CN106967997B - A kind of efficient self-supporting catalysis electrode and its preparation method and application - Google Patents
A kind of efficient self-supporting catalysis electrode and its preparation method and application Download PDFInfo
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- CN106967997B CN106967997B CN201710119624.9A CN201710119624A CN106967997B CN 106967997 B CN106967997 B CN 106967997B CN 201710119624 A CN201710119624 A CN 201710119624A CN 106967997 B CN106967997 B CN 106967997B
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- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
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- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
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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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- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
- C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
- C25B11/031—Porous electrodes
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- 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
Abstract
The invention discloses a kind of efficient self-supporting catalysis electrodes and its preparation method and application, ferronickel molybdenum manganese alloy is prepared first, and wherein the amount percentage of the substance of nickel is 5%-25%, and the amount percentage of the substance of iron is in 5%-25%, for the amount percentage of the substance of molybdenum in 5%-25%, surplus is manganese.The certain alloy strip of thickness or alloy sheets are prepared using the method for rolling and getting rid of band.Using de- alloying process, including chemical removal alloying and electrochemistry removal alloying, efficient self-supporting catalysis electrode is prepared.The advantage of this electrode material is: three-dimensional porous self-supporting, is not necessarily to any supporter and binder；Non-precious Metal Catalysts electrode, material content is abundant, cheap, and preparation condition is controllable；High current steady operation；With double catalysis, it can carry out simultaneously being electrolysed aquatic products hydrogen in alkaline electrolytic bath and produce oxygen, this self-supporting catalytic electrode material can be applied to catalysis and produce hydrogen production oxygen, and the fields such as fuel cell are a kind of new and effective catalysis electrodes.
Description
Technical field
The invention belongs to be catalyzed the technical field of water electrolysis, especially a kind of self-supporting catalysis electrode for being catalyzed water electrolysis and
Preparation method and the application in catalysis water electrolysis simultaneous hydrogen production and in terms of producing oxygen.
Background technique
With social economy's accelerated development, environmental pollution increasingly sharpens with energy crisis, and people are to cleaning, sustainable new
The energy and new energy storage equipment are increasingly paid attention to.Hydrogen is cleaned with it, is efficient, pollution-free by extensive concern.In nature
Hydrogen content is few and impure, therefore extensive hydrogen manufacturing is the most important thing.In known various hydrogen producing technologies, electrolysis water can be incited somebody to action
The new energy forms such as intermittence, uncontrollable solar energy, wind energy and water energy are converted into hydrogen storage to realize and can reconcile controllability.
But in actual production, water electrolysis needs overcome very big overpotential, cause energy consumption high, efficiency decline.By researcher
Be continually striving to, the overpotential of water electrolysis can be effectively reduced using catalysis electrode and improve efficiency to reduce energy consumption for discovery.
Now, the noble metal and iridium, ruthenium oxide of platinum class respectively be electrolysis aquatic products hydrogen and produce the most effective catalysis electrode of oxygen, but they
The shortcomings that reserves are low, price is difficult to realize its extensive use.Therefore, efficient, rich content base metal is researched and developed to urge
Polarizing electrode causes the concern of people.
In recent years, from noble metal to precious metal doping again to non-noble transition metal it is compound/doping, a series of catalysis electrode materials
The exploitation of material be reduce water electrolysis overpotential and effort.For example, metal phosphide, metal carbides, molybdenum disulfide class are contour
Effect catalytic water electrolytic hydrogen production catalytic electrode material (E.J.Popczun, J.R.McKone, C.G.Read, A.J.Biacchi,
A.M.Wiltrout, N.S.Lewis, R.E.Schaak, J.Am.Chem.Soc.135 (2013) 9267e9270)；And phosphatization cobalt,
Transition metal oxide and hydroxide etc. are catalyzed water electrolysis and produce oxygen catalytic electrode material (J.-X.Feng, H.Xu, Y.-
T.Dong, S.-H.Ye, Y.-X.Tong, G.-R.Li, Angew.Chem.128 (2016) 3758e3762).Current many catalysis
Electrode has good catalytic performance under strong acid or basic conditions, but on the one hand meets simultaneously and produce hydrogen and produce the optimal of oxygen
The efficient catalytic electrode of condition is fewer and fewer, and on the other hand, two kinds of optimal operating conditions cannot be used in an electrolytic cell, makes
It obtains cell construction to complicate, increases cost.Therefore, double-function catalyzing electrode is explored under the identical operating condition of an electrolytic cell
It is still a huge challenge that hydrogen, which can be produced, but also produce oxygen.
Summary of the invention
The technical problem to be solved by the present invention is to the overpotential to reduce water electrolysis, improve efficiency, and simplify electrolytic cell knot
Structure proposes a kind of abundant raw material, efficient self-supporting catalysis electrode and preparation method thereof and in catalytic water electrolytic hydrogen production and produces oxygen
The application of aspect, prepared catalysis electrode both can be used as the cathode of catalytic water electrolytic hydrogen production, can be used for catalysis water electrolysis
The anode for producing oxygen is a kind of difunctional catalysis electrode.
In order to solve the above-mentioned technical problem, the technical solution adopted by the present invention is that: a kind of efficient self-supporting catalysis electrode
Preparation method includes the following steps:
(1) prepared by alloy: prepare ferronickel molybdenum manganese alloy, in the alloy, the amount percentage of the substance of nickel is 5%-25%,
The amount percentage of the substance of iron is in 5%-25%, and for the amount percentage of the substance of molybdenum in 5%-25%, surplus is manganese；The alloy quilt
It is processed into alloy strip or alloy sheets of the thickness at 20-500 μm；
(2) alloy that step (1) is prepared is prepared into efficient self-supporting catalysis electrode using de- alloyage process, it is described
Efficient self-supporting catalysis electrode aperture be mainly distributed on 2 nanometers in 500 nanometer ranges, specific surface area is 10~80m2/g。
De- alloyage process in the step (2) is that the de- alloyage process of chemistry or electrochemistry take off alloyage process.
The de- alloyage process of chemistry is alloy strip to be prepared in step (1) or alloy sheets are dipped in acid solution
De- alloying process is carried out, is dried in vacuo after the completion.
It is preferred that the acid solution is concentration 0.005mol/L~2mol/L acid solution.
It is electrode of being worked with alloy strip made from step (1) or alloy sheets that the electrochemistry, which takes off alloyage process, is adopted
Alloying is taken off in faintly acid salting liquid with three-electrode system, taking off alloying voltage is -0.45V~-0.8V, takes off alloying time
It is 500 seconds~40000 seconds.
It is preferred that the faintly acid salt is for the strong acid weak base salting liquid of concentration 0.5mol/L~3mol/L ammonium.
Efficient self-supporting catalysis electrode made from the step (2), according to the amount optimization of substance than being Ni: Fe: Mo=5: 2
: 1 or 2: 1.2: 1 or 3: 1: 1 or 1: 1: 1 or 8: 2: 1.
The alloy of the step (1) is prepared using rolling or the method for getting rid of band.
Efficient self-supporting catalysis electrode made from above-mentioned preparation method.
Efficient application of the self-supporting catalysis electrode in terms of electrolysis water made from above-mentioned preparation method.
The beneficial effects of the present invention are: catalysis electrode 1 obtained) three-dimensional porous self-supporting, without any supporter and viscous
Tie agent；2) Non-precious Metal Catalysts electrode, material content is abundant, cheap, and preparation condition is controllable；3) high current stablizes work
Make, producing current density in hydrogen may be up to 1000mA/cm2More than, it is 100mA/cm in current density2And 200mA/cm2Overpotential point
It Wei not 133mV and 211mV；Produce oxygen in current density be 10mA/cm2And 100mA/cm2Overpotential be respectively 265mV and
367mV, when standard hydrogen potential is 2V, current density is up to 632mA/cm2；4) there are double catalysis, it can be in alkaline electrolysis
Electrolysis aquatic products hydrogen is carried out in slot simultaneously and produces oxygen, when voltage is 1.54V, current density is up to 10mA/cm2, show advantageous
Catalytic performance.The popularity and high current high stability of raw material have been greatly facilitated the popularity and electric energy conversion of application
It is a kind of new and effective double-function catalyzing electrode for the efficient energy conversion of chemical energy.
Detailed description of the invention
Fig. 1 be catalysis electrode obtained in embodiment 1 SEM figure (A be acquisition efficient self-supporting catalysis electrode
SEM exterior view；B is the SEM sectional view of the efficient self-supporting catalysis electrode obtained)；
Fig. 2 is the EDS figure of the efficient self-supporting catalysis electrode obtained in embodiment 1；
Fig. 3 is the catalytic water electrolytic hydrogen production in alkaline electrolyte of the efficient self-supporting catalysis electrode obtained in embodiment 1
Performance curve (i.e. current density is with reversible hydrogen electrode potential change curve)；
Fig. 4 catalytic water electrolytic hydrogen production institute in alkaline electrolyte for the efficient self-supporting catalysis electrode that is obtained in embodiment 1
It obtains catalytic stability curve (i.e. under constant voltage, current density changes over time curve)；
Fig. 5 is that the water electrolysis that is catalyzed in alkaline electrolyte of the efficient self-supporting catalysis electrode obtained in embodiment 1 produces oxygen
Performance curve (i.e. current density is with reversible hydrogen electrode potential change curve)；
Fig. 6 is catalyzed water electrolysis production oxygen institute for the efficient self-supporting catalysis electrode obtained in embodiment 1 in alkaline electrolyte
It obtains catalytic stability curve (i.e. under constant voltage, current density changes over time curve)；
Fig. 7 is that the efficient self-supporting catalysis electrode obtained in embodiment 1 is used as double-function catalyzing electricity in alkaline electrolytic bath
The performance curve of pole electrolysis water.
Fig. 8 is that the efficient self-supporting catalysis electrode obtained in embodiment 1 is used as double-function catalyzing electricity in alkaline electrolytic bath
The stability curve of pole electrolysis water.
Specific embodiment
Invention is further described in detail with reference to the accompanying drawings and detailed description:
The preparation method of efficient self-supporting catalysis electrode of the invention, includes the following steps:
(1) prepared by alloy: prepare ferronickel molybdenum manganese alloy, in the alloy, the amount percentage of the substance of nickel is 5%-25%,
The amount percentage of the substance of iron is in 5%-25%, and for the amount percentage of the substance of molybdenum in 5%-25%, surplus is manganese；The alloy quilt
It is processed into alloy strip or alloy sheets of the thickness at 20-500 μm；
(2) alloy that step (1) is prepared is prepared into efficient self-supporting catalysis electrode using de- alloyage process, it is described
Efficient self-supporting catalysis electrode aperture be mainly distributed as 2 nanometers in 500 nanometer ranges, specific surface area is 10~80m2/g。
De- alloyage process in the step (2) is that the de- alloyage process of chemistry or electrochemistry take off alloyage process.
The de- alloyage process of chemistry is alloy strip to be prepared in step (1) or alloy sheets are dipped in acid solution
De- alloying process is carried out, is dried in vacuo after the completion.
It is preferred that the acid solution is concentration 0.005mol/L~2mol/L acid solution.
It is electrode of being worked with alloy strip made from step (1) or alloy sheets that the electrochemistry, which takes off alloyage process, is adopted
Alloying is taken off in faintly acid salting liquid with three-electrode system, taking off alloying voltage is -0.45V~-0.8V, takes off alloying time
It is 500 seconds~40000 seconds.
It is preferred that the faintly acid salt is the strong acid weak base salting liquid that concentration is 0.5mol/L~3mol/L ammonium.
Efficient self-supporting catalysis electrode made from the step (2), according to the amount optimization of substance than being Ni: Fe: Mo=5: 2
: 1 or 2: 1.2: 1 or 3: 1: 1 or 1: 1: 1 or 8: 2: 1.
The alloy of the step (1) is prepared using rolling or the method for getting rid of band.
Efficient self-supporting catalysis electrode made from above-mentioned preparation method.
Efficient application of the self-supporting catalysis electrode in terms of electrolysis water made from above-mentioned preparation method.
Following embodiment can make those skilled in the art that the present invention, but protection scope of the present invention be more fully appreciated
It is not limited to the following embodiments.
Embodiment 1
(1) prepared by alloy, prepares ferronickel molybdenum manganese alloy, by four kinds of W metals: Fe: Mo: Mn according to amount of substance ratio is 20: 5:
5: 70, it is put into smelting furnace, melting forms alloy in low vacuum smelting furnace；Then band is got rid of in getting rid of band machine obtain alloy bar
Band, the strip width is 2mm, with a thickness of 25 μm.
(2) it takes off alloying and prepares porous metals,
Alloyage process is taken off using electrochemistry:
The obtained alloy of step (1) preparation is taken off into alloyage process using electrochemistry and prepares efficient self-supporting catalysis electricity
Pole takes off alloying step are as follows: 1mol/L ammonium sulfate as de- alloying solution, the test system used for three-electrode system,
Middle alloy strip is used as working electrode, platinized platinum to electrode, and Ag/AgCl electrode is as reference electrode.De- alloying voltage is-
0.6V (vs.Ag/AgCl reference electrode), taking off alloying time is 7200 seconds, and efficient self-supporting catalysis electrode can be obtained.
Fig. 1 is that the SEM of catalysis electrode obtained schemes, it can be seen that the catalyst is the three-dimensional porous knot of two-phase doping
Structure；Fig. 2 is that the EDS of catalysis electrode obtained schemes, it can be seen that Ni: Fe: Mn atomic ratio of catalysis electrode is close to 5: 2: 1.
Catalytic water electrolytic hydrogen production is carried out in standard three electrode electrolytic cell to the catalysis electrode of above method preparation and produces oxygen
It can test；Working electrode is efficient self-supporting catalysis electrode prepared by the present invention in electrolytic cell, reference electrode is silver-colored silver chlorate electricity
Pole is platinized platinum to electrode.It should be noted that all electricity obtained using silver silver chloride electrode as reference electrode in electro-catalysis test
Gesture is converted into reversible hydrogen electrode potential in catalytic performance figure.And the electrolysis water in alkaline electrolytic bath is in two electrode conditions
Lower test, the efficient self-supporting catalysis electrode of preparation produces hydrogen respectively as cathode and anode produces oxygen.
Fig. 3 is the catalytic water electrolytic hydrogen production performance map in alkaline electrolyte for obtaining efficient self-supporting catalysis electrode, can be with
Find out: catalytic water electrolytic hydrogen production is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 133mV and 211mV,
Show the catalysis H2-producing capacity for having excellent.
Fig. 4 is the catalytic water electrolytic hydrogen production stability diagram in alkaline electrolyte for obtaining efficient self-supporting catalysis electrode.It can
To find out (110mA/cm under the conditions of high current density2), material worked by (10 hours) for a long time, and catalytic performance is steady
It is fixed, do not decay substantially.
Fig. 5 is to obtain the water electrolysis that is catalyzed in alkaline electrolyte of efficient self-supporting catalysis electrode to produce oxygen performance map, can be with
Find out: catalysis water electrolysis produces oxygen, is 10mA/cm in current density2And 100mA/cm2Overpotential is respectively 265mV and 367mV,
When standard hydrogen potential is 2V, current density is up to 632mA/cm2, show to be catalyzed to produce in high current that there is outstanding performance in oxygen.
Fig. 6 is the catalysis water electrolysis production oxidative stability figure in alkaline electrolyte for obtaining efficient self-supporting catalysis electrode.It can
To find out (120mA/cm under the conditions of high current density2), material worked by (10 hours) for a long time, and catalytic performance is steady
It is fixed, do not decay substantially.
Fig. 7 be obtain efficient self-supporting catalysis electrode in alkaline electrolytic bath as double-function catalyzing electrolysis water
Performance curve, it can be seen that current density be 10mA/cm2And 100mA/cm2Voltage is respectively 1.54V and 1.77V.
Fig. 8 is the catalysis water electrolysis stability diagram in alkaline (1MKOH) electrolytic cell for obtaining efficient self-supporting catalysis electrode,
It can be seen that can carry out simultaneously electrolysis aquatic products hydrogen in alkaline electrolytic bath and produce oxygen, when voltage is 1.54V, current density is reachable
10mA/cm2, and worked by (10 hours) for a long time, catalytic performance there is no any variation.
Embodiment 2
It is same as Example 1, only de- alloying time is become 1800 seconds.The catalytic performance of gained catalysis electrode: it urges
Change water electrolysis and produce hydrogen, is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 241mV and 340mV；It is catalyzed water power
Solution produces oxygen, in the case where standard hydrogen potential is 2V, current density 304mA/cm2。
Embodiment 3
It is same as Example 1, only de- alloying time is become 3600 seconds.The catalytic performance of gained catalysis electrode: it urges
Change water electrolysis and produce hydrogen, is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 190mV and 315mV；It is catalyzed water power
Solution produces oxygen, in the case where standard hydrogen potential is 2V, current density 480mA/cm2。
Embodiment 4
It is same as Example 1, only de- alloying time is become 10800 seconds.The catalytic performance of gained catalysis electrode: it urges
Change water electrolysis and produce hydrogen, is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 185mV and 312mV；It is catalyzed water power
Solution produces oxygen, in the case where standard hydrogen potential is 2V, current density 496mA/cm2。
Embodiment 5
It is same as Example 1, only de- alloying time is become 14400 seconds.The catalytic performance of gained catalysis electrode: it urges
Change water electrolysis and produce hydrogen, is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 189mV and 320mV；It is catalyzed water power
Solution produces oxygen, in the case where standard hydrogen potential is 2V, current density 476mA/cm2。
Embodiment 6
It is same as Example 1, only 10: 10: 10: 70 are changed to according to amount of substance ratio by Ni: Fe: Mo: Mn.Gained catalysis electricity
The catalytic performance of pole: catalytic water electrolytic hydrogen production is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 226mV
And 353mV；It is catalyzed water electrolysis and produces oxygen, in the case where standard hydrogen potential is 2V, current density 380mA/cm2。
Embodiment 7
It is same as Example 1,15: 15: 10: 60 are changed to according to amount of substance ratio by Ni: Fe: Mo: Mn.Gained catalysis electrode
Catalytic performance: catalytic water electrolytic hydrogen production is 100mA/cm in current density2And 200mA/cm2Overpotential be respectively 259mV and
420mV；It is catalyzed water electrolysis and produces oxygen, in the case where standard hydrogen potential is 2V, current density 334mA/cm2。
Embodiment 8
It is same as Example 1,25: 10: 10: 55 are changed to according to amount of substance ratio by Ni: Fe: Mo: Mn.Gained catalysis electrode
Catalytic performance: catalytic water electrolytic hydrogen production is 100mA/cm in current density2And 200mA/cm2Overpotential be respectively 238mV and
364mV；It is catalyzed water electrolysis and produces oxygen, in the case where standard hydrogen potential is 2V, current density 356mA/cm2。
Embodiment 9
It is same as Example 1, de- alloy approach is only changed to the de- alloy approach of chemistry.The catalytic of gained catalysis electrode
Can: catalytic water electrolytic hydrogen production is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 205mV and 317mV；It urges
Change water electrolysis and produces oxygen, in the case where standard hydrogen potential is 2V, current density 373mA/cm2。
Embodiment 10
It is same as Example 1, de- alloy approach is changed to the de- alloy approach of chemistry, taking off alloying time is 10800 seconds.Institute
The catalytic performance of catalysis electrode: catalytic water electrolytic hydrogen production is obtained, is 100mA/cm in current density2And 200mA/cm2Overpotential difference
For 224mV and 338mV；It is catalyzed water electrolysis and produces oxygen, in the case where standard hydrogen potential is 2V, current density 349mA/cm2。
Embodiment 11
It is same as Example 1, only alloy preparation method is changed to roll.The catalytic performance of gained catalysis electrode: catalysis
Water electrolysis produces hydrogen, is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 178mV and 295mV；It is catalyzed water electrolysis
Oxygen is produced, in the case where standard hydrogen potential is 2V, current density 476mA/cm2。
Efficient self-supporting catalysis electricity is prepared when the ferronickel molybdenum manganese alloy using certain proportion range carries out de- Alloying Treatment
The pole current density more stable and applicable compared to conventional powder cladding process is bigger, and producing current density in hydrogen may be up to 1000mA/cm2
More than, it is 100mA/cm in current density2And 200mA/cm2Overpotential is respectively 133mV and 211mV (Fig. 3)；It produces in oxygen in electricity
Current density is 10mA/cm2And 100mA/cm2Overpotential is respectively 265mV and 367mV, and when standard hydrogen potential is 2V, electric current is close
Degree is up to 632mA/cm2, (Fig. 5)；With double catalysis, electrolysis aquatic products hydrogen and production can be carried out simultaneously in alkaline electrolytic bath
Oxygen, when voltage is 1.54V, current density is up to 10mA/cm2(Fig. 7) shows advantageous catalytic performance.
Embodiment described above is merely to illustrate technical idea and feature of the invention, in the art its object is to make
Technical staff it will be appreciated that the contents of the present invention and implement accordingly, patent model of the invention only cannot be limited with the present embodiment
It encloses, i.e., same changes or modifications made by all disclosed spirit are still fallen in the scope of the patents of the invention.
Claims (5)
1. a kind of preparation method of efficient self-supporting catalysis electrode, which comprises the steps of:
(1) prepared by alloy: preparing ferronickel molybdenum manganese alloy, in the alloy, the amount percentage of the substance of nickel is 5%-25%, iron
The amount percentage of substance is in 5%-25%, and for the amount percentage of the substance of molybdenum in 5%-25%, surplus is manganese；The alloy is used and is got rid of
The method of band is processed to alloy strip or alloy sheets of the thickness at 20-500 μm；
(2) alloy strip or alloy sheets step (1) being prepared take off alloyage process preparation using electrochemistry and efficiently prop up certainly
Catalysis electrode is supportted, in 2 nanometers to 500 nanometer ranges, specific surface area is the efficient self-supporting catalysis electrode pore-size distribution
10~80m2/g；
It is electrode of being worked with alloy strip made from step (1) or alloy sheets that the electrochemistry, which takes off alloyage process, using three
Electrode system takes off alloying in faintly acid salting liquid, and taking off alloying voltage is -0.45V~-0.8V, and de- alloying time is
500 seconds~40000 seconds.
2. the preparation method of efficient self-supporting catalysis electrode according to claim 1, which is characterized in that the faintly acid salt
For the strong acid weak base salting liquid of concentration 0.5mol/L~3mol/L ammonium.
3. the preparation method of efficient self-supporting catalysis electrode according to claim 1, which is characterized in that the step (2)
Efficient self-supporting catalysis electrode obtained is Ni: Fe: Mo=5: 2: 1 or 2: 1.2: 1 or 3: 1: 1 or 1: 1 according to the mass ratio of the material
: 1 or 8: 2: 1.
4. efficient self-supporting catalysis electrode made from preparation method as described in any one of claims 1-3.
5. efficient self-supporting catalysis electrode is in terms of electrolysis water made from preparation method as described in any one of claims 1-3
Using.
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