CN106987859A - The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition - Google Patents
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition Download PDFInfo
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- CN106987859A CN106987859A CN201710292185.1A CN201710292185A CN106987859A CN 106987859 A CN106987859 A CN 106987859A CN 201710292185 A CN201710292185 A CN 201710292185A CN 106987859 A CN106987859 A CN 106987859A
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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
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- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- C25D3/00—Electroplating: Baths therefor
- C25D3/02—Electroplating: Baths therefor from solutions
- C25D3/46—Electroplating: Baths therefor from solutions of silver
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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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Abstract
The invention discloses a kind of method for preparing the different morphologies Ag base oxygen-separating catalyst membrane materials for electrolysis water in a mild condition, this method is under normal temperature, normal pressure, weak basic condition, Ag base catalyst films are prepared by electrochemical method original position, it is a kind of simple to operate, easily controllable technical scheme of course of reaction.Concrete scheme is：The ammoniacal liquor complexing agent that can be complexed with Ag+ is added in organic carboxylate, to change the metal existing forms of Ag+ in the solution, then passes through potentiostatic method in-situ deposition, you can obtain Ag（Ⅱ）Base oxygen-separating catalyst membrane material, and when the addition of ammoniacal liquor complexing agent is different, resulting its pattern of Ag bases catalyst is different.Ag base oxygen-separating catalysts prepared by this method have relatively low overpotential, electrolysis 10h still shows higher catalytic activity and stability in the basic conditions, and preparation technology is simple, provides a kind of new Oxygen anodic evolution material for water electrolysis hydrogen production, is with a wide range of applications.
Description
Technical field
The invention belongs to inorganic functional material and electrochemical technology field, specifically a kind of electro-deposition in situ prepares electrolysis water
The method of Ag base oxygen-separating catalyst membrane materials, particularly one kind prepare different morphologies in organic carboxylate using electrochemical method
Ag base oxygen-separating catalyst membrane material methods.
Background technology
It is well known that traditional fossil energy reserves such as coal, oil, natural gas increasingly fall sharply, and people are to the need of the energy
Asking but gradually increases, it is contemplated that to mid-21st Century, and global Energy Consumption at least increases by 2 times till now, and energy crisis increasingly adds
It is acute；The problem of environmental pollutions such as the greenhouse effects, the haze that are brought by traditional energy are also increasingly highlighted, and develop clean reproducible energy
It is extremely urgent.The recyclability and neutral carbon of solar energy not only can meet energy demand instead of fossil fuel, can also solve
The environmental problem that traditional energy is brought, but there is the defects such as dispersiveness, unstability in solar energy, it is therefore desirable to a kind of economical and effective
Mode convert and store solar energy.Hydrogen Energy so that its is lasting, stably, cleaning, calorific value is high, thermal conductivity is good etc., and advantage turns into preferably
Energy carrier.The water electrolysis hydrogen production technology of Driven by Solar Energy can avoid the defect of solar energy, realize that it is efficiently utilized.Electrolysis water sun
Pole oxygen evolution reaction is the deterministic process of energy conversion and storage, is also the bottleneck of water oxygen hydrogen producing technology, course of reaction is related to 4
The reduction group of individual electronics and catalyst surface, which reacts, makes water be oxidized generation oxygen.The key of oxygen evolution reaction is O-H keys
Fracture and O -- O bond formation；Shown in the half-reaction of water decomposition --- oxygen evolution reaction process such as formula (1).Oxygen anodic evolution catalyst
The avtive spot reacted with 4 electronics need to be provided, its catalytic performance decides power consumption height and hydrogen production efficiency, therefore, system
Standby efficient Oxygen anodic evolution catalyst is the key of the water electrolysis hydrogen production technology of Driven by Solar Energy.
2H2O(l) →O2(g)+4H+(aq)+4e− (1)
Existing Ag bases Oxygen anodic evolution catalyst has relatively low overpotential for oxygen evolution and is easy to the crystal structure of modulation, at present
Develop Ag-B i And Ag-C i Oxygen-separating catalyst [International Journal of Hydrogen Energy. 2011,
36:7374；International Journal of Hydrogen Energy. 2013;38:5251].And electricity is heavy in the original location
Electrolytic anion is both the part of catalyst during product, is the acceptor of PCET process protons again, electrolytic anion is with urging
Bonding action is too strong between agent Ag clusters, is unfavorable for the transfer process of proton, so as to cause its electricity of Ag base Oxygen anodic evolutions catalyst
Solve efficiency relatively relatively low, have a strong impact on its application.Therefore, existing inorganic cushioning liquid electrolytic anion all with Ag+Bonding
Effect is stronger, it is impossible to solve this problem well.
The content of the invention
It is an object of the invention to provide the side that a kind of electro-deposition in situ prepares electrolysis water Ag base oxygen-separating catalyst membrane materials
Method, this method is under normal temperature, normal pressure, weak basic condition, to prepare Ag base catalyst films by electrochemical method original position, be one
Plant simple to operate, the easily controllable technical scheme of course of reaction.It can be complexed by being added in organic carboxylate with Ag+
Ammoniacal liquor complexing agent, to change the metal existing forms of Ag+ in the solution, then passes through potentiostatic method in-situ deposition, you can obtain Ag
（Ⅱ）Base oxygen-separating catalyst membrane material, and when the addition of ammoniacal liquor complexing agent is different, resulting its shape of Ag bases catalyst
Looks are different, and show during electrolysis water excellent catalytic activity and stability.
The technical solution used in the present invention is：
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material, comprises the following steps under a kind of temperate condition：
（1）, electro-conductive glass ITO substrate preparation
Electro-conductive glass is standby after being cleaned by ultrasonic；
（2）, silver nitrate solution preparation
The pure silver nitrate solid of analysis is weighed, silver nitrate solution is prepared；
（3）, electrolyte solution configuration
Take C2H3KO2Be dissolved in ultrasonic water, it is to be dissolved after, add NH3H2O, stirs, now, now the pH of potassium acetate solution
For 10.1 ~ 10.8；Micropore ceramics glass is moved to afterwards as anode, the cathode chamber of the H type electrolytic cells of barrier film；Pipette and match somebody with somebody again afterwards
The silver nitrate of system adds anode chamber, identical with cathode chamber solution volume to anode chamber；
（4）, in situ prepare
Using the electrochemical workstation of three-electrode system, using platinum post electrode as auxiliary electrode, Ag/AgCl electrodes are used as reference electricity
Pole, electro-conductive glass makes electro-conductive glass part be contacted with electrolyzer anode chamber solution, H type electrolytic cells is fixed as working electrode
In Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, catalyst film material is prepared.
It is preferred that, step（4）In, the temperature of Water Tank with Temp.-controlled is 25 DEG C；Decomposition voltage is 1.3 vs. NHE, when by leading
The electricity of electric glass surface stops when being 1.5 coulombs.
Step（3）In, the pH of potassium acetate solution is 10.19, then the product finally prepared is rectangular bulk, rough surface by
Little particle is constituted.
Step（3）In, the pH of potassium acetate solution is 10.40, then the product finally prepared is rectangular bulk, rough surface by
Little particle is constituted.
Step（3）In, the pH of potassium acetate solution is 10.64, then the product finally prepared is the pane for having clipped corner
Shape.
Step（3）In, the pH of potassium acetate solution is 10.72, then the product finally prepared is that knitting wool is spherical, rough surface by
Very macroscopic void is constituted.
The key technology of the inventive method is to select electrolytic anion and Ag+The weaker organic carboxylate of bonding action
Complexing agent NH is added as buffer electrolyte, and by original position3H2O mode, changes Ag+There is shape in metal in the solution
State, makes this problem be well solved.Ag (II) the base oxygen-separating catalyst obtained by constant potential coulomb method original position, it is urged
Change activity and stability is all greatly improved.
The present invention has advantages below compared with prior art：
1st, this method preparation condition is gentle（Normal temperature, normal pressure, pH=10.19 ~ 10.72）, method is simple, easily controllable.
2nd, the present invention prepares Ag base catalyst in organic carboxylate situ electro-deposition, and first passage original position is added
Complexing agent NH3H2O mode, changes Ag+ metallic state, promotes Ag+ anodic deposition.
3rd, the present invention is to prepare Ag base oxygen-separating catalysts in the electro-deposition of potassium acetate situ, according to being total to for organic carboxylate
Property, other organic carboxylates are extended to, are to prepare Ag base catalyst in other organic carboxylates to open direction.
4th, Ag bases catalyst prepared by the present invention is Ag (II) oxide, and Ag (II) oxygen is regulated and controled by the amount of modulation complexing agent
The appearance structure of compound oxygen-separating catalyst.
The present invention is reasonable in design, and the Ag base oxygen-separating catalysts of preparation have relatively low overpotential, are electrolysed in the basic conditions
10h still shows higher catalytic activity and stability, and preparation technology is simple, for water electrolysis hydrogen production provide it is a kind of newly
Oxygen anodic evolution material, is with a wide range of applications.
Brief description of the drawings
Fig. 1 a represent the electron scanning Electronic Speculum SEM figures of the products therefrom of embodiment 2（10μm）.
Fig. 1 b represent the electron scanning Electronic Speculum SEM figures of the products therefrom of embodiment 2（500nm）.
Fig. 2 represents the X ray diffracting spectrum of the products therefrom of embodiment 2（XRD）Figure.
Fig. 3 represents the products therefrom of embodiment 2 in 0.1M K3PO4In chronoa mperometric plot.
Embodiment
The present invention will be further described with reference to the accompanying drawings and examples.
Embodiment 1
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material, comprises the following steps under a kind of temperate condition：
1st, by thickness be 1.8mm, sheet resistance be 8.6 ± 1.0 Ω/sq specifications ITO electro-conductive glass be cut into size be 1cm ×
5cm slide, distinguishes ultrasound 5 minutes by the slide cut out in acetone and absolute ethyl alcohol, is then cleaned with ultra-pure water dry successively
It is net standby.
2nd, the pure silver nitrate solid of analysis of certain mass is weighed, 100mL 0.02mol/L silver nitrate solution is prepared.
3rd, 0.9814g C are weighed2H3KO2Be dissolved in the ultrasonic water of 100mL, it is to be dissolved after, add 3.3mol/L's with liquid-transfering gun
NH3H2The μ L of O 40, stir, and now the pH of potassium acetate solution is 10.19.Micropore ceramics glass is moved to afterwards as the H of barrier film
In type electrolytic cell, anode, cathode chamber respectively add 38mL and 40mL.The silver nitrate that the above-mentioned preparations of 2mL are pipetted with pipette adds sun
Pole room.
4th, using the electrochemical workstation of three-electrode system, using platinum post electrode (φ 1mm × 5mm) as auxiliary electrode,
Ag/AgCl electrodes are as reference electrode, and electro-conductive glass makes electro-conductive glass 1cm × 1cm parts and electrolytic cell sun as working electrode
Pole room solution is contacted, and H type electrolytic cells is fixed in 25 DEG C of Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, decomposition voltage
For 1.3 vs. NHE.Stop when being 1.5 coulombs by the electricity of conductive glass surface.
Experiment shows：In embodiment 1, a thick layer grey black color substance, XRD analysis can be generated on anode ITO surfaces
It is AgO to show it.Sem analysis is carried out to it, it is made up of in rectangular block and rough surface little particle.It is in 0.1M K3PO4
Middle current density is 2.4mA/cm2, and it is electrolysed after 10h, current density is without being decreased obviously.
Embodiment 2
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material, comprises the following steps under a kind of temperate condition：
1st, by thickness be 1.8mm, sheet resistance be 8.6 ± 1.0 Ω/sq specifications ITO electro-conductive glass be cut into size be 1cm ×
5cm slide, distinguishes ultrasound 5 minutes by the slide cut out in acetone and absolute ethyl alcohol, is then cleaned with ultra-pure water dry successively
It is net standby.
2nd, the pure silver nitrate solid of analysis of certain mass is weighed, 100mL 0.02mol/L silver nitrate solution is prepared.
3rd, 0.9814g C are weighed2H3KO2Be dissolved in the ultrasonic water of 100mL, it is to be dissolved after, add 3.3mol/L's with liquid-transfering gun
NH3H2The μ L of O 70, stir, and now the pH of potassium acetate solution is 10.40.Micropore ceramics glass is moved to afterwards as the H of barrier film
In type electrolytic cell, anode, cathode chamber respectively add 38mL and 40mL.The silver nitrate that the above-mentioned preparations of 2mL are pipetted with pipette adds sun
Pole room.
4th, using the electrochemical workstation of three-electrode system, using platinum post electrode (φ 1mm × 5mm) as auxiliary electrode,
Ag/AgCl electrodes are as reference electrode, and electro-conductive glass makes electro-conductive glass 1cm × 1cm parts and electrolytic cell sun as working electrode
Pole room solution is contacted, and H type electrolytic cells is fixed in 25 DEG C of Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, decomposition voltage
For 1.3 vs. NHE.Stop when being 1.5 coulombs by the electricity of conductive glass surface.
Experiment shows：In embodiment 2, a thick layer grey black color substance can be generated on anode ITO surfaces, it is carried out
XRD analysis as shown in Fig. 2 its be AgO, show that we are adding NH3H2Obtained in O potassium acetate by the method for electro-deposition in situ
High price Ag oxides, this is also likely to be the most immediate cause for causing its catalytic activity high.It is carried out sem analysis such as Fig. 1 a and
Shown in 1b, it increases in rectangular block and surface roughness compared with embodiment 1, is made up of little particle, adds itself and electrolyte
Contact area, and then be conducive to its Oxygen anodic evolution.As shown in figure 3, it is in 0.1M K3PO4Middle current density is 3.5mA/cm2, it is
The Ag-B previously prepared i With nearly 2 times of oxygen-separating catalyst current density, Ag-C i Nearly 7 times of oxygen-separating catalyst current density, and
It is electrolysed after 10h, current density shows excellent catalytic activity and stability without decline.
Embodiment 3
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material, comprises the following steps under a kind of temperate condition：
1st, by thickness be 1.8mm, sheet resistance be 8.6 ± 1.0 Ω/sq specifications ITO electro-conductive glass be cut into size be 1cm ×
5cm slide, distinguishes ultrasound 5 minutes by the slide cut out in acetone and absolute ethyl alcohol, is then cleaned with ultra-pure water dry successively
It is net standby.
2nd, the pure silver nitrate solid of analysis of certain mass is weighed, 100 mL 0.02mol/L silver nitrate solution is prepared.
3rd, 0.9814g C are weighed2H3KO2Be dissolved in the ultrasonic water of 100mL, it is to be dissolved after, add 3.3mol/L's with liquid-transfering gun
NH3H2The μ L of O 150, stir, and now the pH of potassium acetate solution is 10.64.Micropore ceramics glass is moved to afterwards as barrier film
In H type electrolytic cells, anode, cathode chamber respectively add 38mL and 40mL.The silver nitrate that the above-mentioned preparations of 2mL are pipetted with pipette adds sun
Pole room.
4th, using the electrochemical workstation of three-electrode system, using platinum post electrode (φ 1mm × 5mm) as auxiliary electrode,
Ag/AgCl electrodes are as reference electrode, and electro-conductive glass makes electro-conductive glass 1cm × 1cm parts and electrolytic cell sun as working electrode
Pole room solution is contacted, and H type electrolytic cells is fixed in 25 DEG C of Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, decomposition voltage
For 1.3 vs. NHE.Stop when being 1.5 coulombs by the electricity of conductive glass surface.
Experiment shows：In embodiment 3, a thick layer grey black color substance, XRD analysis can be generated on anode ITO surfaces
It is AgO to show it.Sem analysis is carried out to it, it seems the irregular rectangular bulk for having clipped corner.It is in 0.1M K3PO4In
Current density is 2.3mA/cm2, and it is electrolysed after 10h, current density is without being decreased obviously.
Embodiment 4
The preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material, comprises the following steps under a kind of temperate condition：
1st, by thickness be 1.8mm, sheet resistance be 8.6 ± 1.0 Ω/sq specifications ITO electro-conductive glass be cut into size be 1cm ×
5cm slide, distinguishes ultrasound 5 minutes by the slide cut out in acetone and absolute ethyl alcohol, is then cleaned with ultra-pure water dry successively
It is net standby.
2nd, the pure silver nitrate solid of analysis of certain mass is weighed, 100mL 0.02mol/L silver nitrate solution is prepared.
3rd, 0.9814g C are weighed2H3KO2Be dissolved in the ultrasonic water of 100mL, it is to be dissolved after, add 3.3mol/L's with liquid-transfering gun
NH3H2The μ L of O 190, stir, and now the pH of potassium acetate solution is 10.72.Micropore ceramics glass is moved to afterwards as barrier film
In H type electrolytic cells, anode, cathode chamber respectively add 38mL and 40mL.The silver nitrate that the above-mentioned preparations of 2mL are pipetted with pipette adds sun
Pole room.
4th, using the electrochemical workstation of three-electrode system, using platinum post electrode (φ 1mm × 5mm) as auxiliary electrode,
Ag/AgCl electrodes are as reference electrode, and electro-conductive glass makes electro-conductive glass 1cm × 1cm parts and electrolytic cell sun as working electrode
Pole room solution is contacted, and H type electrolytic cells is fixed in 25 DEG C of Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, decomposition voltage
For 1.3 vs. NHE.Stop when being 1.5 coulombs by the electricity of conductive glass surface.
Experiment shows：In embodiment 4, a thick layer grey black color substance, XRD analysis can be generated on anode ITO surfaces
It is AgO to show it.Sem analysis is carried out to it, it is that knitting wool is spherical, and rough surface is made up of many holes.It is in 0.1M K3PO4
In analysis oxidative stability it is poor, test 1h after current density significantly decrease, electrolysis 10h after current density drop to 0.9mA/
cm2, and tend towards stability.
All those skilled in the art are obtained according to the present invention in existing technical foundation by logic analysis, reasoning
The technical scheme arrived, should be within the scope of the claims be protected.
Claims (6)
1. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under a kind of temperate condition, it is characterised in that：Including
Following steps：
（1）, electro-conductive glass ITO substrate preparation
Electro-conductive glass is standby after being cleaned by ultrasonic；
（2）, silver nitrate solution preparation
The pure silver nitrate solid of analysis is weighed, silver nitrate solution is prepared；
（3）, electrolyte solution configuration
Take C2H3KO2Be dissolved in ultrasonic water, it is to be dissolved after, add NH3H2O, stirs, now, now the pH of potassium acetate solution
For 10.1 ~ 10.8；Micropore ceramics glass is moved to afterwards as anode, the cathode chamber of the H type electrolytic cells of barrier film；Pipette and match somebody with somebody again afterwards
The silver nitrate of system adds anode chamber, identical with cathode chamber solution volume to anode chamber；
（4）, in situ prepare
Using the electrochemical workstation of three-electrode system, using platinum post electrode as auxiliary electrode, Ag/AgCl electrodes are used as reference electricity
Pole, electro-conductive glass makes electro-conductive glass part be contacted with electrolyzer anode chamber solution, H type electrolytic cells is fixed as working electrode
In Water Tank with Temp.-controlled, using potentiostatic deposition coulometry, catalyst film material is prepared.
2. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition according to claim 1,
It is characterized in that：Step（4）In, the temperature of Water Tank with Temp.-controlled is 25 DEG C；Decomposition voltage is 1.3 vs. NHE, when passing through conductive glass
The electricity on glass surface stops when being 1.5 coulombs.
3. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition according to claim 2,
It is characterized in that：Step（3）In, the pH of potassium acetate solution is 10.19.
4. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition according to claim 2,
It is characterized in that：Step（3）In, the pH of potassium acetate solution is 10.40.
5. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition according to claim 2,
It is characterized in that：Step（3）In, the pH of potassium acetate solution is 10.64.
6. the preparation method of water electrolysis hydrogen production Ag bases oxygen-separating catalyst membrane material under temperate condition according to claim 2,
It is characterized in that：Step（3）In, the pH of potassium acetate solution is 10.72.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108385125A (en) * | 2018-03-08 | 2018-08-10 | 太原理工大学 | Temperate condition prepares Au-BiThe method of Oxygen anodic evolution catalyst and application |
| CN108385146A (en) * | 2018-03-26 | 2018-08-10 | 太原理工大学 | The method for preparing the different crystal face AgO oxygen-separating catalyst membrane materials of exposure in a mild condition |
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| US5248397A (en) * | 1990-02-06 | 1993-09-28 | Olin Corporation | Chlorine dioxide generation from chloric acid - alkali metal chlorate mixtures |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108385125A (en) * | 2018-03-08 | 2018-08-10 | 太原理工大学 | Temperate condition prepares Au-BiThe method of Oxygen anodic evolution catalyst and application |
| CN108385125B (en) * | 2018-03-08 | 2019-08-02 | 太原理工大学 | Temperate condition prepares Au-BiThe method and application of Oxygen anodic evolution catalyst |
| CN108385146A (en) * | 2018-03-26 | 2018-08-10 | 太原理工大学 | The method for preparing the different crystal face AgO oxygen-separating catalyst membrane materials of exposure in a mild condition |
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| CN106987859B (en) | 2018-07-31 |
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