CN111346635B - Intermetallic compound nano catalyst, preparation method and application thereof - Google Patents
Intermetallic compound nano catalyst, preparation method and application thereof Download PDFInfo
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- 229910000765 intermetallic Inorganic materials 0.000 title claims abstract description 64
- 239000011943 nanocatalyst Substances 0.000 title claims abstract description 54
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
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- 239000002904 solvent Substances 0.000 claims abstract description 22
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- 238000006243 chemical reaction Methods 0.000 claims abstract description 17
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 14
- 150000002258 gallium Chemical class 0.000 claims abstract description 14
- 150000002503 iridium Chemical class 0.000 claims abstract description 14
- 239000001301 oxygen Substances 0.000 claims abstract description 14
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 14
- 238000002156 mixing Methods 0.000 claims abstract description 7
- 238000000034 method Methods 0.000 claims description 21
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 18
- 238000002390 rotary evaporation Methods 0.000 claims description 16
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 12
- 239000001257 hydrogen Substances 0.000 claims description 10
- 229910052739 hydrogen Inorganic materials 0.000 claims description 10
- 238000001816 cooling Methods 0.000 claims description 8
- 238000010438 heat treatment Methods 0.000 claims description 7
- 239000011261 inert gas Substances 0.000 claims description 7
- 239000002253 acid Substances 0.000 claims description 6
- CHPZKNULDCNCBW-UHFFFAOYSA-N gallium nitrate Chemical group [Ga+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O CHPZKNULDCNCBW-UHFFFAOYSA-N 0.000 claims description 6
- 229940044658 gallium nitrate Drugs 0.000 claims description 3
- DANYXEHCMQHDNX-UHFFFAOYSA-K trichloroiridium Chemical group Cl[Ir](Cl)Cl DANYXEHCMQHDNX-UHFFFAOYSA-K 0.000 claims description 3
- 239000003054 catalyst Substances 0.000 abstract description 17
- 230000000694 effects Effects 0.000 abstract description 13
- 239000002105 nanoparticle Substances 0.000 abstract description 11
- 230000003197 catalytic effect Effects 0.000 abstract description 9
- 230000002378 acidificating effect Effects 0.000 abstract description 6
- 230000005540 biological transmission Effects 0.000 abstract description 5
- 238000006555 catalytic reaction Methods 0.000 abstract description 5
- 239000000463 material Substances 0.000 abstract description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052799 carbon Inorganic materials 0.000 abstract description 3
- 238000001514 detection method Methods 0.000 description 13
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 8
- 229910045601 alloy Inorganic materials 0.000 description 8
- 239000000956 alloy Substances 0.000 description 8
- 238000000634 powder X-ray diffraction Methods 0.000 description 6
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- 239000007789 gas Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 239000000243 solution Substances 0.000 description 5
- 229910052786 argon Inorganic materials 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 229910021638 Iridium(III) chloride Inorganic materials 0.000 description 3
- 230000004075 alteration Effects 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 230000010287 polarization Effects 0.000 description 3
- 238000001556 precipitation Methods 0.000 description 3
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(IV) oxide Inorganic materials O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
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- 238000004502 linear sweep voltammetry Methods 0.000 description 2
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- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- HTXDPTMKBJXEOW-UHFFFAOYSA-N iridium(IV) oxide Inorganic materials O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 description 1
- 239000003446 ligand Substances 0.000 description 1
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- 229910052697 platinum Inorganic materials 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/62—Platinum group metals with gallium, indium, thallium, germanium, tin or lead
-
- B01J35/33—
-
- 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
-
- 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
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
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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
Abstract
The invention provides a preparation method of an intermetallic compound nano catalyst, which comprises the following steps: s1) mixing carbon black, iridium salt and gallium salt in a solvent, and removing the solvent to obtain a mixture; s2) carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain the intermetallic compound nano catalyst. Compared with the prior art, the IrGa nanoparticles in the intermetallic compound nano-catalyst prepared by the invention have catalytic activity, and the mesopores in the carbon carrier can improve the material transmission rate in the catalytic reaction, so that the IrGa nanoparticles have better activity and stability when used as the catalyst, and have better catalytic activity and application prospect in the acidic oxygen evolution reaction.
Description
Technical Field
The invention belongs to the technical field of electrochemistry, and particularly relates to an intermetallic compound nano catalyst, and a preparation method and application thereof.
Background
Energy sources are the basis for the existence and development of human society. Due to the problems of limited reserves of fossil fuels, time and labor consumption in mining, environmental pollution easily caused in use and the like, the development of renewable clean energy sources is urgent in recent years. Such as solar energy, wind energy, geothermal energy, etc., but these energy forms cannot meet people's needs at any time and any place. Therefore, the development of clean energy technology requires various energy conversion and storage methods including water decomposition, fuel cell, carbon dioxide reduction, and the like. The heart of these energy conversion and storage means is a series of electrochemical reactions, one of the important electrochemical reactions being the oxygen evolution reaction. For example, the electrochemical decomposition of water comprises an anodic Oxygen Evolution Reaction (OER) and a cathodic Hydrogen Evolution Reaction (HER).
To date, research on HER in acidic solutions has been well studied. Of the various HER catalysts, those with the best activity in acidic media are platinum-based catalysts. However, OER has a high reaction energy barrier as one of the key processes for many energy-related applications, and has been attracting attention. The four electron mechanism determines its large reaction overpotential, slow reaction rate and large power consumption, which also indicates that OER is the rate-determining step in the water decomposition process. In practical application, IrO is due to commercial2Lower activity and RuO2The extremely poor stability can not meet the increasing energy and environmental requirements, so that the IrO can be replaced2And RuO2Efficient and stable OER catalysts are essential. A large number of researchersSignificant effort has been devoted to developing Ir-based and Ru-based alloy OER catalysts to replace commercial IrO2And RuO2A catalyst.
In the synthesis and application of numerous catalysts, intermetallic compounds have received much attention from researchers due to their unique advantages. The intermetallic compound has a definite stoichiometric number and crystal structure, and has more remarkable ligand effect, geometric effect and bifunctional mechanism than disordered alloy. Particularly in catalytic reactions, the unique ordered structure of intermetallic compounds allows for uniform separation of the sites of the active metals, providing unique geometric and electronic properties that generally result in significant enhancements in activity, selectivity, and stability. In addition, the regular ordered structure of the intermetallic compound is beneficial to researching the structure-activity relationship between the structure and the performance of the intermetallic compound, and provides a theoretical basis for further guiding the structure design and the synthesis of the novel high-performance catalyst. It is generally considered that the catalytic reaction occurs on the surface of the catalyst, so that the preparation of nano-sized intermetallic compounds can greatly increase the specific surface area thereof, thereby improving the activity. But at present, no intermetallic compound capable of catalyzing and electrolyzing water to produce hydrogen exists.
Disclosure of Invention
In view of the above, the technical problem to be solved by the present invention is to provide an intermetallic compound nano catalyst, a preparation method and an application thereof, wherein the intermetallic compound nano catalyst prepared by the method has a good catalytic activity in an acidic oxygen evolution reaction.
The invention provides a preparation method of an intermetallic compound nano catalyst, which comprises the following steps:
s1) mixing carbon black, iridium salt and gallium salt in a solvent, and removing the solvent to obtain a mixture;
s2) carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain the intermetallic compound nano catalyst.
Preferably, the iridium salt is selected from iridium chloride; the gallium salt is selected from gallium nitrate.
Preferably, the mass ratio of the carbon black to the iridium salt to the gallium salt is (35-45): (10-15): (15-20).
Preferably, the reducing atmosphere comprises hydrogen and an inert gas; the volume ratio of hydrogen to inert gas in the reducing atmosphere is (3-7): (93-97).
Preferably, the temperature of the high-temperature treatment is 750-950 ℃; the time of the high-temperature treatment is 7-9 h.
Preferably, the step S2) is specifically:
and heating the mixture to 750-950 ℃ at a speed of 4-6 ℃/min in a reducing atmosphere, preserving the heat for 7-9 h, and then cooling to 20-30 ℃ at a speed of 4-6 ℃/min to obtain the intermetallic compound nano catalyst.
Preferably, the solvent in step S1) is selected from water; the method for removing the solvent is rotary evaporation.
Preferably, the speed of the rotary evaporation is 85-95 r/min; the temperature of rotary evaporation is 75-85 ℃; the vacuum degree is 55-65 mbar.
The invention also provides the intermetallic compound nano catalyst prepared by the method.
The invention also provides the application of the intermetallic compound nano-catalyst prepared by the method in the acidic oxygen evolution reaction.
The invention provides a preparation method of an intermetallic compound nano catalyst, which comprises the following steps: s1) mixing carbon black, iridium salt and gallium salt in a solvent, and removing the solvent to obtain a mixture; s2) carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain the intermetallic compound nano catalyst. Compared with the prior art, the IrGa nanoparticles in the intermetallic compound nano-catalyst prepared by the invention have catalytic activity, and the mesopores in the carbon carrier can improve the material transmission rate in the catalytic reaction, so that the IrGa nanoparticles have better activity and stability when used as the catalyst, and have better catalytic activity and application prospect in the acidic oxygen evolution reaction.
Drawings
FIG. 1 is a TEM image of the intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention;
fig. 2 is an electron microscope photograph of an atomic resolution aberration corrected high-angle annular dark field image-scanning transmission electron microscope of the intermetallic compound IrGa nano catalyst prepared in example 1 of the present invention;
FIG. 3 is X-ray powder diffraction of the intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention;
FIG. 4 is an element distribution diagram of the intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention;
FIG. 5 shows that the intermetallic compound IrGa nano-catalyst prepared in example 1 of the present invention is in 0.1M HClO4OER polarization profile in solution;
FIG. 6 shows that the intermetallic compound IrGa nano-catalyst prepared in example 1 of the present invention is in 0.1M HClO4OER stability profile in solution.
FIG. 7 shows the X-ray powder diffraction pattern of the intermetallic compound IrGa nanocatalyst prepared in example 2 of the present invention;
FIG. 8 shows that the intermetallic compound IrGa nano-catalyst prepared in example 2 of the present invention is in 0.1M HClO4OER polarization profile in solution;
FIG. 9 shows the X-ray powder diffraction pattern of the intermetallic compound IrGa nanoparticle catalyst prepared in example 3 of the present invention;
FIG. 10 shows that the intermetallic compound IrGa nano-catalyst prepared in example 3 of the present invention is in 0.1M HClO4OER polarization profile in solution.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings of the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a preparation method of an intermetallic compound nano catalyst, which comprises the following steps: s1) mixing carbon black, iridium salt and gallium salt in a solvent, and removing the solvent to obtain a mixture; s2) carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain the intermetallic compound nano catalyst.
The present invention is not particularly limited in terms of the source of all raw materials, and may be commercially available.
Mixing carbon black, iridium salt and gallium salt in a solvent; the carbon black is not particularly limited as long as it is a commercial carbon black well known to those skilled in the art, and in the present invention, a commercial carbon black KJ600 and/or XC-72R; the iridium salt is preferably iridium chloride; the gallium salt is preferably gallium nitrate; the mass ratio of the carbon black to the iridium salt to the gallium salt is preferably (35-45): (10-15): (15-20), more preferably (38-42): (10-12): (15-17), and more preferably 40: 11.38: 16.38; in the present invention, the metal content in the total mass of the carbon black, iridium salt and gallium salt is preferably 18% to 22%, more preferably 20%; the purpose of the solvent is to thoroughly mix the carbon black, iridium salt and gallium salt to obtain a uniform mixture, which can be an organic solvent or water, and is preferably water in the invention; the ratio of the carbon black to the solvent is preferably (35-45) mg: (45-55) mL, more preferably (38-42) mg: (48-52) mL, more preferably 40 mg: 50 mL.
After mixing, removing the solvent to obtain a mixture; the method for removing the solvent is preferably rotary evaporation; the rotary evaporation speed is preferably 85-95 revolutions per minute, more preferably 88-92 revolutions per minute, and further preferably 90 revolutions per minute; the temperature of the rotary evaporation, namely the temperature of the water bath, is preferably 75-85 ℃, more preferably 78-82 ℃ and further preferably 80 ℃; the vacuum degree during rotary evaporation is preferably 55-65 mbar, more preferably 58-62 mbar, and still more preferably 60 mbar.
Carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain an intermetallic compound nano catalyst; the reducing atmosphere preferably comprises hydrogen and an inert gas; the inert gas is preferably argon; the volume ratio of the hydrogen to the inert gas is preferably (3-7): (93-97), more preferably (4-6): (94-96), and more preferably 5: 95; the temperature of the high-temperature treatment is preferably 750-950 ℃, more preferably 780-820 ℃ and further preferably 800 ℃; the heating rate of the high-temperature treatment is preferably 4-6 ℃/min, more preferably 4.5-5.5 ℃/min, and further preferably 5 ℃/min; the time of the high-temperature treatment is preferably 7-9 h, more preferably 7.8-8.2 h, and further preferably 8 h; after high-temperature treatment, preferably cooling to room temperature; the cooling rate is preferably 4-6 ℃/min, more preferably 4.5-5.5 ℃/min, and further preferably 5 ℃/min; in the present invention, this step is preferably embodied as follows: and heating the mixture to 750-950 ℃ at a speed of 4-6 ℃/min in a reducing atmosphere, preserving the heat for 7-9 h, and then cooling to 20-30 ℃ at a speed of 4-6 ℃/min to obtain the intermetallic compound nano catalyst. In the present invention, it is more preferable to lower the temperature to 25 ℃.
The invention provides a method for preparing an intermetallic compound nano catalyst by an impregnation method, the method has the advantages of easily obtained raw materials, simple operation and realization of large-scale treatment, IrGa nanoparticles in the prepared intermetallic compound nano catalyst have catalytic activity, and mesoporous pores in a carbon carrier can improve the material transmission rate in catalytic reaction, so that the IrGa nanoparticles have good activity and stability when used as a catalyst, and have good catalytic activity and application prospect in acid oxygen evolution reaction.
The invention also provides an intermetallic compound nano catalyst prepared by the method; the grain size of the intermetallic nano catalyst is preferably 1-15 nm, more preferably 5-12 nm, and still more preferably 7-9 nm.
The invention also provides an application of the intermetallic compound nano-catalyst prepared by the method in oxygen evolution reaction, preferably in acid oxygen evolution reaction, and the intermetallic compound nano-catalyst can be used as a catalyst in the oxygen evolution reaction of an acid medium.
In order to further illustrate the present invention, the following describes an intermetallic compound nano-catalyst, a preparation method and applications thereof in detail with reference to examples.
The reagents used in the following examples are all commercially available.
Example 1
40.00mg of commercial carbon black KJ600, 11.38mg of IrCl3And 16.38mg Ga (NO)3)3Dispersing in 50mL water, stirring uniformly, and performing rotary evaporation to remove solvent water to obtain a uniform mixture, wherein the rotation speed in the rotary evaporation process is 90 revolutionsMin, water bath temperature 80 deg.C, vacuum degree 60 mbar.
Transferring the obtained uniform mixture into a quartz crucible, putting the quartz crucible into a tube furnace, introducing argon-hydrogen gas as a reducing gas (the volume ratio of the argon gas to the hydrogen gas is 95:5), heating the tube furnace to 800 ℃ at the speed of 5 ℃/min, and preserving the heat for 8 hours; then cooling to room temperature (20-30 ℃) at the speed of 5 ℃/min; and keeping the normal pressure in the tubular furnace to obtain the intermetallic compound IrGa nano catalyst.
The intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention was examined by transmission electron microscopy, and the results are shown in fig. 1. As can be seen from fig. 1, the intermetallic compound IrGa nano-catalyst particles prepared in example 1 were uniformly distributed.
The intermetallic compound IrGa nano catalyst prepared in example 1 of the present invention was subjected to atomic resolution aberration corrected high angle annular dark field image scanning transmission electron microscope detection, and the detection result is shown in fig. 2. As is clear from fig. 2, the light and dark ordered Ir and Ga elements are clearly seen from the spherical aberration chart, and it is confirmed that example 1 synthesizes an ordered intermetallic compound phase.
The intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention was subjected to X-ray powder diffraction detection, and the detection results are shown in fig. 3. As can be seen from fig. 3, the X-ray diffraction pattern matched that of IrGa XRD standard PDF card, demonstrating that example 1 synthesizes an ordered intermetallic compound phase.
The intermetallic compound IrGa nanocatalyst prepared in example 1 of the present invention was subjected to elemental analysis and examined, and the examination results are shown in fig. 4, and it is understood from fig. 4 that the elemental analysis demonstrated that the material synthesized in example 1 contained Ir and Ga elements.
The activity detection of acid oxygen precipitation is carried out on the intermetallic compound IrGa nano catalyst prepared in the embodiment 1 of the invention, and the specific method comprises the following steps:
the catalytic activity was measured by linear sweep voltammetry at a sweep rate of 10 mV. multidot.s-1The rotation rate of the RDE was 1600rpm, and nitrogen was purged to HClO at a concentration of 0.1mol/L4In aqueous solution to achieve anaerobic conditions during the test.
As shown in FIG. 5, it can be seen from FIG. 5 that the overpotential for hydrogen production catalyzed by the intermetallic compound IrGa nano-catalyst (i.e., IrGa-IMC/KJ600 in FIG. 5) prepared in example 1 is the lowest and is 10mA/cm2The overpotential is only 272mV, much less than that of a commercial alloy catalyst (commercial Pt/C308 mV, manufacturer Premetek Corporation, Pt loading 20 wt%).
Ir/KJ600 in FIG. 5 was prepared according to the method of example 1 except that Ga (NO) was not added3)3And the load capacity of Ir in the obtained Ir/KJ600 is 20 wt%; commercial Ir/C manufacturer No. Premetek Corporation, Ir loading was 20 wt%.
The intermetallic compound IrGa nano catalyst prepared in the embodiment 1 of the invention is subjected to stability detection, and an accelerated decay stability test (CV sweeps 3000 circles under the voltage of 1.0-1.6V and then the catalytic activity is measured by linear sweep voltammetry) is adopted; the detection result is shown in fig. 6, and it can be seen from fig. 6 that the alloy catalyst prepared in example 1 of the present invention has good stability, and the activity does not decline significantly after 3000 cycles of CV cycle.
Example 2
40.00mg of commercial carbon black KJ600, 11.38mg of IrCl3And 16.38mg Ga (NO)3)3Dispersing in 50mL of water, stirring uniformly, and performing rotary evaporation to remove solvent water to obtain a uniform mixture, wherein the rotation speed in the rotary evaporation process is 90 revolutions per minute, the water bath temperature is 80 ℃, and the vacuum degree is 60 mbar.
Transferring the obtained uniform mixture into a quartz crucible, putting the quartz crucible into a tube furnace, introducing argon-hydrogen gas as a reducing gas (the volume ratio of the argon gas to the hydrogen gas is 95:5), heating the tube furnace to 800 ℃ at the speed of 5 ℃/min, and preserving the heat for 2 h; then cooling to room temperature (20-30 ℃) at the speed of 5 ℃/min; and keeping the normal pressure in the tubular furnace to obtain the intermetallic compound IrGa nano catalyst.
The intermetallic compound IrGa nano catalyst prepared in example 2 of the present invention was subjected to X-ray powder diffraction detection, and the detection result is shown in fig. 7, where the broad peak of XRD indicates that the IrGa alloy nanoparticles are small in size.
EXAMPLES OF THE INVENTION following the procedure of example 12 the intermetallic compound IrGa nanoparticle material prepared by the invention was subjected to an acidic oxygen precipitation activity test, and the detection result is shown in FIG. 8. from FIG. 8, it can be seen that the alloy catalyst prepared in example 2 of the present invention was at 10mA/cm2The overpotential was 281 mV.
Example 3
40.00mg of commercial carbon black XC-72R, 11.38mg of IrCl3And 16.38mg Ga (NO)3)3Dispersing in 50mL of water, stirring uniformly, and performing rotary evaporation to remove solvent water to obtain a uniform mixture, wherein the rotation speed in the rotary evaporation process is 90 revolutions per minute, the water bath temperature is 80 ℃, and the vacuum degree is 60 mbar.
Transferring the obtained uniform mixture into a quartz crucible, putting the quartz crucible into a tubular furnace, introducing argon-hydrogen gas serving as reducing gas (the volume ratio of the argon to the hydrogen is 95:5), heating the tubular furnace to 400 ℃ at the speed of 5 ℃/min, and preserving the temperature for 5 hours; then cooling to room temperature (20-30 ℃) at the speed of 5 ℃/min; and keeping the normal pressure in the tubular furnace to obtain the intermetallic compound IrGa nano catalyst.
The intermetallic compound IrGa nano catalyst prepared in example 3 of the present invention was subjected to X-ray powder diffraction detection, and the detection result is shown in fig. 9, where the broad peak of XRD indicates that IrV alloy nanoparticles are small in size.
The activity test of acid oxygen precipitation was performed on the intermetallic compound IrGa nanocatalyst prepared in example 3 of the present invention according to the method of example 1, and the detection result is shown in fig. 10, and it can be seen from fig. 10 that the alloy catalyst prepared in example 3 was at 10mA/cm2The overpotential was 291 mV.
Claims (7)
1. The application of the intermetallic compound nano catalyst in the acid oxygen evolution reaction is characterized in that the preparation method of the intermetallic compound nano catalyst comprises the following steps:
s1) mixing carbon black, iridium salt and gallium salt in a solvent, and removing the solvent to obtain a mixture; the mass ratio of the carbon black to the iridium salt to the gallium salt is (35-45): (10-15): (15-20);
s2) carrying out high-temperature treatment on the mixture in a reducing atmosphere to obtain the intermetallic compound nano catalyst.
2. Use according to claim 1, characterized in that said iridium salt is selected from iridium chloride; the gallium salt is selected from gallium nitrate.
3. The use according to claim 1, wherein the reducing atmosphere comprises hydrogen and an inert gas; the volume ratio of hydrogen to inert gas in the reducing atmosphere is (3-7): (93-97).
4. The use according to claim 1, wherein the high temperature treatment is carried out at a temperature of 750 ℃ to 950 ℃; the time of the high-temperature treatment is 7-9 h.
5. The application according to claim 1, wherein the step S2) is specifically:
and heating the mixture to 750-950 ℃ at a speed of 4-6 ℃/min in a reducing atmosphere, preserving the heat for 7-9 h, and then cooling to 20-30 ℃ at a speed of 4-6 ℃/min to obtain the intermetallic compound nano catalyst.
6. Use according to claim 1, wherein the solvent in step S1) is selected from water; the method for removing the solvent is rotary evaporation.
7. The use according to claim 6, wherein the speed of the rotary evaporation is 85-95 revolutions/min; the temperature of rotary evaporation is 75-85 ℃; the vacuum degree is 55-65 mbar.
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