CN111244486A - Preparation and application of graphite type carbon nitride and carbon composite carrier supported Ir catalyst - Google Patents

Preparation and application of graphite type carbon nitride and carbon composite carrier supported Ir catalyst Download PDF

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CN111244486A
CN111244486A CN201811435812.3A CN201811435812A CN111244486A CN 111244486 A CN111244486 A CN 111244486A CN 201811435812 A CN201811435812 A CN 201811435812A CN 111244486 A CN111244486 A CN 111244486A
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catalyst
composite carrier
carbon
graphite type
carbon nitride
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俞红梅
覃博文
高学强
姚德伟
孙昕野
秦晓平
邵志刚
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Dalian Institute of Chemical Physics of CAS
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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
    • H01M4/92—Metals of platinum group
    • H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
    • 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
    • H01M4/92—Metals of platinum group
    • H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
    • H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
    • 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 relates to a preparation method and application of a graphite type carbon nitride and carbon composite carrier loaded Ir catalyst, in particular to preparation of a graphite type carbon nitride and carbon composite carrier, wherein a nitrogen source and a carbon source are used as precursors, a mixed solvent is added, the solvent is dried after stirring, and then the composite carrier is prepared by heat treatment in argon. And then taking the composite carrier into a mixed solvent, adding an iridium precursor after ultrasonic dispersion, stirring and dispersing, drying the solvent, then carrying out heat treatment in hydrogen, and carrying out centrifugal washing and vacuum drying to obtain the graphite type carbon nitride and carbon composite carrier supported Ir catalyst. TEM test shows that: the graphite type carbon nitride and carbon composite carrier loads Ir catalyst, when the loading capacity is not more than 1 wt%, no metal nano-particles exist, and when the loading capacity is more than 1%, metal nano-particles exist. The LSV test shows that: 1% Ir @ g-C3N4(ii)/C and 2% Ir @ g-C3N4The specific mass activity at 50mV overpotential is 43% and 120% of Pt/C.

Description

Preparation and application of graphite type carbon nitride and carbon composite carrier supported Ir catalyst
Technical Field
The invention relates to a preparation method and application of a graphite hydroxide type carbon nitride and carbon composite carrier loaded Ir catalyst for an alkaline anion exchange membrane fuel cell3N4and/C. 1% Ir @ g-C as an alkaline anion exchange membrane fuel cell hydrogen oxidation electrocatalyst3N4Specific Mass Activity at 0.05V for/C was 43% of commercial Pt/C, 2% Ir @ g-C3N4The specific mass activity at 0.05V for/C was 120% of that of commercial Pt/C.
Background
Alkaline Anion Exchange Membrane Fuel Cells (AAEMFC) are a new class of polymer electrolyte membrane fuel cells. Compared with Proton Exchange Membrane Fuel Cells (PEMFCs), the Alkaline Fuel Cell (AFC) cathode Oxygen Reduction Reaction (ORR) has the advantage of fast kinetics, and the cathode is expected to radically get rid of the dependence on noble metal platinum; meanwhile, the solid anionic polymer electrolyte membrane is adopted, so that the problems of KOH leakage, carbonation and the like of a liquid electrolyte in AFC are solved, and the advantages of AFC and PEMFC are combined. Therefore, the AAEMFC has wide application prospect and becomes a new research direction in the field of fuel cells.
Although AAEMFC has the advantage of fast kinetics of the cathode Oxygen Reduction Reaction (ORR) of Alkaline Fuel Cells (AFC), studies have found that: even noble platinum group catalysts are electrocatalysts for anodic oxidation of Hydrogen (HOR) under alkaline conditions, the exchange current density is 2 orders of magnitude slower than under acidic conditions. The pH effect of the anode catalyst seriously hinders the achievement of the target of reducing the noble metal loading of the AAEMFC anode and using the non-noble metal catalyst, so the recent research on the non-platinum or non-noble metal anode hydrogen oxidation catalyst which can be used under the alkaline condition is gradually a new focus.
In the research of alkaline oxyhydrogen electrocatalysts, metallic Ir and its Ir-M alloy catalysts have attracted extensive attention. A Ru-Ir/C catalyst was prepared by j.ohyama et al (j.mater.chem.a,2016,4, 15980). Under alkaline conditions, the catalytic activity of the Ru-Ir/C nanoparticles was found to be 4 times that of Pt/C. Hongsen Wang. et al (J.Am.chem.Soc,2017) introduced a preparation method of IrPdRu/C, and the catalytic activity of the anode catalyst is superior to that of Pt/C. Ir nanowires prepared by Wei luo et al (j.mater.chem.a,2017,5,22959) have good catalytic activity for hydrogen oxidation.
The invention adopts a dipping reduction method to prepare a graphite type carbon nitride and carbon composite carrier supported Ir catalyst, fixes atomic Ir through nitrogen atoms in the graphite type carbon nitride, and simultaneously modulates the electronic structure of the Ir. Meanwhile, the graphite type carbon nitride and carbon composite has better conductivity, the theoretical loading capacity of Ir in the Ir catalyst loaded on the composite carrier is not more than 2%, and the alkaline hydrogen oxidation activity is better.
Disclosure of Invention
The invention aims to provide a graphite hydroxide type carbon nitride and carbon composite carrier loaded Ir catalyst for an alkaline anion exchange membrane fuel cell, and ensure that the oxyhydrogen electrocatalyst prepared by the preparation method of the catalyst can ensure that the alkaline anion exchange membrane fuel cell has better full-cell performance.
In order to achieve the purpose, the invention adopts the technical scheme that:
the invention provides a preparation method of a graphite type carbon nitride and carbon composite carrier supported Ir catalyst, which comprises the following steps:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking a proper amount of nitrogen source and carbon source, adding the nitrogen source and the carbon source into a mixed solvent of ethanol and water, carrying out ultrasonic stirring for 0.5-12 hours, drying the solvent to obtain a mixture, and carrying out heat treatment reaction on the mixture at the temperature of 550-750 ℃ in an argon or nitrogen atmosphere for 2-6 hours to obtain the graphite type carbon nitride and carbon composite carrier;
(2) preparing a graphite type carbon nitride and carbon composite carrier supported Ir catalyst: and adding a certain amount of Ir precursor into the graphite type carbon nitride and carbon composite carrier, performing ultrasonic stirring reaction for 0.5-12 hours, drying the solvent to obtain a mixture, treating the mixture at the temperature of 200-400 ℃ for 2-6 hours in a hydrogen atmosphere, performing centrifugal washing and vacuum drying to obtain the graphite type carbon nitride and carbon composite carrier loaded Ir catalyst.
Based on the technical scheme, preferably, the nitrogen source is at least one of urea, melamine and dicyandiamide; the carbon source is at least one of XC-72, BP2000, graphene oxide and graphene; the precursor of Ir is at least one of chloroiridic acid, iridium acetylacetonate and iridium trichloride.
Based on the technical scheme, the stirring time range in the step (1) is preferably 12 hours; the argon heat treatment temperature is 550 ℃; the mass ratio of the nitrogen source to the carbon source is 4:1-1: 4; the reaction time ranged from 4 hours.
Based on the technical scheme, preferably, the molar concentration of the precursor of Ir in the step (2) is 0.2M; the hydrogen heat treatment temperature was 300 ℃.
The invention also provides a graphite type carbon nitride and carbon composite carrier loaded Ir catalyst prepared by the preparation method, wherein the carrier of the catalyst loaded Ir catalyst is a graphite type carbon nitride and carbon composite, the active center is metal Ir, and the loading amount of the Ir is 0.05-2 wt%; in the carrier, the carbon-nitrogen atom ratio is 41:59-88: 12; the metallic Ir is in the shape of at least one of nanoparticles, sub-nanoclusters or single atoms.
The invention further provides application of the catalyst in anode hydrogen oxidation of the alkaline anion exchange membrane fuel cell.
Advantageous effects
1. The graphite hydroxide type carbon nitride and carbon composite carrier loaded Ir catalyst for the alkaline anion exchange membrane fuel cell prepared by the method has the advantages of small metal consumption, loading capacity of 0.05 wt% -2 wt%, and good catalytic activity of hydrogen oxidation.
2. The mass ratio of melamine and carbon serving as precursors is controlled, and the atomic ratio of carbon to nitrogen elements in the graphite type carbon nitride and carbon composite carrier is regulated and controlled, wherein the range of the atomic ratio of carbon to nitrogen is 40:60-88: 12.
3. Compared with a commercial Pt/C catalyst, the graphite hydroxide type carbon nitride and carbon composite carrier loaded Ir catalyst for the alkaline anion exchange membrane fuel cell prepared by the method has better catalytic activity of hydrogen oxidation under alkaline conditions; 1% Ir @ g-C3N4The specific mass activity of the Pt/C at 50mV is 43% of that of Pt/C, 2% Ir @ g-C3N4The specific mass activity at 50mV of/C is 120% of Pt/C. Has important application value in the anode catalyst of the alkaline anion exchange membrane fuel cell.
Drawings
FIG. 1 is a schematic diagram of a graphite type carbon nitride and carbon composite carrier loaded low-loading Ir catalyst.
FIG. 2 shows a graphite type carbon nitride and carbon composite carrier supported low-loading Ir catalyst (1% Ir @ g-C) prepared as described in example 13N4XRD pattern of/C).
FIG. 3 shows a graphite-type carbon nitride and carbon composite carrier supported low-loading Ir catalyst (1% Ir @ g-C) prepared as described in example 13N4TEM image of/C).
FIG. 4 shows a graphite-type carbon nitride and carbon composite carrier supported low-loading Ir catalyst (1% Ir @ g-C) prepared by the procedure described in example 13N4(a) SEM picture and (b) EDS Mapping picture of/C).
FIG. 5 is a graph of a graphitic carbon nitride and carbon composite supported low-loading Ir catalyst (1% Ir @ g-C) prepared according to the procedures described in example 1, example 2, example 3, example 4 and example 53N4/C)、(2％Ir@g-C3N4/C)、(0.5％Ir@g-C3N4/C)、(0.25％Ir@g-C3N4/C) and (0.05% Ir @ g-C3N4Polarization curve obtained by cyclic voltammetric scanning of/C).
FIG. 6 is a graph of a graphitic carbon nitride and carbon composite supported low-loading Ir catalyst (1% Ir @ g-C) prepared as described in examples 1, 2, 3, 4 and 53N4/C)、(2％Ir@g-C3N4/C)、(0.5％Ir@g-C3N4/C)、(0.25％Ir@g-C3N4/C) and (0.05% Ir @ g-C3N4and/C) polarization curves obtained by performing linear voltammetric scanning.
FIG. 7 is a graph of a graphitic carbon nitride and carbon composite support supported low-loading Ir catalyst (1% Ir @ g-C) prepared according to the procedures described in examples 1, 6 and 73N4Polarization curve obtained by cyclic voltammetric scanning of/C).
FIG. 8 is a graph of a graphitic carbon nitride and carbon composite support supported low-loading Ir catalyst (1% Ir @ g-C) prepared according to the procedures described in examples 1, 6 and 73N4Polarization curve obtained by cyclic voltammetric scanning of/C).
FIG. 9 is a plot of the polarization from cyclic voltammetric scans of a commercial 20% Pt/C catalyst.
FIG. 10 is a plot of the polarization from a linear voltammetric scan of a commercial 20% Pt/C catalyst.
Detailed Description
The preparation method, characteristics and application of the graphite hydroxide type carbon nitride and carbon composite carrier supported Ir catalyst for the alkaline anion exchange membrane fuel cell are further explained by combining the attached drawings as follows:
example 1
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 0.5g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing the mixture in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N being 88:12 a graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and centrifugally washing and vacuum drying the mixture to obtain the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst, wherein the mass fraction of the metal Ir is 1%.
XRD testing of fig. 2 shows that: 1% Ir @ g-C3N4C does not haveThe characteristic peak of the Ir nanocrystal is obvious, which indicates that the Ir is in an amorphous state or the Ir can be in a sub-nanometer structure or a single atom.
The TEM test of fig. 3 shows: 1% Ir @ g-C3N4the/C has no nanoparticles and the metal morphology may be sub-nanoparticles or monoatomic.
The SEM of fig. 4a and EDS of fig. 4b indicate: 1% Ir @ g-C3N4The Ir, N and C elements in the/C are uniformly distributed.
The CV test of fig. 5 shows: 1% Ir @ g-C3N4the/C has no obvious absorption and desorption peak in the absorption and desorption area of hydrogen, and further indicates that Ir is a sub-nano structure or a single atom.
The LSV test of fig. 6 shows: 1% Ir @ g-C3N4The limiting diffusion current of/C is 1.0mAcm-2Thus, the compound has a better hydrogen oxidation activity.
Example 2
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 0.5g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing the mixture in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N being 88:12 a graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and centrifugally washing and vacuum drying the mixture to obtain the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst, wherein the mass fraction of the metal Ir is 2%.
The CV test of fig. 5 shows: 2% Ir @ g-C3N4the/C has an obvious absorption and desorption peak in the absorption and desorption area of the hydrogen, which shows that when the loading capacity is 2%, the shape of Ir is a nano particle and is a crystalline state.
The LSV test of fig. 6 shows: 2% Ir @ g-C3N4The limiting diffusion current of/C is 2.5mAcm-2Has the advantages ofGood hydrogen oxidation activity.
Example 3
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 0.5g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing the mixture in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N being 88:12 a graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and centrifugally washing and vacuum drying the mixture to obtain the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst, wherein the mass fraction of the metal is 0.5%.
The CV test of fig. 5 shows: 0.5% Ir @ g-C3N4the/C has no obvious absorption and desorption peak in the absorption and desorption area of hydrogen, and the Ir is a sub-nano structure or a single atom.
The LSV test of fig. 6 shows: 0.5% Ir @ g-C3N4The limiting diffusion current of/C is 0.5mAcm-2Has certain hydrogen oxidation activity.
Example 4
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 0.5g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing the mixture in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N being 88:12 a graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and preparing the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst through centrifugal washing and vacuum drying, wherein the mass fraction of the obtained metal is 0.25%.
The CV test of fig. 5 shows: 0.25% Ir @ g-C3N4the/C has no obvious absorption and desorption peak in the absorption and desorption area of hydrogen, and further indicates that Ir is a sub-nano structure or a single atom.
The LSV test of fig. 6 shows: 0.25% Ir @ g-C3N4the/C has no obvious hydrogen oxidation activity.
Example 5
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 0.5g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing the mixture in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N being 88:12 a graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and preparing the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst through centrifugal washing and vacuum drying, wherein the mass fraction of the obtained metal is 0.05%.
The CV test of fig. 5 shows: 0.05% Ir @ g-C3N4the/C has no obvious absorption and desorption peak in the absorption and desorption area of hydrogen, and further indicates that Ir is a sub-nano structure or a single atom.
The LSV test of fig. 6 shows: 0.05% Ir @ g-C3N4the/C has no obvious hydrogen oxidation activity.
Example 6
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 1g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition, wherein the atomic ratio of C to N is 74:26 graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and centrifugally washing and vacuum drying the mixture to obtain the graphite type carbon nitride and carbon composite carrier loaded low-load Ir catalyst, wherein the mass fraction of the metal is 1%.
The CV test of fig. 7 shows: 1% Ir @ g-C3N4and/C (C: N ═ 74:26) has no obvious absorption and desorption peaks in the absorption and desorption regions of hydrogen, and Ir is shown to be a sub-nano structure or a single atom.
The LSV test of fig. 8 shows: 1% Ir @ g-C3N4The limiting current of/C (C: N: 74:26) is 0.8mAcm-2The increase in nitrogen element may cause a decrease in catalyst activity and a deterioration in conductivity.
Example 7
Preparation:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking 2g of melamine, 1g of XC-72, 10mL of ethanol and 10mL of water in a 50mL beaker, carrying out ultrasonic treatment for 30 minutes, stirring for 12 hours, drying the solvent at 60 ℃, grinding, placing in a quartz boat in an argon atmosphere, and reacting for 4 hours at 550 ℃ to prepare the melamine-formaldehyde resin composition with the atomic ratio of C to N of 59:41 graphite type carbon nitride and carbon composite support.
(2) The graphite type carbon nitride and carbon composite carrier supported Ir catalyst: taking 50mg of the graphite type carbon nitride and carbon composite carrier prepared in the step (1), adding a certain amount of chloroiridic acid, and stirring for 12 hours. Then grinding and placing the mixture in a quartz boat in a hydrogen atmosphere, reacting for 2 hours at 300 ℃, and centrifugally washing and vacuum drying the mixture to prepare the graphite type carbon nitride and carbon composite carrier supported Ir catalyst, wherein the mass fraction of the metal is 1%.
The CV test of fig. 7 shows: 1% Ir @ g-C3N4and/C (C: N: 59:41) has no obvious absorption and desorption peak in the absorption and desorption region of hydrogen.
The LSV test of fig. 8 shows: 1% Ir @ g-C3N4the/C (C: N: 59:41) had no significant hydro-oxidation activity.

Claims (6)

1. A preparation method of a graphite type carbon nitride and carbon composite carrier supported Ir catalyst is characterized by comprising the following steps:
(1) preparing a graphite type carbon nitride and carbon composite carrier: taking a proper amount of nitrogen source and carbon source, adding the nitrogen source and the carbon source into a mixed solvent of ethanol and water, carrying out ultrasonic stirring for 0.5-12 hours, drying the solvent to obtain a mixture, and carrying out heat treatment reaction on the mixture at the temperature of 550-750 ℃ in an argon or nitrogen atmosphere for 2-6 hours to obtain the graphite type carbon nitride and carbon composite carrier;
(2) preparing a graphite type carbon nitride and carbon composite carrier supported Ir catalyst: adding a certain amount of Ir precursor into the graphite type carbon nitride and carbon composite carrier, performing ultrasonic stirring reaction for 0.5-12, drying the solvent to obtain a mixture, treating the mixture at the temperature of 200-400 ℃ for 2-6 hours in a hydrogen atmosphere, performing centrifugal washing and vacuum drying to obtain the graphite type carbon nitride and carbon composite carrier loaded Ir catalyst.
2. The method of claim 1, wherein: the nitrogen source is at least one of urea, melamine and dicyandiamide; the carbon source is at least one of XC-72, BP2000, graphene oxide and graphene; the precursor of Ir is at least one of chloroiridic acid, iridium acetylacetonate and iridium trichloride.
3. The method of claim 1, wherein: the stirring time range in the step (1) is 12 hours; the argon heat treatment temperature is 550 ℃; the mass ratio of the nitrogen source to the carbon source is 4:1-1: 4; the reaction time ranged from 4 hours.
4. The method of claim 1, wherein: the molar concentration of the precursor of Ir in the step (2) is 0.01-0.1M; the hydrogen heat treatment temperature was 300 ℃.
5. A graphitic carbon nitride and carbon composite carrier-supported Ir catalyst prepared according to the preparation method of any one of claims 1 to 4, characterized in that: the catalyst supported catalyst has a carrier which is a graphite carbon nitride and carbon compound, an active center which is metal Ir, and the loading capacity of the Ir is 0.05 wt% -2 wt%; in the carrier, the carbon-nitrogen atom ratio is 41:59-88: 12; the metallic Ir is in the shape of at least one of nanoparticles, sub-nanoclusters or single atoms.
6. Use of the catalyst of claim 5 in the anodic oxidation of hydrogen in an alkaline anion exchange membrane fuel cell.
CN201811435812.3A 2018-11-28 2018-11-28 Preparation and application of graphite type carbon nitride and carbon composite carrier supported Ir catalyst Pending CN111244486A (en)

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