CN111137855B - Energy storage and conversion system based on hydrogen loading-hydrogen production of liquid ammonia - Google Patents
Energy storage and conversion system based on hydrogen loading-hydrogen production of liquid ammonia Download PDFInfo
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- CN111137855B CN111137855B CN202010139624.7A CN202010139624A CN111137855B CN 111137855 B CN111137855 B CN 111137855B CN 202010139624 A CN202010139624 A CN 202010139624A CN 111137855 B CN111137855 B CN 111137855B
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 204
- 239000001257 hydrogen Substances 0.000 title claims abstract description 192
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 192
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 164
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 48
- 238000006243 chemical reaction Methods 0.000 title claims abstract description 36
- 238000004146 energy storage Methods 0.000 title claims abstract description 21
- 229910021529 ammonia Inorganic materials 0.000 claims abstract description 60
- 238000003860 storage Methods 0.000 claims abstract description 49
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 47
- 238000000926 separation method Methods 0.000 claims abstract description 24
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 23
- 230000003197 catalytic effect Effects 0.000 claims abstract description 21
- 238000002309 gasification Methods 0.000 claims abstract description 15
- 239000012535 impurity Substances 0.000 claims abstract description 15
- 239000003507 refrigerant Substances 0.000 claims abstract description 14
- 238000011084 recovery Methods 0.000 claims abstract description 12
- 238000000746 purification Methods 0.000 claims abstract description 11
- 238000010438 heat treatment Methods 0.000 claims abstract description 9
- 238000004523 catalytic cracking Methods 0.000 claims abstract description 7
- 230000001105 regulatory effect Effects 0.000 claims abstract description 7
- 239000002912 waste gas Substances 0.000 claims abstract description 7
- 238000001035 drying Methods 0.000 claims abstract description 6
- 238000012546 transfer Methods 0.000 claims abstract description 5
- 239000012528 membrane Substances 0.000 claims description 22
- 238000005336 cracking Methods 0.000 claims description 19
- 239000003054 catalyst Substances 0.000 claims description 17
- 239000002808 molecular sieve Substances 0.000 claims description 9
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 9
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 8
- 239000003463 adsorbent Substances 0.000 claims description 6
- 238000000354 decomposition reaction Methods 0.000 claims description 6
- 239000007787 solid Substances 0.000 claims description 6
- 229910052751 metal Inorganic materials 0.000 claims description 5
- 239000002184 metal Substances 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 5
- 229910052763 palladium Inorganic materials 0.000 claims description 4
- 239000000956 alloy Substances 0.000 claims description 3
- 229910045601 alloy Inorganic materials 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N ethylene glycol Natural products OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 3
- 125000003827 glycol group Chemical group 0.000 claims description 3
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 claims description 3
- 230000000630 rising effect Effects 0.000 claims description 3
- 239000007789 gas Substances 0.000 abstract description 13
- 238000000034 method Methods 0.000 description 17
- 230000008569 process Effects 0.000 description 11
- 239000002826 coolant Substances 0.000 description 10
- 238000005516 engineering process Methods 0.000 description 10
- 239000002994 raw material Substances 0.000 description 8
- 238000005265 energy consumption Methods 0.000 description 7
- 239000007788 liquid Substances 0.000 description 7
- 239000000243 solution Substances 0.000 description 5
- 239000002918 waste heat Substances 0.000 description 5
- 238000010586 diagram Methods 0.000 description 4
- 239000002803 fossil fuel Substances 0.000 description 4
- 238000004064 recycling Methods 0.000 description 4
- 238000013461 design Methods 0.000 description 3
- 150000004678 hydrides Chemical class 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 238000005868 electrolysis reaction Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000004880 explosion Methods 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 231100000572 poisoning Toxicity 0.000 description 2
- 230000000607 poisoning effect Effects 0.000 description 2
- 238000000197 pyrolysis Methods 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000003421 catalytic decomposition reaction Methods 0.000 description 1
- 238000007233 catalytic pyrolysis Methods 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000001651 catalytic steam reforming of methanol Methods 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 230000014509 gene expression Effects 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000008676 import Effects 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000005086 pumping Methods 0.000 description 1
- 238000002407 reforming Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 239000006200 vaporizer Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- 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
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/047—Decomposition of ammonia
-
- C—CHEMISTRY; METALLURGY
- 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
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
- F28D7/00—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
- F28D7/08—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits being otherwise bent, e.g. in a serpentine or zig-zag
- F28D7/082—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits being otherwise bent, e.g. in a serpentine or zig-zag with serpentine or zig-zag configuration
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0405—Purification by membrane separation
- C01B2203/041—In-situ membrane purification during hydrogen production
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/042—Purification by adsorption on solids
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/0495—Composition of the impurity the impurity being water
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/06—Integration with other chemical processes
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- 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
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
- C01B2203/0872—Methods of cooling
- C01B2203/0883—Methods of cooling by indirect heat exchange
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- 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
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract
The invention provides an energy storage and conversion system based on liquid ammonia hydrogen-carrying and hydrogen production, which comprises: the liquid ammonia storage, gasification, impurity removal and ammonia gas heating unit comprises a liquid ammonia storage tank, a gasifier, a pressure regulating valve group, a drying filter, an ammonia gas preheater and a heater which are sequentially communicated; the catalytic cracking conversion hydrogen production and separation purification unit comprises an ammonia catalytic cracking-hydrogen separator, a purifier, a cooler and a secondary refrigerant pump which are sequentially communicated; the ammonia catalytic cracking-hydrogen separator is communicated with the ammonia preheater, and high-temperature nitrogen in the waste gas generated by the ammonia catalytic cracking-hydrogen separator is subjected to energy recovery through the ammonia preheater to transfer heat to ammonia so as to heat the ammonia; and circulating the secondary refrigerant between the cooler and the gasifier through the secondary refrigerant pump. The existing hydrogen production process has the problems of large pollution discharge amount, high power consumption and complex storage and transportation after gas production.
Description
Technical Field
The invention relates to the field of heat exchange networks and equipment for carrying hydrogen to prepare hydrogen by liquid ammonia, in particular to an energy storage and conversion system for carrying hydrogen to prepare hydrogen by liquid ammonia.
Background
The shortage of energy sources, environmental pollution and climate warming bring great pressure to human society, so that the reasonable development of efficient clean energy sources and related conversion technologies for optimizing the energy source use efficiency are key problems to be solved at present in the transition from traditional heavy-pollution fossil fuels to environment-friendly renewable non-fossil energy sources. Among the renewable energy sources, hydrogen energy is known as "pearl on energy crown" which is a completely clean renewable final energy source. Although the hydrogen is widely distributed, the free hydrogen exists in a very small amount in a natural state, and how to economically and economically enrich and purify the hydrogen in a low-carbon environment-friendly way so as to manufacture the hydrogen is a great difficulty in the popularization of the hydrogen energy at present. The industrial artificial large-scale hydrogen production can be divided into fossil fuel, renewable water electrolysis, biotechnology manufacturing and the like. However, the hydrogen production processes are limited by technology, so that environmental and economic problems such as larger pollution emission, higher power consumption and the like exist, or the large-scale production stability is poor. In addition, the storage and transportation after the hydrogen manufacture is complex and extremely expensive, the hydrogen storage tank with the design pressure of 98MPa is required to be produced for the gaseous pressure hydrogen storage, the liquid hydrogen storage and transportation needs to be liquefied by reducing the hydrogen to minus 253 ℃ under normal pressure, and the technical difficulty of the tank storage is extremely high. There is therefore an urgent need to find alternative methods for producing hydrogen from hydrogen storage with economy in the event that the above technology is not mature.
Ammonia, which is an organic substance with a mass fraction of 17.6% of hydrogen, is widely used for agricultural industrial basic products and chemical raw materials, has a narrow explosion limit (16-27%) in air, has an easy discovery of pungent smell, has mature production technology and low storage and transportation price, is completely cracked into hydrogen and nitrogen by adding a conventional catalyst at about 600 ℃ and normal pressure, has a conversion efficiency of 99.9%, and has great hydrogen production potential. Ammonia can be liquefied only at normal temperature of-33 ℃ and does not generate hydrogen embrittlement reaction with metal, and the volume energy density of liquid ammonia is 1.53 times that of liquid hydrogen. The volume energy density of the liquid ammonia is 1.53 times that of the liquid hydrogen, and the energy storage and transportation rate is higher under the same volume condition. At present, the price of hydrogen in domestic hydrogen stations is about 70 yuan per kilogram, the price of liquid ammonia is about 3000 yuan per ton, the hydrogen obtained by decomposition is about 16.7 yuan per kilogram, and the difference of the costs of hydrogen and ammonia in storage, transportation, decomposition and the like is not compared. Thus, ammonia is a source of feed gas for hydrogen storage-production and a promising and new attractive technical form.
The existing hydrogen production-storage technology is concentrated on the aspects of high energy consumption and high emission, and the technology of hydrogen production and hydrogen storage is purely split, such as fossil fuel reforming, water electrolysis is performed after a large amount of energy is consumed and hydrogen is produced, compared with the technology without subsequent hydrogen storage and transportation, so that subsequent compression, liquefaction and hydride storage and transportation are performed again for energy consumption, the cost of the current large-scale hydrogen production is acceptable, the energy consumption and the cost of the subsequent hydrogen storage and transportation are too high, the mode of the technology leads the final hydrogen consumption cost of the whole hydrogen production-storage industry to be far greater than the cost of fossil fuel and related emission treatment, and the energy efficiency when hydrogen is used does not counteract the energy consumption emission when hydrogen production-hydrogen storage is not carried out, so the technology is quite unreasonable at present.
Disclosure of Invention
According to the technical problems that the existing hydrogen production process has the environmental and economic problems of large pollution discharge amount, high electricity consumption and the like, and the storage and transportation after the hydrogen production is complex and extremely expensive, the energy storage and conversion system based on the liquid ammonia hydrogen loading-hydrogen production is provided. The hydrogen storage method takes hydride storage and transportation as the beginning hydrogen production as the terminal, breaks through the complex process of the traditional method of firstly producing hydrogen and then storing and transporting and extremely high cost, takes hydrogen-rich liquid ammonia (17.6 percent of hydrogen storage amount per unit mass) as a hydrogen storage carrier, breaks through the traditional hydrogen carrying systems such as electrolyzed water (11.1 percent), methanol steam reforming (12.4 percent), organic hydride hydrolysis (5.2 to 8.6 percent) and the like; through the steps of liquid ammonia gasification, ammonia preheating, heating, catalytic decomposition, final hydrogen purification and the like, a series of energy conversion processes can effectively and economically store and transport hydrogen-rich media and produce hydrogen with the purification rate of more than 99.9 percent on site, and the cold and waste heat in the process are recovered by utilizing an integrated heat exchange network so as to reduce the hydrogen production energy consumption, and meanwhile, the device also has the advantages of no pollution of waste gas, compact structure and capability of meeting the hydrogen demand of a site hydrogenation station and related chemical equipment during the starting.
The invention adopts the following technical means:
An energy storage and conversion system for hydrogen-producing based on liquid ammonia, comprising:
The liquid ammonia storage, gasification, impurity removal and ammonia gas heating unit comprises a liquid ammonia storage tank, a gasifier, a pressure regulating valve group, a drying filter, an ammonia gas preheater and a heater which are sequentially communicated;
The catalytic cracking conversion hydrogen production and separation purification unit comprises an ammonia catalytic cracking-hydrogen separator, a purifier, a cooler and a secondary refrigerant pump which are sequentially communicated; the ammonia catalytic cracking-hydrogen separator is communicated with the ammonia preheater, and high-temperature nitrogen in the waste gas generated by the ammonia catalytic cracking-hydrogen separator 7 is subjected to energy recovery through the ammonia preheater to transfer heat to ammonia so as to heat the ammonia; and the refrigerating medium is pumped between the cooler and the gasifier through the refrigerating medium pump, the refrigerating medium recovers the cold energy generated by the gasification of the liquid ammonia in the gasifier, and the cooler cools the hydrogen through the refrigerating medium.
Further, the gasifier, the ammonia gas preheater and the cooler are plate-fin, plate, wound tube or shell-and-tube heat exchangers.
Further, the ammonia catalytic cracking-hydrogen separator comprises an inlet manifold, an outlet manifold and a shell-and-tube cracking separation device; the shell-and-tube cracking separation device is filled with a catalyst; the shell-and-tube cracking separation device is provided with a nitrogen outlet; the inlet manifold is communicated with the inside of the shell-and-tube cracking separation device; the outlet manifold extends into the shell-and-tube cracking separation device; the inner wall of the outlet manifold is attached with a hydrogen permeable membrane.
Further, the catalyst is a metal-based ammonia decomposition catalyst.
Further, the purifier is a sleeve type, and comprises an outer tube and an inner tube, wherein the outer tube is provided with a hydrogen inlet, the outer tube is filled with a porous solid molecular sieve adsorbent, the inner tube is attached with a hydrogen permeable membrane, and hydrogen is led out from the inner tube through the hydrogen permeable membrane after passing through the porous solid molecular sieve adsorbent to adsorb impurities.
Further, the hydrogen permeable membrane is a palladium-based alloy membrane.
Further, the secondary refrigerant is glycol aqueous solution or nitrogen.
Further, the heater is fully operated when the liquid ammonia storage, gasification, impurity removal and ammonia gas temperature rising unit starts hydrogen production, and becomes a small-load operation or an intermittent operation mode after hydrogen is produced.
Compared with the prior art, the invention has the following advantages:
1. the energy storage and conversion system based on liquid ammonia hydrogen loading-hydrogen production provided by the invention abandons the unreasonable situation that the prior pure hydrogen production and hydrogen storage technology is split (namely hydrogen production is firstly carried out and then hydrogen storage is carried out), initially provides the technical flow of hydrogen raw material loading firstly and hydrogen production in a field is reproduced, and overcomes the technical engagement of no subsequent hydrogen storage and transportation after large-scale energy consumption hydrogen production in the prior art, so that the compression, liquefaction, storage and transportation of hydrogen are carried out again for a large amount of energy consumption and even worse than the hydrogen production economy.
2. The energy storage and conversion system based on the hydrogen carrying and hydrogen production of the liquid ammonia provided by the invention overcomes the defects of high cost, inflammability, explosiveness and the like of the existing hydrogen and liquid hydrogen storage and transportation, utilizes the hydrogen carrying raw material liquid ammonia to carry out storage and transportation, and has the advantages that the liquid ammonia acquisition way is wide, the cost is low (< 3000 per ton), the converted hydrogen is 16.7 per kg, the hydrogen price of the existing hydrogen station is about 70 per kg, and the hydrogen storage amount per unit mass is higher (17.6%) than that of other hydrogen carrying systems. In addition, the volume energy density of the liquid ammonia is 1.53 times of that of the liquid hydrogen, and if the same volume of fuel is adopted, the endurance mileage of the liquid ammonia is 1.53 times of that of the liquid hydrogen.
3. The invention has the unique design that the hydrogen gas cooling system comprises two energy recovery heat exchange networks, wherein the cold energy recovery heat exchange networks respectively recycle the cold energy of the gasification of the liquid ammonia of the gasifier by pumping the secondary refrigerant so as to cool the hydrogen gas with higher temperature in the cooler; the heat recovery heat exchange network utilizes the low Wen Anqi of decomposed high-temperature nitrogen gas after being circularly heated and gasified in the preheater so as to save the power consumption of the heater, the design enables the system to be more energy-saving and environment-friendly, power consumption components of the system are only a cold recovery circulating pump and an ammonia heater, no other power consumption equipment exists, the heater works in full load when the system is started in a circulating mode, and the heater is changed into a small-load working mode or an intermittent working mode after hydrogen is produced.
4. In order to prevent the danger of inflammability and explosiveness when hydrogen is cooled down, the invention does not directly utilize the decomposed hydrogen waste heat to gasify raw gas in the system, but skillfully sets other explosion-proof secondary refrigerant as medium to transfer and convert heat between the gasifier and the cooler.
5. According to the energy storage and conversion system based on liquid ammonia hydrogen loading-hydrogen production, the gasifier, the preheater and the cooler are packaged and integrated in the same multi-channel heat exchanger to form the integrated circulating heat conversion device, so that compact modularized installation is facilitated.
In conclusion, the system provided by the invention is compact, safe and efficient, and the heat exchange network and the cracking purification device which are skillfully designed are used for enabling the liquid ammonia to be energy-saving and environment-friendly in the processes of gasifying, heating and cracking to generate hydrogen for recovering temperature and discharging tail gas. Therefore, the technical scheme of the invention solves the problems of large pollution discharge, high power consumption and the like in the existing hydrogen production process, and the problems of complex storage and transportation after hydrogen production and extremely high cost.
Based on the reasons, the method can be widely popularized in the fields of liquid ammonia hydrogen-carrying-hydrogen production, related hydrogen energy automobiles, ships and the like.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described, and it is obvious that the drawings in the following description are some embodiments of the present invention, and other drawings may be obtained according to the drawings without inventive effort to a person skilled in the art.
FIG. 1 is a schematic diagram of the structure and principle of the energy storage and conversion system based on liquid ammonia hydrogen-carrying-hydrogen production according to the present invention.
Fig. 2 is a schematic diagram of a flow path structure of an energy recovery heat exchange network.
FIG. 3 is a schematic diagram of the ammonia catalytic cracking-hydrogen separator according to the present invention.
FIG. 4 is a schematic diagram of a purifier according to the present invention.
In the figure: 1. a liquid ammonia storage tank; 2. a gasifier; 3. a pressure regulating valve block; 4. drying the filter; 5. an ammonia preheater; 6. a heater; 7. an ammonia catalytic cracking-hydrogen separator; 71. an inlet manifold; 72. a shell-and-tube cracking separation device; 73. an outlet manifold; 74. a nitrogen outlet; 8. a purifier; 81. an inner tube; 82. an outer tube; 9. a cooler; 10. a coolant pump.
Detailed Description
It should be noted that, without conflict, the embodiments of the present invention and features of the embodiments may be combined with each other. The invention will be described in detail below with reference to the drawings in connection with embodiments.
For the purpose of making the objects, technical solutions and advantages of the embodiments of the present invention more apparent, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, not all embodiments. The following description of at least one exemplary embodiment is merely exemplary in nature and is in no way intended to limit the invention, its application, or uses. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the present invention. As used herein, the singular is also intended to include the plural unless the context clearly indicates otherwise, and furthermore, it is to be understood that the terms "comprises" and/or "comprising" when used in this specification are taken to specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof.
The relative arrangement of the components and steps, numerical expressions and numerical values set forth in these embodiments do not limit the scope of the present invention unless it is specifically stated otherwise. Meanwhile, it should be clear that the dimensions of the respective parts shown in the drawings are not drawn in actual scale for convenience of description. Techniques, methods, and apparatus known to those of ordinary skill in the relevant art may not be discussed in detail, but are intended to be part of the specification where appropriate. In all examples shown and discussed herein, any specific values should be construed as merely illustrative, and not a limitation. Thus, other examples of the exemplary embodiments may have different values. It should be noted that: like reference numerals and letters denote like items in the following figures, and thus once an item is defined in one figure, no further discussion thereof is necessary in subsequent figures.
In the description of the present invention, it should be understood that the azimuth or positional relationships indicated by the azimuth terms such as "front, rear, upper, lower, left, right", "lateral, vertical, horizontal", and "top, bottom", etc., are generally based on the azimuth or positional relationships shown in the drawings, merely to facilitate description of the present invention and simplify the description, and these azimuth terms do not indicate and imply that the apparatus or elements referred to must have a specific azimuth or be constructed and operated in a specific azimuth, and thus should not be construed as limiting the scope of protection of the present invention: the orientation word "inner and outer" refers to inner and outer relative to the contour of the respective component itself.
Spatially relative terms, such as "above … …," "above … …," "upper surface on … …," "above," and the like, may be used herein for ease of description to describe one device or feature's spatial location relative to another device or feature as illustrated in the figures. It will be understood that the spatially relative terms are intended to encompass different orientations in use or operation in addition to the orientation depicted in the figures. For example, if the device in the figures is turned over, elements described as "above" or "over" other devices or structures would then be oriented "below" or "beneath" the other devices or structures. Thus, the exemplary term "above … …" may include both orientations "above … …" and "below … …". The device may also be positioned in other different ways (rotated 90 degrees or at other orientations) and the spatially relative descriptors used herein interpreted accordingly.
In addition, the terms "first", "second", etc. are used to define the components, and are only for convenience of distinguishing the corresponding components, and the terms have no special meaning unless otherwise stated, and therefore should not be construed as limiting the scope of the present invention.
Example 1
The present invention provides an energy storage and conversion system for hydrogen-producing based on liquid ammonia hydrogen loading, as shown in fig. 1-4, comprising:
The liquid ammonia storage, gasification, impurity removal and ammonia gas heating unit comprises a liquid ammonia storage tank 1, a gasifier 2, a pressure regulating valve group 3, a drying filter 4, an ammonia gas preheater 5 and a heater 6 which are sequentially communicated; all the equipment of the liquid ammonia storage, gasification, impurity removal and ammonia gas heating unit are communicated through pipelines;
the catalytic cracking conversion hydrogen production and separation purification unit comprises an ammonia catalytic cracking-hydrogen separator 7, a purifier 8, a cooler 9 and a secondary refrigerant pump 10 which are sequentially communicated; all the devices of the catalytic pyrolysis conversion hydrogen production, separation and purification units are communicated through pipelines;
The ammonia catalytic cracking-hydrogen separator 7 is communicated with the ammonia preheater 5, and high-temperature nitrogen in the waste gas generated by the ammonia catalytic cracking-hydrogen separator 7 is subjected to energy recovery through the ammonia preheater 5 to transfer heat to ammonia so as to heat the ammonia; the coolant is pumped between the cooler 9 and the gasifier 2 by the coolant pump 10, the coolant recovers the cold energy generated by the gasification of the liquid ammonia in the gasifier 2, and the cooler 9 cools the hydrogen by the coolant.
When the system works, a liquid ammonia storage tank 1 is connected with a gasifier 2 through a low-temperature pipeline and receives liquid ammonia from the storage tank, and a pressure regulating valve 3 controls the pressure in the storage tank and the gasifier and the flow of ammonia output outwards; the gasifier 2 is connected with an ammonia drier filter 4, a preheater 5 and a heater 6 in sequence through pipelines, and the raw material gas ammonia gas reaches the catalytic cracking temperature through preheating and heating;
The raw material gas is introduced into an ammonia catalytic cracking-hydrogen separator 7, and is decomposed into hydrogen and nitrogen by a catalyst reaction at a certain temperature; the hydrogen enters a purifier 8 through a hydrogen permeable membrane for enrichment and purification, and the nitrogen enters the mentioned preheater 5 as tail gas for recycling waste heat to preheat ammonia; the purified hydrogen enters a cooler 9 to exchange heat and cool with the secondary refrigerant in the gasifier 2; the coolant is circulated in the above-described system vaporizer 2 and cooler 9 by a coolant pump 10 to vaporize liquid ammonia and cool hydrogen.
Further, the gasifier 2, the ammonia preheater 5 and the cooler 9 are plate-fin, plate, wound tube or shell-and-tube heat exchangers.
Further, the internal channels of the gasifier 3 may be corrugated fins, and the internal channels of the ammonia preheater 5 and the cooler 9 may be zigzag fins.
Furthermore, the gasifier 3, the ammonia gas preheater 5 and the cooler 9 are packaged and integrated in the same multi-channel heat exchanger to form an integrated circulating heat conversion device, so that the device is convenient to install.
Further, as shown in fig. 3, the ammonia catalytic cracking-hydrogen separator 7 includes an inlet manifold 71, an outlet manifold 73, and a shell-and-tube cracking separation device 72; the shell-and-tube cracking separation device 72 is filled with a catalyst; the shell-and-tube cracking separation device 72 is provided with a nitrogen outlet 74; the inlet manifold 71 is in communication with the interior of the shell-and-tube cracking separation device 72; the outlet manifold 73 extends into the interior of the shell-and-tube pyrolysis separation unit 72; a hydrogen permeable membrane is attached to the inner wall of the outlet manifold 73;
The ammonia catalytic cracking-hydrogen separator 7 is a unit device for separating and integrating raw material gas into hydrogen and waste gas nitrogen. Through setting up the manifold, can increase reaction area and reduce catalyst poisoning inefficacy phenomenon, make ammonia be divided into several strands and let in the shell-and-tube pyrolysis separator in through the import manifold, by catalyst schizolysis into hydrogen and nitrogen, export manifold is with hydrogen membrane only hydrogen can get into in the pipe and export, and the hydrogen of each strand of export is assembled by the exit end manifold of export manifold and is discharged.
Further, the catalyst is a metal-based ammonia decomposition catalyst such as Ru, ni, fe and the like or other compound components.
Further, as shown in fig. 4, the purifier 8 is a sleeve, and includes an outer tube 82 and an inner tube 81, the outer tube 82 is provided with a hydrogen inlet, the outer tube 82 is filled with a porous solid molecular sieve adsorbent, the inner tube 81 is attached with a hydrogen permeable membrane, and hydrogen is led out from the inner tube 81 through the hydrogen permeable membrane after passing through the porous solid molecular sieve adsorbent to adsorb impurities.
Specifically, hydrogen enters the purifier 8 from the outer tube, wherein tiny moisture impurities, ammonia, nitrogen and the like are adsorbed by the molecular sieve, the remaining hydrogen is led out from the inner tube through the hydrogen permeable membrane II 81, and the purified hydrogen can be expected to reach 99.99%.
Further, the hydrogen permeable membrane is a palladium-based alloy membrane or other relevant hydrogen permeable membranes.
Further, the coolant is glycol aqueous solution, nitrogen or other explosion-proof coolant to cool the hydrogen gas to prevent the cooler from hydrogen explosion.
Further, the system power consumption components are only the coolant pump 10 and the heater 6, and no other power consumption equipment exists; the heater 6 is fully operated when the liquid ammonia storage, gasification, impurity removal and ammonia heating unit starts hydrogen production, and the heater 6 is changed into a small-load operation or an intermittent operation mode after hydrogen is produced.
The working process of the energy storage and conversion system based on liquid ammonia hydrogen loading-hydrogen production specifically comprises the following steps:
(1) Liquid ammonia storage and transportation gasification process
The ammonia gas is converted into liquid state to be stored in a liquid ammonia storage tank 1 under normal temperature pressurization of 0.86MPa or normal pressure and low temperature of minus 33 ℃, wherein the liquid ammonia is gasified and cold energy is recovered in the liquid ammonia through a gasifier 2, and then the pressure in the storage tank and the gasifier and the flow of the gasified ammonia gas which is output outwards are controlled through a pressure regulating valve group 3.
(2) Ammonia drying impurity removal and temperature rising process
The gasified ammonia gas is connected with a dryer filter 4 through a pipeline to dry and remove impurities, then the ammonia gas is preheated to about 500 ℃ by using waste heat recovered by system waste gas through an ammonia gas preheater 5, and then the ammonia gas passes through a heater 6 with a set temperature to enable the ammonia gas of raw material gas to reach about 650 ℃ of catalytic cracking temperature.
(3) Catalytic cracking separation of ammonia and hydrogen purification process
The raw material gas under the process condition enters the ammonia catalytic cracking-hydrogen separator 7, and is reacted and decomposed into hydrogen and nitrogen by a catalyst at a certain temperature of about 650 ℃ and under normal pressure, and the process can be represented as follows:
The process is an endothermic expansion reaction, namely, unit mole ammonia gas is cracked into 75% hydrogen and 25% ammonia gas under the catalysis of a certain temperature and absorbs 47.3kJ heat, so that the dynamic decomposition of ammonia is facilitated by increasing the temperature and reducing the pressure, and the ammonia cracking conversion rate can reach 99.9% at the temperature of about 650 ℃ under normal pressure generally.
In order to increase the reaction area and reduce the poisoning failure phenomenon of the catalyst, the ammonia gas in the ammonia catalytic cracking-hydrogen separator 7 is divided into 3 strands which are respectively cracked into hydrogen and nitrogen by the catalyst in the manifold, each end of the manifold is provided with a shell-and-tube cracking separation device, the shell side of the separation device is filled with the catalyst, the tube layer is attached with a palladium metal-based hydrogen permeable membrane, only hydrogen gas after decomposed gas passes through the hydrogen permeable membrane can enter the purifier 8 and is subjected to pressure swing adsorption purification enrichment by utilizing a molecular sieve, the separated hydrogen enters the purifier from the outer tube, tiny moisture impurities, ammonia, nitrogen and the like are adsorbed by the molecular sieve, and the rest hydrogen gas is led out from the inner tube through the hydrogen permeable membrane.
(4) System heat exchange network energy recycling process
The separated nitrogen and the purified hydrogen enter a heat exchange network of the system for energy recycling, wherein the nitrogen is taken as tail gas to enter a pre-heater 5 before the tail gas is used for recycling waste heat so as to pre-heat ammonia gas to be reacted in the system, and the ammonia gas is discharged to the atmosphere after the temperature of the ammonia gas is reduced; the purified hydrogen enters a cooler 9 to exchange heat with the secondary refrigerant in the gasifier, and the recovered cold energy is used for self cooling and then is supplied to a fuel cell of a using device, an internal combustion engine or is introduced into a hydrogen storage tank through a booster valve group.
The system comprises two energy recovery heat exchange networks, wherein the cold energy recovery heat exchange network utilizes a secondary refrigerant pump 10 to pump the secondary refrigerant to recycle the cold energy of the gasification of the liquid ammonia of the gasifier 3 so as to cool the hydrogen with higher temperature in a cooler 9; the heat recovery heat exchange network circularly heats gasified low Wen Anqi in the preheater 5 by utilizing decomposed high-temperature nitrogen, thereby saving the power consumption of the heater 6.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some or all of the technical features thereof can be replaced with equivalents; such modifications and substitutions do not depart from the spirit of the technical solutions according to the embodiments of the present invention.
Claims (8)
1. An energy storage and conversion system for hydrogen production based on liquid ammonia, comprising:
The liquid ammonia storage, gasification, impurity removal and ammonia gas heating unit comprises a liquid ammonia storage tank (1), a gasifier (2), a pressure regulating valve group (3), a drying filter (4), an ammonia gas preheater (5) and a heater (6) which are sequentially communicated;
the catalytic cracking conversion hydrogen production and separation purification unit comprises an ammonia catalytic cracking-hydrogen separator (7), a purifier (8), a cooler (9) and a secondary refrigerant pump (10) which are sequentially communicated; the ammonia catalytic cracking-hydrogen separator (7) is communicated with the ammonia preheater (5), and high-temperature nitrogen in the waste gas generated by the ammonia catalytic cracking-hydrogen separator (7) is subjected to energy recovery through the ammonia preheater (5) to transfer heat to ammonia so as to raise the temperature; the refrigerating medium is pumped and circulated between the cooler (9) and the gasifier (2) through the refrigerating medium pump (10), the refrigerating medium recovers the cold energy generated by the gasification of the liquid ammonia in the gasifier (2), and the cooler (9) cools the hydrogen through the refrigerating medium.
2. Energy storage and conversion system based on liquid ammonia hydrogen-production according to claim 1, characterized in that the gasifier (2), the ammonia preheater (5) and the cooler (9) are plate-fin, plate, wound tube or shell-and-tube heat exchangers.
3. The energy storage and conversion system based on liquid ammonia hydrogen-production according to claim 1, characterized in that the ammonia catalytic cracking-hydrogen separator (7) comprises an inlet manifold (71), an outlet manifold (73) and a shell-and-tube cracking separation device (72); the shell-and-tube cracking separation device (72) is filled with a catalyst; the shell-and-tube cracking separation device (72) is provided with a nitrogen outlet (74); the inlet manifold (71) is communicated with the inside of the shell-and-tube cracking separation device (72); the outlet manifold (73) extends into the interior of the shell-and-tube cracking separation device (72); a hydrogen permeable membrane is attached to the inner wall of the outlet manifold (73).
4. The hydrogen-producing energy storage and conversion system based on liquid ammonia according to claim 3, wherein the catalyst is a metal-based ammonia decomposition catalyst.
5. The energy storage and conversion system based on liquid ammonia hydrogen-carrying hydrogen production according to claim 1, wherein the purifier (8) is a sleeve type, comprising an outer tube (82) and an inner tube (81), the outer tube (82) is provided with a hydrogen inlet, the outer tube (82) is filled with a porous solid substance molecular sieve adsorbent, the inner tube (81) is attached with a hydrogen permeable membrane, and hydrogen is led out from the inner tube (81) through the hydrogen permeable membrane after passing through impurities adsorbed by the porous solid substance molecular sieve adsorbent.
6. The energy storage and conversion system for hydrogen production based on liquid ammonia carrier hydrogen according to claim 3 or 5, wherein the hydrogen permeable membrane is a palladium-based alloy membrane.
7. The energy storage and conversion system for hydrogen production based on liquid ammonia according to claim 1, wherein the secondary refrigerant is glycol aqueous solution or nitrogen.
8. The energy storage and conversion system based on hydrogen production by liquid ammonia according to claim 1, wherein the heater (6) is operated at full load when the liquid ammonia storage, gasification, impurity removal and ammonia gas temperature rising unit starts hydrogen production, and the heater (6) is changed to a small load operation or an intermittent operation mode when hydrogen is produced.
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| CN111998225B (en) * | 2020-07-07 | 2022-04-26 | 金华职业技术学院 | High-temperature nitrogen recovery system and control method thereof |
| KR102486171B1 (en) * | 2020-12-15 | 2023-01-09 | 주식회사 원익홀딩스 | Gas generator apparatus having pre-heater for supplying heat source of input gas to reformer |
| CN112901339B (en) * | 2021-01-15 | 2022-04-26 | 河北工业大学 | Direct injection natural gas engine system based on ammonia pyrolysis device and control method thereof |
| CN113451615A (en) * | 2021-05-18 | 2021-09-28 | 青岛创启新能催化科技有限公司 | Liquid ammonia cracking power generation system and method |
| CN114233526A (en) * | 2021-08-11 | 2022-03-25 | 哈尔滨工程大学 | Ammonia reforming system and method for inhibiting natural gas engine knocking and misfiring |
| CN115818567B (en) * | 2022-12-16 | 2023-07-21 | 天津大学 | Large-scale green ammonia pyrolysis hydrogen production system and hydrogen production method |
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