CN110273161A - A kind of electrolysis ammonia hydrogen generating system - Google Patents
A kind of electrolysis ammonia hydrogen generating system Download PDFInfo
- Publication number
- CN110273161A CN110273161A CN201910540176.9A CN201910540176A CN110273161A CN 110273161 A CN110273161 A CN 110273161A CN 201910540176 A CN201910540176 A CN 201910540176A CN 110273161 A CN110273161 A CN 110273161A
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- Prior art keywords
- hydrogen
- anode
- cathode
- layer
- ammonia
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 205
- 239000001257 hydrogen Substances 0.000 title claims abstract description 167
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 167
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 157
- 229910021529 ammonia Inorganic materials 0.000 title claims abstract description 103
- 238000005868 electrolysis reaction Methods 0.000 title claims abstract description 36
- 239000007789 gas Substances 0.000 claims abstract description 82
- 238000004519 manufacturing process Methods 0.000 claims abstract description 72
- 239000003792 electrolyte Substances 0.000 claims abstract description 51
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 34
- 238000003860 storage Methods 0.000 claims abstract description 17
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 16
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 12
- 239000001301 oxygen Substances 0.000 claims description 12
- 229910052760 oxygen Inorganic materials 0.000 claims description 12
- 239000007787 solid Substances 0.000 claims description 12
- 239000004020 conductor Substances 0.000 claims description 11
- 239000010416 ion conductor Substances 0.000 claims description 11
- 230000005611 electricity Effects 0.000 claims description 6
- 238000000354 decomposition reaction Methods 0.000 claims description 4
- 238000000605 extraction Methods 0.000 claims description 2
- 230000003447 ipsilateral effect Effects 0.000 claims 2
- 150000002431 hydrogen Chemical class 0.000 abstract description 8
- 239000000463 material Substances 0.000 description 17
- 238000006243 chemical reaction Methods 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 6
- 238000010586 diagram Methods 0.000 description 4
- 239000002803 fossil fuel Substances 0.000 description 4
- XMHIUKTWLZUKEX-UHFFFAOYSA-N hexacosanoic acid Chemical compound CCCCCCCCCCCCCCCCCCCCCCCCCC(O)=O XMHIUKTWLZUKEX-UHFFFAOYSA-N 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 3
- 229910052788 barium Inorganic materials 0.000 description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 3
- 229910000420 cerium oxide Inorganic materials 0.000 description 3
- RIVZIMVWRDTIOQ-UHFFFAOYSA-N cobalt iron Chemical compound [Fe].[Co].[Co].[Co] RIVZIMVWRDTIOQ-UHFFFAOYSA-N 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 3
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 3
- 229910052726 zirconium Inorganic materials 0.000 description 3
- -1 Oxonium ion Chemical class 0.000 description 2
- 238000005915 ammonolysis reaction Methods 0.000 description 2
- UZFMKSXYXFSTAP-UHFFFAOYSA-N barium yttrium Chemical compound [Y].[Ba] UZFMKSXYXFSTAP-UHFFFAOYSA-N 0.000 description 2
- 229910021523 barium zirconate Inorganic materials 0.000 description 2
- 229910001873 dinitrogen Inorganic materials 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 2
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 2
- 238000005373 pervaporation Methods 0.000 description 2
- 238000010992 reflux Methods 0.000 description 2
- 239000004575 stone Substances 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 241000968352 Scandia <hydrozoan> Species 0.000 description 1
- WGQUMWUZQOHZIO-UHFFFAOYSA-N [Co].[Ba].[Pr] Chemical compound [Co].[Ba].[Pr] WGQUMWUZQOHZIO-UHFFFAOYSA-N 0.000 description 1
- OYVYTMATAYLZSM-UHFFFAOYSA-N [Co].[Sr].[Sm] Chemical compound [Co].[Sr].[Sm] OYVYTMATAYLZSM-UHFFFAOYSA-N 0.000 description 1
- XGPJPLXOIJRLJN-UHFFFAOYSA-N [Mn].[Sr].[La] Chemical compound [Mn].[Sr].[La] XGPJPLXOIJRLJN-UHFFFAOYSA-N 0.000 description 1
- FZJJTYLFARYPAT-UHFFFAOYSA-N [Ni].[Sr].[La] Chemical compound [Ni].[Sr].[La] FZJJTYLFARYPAT-UHFFFAOYSA-N 0.000 description 1
- DAGLJEVWOYUGCC-UHFFFAOYSA-N [Ni].[Sr].[Pr] Chemical compound [Ni].[Sr].[Pr] DAGLJEVWOYUGCC-UHFFFAOYSA-N 0.000 description 1
- WOIHABYNKOEWFG-UHFFFAOYSA-N [Sr].[Ba] Chemical compound [Sr].[Ba] WOIHABYNKOEWFG-UHFFFAOYSA-N 0.000 description 1
- PACGUUNWTMTWCF-UHFFFAOYSA-N [Sr].[La] Chemical compound [Sr].[La] PACGUUNWTMTWCF-UHFFFAOYSA-N 0.000 description 1
- UYPAYADJAOQPLA-UHFFFAOYSA-N [Sr].[Pr] Chemical compound [Sr].[Pr] UYPAYADJAOQPLA-UHFFFAOYSA-N 0.000 description 1
- QQGYPWFMCHMCJD-UHFFFAOYSA-N [Yb].[Y].[Zr] Chemical compound [Yb].[Y].[Zr] QQGYPWFMCHMCJD-UHFFFAOYSA-N 0.000 description 1
- DQBAOWPVHRWLJC-UHFFFAOYSA-N barium(2+);dioxido(oxo)zirconium Chemical compound [Ba+2].[O-][Zr]([O-])=O DQBAOWPVHRWLJC-UHFFFAOYSA-N 0.000 description 1
- 238000007233 catalytic pyrolysis Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000002848 electrochemical method Methods 0.000 description 1
- 239000002001 electrolyte material Substances 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- LNTHITQWFMADLM-UHFFFAOYSA-N gallic acid Chemical compound OC(=O)C1=CC(O)=C(O)C(O)=C1 LNTHITQWFMADLM-UHFFFAOYSA-N 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 238000010303 mechanochemical reaction Methods 0.000 description 1
- 229910002119 nickel–yttria stabilized zirconia Inorganic materials 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- HJGMWXTVGKLUAQ-UHFFFAOYSA-N oxygen(2-);scandium(3+) Chemical compound [O-2].[O-2].[O-2].[Sc+3].[Sc+3] HJGMWXTVGKLUAQ-UHFFFAOYSA-N 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
Abstract
The present invention discloses a kind of electrolysis ammonia hydrogen generating system, including ammonia storage tank, Hydrogen collection device and hydrogen manufacturing component, the hydrogen manufacturing component includes shell, is set to the shell cylinder electrolyte layer and is set to the anode layer and cathode layer of the electrolyte layer opposite sides, the anode of the connection of the cathode of the anode layer and power supply, the cathode layer and power supply connects.The electrolysis ammonia hydrogen generating system that the present invention uses prepares hydrogen, generates hydrogen in cathode layer, anode layer generates nitrogen and directly obtains the hydrogen of high yield high-purity to efficiently separate the nitrogen and hydrogen prepared.Residue ammonia of the invention is back to anode inlet by pipeline from anode gas outlet, and the hydrogen that will not be generated with cathode mixes.
Description
Technical field
The invention belongs to technical field of hydrogen preparation, and in particular to a kind of electrolysis ammonia hydrogen generating system.
Background technique
The energy is the basic assurance of modern social development, is the foundation stone of human civilization.However, existing be with fossil fuel
The energy resource system on basis not only brings serious problem of environmental pollution to us, but also fossil fuel is largely exploited, and is faced withered
It exhausts.The new energy for finding alternative fossil fuel is the important goal of countries nowadays energy development.Hydrogen is as a kind of cleaning energy
Source carrier and be concerned, the development and utilization of Hydrogen Energy must solve the source problem that comes of hydrogen, develop safe and efficient, economic hydrogen supply,
Hydrogen storage technology is the basic of realization hydrogen utilization.Nowadays there are two types of main sources, i.e. water electrolysis and fossil fuel production for hydrogen.Water
The technical process of electrolytic hydrogen production is simple, pollution-free, but its cost is excessively high, and conversion hydrogen needs to consume a large amount of electric energy；Utilize change
Stone fuel production hydrogen then needs to consume a large amount of non-renewable energy resources, while a large amount of greenhouse gases can be discharged into environment,
It is disagreed with purpose of the hydrogen as the energy is used, these reasons limit a kind of extensive use of the hydrogen as alternative energy source.
Ammonia be a kind of hydrogeneous mass fraction up to 17.8% hydrogen-rich materials, since its is cheap, while in pressurization and low
Can be converted to when warm environment liquid it is easily stored and transport, be of concern in recent years as the raw material of hydrogen manufacturing.Utilize ammonia system
The tail gas that hydrogen generates is pollution-free and stable structure nitrogen, and is suitable for nowadays environmentally friendly requirement.Obtaining hydrogen by ammonia mainly has
Three kinds of modes: thermal decomposition or catalytic pyrolysis ammonia, mechanochemical reaction decompose ammonia and electrochemical method decomposition ammonia.
Traditional ammonolysis craft needs to remove by low concentration ammonia and hydrogen nitrogen separating step.Especially hydrogen nitrogen separates, and needs to pass through
The technologies such as PSA or UF membrane carry out hydrogen and nitrogen gas separation.Wherein, PSA unit scale is larger, and expensive, although can get 99.9%
Hydrogen, but yield only 50~70%；And UF membrane yield is up to 90% or more, but purity is only 93~95%, in order to obtain height
Yield high-purity hydrogen needs complicated purification system, sufficiently expensive.Therefore, it needs a kind of high yield and high-purity hydrogen can be obtained
Hydrogen generating system.
Summary of the invention
Therefore, the technical problem to be solved in the present invention is that when ammonolysis craft in the prior art being overcome to prepare hydrogen yield and
Purity can not reach simultaneously the defect of requirement, to provide a kind of electrolysis ammonia hydrogen generating system.
The present invention adopts the following technical scheme:
The present invention provides a kind of electrolysis ammonia hydrogen generating system, including,
Ammonia storage tank；
Hydrogen manufacturing component, including shell, it is placed in the intracorporal electrolytic tank of solid oxide of the shell, the solid oxide electrolyte
Pond includes electrolyte layer and the anode layer and cathode layer for being set to the electrolyte layer opposite sides, the anode layer and power supply
The anode of cathode connection, the cathode layer and power supply connects, and the anode layer and cathode layer are connected with load respectively；It is close
Anode inlet is set in the housing sidewall of the anode layer, and the anode inlet is connected to the ammonia storage tank, close
Cathode gas outlet is set on the cathode layer and the housing sidewall opposite with the anode layer；
Hydrogen collection device is connected to, to collect hydrogen with the cathode gas outlet.
Preferably, the electrolytic tank of solid oxide is anode support type, electrolyte layer thickness in the anode support type
It is 10-30 μm；Anode layer thickness is 300-1000 μm；The cathode electrode layer thickness is 10-50 μm；
Alternatively, the electrolytic tank of solid oxide is electrolyte-supporting type, electrolyte thickness in the electrolyte-supporting type
Degree is 300-1000 μm；Anode layer thickness is 10-50 μm；The cathode electrode layer thickness is 10-50 μm.
Preferably, further include,
Anode gas outlet is disposed in proximity in the housing sidewall of the anode layer, and same with the anode inlet
Side setting by ammonia remaining in the hydrogen manufacturing component and decomposes the nitrogen extraction generated.
Preferably, further include,
Expander, First Heat Exchanger and the second heat exchanger, the ammonia storage tank, the expander and First Heat Exchanger successively connect
Logical setting；
The electrolyte layer be oxygen ion conductor electrolyte layer when, the First Heat Exchanger respectively with the anode inlet
It is connected to anode gas outlet, so that the nitrogen that ammonia is generated with ammonia remaining in the hydrogen manufacturing component and decomposition is described
Indirect heat exchange in First Heat Exchanger；Second heat exchanger is connected to drier, second heat exchanger and the cathode outlet
Mouth connection, the drier are connected to the Hydrogen collection device, so that the hydrogen from the cathode gas outlet passes through second
Enter in the Hydrogen collection device after heat exchanger and drier heat exchange；Alternatively,
The electrolyte layer be proton conductor electrolyte layer when, the expander successively with second heat exchanger, first
Heat exchanger is connected with anode inlet, and the cathode gas outlet is successively connect with second heat exchanger and Hydrogen collection device,
The anode gas outlet is connect with the First Heat Exchanger, so that the ammonia in the ammonia storage tank is in second heat exchanger
Interior and hydrogen exchanges heat, and enters back into interior and remaining in the hydrogen manufacturing component ammonia of the First Heat Exchanger and decomposes generation
Nitrogen heat exchange.
Preferably, when the electrolyte layer is oxygen ion conductor electrolyte layer, further include,
Cathode inlet mouth is disposed in proximity in the housing sidewall of the cathode layer, and same with the cathode gas outlet
Side setting；
Be sequentially communicated water pot and evaporator, the steam outlet of the evaporator successively with second heat exchanger and cathode
Air inlet connection, so that vapor enters in second heat exchanger and after the hydrogen heat exchange from the cathode gas outlet
In the cathode inlet mouth.
Preferably, the anode gas outlet is connected to the anode inlet in hydrogen manufacturing component outer, by the hydrogen manufacturing
Remaining part ammonia is back to the hydrogen manufacturing component in component.
It preferably, further include the anode gas flow channels being coated on the outside of anode layer, the anode inlet and anode outlet
Mouth is connected in hydrogen manufacturing components interior with the anode gas flow channels, is reacted at anode layer so that ammonia enters and makes nitrogen
Gas and remaining ammonia leave hydrogen manufacturing component by anode gas outlet.
It preferably, further include the cathode gas flow channels being coated on the outside of cathode layer,
When the electrolyte layer is oxygen ion conductor electrolyte layer, cathode inlet mouth and cathode gas outlet are in hydrogen manufacturing component
Portion is connected to the cathode gas flow channels, is reacted so that vapor enters at cathode layer and makes hydrogen and residual water vapor
Hydrogen manufacturing component is left by cathode gas outlet；Alternatively,
The electrolyte layer is that proton conductor electrolyte layer is that cathode gas outlet is in hydrogen manufacturing components interior and the cathode gas
Body runner connection, so that hydrogen leaves hydrogen manufacturing component by cathode gas outlet.
Overall reaction of the present invention is 2NH3=N2+3H2。
Electrolyte used in the present invention is different, and anode and cathode half-reaction is not also identical,
If electrolyte includes being not limited to the YSZ (oxidation of stabilized with yttrium oxide using oxygen ion conductor electrolyte
Zirconium), ScSZ (zirconium oxide of scandia stabilized), GDC (cerium oxide of Gd2 O3), SDC (cerium oxide of strontium doping) or LSGM (strontium
One of with the lanthanum gallate of magnesium doping), specific half-reaction are as follows:
Anode: 2NH3+3O2-=N2+3H2O+6e-
Cathode: 3H2O+6e-=3H2+3O2-；
Anode layer material is the conductor material that Ni and electrolyte mix, cathode layer materials be include but is not limited to Ni,
The conductor material of one of LSM (lanthanum-strontium manganese) and LSCF (lanthanum-strontium ferro-cobalt) and electrolyte mixing.
If electrolyte includes being not limited to barium cerate or barium zirconate based perovskite material using proton conductor electrolyte
Material (barium cerate, the doped yttrium barium zirconate of zirconium and doped yttrium barium cerate, the doping of zirconium yttrium ytterbium), specific half-reaction are as follows:
Anode: 2NH3=N2+6H++6e-
Cathode: 6e-+6H+=3H2；
Anode layer material is the conductor material that Ni and electrolyte mix, cathode layer materials be include but is not limited to Ni,
BSCF (barium strontium ferro-cobalt), LSCF, PSCF (praseodymium strontium ferro-cobalt), SSC (samarium strontium cobalt), LSN (lanthanum-strontium nickel), PSN (praseodymium strontium nickel) or PBC
The conductor material of one of (praseodymium barium cobalt) and electrolyte mixing.
Technical solution of the present invention has the advantages that
1. electrolysis ammonia system used in the present invention prepares hydrogen, hydrogen is generated in cathode layer, anode layer generates nitrogen,
To efficiently separate the nitrogen and hydrogen prepared, the hydrogen of high yield high-purity is directly obtained.
2. residue ammonia of the invention is back to anode inlet by pipeline from anode gas outlet, will not be generated with cathode
Hydrogen mixes.
3. present invention setting heat exchanger, so that the high-temperature gas that reaction generates transfers heat to the unstripped gas before reaction
Body, preheating material gas, energy saving in advance.
4. ammonia is also used as the fuel of electrolytic tank of solid oxide to provide electricity for electrolysis hydrogen while present invention electrolysis ammonia
Can, it can also externally generate electricity under hypopolarization；It only needs to input a small amount of electric energy and overcomes polarizing voltage, that is, can reach ideal production hydrogen
Rate.
Detailed description of the invention
It, below will be to specific in order to illustrate more clearly of the specific embodiment of the invention or technical solution in the prior art
Embodiment or attached drawing needed to be used in the description of the prior art be briefly described, it should be apparent that, it is described below
Attached drawing is some embodiments of the present invention, for those of ordinary skill in the art, before not making the creative labor
It puts, is also possible to obtain other drawings based on these drawings.
Fig. 1 is the structural schematic diagram that ammonia device for producing hydrogen is electrolysed in the embodiment of the present invention 1 and 3；
Fig. 2 is the structural schematic diagram that ammonia device for producing hydrogen is electrolysed in the embodiment of the present invention 2；
Fig. 3 is the structural schematic diagram of hydrogen manufacturing component in the embodiment of the present invention 1 and 3；
Fig. 4 is the structural schematic diagram of hydrogen manufacturing component in the embodiment of the present invention 2.
Description of symbols:
1- hydrogen manufacturing component；2- ammonia storage tank；3- Hydrogen collection device；4- expander；5- First Heat Exchanger；6- second exchanges heat
Device；The defeated ammonia pipeline of 7-；8- anode escape pipe；9- cathode escape pipe；10- anode inlet；11- anode gas outlet；12- cathode goes out
Port；13- water pot；14- evaporator；15- aqueduct；16- cathode inlet mouth；17- drier；
101- electrolyte layer；102- anode layer；103- cathode layer；104- power supply；105- shell；106- anodic gas stream
Road；107- cathode gas flow channels；108- load.
Specific embodiment
Technical solution of the present invention is clearly and completely described below in conjunction with attached drawing, it is clear that described implementation
Example is a part of the embodiment of the present invention, instead of all the embodiments.Based on the embodiments of the present invention, ordinary skill
Personnel's every other embodiment obtained without making creative work, shall fall within the protection scope of the present invention.
In the description of the present invention, it should be noted that term " center ", "upper", "lower", "left", "right", "vertical",
The orientation or positional relationship of the instructions such as "horizontal", "inner", "outside" be based on the orientation or positional relationship shown in the drawings, merely to
Convenient for description the present invention and simplify description, rather than the device or element of indication or suggestion meaning must have a particular orientation,
It is constructed and operated in a specific orientation, therefore is not considered as limiting the invention.In addition, term " first ", " second ",
" third " is used for descriptive purposes only and cannot be understood as indicating or suggesting relative importance.
In the description of the present invention, it should be noted that unless otherwise clearly defined and limited, term " installation ", " phase
Even ", " connection " shall be understood in a broad sense, for example, it may be being fixedly connected, may be a detachable connection, or be integrally connected；It can
To be mechanical connection, it is also possible to be electrically connected；It can be directly connected, can also can be indirectly connected through an intermediary
Connection inside two elements.For the ordinary skill in the art, above-mentioned term can be understood at this with concrete condition
Concrete meaning in invention.
As long as in addition, the non-structure each other of technical characteristic involved in invention described below different embodiments
It can be combined with each other at conflict.
Embodiment 1
The present embodiment discloses a kind of electrolysis ammonia hydrogen generating system, uses oxygen ion conductor as electrolyte.
As shown in figure 3, hydrogen manufacturing component 1, including shell 105, it is set to the 105 Inner electrolysis matter layer 101 of shell and setting
In the anode layer 102 and cathode layer 103 of 101 opposite sides of electrolyte layer, the cathode of the anode layer 102 and power supply 104
Connection, the positive of the cathode layer 103 and power supply 104 connect, and the anode layer 102 and cathode layer 103 respectively with load
108 both ends are connected；Anode layer surface is coated with anode gas flow channels 106, and cathode layer is coated with cathode gas flow channels 107, sun
Pole air inlet 10 and anode gas outlet 11 are connected in 1 inside of hydrogen manufacturing component with the anode gas flow channels 106, cathode inlet mouth 16
It is connected in 1 inside of hydrogen manufacturing component with the cathode gas flow channels 107 with cathode gas outlet 12.
The present embodiment electrolytic tank of solid oxide is anode support type, wherein 101 material of oxygen ion conductor electrolyte layer are as follows:
YSZ (zirconium oxide of stabilized with yttrium oxide), anode layer 102 are as follows: Ni-YSZ, the material of cathode layer 103 are as follows: LSM-YSZ；Oxonium ion is led
The thickness of body electrolyte layer 101 are as follows: 15 μm, the thickness of anode layer 102 are as follows: 700 μm, the thickness of cathode layer 103 are as follows: 20 μm；Electricity
104 voltage of source are as follows:+0.3V.
As shown in Fig. 2, the defeated ammonia pipeline 7 that ammonia storage tank 2 is extended in the electrolysis ammonia hydrogen generating system of the present embodiment passes through expansion
The anode inlet 10 of hydrogen manufacturing component 1 is connected to after device 4 by First Heat Exchanger 5；The aqueduct 15 that water pot 13 extends is logical
The cathode inlet mouth 16 of hydrogen manufacturing component 1 is connected to after pervaporation device 14 by the second heat exchanger 6；The anode outlet of hydrogen manufacturing component 1
It is two that the anode escape pipes 8 that mouth 11 extends, which are divided to, and one communicates after First Heat Exchanger 5 with air, one and defeated ammonia pipe
Road 7 is connected；The cathode escape pipe 9 that the cathode gas outlet 12 of hydrogen manufacturing component 1 is extended 6 passes through drier after the second heat exchanger
17 are connected with Hydrogen collection device 3.
After tested, through this embodiment in device carry out ammonia decomposing hydrogen-production, hydrogen yield > 93%, obtained hydrogen
Purity >=99.99%.
Embodiment 2
The present embodiment discloses another electrolysis ammonia hydrogen generating system, uses proton conductor as electrolyte.
As shown in figure 4, hydrogen manufacturing component 1, including shell 105, it is set to the 105 Inner electrolysis matter layer 101 of shell and setting
In the anode layer 102 and cathode layer 103 of 101 opposite sides of electrolyte layer, the cathode of the anode layer 102 and power supply 104
Connection, the positive of the cathode layer 103 and power supply 104 connect, and the anode layer 102 and cathode layer 103 respectively with load
108 both ends are connected；Anode layer surface is coated with anode gas flow channels 106, and cathode layer is coated with cathode gas flow channels 107, sun
Pole air inlet 10 and anode gas outlet 11 are connected in 1 inside of hydrogen manufacturing component with the anode gas flow channels 106, cathode gas outlet 12
It is connected in 1 inside of hydrogen manufacturing component with the cathode gas flow channels 107.
The present embodiment electrolytic tank of solid oxide is anode support type, wherein 101 material of proton conductor electrolyte layer are as follows:
BCZY (barium cerate of zirconium and doped yttrium), anode layer 102 are as follows: Ni-BCZY, the material of cathode layer 103 are as follows: Ni-BCZY；Proton is led
The thickness of body electrolyte layer 101 are as follows: 20 μm, the thickness of anode layer 102 are as follows: 500 μm, the thickness of cathode layer 103 are as follows: 30 μm；Electricity
104 voltage of source are as follows:+0.3V.
As shown in figure 3, the defeated ammonia pipeline 7 that ammonia storage tank 2 is extended in the electrolysis ammonia hydrogen generating system of the present embodiment passes through expansion
The anode inlet 10 of hydrogen manufacturing component 1 is successively connected to after device 4 by the second heat exchanger 6 and First Heat Exchanger 5；Hydrogen manufacturing component 1
The anode escape pipe 8 that extends of anode gas outlet 11 to be divided to be two, one communicates after First Heat Exchanger 5 with air, one
Branch is connected with defeated ammonia pipeline 7；The cathode escape pipe 9 that the cathode gas outlet 12 of hydrogen manufacturing component 1 is extended is 6 after the second heat exchanger
It is connected with Hydrogen collection device 3.
After tested, through this embodiment in device carry out ammonia decomposing hydrogen-production, hydrogen yield > 93%, obtained hydrogen
Purity >=99.99%.
Embodiment 3
The present embodiment discloses a kind of electrolysis ammonia hydrogen generating system, uses oxygen ion conductor as electrolyte.
As shown in figure 3, hydrogen manufacturing component 1, including shell 105, it is set to the 105 Inner electrolysis matter layer 101 of shell and setting
In the anode layer 102 and cathode layer 103 of 101 opposite sides of electrolyte layer, the cathode of the anode layer 102 and power supply 104
Connection, the cathode layer 103 are connect with the anode of power supply 104；Anode layer surface is coated with anode gas flow channels 106, cathode layer
Cathode gas flow channels 107, anode inlet 10 and anode gas outlet 11 are coated in 1 inside of hydrogen manufacturing component and the anodic gas
Runner 106 is connected to, and cathode inlet mouth 16 and cathode gas outlet 12 connect in 1 inside of hydrogen manufacturing component with the cathode gas flow channels 107
It is logical.
The present embodiment electrolytic tank of solid oxide is electrolyte-supporting type, wherein 101 material of oxygen ion conductor electrolyte layer
Are as follows: GDC (cerium oxide of Gd2 O3), anode layer 102 are as follows: Ni-GDC, the material of cathode layer 103 are as follows: LSCF-GDC；Oxonium ion is led
The thickness of body electrolyte layer 101 are as follows: 700 μm, the thickness of anode layer 102 are as follows: 25 μm, the thickness of cathode layer 103 are as follows: 40 μm；Electricity
104 voltage of source are as follows: -0.1V.
As shown in Fig. 2, the defeated ammonia pipeline 7 that ammonia storage tank 2 is extended in the electrolysis ammonia hydrogen generating system of the present embodiment passes through expansion
The anode inlet 10 of hydrogen manufacturing component 1 is connected to after device 4 by First Heat Exchanger 5；The aqueduct 15 that water pot 13 extends is logical
The cathode inlet mouth 16 of hydrogen manufacturing component 1 is connected to after pervaporation device 14 by the second heat exchanger 6；The anode outlet of hydrogen manufacturing component 1
It is two that the anode escape pipes 8 that mouth 11 extends, which are divided to, and one communicates after First Heat Exchanger 5 with air, one and defeated ammonia pipe
Road 7 is connected；The cathode escape pipe 9 that the cathode gas outlet 12 of hydrogen manufacturing component 1 is extended 6 passes through drier after the second heat exchanger
17 are connected with Hydrogen collection device 3.
After tested, through this embodiment in device carry out ammonia decomposing hydrogen-production, hydrogen yield > 93%, obtained hydrogen
Purity >=99.99%.
Embodiment 4
The present embodiment discloses the hydrogen production process that embodiment 1 and 3 is electrolysed ammonia hydrogen generating system.
Liquefied ammonia is entered in expander 4 by defeated ammonia pipeline into 7 from ammonia storage tank 2, is gasified as ammonia, is next proceeded through defeated ammonia pipe
Road 7 enters hydrogen manufacturing component 1 from anode inlet 10 by First Heat Exchanger 5；Water, which is entered from water pot 13 by aqueduct 15, to be steamed
It sends out in device 14, heating evaporation is vapor, next proceeds through aqueduct 15 and passes through the second heat exchanger 6 from cathode inlet mouth 16
Into hydrogen manufacturing component 1；
In hydrogen manufacturing component 1, following reaction occurs:
Anode: 2NH3+3O2-=N2+3H2O+6e-
Cathode: 3H2O+6e-=3H2+3O2-；
Enter anode escape pipe 8 from anode gas outlet 11 in anode gas flow channels 106 in the nitrogen that anode layer 102 generates
In, it is partially reentered into reflux in defeated ammonia pipeline 7 and eliminates remaining ammonia in anode inlet 10, partially changed by first
The ammonia in defeated ammonia pipeline 7 is transferred heat to by First Heat Exchanger 5 when hot device 5, then drains into air；In cathode layer 103
The hydrogen of generation enters in cathode escape pipe 9 in cathode gas flow channels 107 from cathode gas outlet 12, when by the second heat exchanger 6
The vapor in aqueduct 15 is transferred heat to by the second heat exchanger 6, extra water is then removed by drier 17
Point, it is collected later by Hydrogen collection device 3.
Embodiment 5
The present embodiment discloses the hydrogen production process that embodiment 2 is electrolysed ammonia hydrogen generating system.
Liquefied ammonia is entered in expander 4 by defeated ammonia pipeline into 7 from ammonia storage tank 2, is gasified as ammonia, is next proceeded through defeated ammonia pipe
Road 7 enters hydrogen manufacturing component 1 from anode inlet 10 by First Heat Exchanger 5；
In hydrogen manufacturing component 1, following reaction occurs:
Anode: 2NH3=N2+6H++6e-
Cathode: 6e-+6H+=3H2。
Enter in anode escape pipe 8 in the nitrogen that anode layer 102 generates from anode gas outlet 11, partially enters defeated ammonia pipeline
Reflux, which reenters, in 7 eliminates remaining ammonia in anode inlet 10, by the first heat exchange when partially passing through First Heat Exchanger 5
Device 5 transfers heat to the ammonia in defeated ammonia pipeline 7, then drains into air；In the hydrogen that cathode layer 103 generates from cathode outlet
Mouth 12 enters in cathode escape pipe 9, transfers heat in defeated ammonia pipeline 7 by passing through the second heat exchanger 6 when the second heat exchanger 6
Ammonia, collected later by Hydrogen collection device 3.
Comparative example
This comparative example is compared with embodiment 1, and difference place is that this comparative example prepares hydrogen using electrolysis water, device and
The difference of embodiment 1 is no ammonia storage tank, expander, First Heat Exchanger, defeated ammonia pipeline and anode inlet.
Water is entered in evaporator from water pot by aqueduct, and heating evaporation is vapor, next proceeds through water-supply-pipe
Road enters hydrogen manufacturing component from cathode inlet mouth by heat exchanger；
In hydrogen manufacturing component 1, following reaction occurs:
Anode: 3O2-=3/2O2+6e-
Cathode: 3H2O+6e-=3H2+3O2-；
Enter in anode escape pipe in anode gas flow channels from anode gas outlet in the oxygen that anode layer generates, then arranges
Enter air；Enter in cathode escape pipe in cathode gas flow channels from cathode gas outlet in the hydrogen that cathode layer generates, by heat exchange
The vapor in aqueduct is transferred heat to by heat exchanger when device, extra moisture is then removed by drier, it
It is collected afterwards by Hydrogen collection device.
Test example
Hydrogen manufacturing test is carried out with the water electrolysis hydrogen production system of the electrolysis ammonia hydrogen generating system of embodiment 1-3 and comparative example, is measured
The power consumption situation of each system when same hydrogen prepares rate, as a result as shown in the table:
Table 1
| Power consumption (W) | |
| Embodiment 1 | 4.0 |
| Embodiment 2 | 3.2 |
| Embodiment 3 | - 0.4 (power generation) |
| Comparative example | 16.5 |
The present invention can be in electrolysis due to ammonia and a kind of energy carrier of high-energy density using electrolysis ammonia hydrogen manufacturing
It is used as the energy simultaneously, electrolysis energy consumption can be significantly reduced, as seen from the above table, the power consumption of embodiment 1-3 is significantly less than comparative example,
Middle 3 ammonia of embodiment is greater than the energy consumed when hydrogen manufacturing as the energy that fuel generates, and dump energy is converted into electric energy and is supplied to
Load.
Obviously, the above embodiments are merely examples for clarifying the description, and does not limit the embodiments.It is right
For those of ordinary skill in the art, can also make on the basis of the above description it is other it is various forms of variation or
It changes.There is no necessity and possibility to exhaust all the enbodiments.And it is extended from this it is obvious variation or
It changes still within the protection scope of the invention.
Claims (9)
1. a kind of electrolysis ammonia hydrogen generating system, which is characterized in that including,
Ammonia storage tank；
Hydrogen manufacturing component, including shell, it is set to electrolytic tank of solid oxide in the shell, the electrolytic tank of solid oxide packet
It includes electrolyte layer and is set to the anode layer and cathode layer of the electrolyte layer opposite sides, the cathode of the anode layer and power supply
The anode of connection, the cathode layer and power supply connects, and the anode layer and cathode layer are connected with load respectively；Close to described
Anode inlet is set in the housing sidewall of anode layer, and the anode inlet is connected to the ammonia storage tank, close to described
Cathode gas outlet is set on cathode layer and the housing sidewall opposite with the anode layer；
Hydrogen collection device is connected to, to collect hydrogen with the cathode gas outlet.
2. electrolysis ammonia hydrogen generating system according to claim 1, which is characterized in that the electrolytic tank of solid oxide is anode
Support type, electrolyte layer is with a thickness of 10-30 μm in the anode support type；Anode layer thickness is 300-1000 μm；The cathode
Layer is with a thickness of 10-50 μm.
3. electrolysis ammonia hydrogen generating system according to claim 1, which is characterized in that the electrolytic tank of solid oxide is electrolysis
Matter support type, electrolyte layer is with a thickness of 300-1000 μm in the electrolyte-supporting type；Anode layer thickness is 10-50 μm；It is described
Cathode electrode layer thickness is 10-50 μm.
4. electrolysis ammonia hydrogen generating system according to claim 3, which is characterized in that further include,
Anode gas outlet is disposed in proximity in the housing sidewall of the anode layer, and with the anode inlet is ipsilateral sets
It sets, by ammonia remaining in the hydrogen manufacturing component and decomposes the nitrogen extraction generated.
5. electrolysis ammonia hydrogen generating system according to claim 4, which is characterized in that further include,
Expander, First Heat Exchanger and the second heat exchanger, the ammonia storage tank, the expander and First Heat Exchanger are sequentially communicated and set
It sets；
The electrolyte layer be oxygen ion conductor electrolyte layer when, the First Heat Exchanger respectively with the anode inlet and sun
Pole gas outlet connection, so that the nitrogen that ammonia and ammonia remaining in the hydrogen manufacturing component and decomposition generate is described first
Indirect heat exchange in heat exchanger；Second heat exchanger is connected to drier, and second heat exchanger and the cathode gas outlet connect
Logical, the drier is connected to the Hydrogen collection device, so that the hydrogen from the cathode gas outlet is by the second heat exchange
Enter in the Hydrogen collection device after device and drier heat exchange；Alternatively,
When the electrolyte layer is proton conductor electrolyte layer, the expander successively exchanges heat with second heat exchanger, first
Device is connected with anode inlet, and the cathode gas outlet is successively connect with second heat exchanger and Hydrogen collection device, described
Anode gas outlet is connect with the First Heat Exchanger so that the ammonia in the ammonia storage tank in second heat exchanger with
Hydrogen heat exchange enters back into the nitrogen generated in the First Heat Exchanger with ammonia remaining in the hydrogen manufacturing component and decomposition
Heat exchange.
6. electrolysis ammonia hydrogen generating system according to claim 5, which is characterized in that the electrolyte layer is oxygen ion conductor electricity
When solving matter layer, further include,
Cathode inlet mouth is disposed in proximity in the housing sidewall of the cathode layer, and with the cathode gas outlet is ipsilateral sets
It sets；
Be sequentially communicated water pot and evaporator, the steam outlet of the evaporator successively with second heat exchanger and cathode inlet
Mouthful connection, so that vapor is in second heat exchanger and after the hydrogen heat exchange from the cathode gas outlet, into described
In cathode inlet mouth.
7. electrolysis ammonia hydrogen generating system according to claim 6, which is characterized in that the anode gas outlet and the anode into
Port is connected in hydrogen manufacturing component outer, and part ammonia remaining in the hydrogen manufacturing component is back to the hydrogen manufacturing component.
8. electrolysis ammonia hydrogen generating system according to claim 7, which is characterized in that further include the sun being coated on the outside of anode layer
Pole gas flow, the anode inlet and anode gas outlet are connected in hydrogen manufacturing components interior with the anode gas flow channels, with
Entering ammonia is reacted at anode layer and is made nitrogen and remaining ammonia to leave hydrogen manufacturing component by anode gas outlet.
9. electrolysis ammonia hydrogen generating system according to claim 8, which is characterized in that further include the yin being coated on the outside of cathode layer
Pole gas flow,
When the electrolyte layer is oxygen ion conductor electrolyte layer, cathode inlet mouth and cathode gas outlet are in hydrogen manufacturing components interior
It is connected to the cathode gas flow channels, is reacted and made hydrogen and residual water vapor logical so that vapor enters at cathode layer
It crosses cathode gas outlet and leaves hydrogen manufacturing component；Alternatively,
It is that cathode gas outlet is in hydrogen manufacturing components interior and the cathode gas when the electrolyte layer is proton conductor electrolyte layer
Runner connection, so that hydrogen leaves hydrogen manufacturing component by cathode gas outlet.
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