure hydrogen sectional purification treatment method and device for fuel cell |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113666337A (en) * | 2021-07-30 | 2021-11-19 | 清华大学 | Non-pure hydrogen sectional purification treatment method and device for fuel cell |
| CN113666337B (en) * | 2021-07-30 | 2023-08-15 | 清华大学 | Method and device for purifying non-pure hydrogen in segments for fuel cell |
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Effective date of registration: 20221125 Address after: 512029 Building 42, Huangshaping Innovation Park, Guanshaocheng Phase I, Shaoguan, Guangdong Patentee after: Guangdong Carbon Neutralization Research Institute (Shaoguan) Address before: 017200 5th floor, building a, entrepreneurship building, aletengxire Town, ejinholo banner, Ordos City, Inner Mongolia Autonomous Region Patentee before: Ordos Guoke Energy Co.,Ltd. |