CN110459775A - Light inorganic element doping nickel-base material and the preparation method and application thereof - Google Patents
Light inorganic element doping nickel-base material and the preparation method and application thereof Download PDFInfo
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- CN110459775A CN110459775A CN201910740391.3A CN201910740391A CN110459775A CN 110459775 A CN110459775 A CN 110459775A CN 201910740391 A CN201910740391 A CN 201910740391A CN 110459775 A CN110459775 A CN 110459775A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
- H01M4/8652—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites as mixture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
- H01M4/8673—Electrically conductive fillers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
- H01M4/8882—Heat treatment, e.g. drying, baking
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic 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
- Y02E60/50—Fuel cells
Abstract
The invention discloses a kind of preparation methods of light inorganic element doping nickel-base material, comprising the following steps: S1, provides nickel persursor material；S2, make the nickel persursor material hydrogenation, boronation, carbonization or nitridation to get the nickel-base material for arriving the light inorganic element doping；Wherein, the nickel persursor material includes nickel salt, nickel complex, inorganic nickel persursor material and nickel metal-organic framework material.The present invention also provides the light inorganic element doping nickel-base materials prepared by the method, and its as the application of oxidation of hydrogen reaction/hydrogen evolution reaction elctro-catalyst.Light inorganic element doping nickel-base material of the invention has excellent hydrogen electro catalytic activity, the ability that good stability and anti-carbon monoxide poison；And it is low in cost, preparation is simple, therefore has extensive commercial application prospect.
Description
Technical field
The present invention relates to electro-catalysis and energy conversion technical fields, and in particular to a kind of Ni-based material of light inorganic element doping
Material, preparation method and as the application of oxidation of hydrogen reaction/hydrogen evolution reaction elctro-catalyst.
Background technique
A kind of energy of the hydrogen as clean and effective, in modern industry field, application value is high.Hydrogen expanding economy master
It to include that two aspects are related to two and half electrochemical reactions: the storage of hydrogen-oxidation of hydrogen reaction and the utilization of hydrogen-hydrogen analysis
It reacts out, such as hydrogen-oxygen fuel cell and electrolysis water.Since oxidation of hydrogen reaction/hydrogen evolution reaction dynamic process is slow,
Therefore needing to develop electrochemical catalyst accelerates its reaction rate.It lives currently, platinum based catalyst presents preferable hydrogen electro-catalysis
Property, but Precious Metals Resources are rare, and it is at high price, prevent its large-scale commercial applications.In addition, platinum based catalyst is easy quilt
Carbon monoxide poisons.Therefore, promote hydrogen electrochemical reaction for realizing that hydrogen economy is of great significance using non-platinum catalyst.
In order to develop alkaline system non noble metal oxygen reduction catalyst, alkaline polymer electrolyte fuel cell meet the tendency of and
It is raw.Unfortunately, the best platinum based catalyst oxidation of hydrogen reaction/hydrogen evolution reaction of hydrogen electro catalytic activity under alkaline condition
Active ratio reduces two orders of magnitude in acid condition, needs higher load capacity.Develop Cheap highly effective under alkaline system
Non-platinum catalyst faces severe challenge.
Under alkaline system, some non-platinum liberation of hydrogen catalyst advantageously, it has been found that but hydro-oxidation catalyst be rarely reported.Nickel
It is that uniquely there is the active base metal of oxidation of hydrogen, the Raney Ni occurred earliest can more strongly active and platinum due to Surface Hydrogen combination
Base catalyst differs greatly.The hydrogen combination energy of metal nickel surface can be effectively reduced in metal-doped and supporting carrier effect.For example,
Nickel-transition metal (transition metal is chromium, molybdenum, copper, iron, zinc etc.) cobalt nickel molybdenum is a kind of efficient hydrogen oxidation catalyst, carbon nitrogen
The nickel of codope also presents preferable oxidation of hydrogen activity.However, the activity of nickel-base material still has gap with platinum.
Summary of the invention
In order to improve the base metal catalytic activity that hydrogen electricity reacts under alkaline system, stability and anti-carbon monoxide poison
A series of problems, such as, the invention proposes a kind of nickel-base materials of light inorganic element doping, using it as alkalinity and neutrality hydrogen
Oxidation reaction/hydrogen evolution reaction elctro-catalyst has excellent hydrogen electro catalytic activity, good stability and anti-carbon monoxide
The ability poisoned；As base metal nickel-base material, the nickel-base material of gap doping is low in cost, and preparation is simple, therefore has
Extensive commercial application prospect.
In order to solve the above-mentioned technical problems, the present invention provides a kind of preparation method of light inorganic element nickel-base material, packets
Include following steps:
S1, nickel persursor material is provided；
S2, make the nickel persursor material hydrogenation, boronation, carbonization or nitridation to get the nickel-base material is arrived；
Wherein, the nickel persursor material includes that nickel salt, nickel complex, inorganic nickel persursor material and nickel metal are organic
Frame material.
Further, the nickel persursor material includes nickel nitrate, nickel sulfate, nickel acetate, the nickel halogenide etc. that business is bought
Nickel salt；The nickel complexes such as ammino compound, cyanogen complex, carbonyl complex, chelate；It can be obtained by preparation
The inorganic nickel persursor materials such as nickel oxide, the nickel hydroxide obtained；And the organic ligands such as 1,3,5-Benzenetricarboxylic acid, terephthalic acid (TPA) and gold
Belong to nickel and is coordinated the nickel metal-organic framework material to be formed.
Further, high-temperature calcination or direct introduction method, which can be used, makes the nickel persursor material hydrogenation, boronation, carbonization
Or nitridation.Wherein, nitridation/hydrogenation/boronation process can use direct introduction method, and the direct introduction method is specifically, before nickel
Ammonium hydroxide, dicyandiamide, ammonium chloride etc. is added in solution before drive body is formed and is introduced directly into the small molecules such as nitrogen/hydrogen/boron.
Further, the hydrogen source of introducing includes hydrogen, ammonia and hydrogen peroxide；The boron source of introducing includes borax, hydroboration
Sodium and boric acid；The carbon source of introducing includes the carbon-rich gas such as methane, ethane, carbon monoxide, the solid carbonaceous materials such as urea, graphite, with
And the carbon containing organic ligand material such as 1,3,5-Benzenetricarboxylic acid, terephthalic acid (TPA)；The nitrogen source of introducing includes urea, ammonium chloride, dicyandiamide, hydrogen
Amine-oxides, ammonia and nitrogen.
Further, transition metal element can also be added during the preparation process in nickel-base material to adjust the electronic state of nickel,
The transition metal element can be one or more of metals such as iron, copper, zinc, chromium, manganese, cobalt, molybdenum.
Further, the temperature of high-temperature calcination needed for adulterating different elements is different, and calcination temperature is preferably 300~600
DEG C, the temperature and time of calcining determines material doped degree.
Further, conductive agent can also be added during the preparation process in nickel-base material and improves material conductivity.The conduction
Agent can be the carbon black conductives agent, KS-6, KS- such as Ketjen black, acetylene black, carbon nanotube, carbon fiber, Super P, Super S, 350G
15, the agent of the graphites such as SFG-6, SFG-15 or graphene.
Further, surfactant can also be added during the preparation process in nickel-base material, to adjust the size shape of material
Looks.The surfactant includes cetyl trimethylammonium bromide, hexadecyltrimethylammonium chloride, trimethyl
The cationic surface active agents such as ammonium bromide；Sodium citrate, Triton X-100, polyoxyethylene sorbitan fat
The nonionic surface active agent such as acid esters；Dodecyl sodium sulfate, lauryl sodium sulfate, neopelex etc. yin from
Subtype surfactant；The high molecular surfactants such as polyvinylpyrrolidone, carboxymethyl cellulose, carbopol；And miaow
The amphoteric surfactantes such as oxazoline derivative, glycine betaine, sulfobetaines.
Another aspect of the present invention additionally provides the nickel-base material being prepared by the method.Due to hydrogen, boron, carbon, nitrogen without
The transition metal elements such as machine light element or iron, cobalt, copper, zinc, chromium, molybdenum, tungsten enter nickel lattice and form the Ni-based of Heteroatom doping
Material, the hydrogen for greatly reducing nickel surface combine energy, are conducive to conduction hydroxy in alkaline electrolyte, to improve catalysis
The activity of agent, and in neutral conditions also with certain oxidation of hydrogen activity.
Further, the pattern of the nickel-base material can for nano particle, nanometer sheet, nanosphere, nanometer rods, nano wire or
Nanotube.
The present invention also provides above-mentioned molecular dopant nickel-base materials to be used as oxidation of hydrogen to react under alkaline or neutral conditions
With hydrogen evolution reaction catalyst.
Further, the nickel-base material of the molecular dopant, which can be supported in electrode base materials, evaluates its hydrogen electrocatalysis
Can, base material includes glass-carbon electrode, carbon paper, gas-diffusion electrode, metal foam electrode, metal foil electrode etc..
Beneficial effects of the present invention:
1, present invention firstly provides light inorganic element hydrogen, boron, carbon, N doping or iron, cobalt, copper, zinc, manganese, chromium, molybdenum, tungsten
Etc. transition metal element doped nickel-base material as oxidation of hydrogen catalysts, while there is excellent catalytic hydrogen evolution reaction
Activity.Activity greatly improves compared with hydro-oxidation catalyst base metal nickel in existing alkaline system, under double-charge even
The best noble metal platinum of activity can be caught up with and surpassed, there is lower overpotential than platinum under same current density for evolving hydrogen reaction.
And in neutral conditions also with certain oxidation of hydrogen activity.
2, light inorganic element hydrogen, boron, carbon, N doping or the iron prepared by the present invention, cobalt, copper, zinc, manganese, chromium, molybdenum, tungsten
It is high etc. the transition metal element doped hydrogen catalyzed oxidation reaction mass activity of nickel-base material.Nitrogen prepared by the present invention simultaneously
Change Raney nickel and shows preferable hydrogen evolution activity.Its catalytic activity considerably beyond other existing base metal hydrogen elctro-catalysts,
The rare pressure of Precious Metals Resources can be alleviated, and nitridation process for preparing nickel provided by the present invention is simple, can substantially reduce
The cost of fuel cell has stronger application value in energy storage conversion art.
3, light inorganic element hydrogen, boron, carbon, N doping or the iron prepared by the present invention, cobalt, copper, zinc, manganese, chromium, molybdenum, tungsten
Etc. transition metal element doped nickel-base catalyst present in oxidation of hydrogen reaction and hydrogen evolution reaction during it is good
Stability and stronger anti-carbon monoxide poison ability.Carbon monoxide, the activity of metal platinum are passed through during stability test
Be decreased obviously and nickel oxide activity reduce almost can be ignored.Its excellent anti-carbon monoxide, which poisons ability, to be made it have
Higher commercial application value, solution are poisoned in Proton Exchange Membrane Fuel Cells and direct methanol fuel cell by carbon monoxide
Efficiency decrease problem is expected to the noble metal platinum for replacing activity best in hydrogen electro-catalysis field.
Detailed description of the invention
Fig. 1 is the TEM image (a, b) and XRD diagram picture (c) of the nickel coordination polymer in embodiment 1；
Fig. 2 is XRD diagram picture (a), SEM image (b) and the TEM image (c) of the nitridation nano nickel particles in embodiment 1；
Fig. 3 hydrogen catalyzed oxidation reaction polarization curve under different rotating speeds for the nitridation nano nickel particles in embodiment 1
(left side) and evolving hydrogen reaction polarization curve (right side)；
Fig. 4 is that the anti-carbon monoxide of nitridation nano nickel particles and noble metal platinum poisons stability curve figure in embodiment 1；
Fig. 5 is to nitrogenize nano nickel particles, metallic nickel nano granule and noble metal platinum catalysis hydrogen in embodiment 1 to be precipitated instead
Answer polarization curve.
Specific embodiment
The present invention will be further explained below with reference to the attached drawings and specific examples, so that those skilled in the art can be with
It more fully understands the present invention and can be practiced, but illustrated embodiment is not as a limitation of the invention.
Following embodiment obtains the nothings such as nitrogen, hydrogen, carbon by nitridation/hydrogenation/carbonization method using different nickel presomas
The transition metal element doped nickel nano material such as the doping of machine light element or iron, cobalt, copper, zinc, manganese, chromium, molybdenum, tungsten.It will catalysis
Agent, which is supported on glass-carbon electrode, tests oxidation of hydrogen and hydrogen precipitation activity, and electrolyte uses 0.1M potassium hydroxide, in three electrodes
It is to electrode with carbon-point under system, saturated calomel electrode is reference electrode, and the conductive substrates of slurries coating are working electrode test
Polarization curve is precipitated in oxidation of hydrogen and hydrogen.Oxidation of hydrogen and hydrogen be precipitated linear sweep voltammetry curve sweep speed be respectively 1mV/s,
5mV/s, electrochemistry compensation 95%.Poison the CO/N that gas uses 5%2Gaseous mixture.
Slurries preparation: weighing 2mg nickel nano material, and 200 μ L ethyl alcohol, 8 μ L naphthols, configuration catalysis is added in 0.3mg Ketjen black
Agent slurries drip 10 μ L, 20 μ L on glass-carbon electrode respectively, spontaneously dry in air.
Electrochemical Test Procedure:
(1) oxidation of hydrogen performance test: before test, hydrogen 30min is passed through into 0.1M potassium hydroxide electrolyte and is extremely saturated,
It keeps hydrogen to be constantly passed through in test process, CV activation a period of time is first swept under three-electrode system, then tests different rotating speeds
The oxidation of hydrogen linear sweep voltammetry curve of lower electrochemistry compensation 95%.
(2) performance test is precipitated in hydrogen: before test, being passed through nitrogen 30min toward 1M potassium hydroxide, air is discharged.It tested
Nitrogen is kept constantly to lead on liquid level in journey, test 1600rpm lower linear scans volt-ampere curve, and sweeping speed is 5mV/s, electrification
Learn compensation 95%.
Embodiment 1: using nickel coordination polymer as precursor synthesis nickel oxide
Six water nickel nitrate of 0.6mmol and 0.3g polyvinylpyrrolidone are dissolved in 20mL deionized water and obtain solution A,
0.4mmol nickel potassium cyanide is dissolved as obtaining precipitating reagent B in 20mL deionized water, and solution A is placed on blender and is vigorously stirred
5min is slowly dropped into precipitating reagent B, after being added dropwise to complete, continues to stir 2min, is then stored at room temperature aging for 24 hours, and centrifugation washs, is true
Sky freeze-drying, obtains nickel coordination polymer presoma, nickel coordination polymer is placed in vacuum tube furnace in ammonia atmosphere 450 DEG C
1h is calcined, nitridation nano nickel particles are made.
Nickel coordination polymer is 100~200nm square thin slice in irregular shape as shown in Figure 1.As shown in Figure 2 through high temperature
After ammonification, the broken nitridation nano nickel particles for obtaining a small amount of carbon-coating package of the positive square piece of nickel, these nitridation nano nickel particles uniformly divide
Cloth, average-size 12.5nm, average diameter are 10~20nm or so.Nitrogen enters nickel lattice and forms nickel oxide, greatly reduces
The hydrogen of nickel surface combines energy, in addition, the nitridation nano nickel particles under carbon-coating protection, extremely difficult in air to be oxidized, mixes nitrogen
Hydrogen electro catalytic activity and good stability of the miscellaneous nickel class catalyst with superelevation.A small amount of carbon-coating is increasing the same of electric conductivity
When play the role of supporting carrier again, be conducive to conduction hydroxy in alkaline electrolyte, to improve the activity of catalyst.
Fig. 3 is that polarization curve is precipitated in the oxidation of hydrogen for nitrogenizing nano nickel particles and hydrogen, it is known that nitridation nano nickel particles tool
Catalytic activity is precipitated in the oxidation of hydrogen and hydrogen for having superelevation.For oxidation of hydrogen, when revolving speed is 1600rpm, in 50mV
Under, current density can achieve 1.7mA cmdisk -2.For liberation of hydrogen, when current density is 10mA cm-2When, required mistake
Potential is only 68mV.
Referring to fig. 4, compared with noble metal platinum, the nitridation nano nickel particles in embodiment 1 have remained stronger anti-one
Carbonoxide poisons ability.
From fig. 5, it can be seen that the nitridation nano nickel particles in embodiment 1 presented during evolving hydrogen reaction it is good steady
It is qualitative.
Embodiment 2: the nickel adulterated using Ni-MOF74 as precursor synthesis carbon
Weigh 0.043g 2,5-Dihydroxyterephthalic acid, 0.13g nickel nitrate, 0.007g salicylic acid, with reacting for 45ml
In kettle, in 18ml ethyl alcohol: n,N-Dimethylformamide: ultrasonic dissolution is complete in water=1:1:1 solution.Reaction kettle is placed on
120 DEG C of reaction 8h in baking oven are centrifuged, and washing, vacuum drying obtains Ni-MOF74 presoma.Ni-MOF74 is placed in vacuum tube
The interior 450 DEG C of calcining 1h in argon atmosphere of formula furnace, are made the nickel nano material of carbon doping.
Embodiment 3: using nickel hydroxide as the nickel of precursor synthesis hydrogen doping
4mmol nickel nitrate is dissolved in the deionized water of 10ml, 5ml ammonium hydroxide is added, obtains soluble nickel ammine,
Nickel ammine is quickly transferred in 45ml diethylene glycol (DEG), 100 DEG C of oil bath 30min release ammonia, obtain nickel hydroxide forerunner
Body.By nickel hydroxide presoma in atmosphere of hydrogen 350 DEG C of calcining 1h, be made hydrogen doping nickelous cyanide nano material.
Embodiment described above is only to absolutely prove preferred embodiment that is of the invention and being lifted, protection model of the invention
It encloses without being limited thereto.Those skilled in the art's made equivalent substitute or transformation on the basis of the present invention, in the present invention
Protection scope within.Protection scope of the present invention is subject to claims.
Claims (10)
1. a kind of preparation method of light inorganic element doping nickel-base material, which comprises the following steps:
S1, nickel persursor material is provided；
S2, make the nickel persursor material hydrogenation, boronation, carbonization or nitridation to get the nickel-base material for arriving the doping；
Wherein, the nickel persursor material includes nickel salt, nickel complex, inorganic nickel persursor material and nickel metal organic frame
Material.
2. the preparation method of nickel-base material as described in claim 1, which is characterized in that the nickel salt include nickel nitrate, nickel sulfate,
Nickel acetate, nickel halogenide；The nickel complex include the ammino compound of nickel, cyanogen complex, carbonyl complex with
And chelate；The inorganic nickel presoma includes nickel oxide, nickel hydroxide；The nickel metal-organic framework material includes isophthalic three
Formic acid, terephthalic acid (TPA) and metallic nickel are coordinated the organic framework materials to be formed.
3. the preparation method of nickel-base material as described in claim 1, which is characterized in that in step S2, using high-temperature calcination
Or direct introduction method makes the nickel persursor material hydrogenation, boronation, carbonization or nitridation；
The hydrogen source of introducing includes hydrogen, ammonia, hydrogen peroxide；The boron source of introducing includes borax, sodium borohydride, boric acid；It introduces
Carbon source includes carbon-rich gas, solid carbonaceous material, carbon containing organic ligand material；The nitrogen source of introducing includes urea, ammonium chloride, double cyanogen
Amine, ammonium hydroxide, ammonia, nitrogen；
Wherein, the carbon-rich gas includes methane, ethane, carbon monoxide；The solid carbonaceous material includes urea, graphite；It is described
Carbon containing organic ligand material includes 1,3,5-Benzenetricarboxylic acid and terephthalic acid (TPA).
4. the preparation method of nickel-base material as claimed in claim 3, which is characterized in that the nickel-base material is gone back during the preparation process
Transition metal element is added, the transition metal element is selected from one of iron, cobalt, copper, zinc, chromium, manganese, molybdenum, tungsten or a variety of.
5. the preparation method of nickel-base material as claimed in claim 4, which is characterized in that the temperature of high-temperature calcination is 300~600
℃。
6. the preparation method of nickel-base material as described in claim 1, which is characterized in that the nickel-base material is during the preparation process
It is also added into conductive agent, the conductive agent is selected from least one of carbon black conductive agent, graphite agent, graphene.
7. the preparation method of nickel-base material as described in claim 1, which is characterized in that the nickel-base material is during the preparation process
It is also added into surfactant.
8. the nickel-base material that method according to claim 1-7 is prepared.
9. nickel-base material as claimed in claim 8, which is characterized in that the nickel-base material is nano particle, nanometer sheet, nanometer
Ball, nanometer rods, nano wire or nanotube.
10. nickel-base material as claimed in claim 9 is urged as the alkaline oxidation of hydrogen under neutrallty condition and hydrogen evolution reaction
Agent.
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| CN111575764A (en) * | 2020-05-19 | 2020-08-25 | 中国科学技术大学 | Composite nickel-tungsten-copper alloy, preparation method and application thereof |
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| CN113584520A (en) * | 2021-07-26 | 2021-11-02 | 中国科学院广州能源研究所 | Super-hydrophilic molybdenum-doped tungsten carbide nano array material and preparation method thereof |
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| CN115007169A (en) * | 2022-01-12 | 2022-09-06 | 渤海大学 | Catalyst for electrochemical oxidation reaction of ammonia, preparation method and application thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111847400A (en) * | 2020-05-14 | 2020-10-30 | 清华大学 | Method for preparing non-noble metal hydrogen fuel cell cathode material |
| CN111575764A (en) * | 2020-05-19 | 2020-08-25 | 中国科学技术大学 | Composite nickel-tungsten-copper alloy, preparation method and application thereof |
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| CN112058299A (en) * | 2020-09-10 | 2020-12-11 | 中山大学 | Multi-shell nickel-based nitride nano composite material and preparation method and application thereof |
| CN113584520A (en) * | 2021-07-26 | 2021-11-02 | 中国科学院广州能源研究所 | Super-hydrophilic molybdenum-doped tungsten carbide nano array material and preparation method thereof |
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| CN114220980B (en) * | 2021-12-08 | 2024-03-26 | 华中科技大学 | Nitrogen-embedded nickel ultrathin nanosheet and preparation method and application thereof |
| CN115007169A (en) * | 2022-01-12 | 2022-09-06 | 渤海大学 | Catalyst for electrochemical oxidation reaction of ammonia, preparation method and application thereof |
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Application publication date: 20191115 |