CN109650336B - Hydrogen purification system in on-site hydrogen production fuel cell device - Google Patents
Hydrogen purification system in on-site hydrogen production fuel cell device Download PDFInfo
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- CN109650336B CN109650336B CN201910120994.3A CN201910120994A CN109650336B CN 109650336 B CN109650336 B CN 109650336B CN 201910120994 A CN201910120994 A CN 201910120994A CN 109650336 B CN109650336 B CN 109650336B
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- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/501—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion
- C01B3/503—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion characterised by the membrane
- C01B3/505—Membranes containing palladium
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/06—Integration with other chemical processes
- C01B2203/066—Integration with other chemical processes with fuel cells
- C01B2203/067—Integration with other chemical processes with fuel cells the reforming process taking place in the fuel cell
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
The invention relates to a hydrogen purification system in a fuel cell device for on-site hydrogen production, which mainly comprises a heat exchanger, an electric heating device, a palladium membrane purification assembly, a starting power supply, a vacuum pump, an on-site hydrogen production unit, a combustion chamber and a hydrogen fuel cell unit. Under the condition of on-site hydrogen production without commercial power, the environmental temperature of the palladium membrane is accurately controlled by combining a chemical power supply and the power supply of a hydrogen fuel cell, and the stability of a hydrogen purification system is improved. The special structural design of the hydrogen purification system, especially the structural design of the heat exchanger, reduces the heat loss of the electric heating device, reduces the operation energy consumption of the hydrogen purification system, and improves the external power generation efficiency of the hydrogen fuel cell unit in the field hydrogen production fuel cell device.
Description
Technical Field
The invention belongs to the field of gas purification, relates to a hydrogen purification system, and particularly relates to a hydrogen purification system in a fuel cell device for on-site hydrogen production.
Background
As the most promising clean energy, hydrogen energy plays an increasing role in the fields of transportation, communication, military, aerospace, and the like. The application of hydrogen energy does not leave links such as hydrogen production, separation and purification of hydrogen, hydrogen storage, hydrogen transportation and the like. The preparation method of the hydrogen mainly comprises water electrolysis and organic matter cracking, steam reforming, coal hydrogen production and the like, except for the water electrolysis hydrogen production method, the concentration of the hydrogen prepared by other conventional hydrogen production methods is generally not more than 80%, and separation and purification are required to meet further application. Common hydrogen separation methods include cryogenic methods, pressure swing adsorption methods, membrane separation methods, and the like. The membrane separation method has the outstanding advantages of small volume and simple and convenient operation, and particularly meets the requirements of hydrogen energy on hydrogen sources. Palladium and its alloy membranes (hereinafter simply referred to as palladium membranes) are the membrane materials that were first applied to hydrogen purification, and have good hydrogen permeability and high temperature stability. Hydrogen is dissolved in metal palladium or palladium alloy to form hydride, and hydrogen is easily subjected to hydrogen embrittlement effect when the metal is dissolved too much, namely, the metal absorbs hydrogen to expand to generate lattice distortion, so that the film becomes brittle and cracks; on the other hand, if the operating temperature is too high, voids are generated in the membrane due to the high-temperature sintering effect between the crystal grains of the palladium membrane, or the membrane is broken due to sintering stress. Therefore, in order to ensure that the palladium membrane can be better applied to a hydrogen purification system, a stable palladium membrane ambient temperature must be provided.
The optimum working temperature for palladium membranes is generally in the range from 350 to 500 ℃. Commonly used methods for heating palladium membranes are typically combustion heating [ Warward, doffman, sunjing. Instant Hydrogen production and Power Generation System and method CN103618100B ] and electric heating [ Hani W.Abu El Hawa, sean-Thomas B.Lundin, neil S.Patki, J.Douglas way.Steam methyl reforming in a Pd-Au membrane reactor: long-term assessment.int.J.hydrogen Energy,2016 10193-10201 ]. The combustion heating can be divided into direct combustion heating and heat conducting medium heating [ Wu Fei, fan Jing, zhouyangning, etc. ] according to the heating mode, a heating system for methanol reforming hydrogen production reaction CN105967144A ]. However, the direct combustion heating has the problems of large temperature fluctuation and local temperature unevenness, so the direct combustion heating can be used in the occasions with low sensitivity to temperature fluctuation, but is not suitable for heating the palladium membrane; if the heat-conducting medium is used for heating the palladium membrane, the working temperature of the palladium membrane is generally 350-500 ℃, and a high-temperature molten salt medium (such as common potassium nitrate molten salt) is required for heating, the uniformity of the molten salt and the temperature distribution of the system is improved through a high-temperature molten salt circulating pump, so that the system is complex and high in manufacturing cost, regular inspection is required in the operation process to prevent molten salt leakage, and certain potential safety hazards exist. The electric heating has the advantages of simple operation and accurate temperature control, but in the field of on-site hydrogen production, particularly when the power supply of a power grid is lacked, the electric heating mode is usually abandoned due to high power consumption. If the electric energy output by the fuel cell is directly applied to supply power to the heating device, the electric energy generated by the fuel cell can be greatly consumed due to the problem of self power consumption when the electric heating device operates, and the external output power of the field hydrogen production fuel cell device is reduced; the fuel generator is adopted to provide power, so that the original purpose of hydrogen power generation is completely violated, and the problems of noise pollution and emission pollution exist.
Therefore, a stable and reliable hydrogen purification system with low energy consumption is urgently needed to be designed for the field hydrogen production fuel cell device which is separated from the power grid.
Disclosure of Invention
The invention aims to provide a stable and reliable hydrogen purification system in a fuel cell device for on-site hydrogen production, and improve the overall operation stability of the fuel cell device for on-site hydrogen production.
The invention adopts the specific technical scheme that: a hydrogen purification system in a fuel cell device for on-site hydrogen production mainly comprises a heat exchanger, an electric heating device, a palladium membrane purification assembly, a starting power supply, a vacuum pump, an on-site hydrogen production unit, a combustion chamber and a hydrogen fuel cell unit.
The heat exchanger is used for recovering the heat of the pure hydrogen after the palladium membrane separation and preheating the hydrogen production raw material, the center of the heat exchanger is provided with a hole for placing an electric heating device, the heat source of the heat exchanger is the high-purity hydrogen after the palladium membrane separation, and the cold source of the heat exchanger is the hydrogen production raw material.
The electric heating device is an electric heating belt, an electric heating sleeve or an electric heating furnace containing a heat-insulating layer, the electric heating device is used for heating the palladium membrane, and the electric heating device is placed in the central hole of the heat exchanger after wrapping the palladium membrane. By utilizing the heat of the heat source of the heat exchanger, the external environment temperature of the heat insulation layer of the electric heating device is improved, and the heat loss in the heating and heat insulation processes of the electric heating device is reduced, so that the energy consumption of the electric heating device is reduced, and the fuel cell is promoted to output more electric energy to the outside. The lower the thermal conductivity coefficient of the thermal insulation material of the thermal insulation layer of the electric heating device is, and the thicker the thermal insulation layer is, the more ideal the thermal insulation effect is, and the lower the power consumption is in stable operation.
The palladium membrane is a palladium membrane or a palladium alloy membrane packaged in advance, mixed hydrogen output by the on-site hydrogen production unit is taken as a separation raw material, hydrogen-containing tail gas separated by the palladium membrane enters a combustion chamber for combustion to provide heat required by reaction for the on-site hydrogen production unit, and high-purity hydrogen separated by the palladium membrane enters a heat exchanger to exchange heat with the hydrogen production raw material, so that the energy efficiency of the whole device is improved; the working temperature of the palladium membrane is 300-500 ℃.
The starting power supply is a chemical power supply capable of being charged and discharged for multiple times, and is used as a working power supply of the hydrogen purification system when the hydrogen fuel cell unit does not output electric energy. The power storage quantity of the starting power supply needs to meet the power consumption quantity before the hydrogen production fuel cell device on site stably outputs electric energy. When the hydrogen fuel cell unit in the on-site hydrogen production fuel device stably outputs electric energy, the unit charges the starting power supply and maintains the full-power state of the starting power supply.
The vacuum pump is used for vacuumizing a system pipeline when the hydrogen purification system starts to work and finishes working.
The on-site hydrogen production unit is used for preparing mixed hydrogen by reacting hydrogen production raw materials.
The combustion chamber is used for combusting hydrogen-containing tail gas after palladium membrane separation.
The hydrogen fuel cell unit is used for outputting electric energy to the outside and supplying power to the electric heating device and the starting power supply.
A hydrogen purification system in an on-site hydrogen production fuel cell device comprises the following specific operation steps:
a. when the hydrogen purification system starts to work, a vacuum pump is started firstly, and a system pipeline is vacuumized;
b. heating the palladium membrane by an electric heating device until the temperature of the palladium membrane rises to the working temperature and the on-site hydrogen production unit reaches the hydrogen production condition;
c. hydrogen production raw materials flow through a heat exchanger and an on-site hydrogen production unit in sequence, and then are converted into mixed hydrogen to enter a palladium membrane through reaction;
d. hydrogen-containing tail gas separated by the palladium membrane enters a combustion chamber for combustion to provide a heat source for the on-site hydrogen production unit;
e. the high-purity hydrogen separated by the palladium membrane firstly enters a heat exchanger to exchange heat with a hydrogen production raw material of the on-site hydrogen production unit to recover energy, then enters a hydrogen fuel cell unit, is externally output with electric energy by the hydrogen fuel cell unit, and supplies power to an electric heating device and a starting power supply;
f. when the hydrogen purification system finishes working, firstly starting a vacuum pump to vacuumize a system pipeline, then closing an electric heating device, and naturally cooling to room temperature.
Compared with the prior art, the invention has the innovation points that: 1. under the condition of no commercial power, the method ingeniously combines a chemical power supply with the power supply of a hydrogen fuel cell, realizes the accurate control of the environmental temperature of the palladium membrane, optimizes the working environment of the palladium membrane, prolongs the service life of the palladium membrane and is beneficial to the commercial application of the palladium membrane; 2. through the design of a unique hydrogen purification system, particularly the structural design of a heat exchanger therein, the heat loss of an electric heating device is reduced, the operation energy consumption of the hydrogen purification system is reduced, and the external electric energy output efficiency of the field hydrogen production fuel cell device is improved.
Has the advantages that: the hydrogen purification system provided by the invention can enable the ideal working environment of the palladium membrane to be free from the restriction of commercial power, prolong the service life of the palladium membrane, reduce the practical application difficulty of the palladium membrane, improve the stability of the hydrogen purification system, and further improve the overall operation stability of the on-site hydrogen production fuel cell device, and the unique structural design of the hydrogen purification system promotes the energy consumption of the overall device to be reduced.
The invention is described in detail below with reference to the figures and specific embodiments. It is intended that the scope of the invention be limited not by this detailed description, but rather by the claims appended hereto.
Drawings
FIG. 1 is a schematic diagram of a hydrogen purification system in an on-site hydrogen production fuel cell device.
Fig. 2 is a schematic diagram of a heat exchanger.
FIG. 3 is a schematic diagram of the electrical energy transfer of a hydrogen purification system in an on-site hydrogen production fuel cell device.
Detailed Description
Example 1
Fig. 1 is a schematic diagram showing a hydrogen purification system in an on-site hydrogen production fuel cell device. A hydrogen purification system in a fuel cell device for on-site hydrogen production specifically comprises a heat exchanger 1, an electric heating device 2, a palladium membrane 3, a starting power supply 4, a vacuum pump 5, an on-site hydrogen production unit 6, a combustion chamber 7 and a hydrogen fuel cell unit 8.
The specific operation steps of a hydrogen purification system in an on-site hydrogen production fuel cell device are as follows:
a. when the hydrogen purification system starts to work, the vacuum pump 5 is started firstly, and the system pipeline is vacuumized;
b. heating the palladium membrane 3 by the electric heating device 2, and after the temperature of the palladium membrane 3 rises to a proper temperature, enabling the on-site hydrogen production unit to reach a hydrogen production condition;
c. after the hydrogen production raw material sequentially flows through the heat exchanger 1 and the on-site hydrogen production unit 6, the hydrogen production raw material is converted into mixed hydrogen through reaction and enters the palladium membrane 3;
d. hydrogen-containing tail gas separated by the palladium membrane 3 enters a combustion chamber 7 for combustion to provide a heat source for the on-site hydrogen production unit 6;
e. the high-purity hydrogen separated by the palladium membrane 3 firstly enters the heat exchanger 1 to exchange heat with a hydrogen production raw material of the on-site hydrogen production unit 6 to recover energy, then enters the hydrogen fuel cell unit 8, is externally output by the hydrogen fuel cell unit 8 and supplies power to the electric heating device 2 and the starting power supply 4;
f. when the hydrogen purification system finishes working, the vacuum pump 5 is started to vacuumize the system pipeline, then the electric heating device 2 is closed, and the system is naturally cooled to room temperature.
The structure of the heat exchanger 1 is shown in fig. 2, and comprises a cold source inlet 11, a cold source outlet 12, a heat source inlet 13, a heat source outlet 14 and a central hole 15; the cold source is a hydrogen production raw material, and the heat source is high-purity hydrogen separated by a palladium membrane; hydrogen production raw materials enter the heat exchanger through a cold source inlet 11 and are conveyed to the on-site hydrogen production unit 6 through a cold source outlet 12, high-purity hydrogen enters the heat exchanger through a heat source inlet 13 and is conveyed to the hydrogen fuel cell unit 8 through a heat source outlet 14, and electric energy is output outwards; the hole 15 is used for placing the electric heating device 2; the electric heating device 2 is an electric heating jacket with rated voltage of 12V and rated power of 500W, the thickness of an insulating layer of the electric heating jacket is 10cm, the palladium membrane 3 wrapped by the electric heating jacket is placed in the hole 15 of the heat exchanger 1, when the temperature rise is finished and the heat preservation stage is started, the environmental temperature fluctuation of the palladium membrane 3 is only plus or minus 1 ℃, the actual power consumption of the electric heating jacket is 100W and is only 20% of the rated power; the on-site hydrogen production unit 6 is a methanol reforming on-site hydrogen production unit, the pressure of the delivered mixed gas is 1MPa, and the concentration of hydrogen in the mixed gas is 65 percent; the palladium membrane 3 is a palladium/copper alloy membrane packaged in advance, the purity of high-purity hydrogen separated by the palladium membrane is 99.999%, and hydrogen-containing tail gas separated by the palladium membrane enters the combustion chamber 7 to be combusted so as to provide heat energy for the on-site hydrogen production unit 6; the starting power supply 4 is a lead-acid storage battery with nominal voltage of 12V and capacity of 100 Ah; the vacuum pump 5 is a 12V micro diaphragm pump; the rated output power of the hydrogen fuel cell unit 8 per unit time is 2kwh, wherein only 5% of the output power is used for supplying power to the electric heating device 2, the rest power is used for charging the starting power supply 4 and outputting the power to the outside, and the power transmission route of a hydrogen purification system in the on-site hydrogen production fuel cell device is shown in fig. 3.
Example 2
The electric heating device 2 is a miniature electric heating furnace with rated voltage of 24V and rated power of 500W, the thickness of the heat-insulating layer of the electric heating furnace is 5cm, and the electric heating furnace is coveredThe palladium-wrapped film 3 is placed in a hole 15 of the heat exchanger 1, and when the temperature is raised and the heat preservation stage is started, the power consumption of the electric heating furnace is 180W, and the rated power is 36%; the on-site hydrogen production unit 6 is an ethanol reforming on-site hydrogen production unit, the pressure of the conveyed mixed gas is 0.8MPa, and the concentration of hydrogen in the mixed gas is 55 percent; the palladium membrane 3 is two palladium composite membranes connected in series, and the hydrogen purification rate is 1m 3 H, the purity of the high-purity hydrogen separated by the palladium membrane is 99.995%, and the hydrogen-containing tail gas separated by the palladium membrane enters a combustion chamber 7 for combustion to provide heat energy for the on-site hydrogen production unit 6; the starting power supply 4 is a lithium battery with nominal voltage of 24V and capacity of 50 Ah; the vacuum pump 5 is a 24V micro diaphragm pump. The rated output power of the hydrogen fuel cell unit 8 per unit time is 1.2kwh, 15% of the output power is used for supplying power to the electric heating device 2, and the rest of the output power is used for charging and outputting the starting power supply 4.
Example 3
The electric heating device 2 is an electric heating belt with rated voltage of 220V and rated power of 2000W, the thickness of a heat insulation layer of the electric heating belt is 15cm, the palladium membrane 3 wrapped by the electric heating belt is placed in the hole 15 of the heat exchanger 1, and when the temperature rise is finished and the heat insulation stage is started, the power consumption of the electric heating belt is 300W and reaches 15% of the rated power; the on-site hydrogen production unit 6 is a methane reforming on-site hydrogen production unit, the pressure of the conveyed mixed gas is 0.8MPa, and the concentration of hydrogen in the mixed gas is 60 percent; the palladium membrane 3 is a palladium composite membrane with four palladium membranes connected in series, the hydrogen purification rate is 5m < 3 >/h, the purity of the high-purity hydrogen separated by the palladium membrane is 99.999 percent, and hydrogen-containing tail gas separated by the palladium membrane enters a combustion chamber 7 to be combusted so as to provide heat energy for the on-site hydrogen production unit 6; the starting power supply 4 is a lithium battery with nominal voltage of 48V and capacity of 100 Ah; the vacuum pump 5 is a 24V micro diaphragm pump. The rated output power of the hydrogen fuel cell unit 8 per unit time is 6kwh, of which only 5% is used for supplying power to the electric heating device 2, and the rest is used for charging and outputting the starting power supply 4.
Claims (6)
1. A hydrogen purification system in an on-site hydrogen production fuel cell device mainly comprises a heat exchanger, an electric heating device, a palladium membrane purification assembly, a starting power supply, a vacuum pump, an on-site hydrogen production unit, a combustion chamber and a hydrogen fuel cell unit, wherein the heat exchanger is used for recovering heat of high-purity hydrogen separated by a palladium membrane and preheating a hydrogen production raw material, the heat exchanger is provided with a central hole for placing the electric heating device, a heat source of the heat exchanger is the high-purity hydrogen separated by the palladium membrane, a cold source of the heat exchanger is the hydrogen production raw material, the electric heating device is an electric heating belt, an electric heating sleeve or an electric heating furnace containing a heat insulation layer, the electric heating device wraps the palladium membrane and then is placed in the central hole of the heat exchanger, the palladium membrane is a palladium membrane or a palladium alloy membrane packaged in advance, mixed hydrogen output by the on-site hydrogen production unit is used as a separation raw material, hydrogen-containing tail gas separated by the palladium membrane enters the combustion chamber for combustion, and the high-purity hydrogen separated by the palladium membrane enters the heat exchanger.
2. A system for hydrogen purification in an on-site hydrogen-producing fuel cell device as claimed in claim 1, wherein: the starting power supply is a chemical power supply capable of being charged and discharged for many times, and serves as a working power supply of the hydrogen purification system when the hydrogen fuel cell unit does not output electric energy, and the electricity storage quantity of the starting power supply needs to meet the electricity consumption quantity before the hydrogen production fuel cell device stably outputs the electric energy.
3. A hydrogen purification system in an on-site hydrogen production fuel cell device according to claim 1, wherein: the vacuum pump is used for vacuumizing a system pipeline when the hydrogen purification system starts to work and finishes working.
4. A hydrogen purification system in an on-site hydrogen production fuel cell device according to claim 1, wherein: the on-site hydrogen production unit is used for preparing mixed hydrogen by reacting hydrogen production raw materials.
5. A hydrogen purification system in an on-site hydrogen production fuel cell device according to claim 1, wherein: the combustion chamber is used for combusting the hydrogen-containing tail gas after the palladium membrane separation.
6. A hydrogen purification system in an on-site hydrogen production fuel cell device according to claim 1, wherein: the hydrogen fuel cell unit is used for outputting electric energy to the outside and supplying power to the electric heating device and the starting power supply.
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