CN106757129B - A kind of tubular type double ion type electrolytic cell - Google Patents
A kind of tubular type double ion type electrolytic cell Download PDFInfo
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- CN106757129B CN106757129B CN201710064333.4A CN201710064333A CN106757129B CN 106757129 B CN106757129 B CN 106757129B CN 201710064333 A CN201710064333 A CN 201710064333A CN 106757129 B CN106757129 B CN 106757129B
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- 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
- C25B9/70—Assemblies comprising two or more cells
- C25B9/73—Assemblies comprising two or more cells of the filter-press type
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- 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
- C25B1/04—Hydrogen or oxygen by electrolysis of water
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- 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
- C25B13/00—Diaphragms; Spacing elements
- C25B13/02—Diaphragms; Spacing elements characterised by shape or form
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- 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
- C25B13/00—Diaphragms; Spacing elements
- C25B13/04—Diaphragms; Spacing elements characterised by the material
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- 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
- C25B9/05—Pressure cells
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- 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
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- 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
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
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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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- Inorganic Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The present invention provides a kind of tubular type double ion type electrolytic cells, including metal tube, oxygen channel, cathode, catholyte layer, water vapor channel, anodolyte layer, anode and hydrogen paths are set gradually with tubular structure from the inner casing of the metal tube toward metal tube center position.A kind of tubular type double ion type electrolytic cell of the present invention, simple in structure, gas concentration polarization potential can substantially reduce, and the efficiency of hydrolytic hydrogen production can be increased to 70% or more.
Description
Technical field
The present invention relates to a kind of electrolytic cell, more particularly to a kind of tubular type double ion type electrolytic cell.
Background technology
Power-to-Gas is one of distributed energy technology trends, and being converted electric energy to by electrolysis water can be steady
Surely the hydrogen stored.Hydrogen by Natural Gas Pipeline Transportation, can also compression hydrogen to high pressure gas holder, transported by the vehicles
To electricity usage region, off grid power demand is solved.When the effect of hydrogen can also be embodied in electric power low ebb, low-price electricity is converted
It is stored at stable chemical substance, carries out supply of electric power in power tense period, play the role of electricity consumption peak load shifting.
Common electrolysis water technology is divided into alkali formula electrolysis water technology and high-temperature electrolysis water technology, from the angle of thermodynamics and kinetics
It is said on degree, high-temperature electrolysis hydrogen manufacturing can convert electric energy to chemical energy with greater efficiency.Such as high-temperature electrolysis sink can reach
Close to 100% transformation efficiency, part energy generates heat, and a part is converted into chemical energy：Hydrogen.Polymer film electrolysis effect
Rate is generally 50% or so, and alkaline electrolysis technical efficiency is lower.
High temperature electrolyser usually has three-decker：Anode, cathode, electrolyte.Using pure water as electrolyte, reaction equation is：Anode is vapor reacting environment and the place that hydrogen generates, and cathode is the place that oxygen generates,
Electrolyte is the medium that oxonium ion transmits.Usual anode, cathode are porous electrodes, should meet gas and be spread in electrode,
Meet the transmission of the proton (or oxonium ion) after electronics, ionization.And electrolyte is compacted zone, in addition to meeting oxygen ion transport, also
Play the role of detaching yin, yang the two poles of the earth gas.The work area of single electrolytic cell is limited, in order to reach scale electrolysis water system
Hydrogen usually gets up several electrolytic cell connection in series-parallel, and reaction gas vapor and hydrogen product mix in electrolytic cell
Flowing, one side mixed gas can reduce the reaction rate of vapor, and another aspect mixed gas also counteracts that hydrogen is arranged in time
Go out, this namely so-called gas concentration polarization potential.
Traditional electrolytic cell three-decker design cannot solve gas concentration polarization potential, only be set by new structure
Reactant, product separation could thoroughly be solved for meter.The heat safe cermet of material generally use of high temperature electrolyser, knot
There is flat and tubular structure using more in terms of structure.Compared to more flat, tubular structure connection is simple, need not seal.
Since the cost of cell materials under hot conditions is higher, the service life is also relatively short, and therefore, further improving electrolytic efficiency is
The trend of high-temperature electrolysis water technology development.
The entitled production hydrogen battery (Patent No. CN201180061466.7) including high temperature steam electrolytic pond battery it is special
It includes metal tube that sharp document, which discloses the battery with tubular geometry, and is placed sequentially in the lateral surface week of the metal tube
The porous anode of the high temperature steam electrolytic pond battery enclosed, the dense electrolyte in high temperature steam electrolytic pond, high temperature steam electrolytic pond
Porous cathode, the porous thick-layer with open-cell porosity, the porous anode of electrochemical pump, the dense electrolyte of electrochemical pump, electricity
The porous cathode and external metallization pipe of chemical pumping.Vapor is after the porous thick-layer entrance with open-cell porosity in high-temperature steam
Resolve into hydrogen and oxonium ion on the porous cathode of electrolytic cell, hydrogen after the porous anode of electrochemical pump is converted to hydrogen ion according to
Enter the porous cathode of the one layer of electrochemical pump in outside after the secondary dense electrolyte by electrochemical pump and is reduced into porous cathode
It is flowed out after hydrogen, to the porous sun of high temperature steam electrolytic pond battery after the dense electrolyte that oxonium ion passes through high temperature steam electrolytic pond
Pole spreads and is oxidized to oxygen in porous anode, and oxygen is flowed into metal tube from the hole of metal tube and flowed out from metal tube.
Battery structure in the patent document is more complex, and the active layer of water electrolysis reaction is the porous cathode and high-temperature steam of electrochemical pump
The porous anode of electrolyzer cells, the intermediate porous thick-layer being mingled with simultaneously are not involved in reaction, and such a structure increases gas diffusion poles
Electrochemical potential affects the transformation efficiency of hydrogen.
Invention content
The present invention is intended to provide the tubular type of a kind of efficiency simple in structure, that hydrolytic hydrogen production can be improved, raising hydrogen conversion
Double ion type electrolytic cell.The present invention is realized by following scheme：
A kind of tubular type double ion type electrolytic cell, including metal tube, from the inner casing of the metal tube toward metal tube center position
Oxygen channel, cathode, catholyte layer, water vapor channel, anodolyte layer, anode and hydrogen are set gradually with tubular structure
Gas channel.
Further, in the oxygen channel, water vapor channel and hydrogen paths gas flowing use inert gas for
The pressure general control of carrier, the oxygen channel, water vapor channel and hydrogen paths is 0.5~1.0bar, by detecting
Mouth pressure realizes channel pressure control.Oxygen channel is used for the outflow of product oxygen, and hydrogen paths are used for the outflow of hydrogen product,
Water vapor channel is used to be electrolysed the inflow of vapor.Oxygen channel, water vapor channel and hydrogen paths pass through segregative inertia
Gas can obtain the product of higher concentration as carrier, and channel pressure may be implemented by controlling flow rate of carrier gas, can also reduce
Polarization potential.Inert gas is generally or mixtures thereof nitrogen, argon gas, it is contemplated that cost problem, it is generally preferable to nitrogen.
Further, the gas flow in the oxygen channel and hydrogen paths with the gas in the water vapor channel
Flow direction is opposite, and such design can make the distribution of electrolytic cell reaction gases concentration difference minimum.
Further, the catholyte layer is cerium oxide (YDC) ceramic material of the yttrium stabilization of filming densification, institute
State barium cerate (BCY) ceramic material that anodolyte layer is filming densification, the catholyte layer and anodolyte
The thickness of layer is 10~50 μm.Anodolyte layer only transmits hydrogen ion H+, catholyte layer only transmits oxonium ion O2-, and
Two layers of electrolyte layer is compact texture, is not in phenomenon of collaborating in this way.
Further, the cathode is made of foamed nickel supported yttria stabilized zirconia (being abbreviated as Ni/YSZ),
Thickness is 100~200 μm, and porosity is 40~60%；The anode uses foamed nickel supported barium cerate (being abbreviated as Ni/BCY)
It is made, thickness is 50~100 μm, and porosity is 40~60%；The water vapor channel using titanium foam load barium cerate and
The mixture (being abbreviated as Ti/ (BCY+YDC)) for the cerium oxide composition that yttrium is stablized is made, and thickness is 100~500 μm.Ni/YSZ、
Ni/BCY and Ti/ (BCY+YDC) is porous metalloceramic composite material.
The shell of the metal tube is made of heat safe metal or composite material, and resistance to pressure pressure is 5~10bar；
The inner casing of metal tube is made of composite material, and resistance to pressure pressure is 10~20bar.Hydrogen is separated from hydrogen paths, is examined
Vapor is considered to the corrosion-free effect of the shell of the metal tube of electrolytic cell, thus metal or composite wood may be used in metal tube envelope
Material is made.
It is compared with the patent document of the entitled production hydrogen battery including high temperature steam electrolytic pond battery, a kind of pipe of the invention
Formula double ion type electrolytic cell, it is simple in structure, two layers of compacted zone i.e. anodolyte layer and catholyte layer are devised, is passed respectively
Hydrogen ion and oxonium ion are led, three layers of porous layer, that is, water vapor channel, anode and cathode are used separately as vapor conversion zone, hydrogen
Generation layer and oxygen generation layer, hydrogen ion are only needed by being reduced into hydrogen after anodolyte layer on anode, hydrogen from
Hydrogen paths flow out, and the present invention is compared with the document of comparison patent No. CN201180061466.7, because electrochemistry is omitted
The porous anode of pump reduces the thickness of water electrolysis layer, to which the formation efficiency of hydrogen can be improved.In addition, comparison patent document
In (Patent No. CN201180061466.7), hydrogen is flowed out from the porous cathode of outermost electrochemical pump, and oxygen is from most interior
The metal tube outflow of layer；And in the present invention, oxygen channel is designed in outermost layer, in this way can to the requirement of the material selection of metal tube
To reduce；Water vapor channel, that is, hydrolysis layer, design hydrolysis under centre position, high temperature need not use precious metal catalyst
Agent, water vapor channel are made using foam metal material；By hydrogen runner design in innermost layer, on the one hand can effectively control
Hydrogen is revealed, and anode active area, the design of the hydrogen of the two and the flow pass of oxygen on the other hand can be effectively increased
It is completely opposite.It designing through the invention, gas concentration polarization potential can substantially reduce, to optimize the efficiency of hydrolytic hydrogen production,
Hydrogen formation efficiency is up to 70% or more.The tubular type double ion type electrolytic cell of the present invention, Seal Design is simple, without series connection, passes through
Several long tubes are simultaneously unified into pile realization relatively high power output.
Description of the drawings
Fig. 1 is the cross-sectional view of tubular type double ion type electrolytic cell in embodiment 1.
Specific implementation mode
Invention is further described in detail with reference to the accompanying drawings and examples, but the invention is not limited in embodiments
Statement.
Embodiment 1
A kind of tubular type double ion type electrolytic cell, as shown in Figure 1, including metal tube 1, from the inner casing of metal tube 1 toward metal tube 1
Center position sets gradually oxygen channel 2, cathode 3, catholyte layer 4, water vapor channel 5, anode electrolysis with tubular structure
The shell of matter layer 6, anode 7 and hydrogen paths 8, metal tube 1 is made of heat safe metal or composite material, resistance to pressure pressure
For 5bar；The inner casing of metal tube 1 is made of composite material, and resistance to pressure pressure is 10bar, and the length of metal tube 1 is about 1m, gold
The outer diameter (outer diameter of i.e. entire electrolytic cell) for belonging to pipe shell is about 1cm, the internal diameter (internal diameter of i.e. entire electrolytic cell) of hydrogen runner
About 0.4cm；Catholyte layer 4 is the YDC ceramic materials of filming densification, and anodolyte layer 6 is that filming is fine and close
The thickness of BCY ceramic materials, catholyte layer 4 and anodolyte layer 6 is 10 μm；Cathode 3 uses porous metalloceramic
Composite material Ni/YSZ is made, and thickness is 100 μm, porosity 40%；Anode 7 uses porous metalloceramic composite material
Ni/BCY is made, and thickness is 50 μm, porosity 40%；Water vapor channel 5 is using porous metalloceramic composite material Ti/
(BCY+YDC) it is made, thickness is 100 μm；Gas flowing in oxygen channel 2, water vapor channel 5 and hydrogen paths 8 is adopted
It is carrier with nitrogen, the pressure control of oxygen channel 2, water vapor channel 5 and hydrogen paths 8 is 0.5bar, oxygen channel 2 and hydrogen
Gas flow in gas channel 8 is opposite with the gas flow in water vapor channel 5.
By the formation electrolytic cell group together parallel with one another of the tubular type double ion type electrolytic cell in 50 the present embodiment 1, work
It is 750 DEG C to make temperature design, and electrolysis operating voltage is set as 1.5V, working current density 1.5A/cm2, using the electrolytic cell group,
Hydrogen output can reach 7.8Nm3/ h, water electrolysis transformation efficiency reach 90% or so, and hydrogen formation efficiency is up to 75% or so.
Embodiment 2
A kind of tubular type double ion type electrolytic cell, structure and a kind of tubular type double ion type electrolytic cell in embodiment 1 are similar
Seemingly, the difference is that：
1, the resistance to pressure pressure of the shell of metal tube is 7.5bar, and the resistance to pressure pressure of the inner casing of metal tube is 15bar；
2, the thickness of cathode is 150 μm, porosity 50%；The thickness of anode is 75 μm, porosity 50%；Vapor
The thickness in channel is 300 μm；
3, the pressure control of oxygen channel, water vapor channel and hydrogen paths is 0.75bar；
4, the thickness of catholyte layer and anodolyte layer is 30 μm；
5, it is carrier that gas flowing, which is all made of argon gas, in oxygen channel, water vapor channel and hydrogen paths.
Embodiment 3
A kind of tubular type double ion type electrolytic cell, structure and a kind of tubular type double ion type electrolytic cell in embodiment 1 are similar
Seemingly, the difference is that：
1, the resistance to pressure pressure of the shell of metal tube is 10bar, and the resistance to pressure pressure of the inner casing of metal tube is 20bar；
2, the thickness of cathode is 200 μm, porosity 60%；The thickness of anode is 100 μm, porosity 60%；Water steams
The thickness in gas channel is 500 μm；
3, the pressure control of oxygen channel, water vapor channel and hydrogen paths is 1.0bar；
4, the thickness of catholyte layer and anodolyte layer is 50 μm；
5, in oxygen channel, water vapor channel and hydrogen paths gas flowing use the mixed gas of nitrogen and argon gas for
Carrier.
Claims (6)
1. a kind of tubular type double ion type electrolytic cell, including metal tube, it is characterised in that：From the inner casing of the metal tube toward metal tube
Center position with tubular structure set gradually oxygen channel, cathode, catholyte layer, water vapor channel, anodolyte layer,
Anode and hydrogen paths.
2. a kind of tubular type double ion type electrolytic cell as described in claim 1, it is characterised in that：The oxygen channel, vapor
Gas flowing in channel and hydrogen paths uses inert gas for carrier, and the oxygen channel, water vapor channel and hydrogen are logical
The pressure control in road is 0.5~1.0bar.
3. a kind of tubular type double ion type electrolytic cell as claimed in claim 2, it is characterised in that：The oxygen channel and hydrogen are logical
Gas flow in road is opposite with the gas flow in the water vapor channel.
4. a kind of tubular type double ion type electrolytic cell as described in claim 1, it is characterised in that：The catholyte layer is thin
The ceria oxide ceramics material that the yttrium of membranization densification is stablized, the anodolyte layer are the barium cerate ceramics material of filming densification
The thickness of material, the catholyte layer and anodolyte layer is 10~50 μm.
5. a kind of tubular type double ion type electrolytic cell as described in claim 1, it is characterised in that：The cathode is negative using nickel foam
It carries yttria stabilized zirconia to be made, thickness is 100~200 μm, and porosity is 40~60%；The anode uses nickel foam
Load barium cerate is made, and thickness is 50~100 μm, and porosity is 40~60%；The water vapor channel is negative using titanium foam
The mixture for carrying the cerium oxide composition that barium cerate and yttrium are stablized is made, and thickness is 100~500 μm.
6. a kind of tubular type double ion type electrolytic cell as described in Claims 1 to 5 is any, it is characterised in that：The metal tube
Shell is made of heat safe metal or composite material, and resistance to pressure pressure is 5~10bar；The inner casing of metal tube is using compound
Material is made, and resistance to pressure pressure is 10~20bar.
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5350496A (en) * | 1992-08-13 | 1994-09-27 | United Technologies Corporation | Solid state high pressure oxygen generator and method of generating oxygen |
| CN1129746A (en) * | 1994-10-28 | 1996-08-28 | 日本电气株式会社 | Electrolytic ionized water producing apparatus |
| CN101886270A (en) * | 2009-04-30 | 2010-11-17 | 通用汽车环球科技运作公司 | Be used for from the high pressure electrolysis cell of water hydrogen manufacturing |
| CN102186781A (en) * | 2008-10-17 | 2011-09-14 | 有限会社春天 | Apparatus for producing hydrogen-dissolved drinking water and process for producing the dissolved drinking water |
| CN103261483A (en) * | 2010-12-20 | 2013-08-21 | 法国原子能及替代能源委员会 | Cell for producing hydrogen comprising high-temperature steam electrolysis cell |
| CN103613066A (en) * | 2013-11-22 | 2014-03-05 | 山东理工大学 | Technique for preparing synthetic gas from wet carbon dioxide by electrocatalysis |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP6069412B2 (en) * | 2015-05-28 | 2017-02-01 | 株式会社ＴｒアンドＫ | Simple electrolytic hydrogen gas generator |
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2017
- 2017-02-04 CN CN201710064333.4A patent/CN106757129B/en active Active
Patent Citations (6)
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|---|---|---|---|---|
| US5350496A (en) * | 1992-08-13 | 1994-09-27 | United Technologies Corporation | Solid state high pressure oxygen generator and method of generating oxygen |
| CN1129746A (en) * | 1994-10-28 | 1996-08-28 | 日本电气株式会社 | Electrolytic ionized water producing apparatus |
| CN102186781A (en) * | 2008-10-17 | 2011-09-14 | 有限会社春天 | Apparatus for producing hydrogen-dissolved drinking water and process for producing the dissolved drinking water |
| CN101886270A (en) * | 2009-04-30 | 2010-11-17 | 通用汽车环球科技运作公司 | Be used for from the high pressure electrolysis cell of water hydrogen manufacturing |
| CN103261483A (en) * | 2010-12-20 | 2013-08-21 | 法国原子能及替代能源委员会 | Cell for producing hydrogen comprising high-temperature steam electrolysis cell |
| CN103613066A (en) * | 2013-11-22 | 2014-03-05 | 山东理工大学 | Technique for preparing synthetic gas from wet carbon dioxide by electrocatalysis |
Non-Patent Citations (1)
| Title |
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| "EDTA-柠檬酸络合法制备(Ce0.8Y0.2-XNdxO1.9)0.99(ZnO)0.01电解质材料及其性能研究";李淑君 等;《无机材料学报》;20120214;第27卷(第3期);第265-270页 * |
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