CN114990573A - Preparation method of self-assembled two-dimensional Ir metallocene electrocatalyst - Google Patents
Preparation method of self-assembled two-dimensional Ir metallocene electrocatalyst Download PDFInfo
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- CN114990573A CN114990573A CN202210627409.0A CN202210627409A CN114990573A CN 114990573 A CN114990573 A CN 114990573A CN 202210627409 A CN202210627409 A CN 202210627409A CN 114990573 A CN114990573 A CN 114990573A
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- C25B1/00—Electrolytic production of inorganic compounds or non-metals
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- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
- C25B11/081—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound the element being a noble metal
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Abstract
The invention relates to a self-assembled two-dimensional Ir metallocene electrocatalyst and a preparation method thereof, belonging to the field of preparation of novel nano catalytic materials. The material synthesis method used in the invention is a gas/liquid interface self-assembly method. The method comprises the following specific steps: firstly, dissolving polyvinylpyrrolidone and iridium chloride trihydrate into ethylene glycol, adding ultrapure water into the solution, fully mixing, transferring the solution into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and putting the kettle into a constant-temperature air-blast drying oven for heating reaction. And centrifuging, washing and drying the obtained product to obtain a black powdery solid, namely the self-assembled two-dimensional Ir metallocene electrocatalyst. The preparation method is simple and easy to implement, the synthesized catalytic material has stable performance, the experimental conditions are green and environment-friendly, and the experimental conditions are mild and suitable for large-scale production.
Description
Technical Field
The invention relates to a preparation method of a self-assembled two-dimensional Ir metallocene electrocatalyst, belonging to the technical field of novel functional materials.
Background
With the urgent need of the human society for renewable clean energy, new technologies for sustainable energy conversion and production have attracted great attention. The water electrolysis hydrogen production technology is the most potential hydrogen energy preparation technology recognized at present, and as an oxidation process essential in water electrolysis, Oxygen Evolution Reaction (OER) is widely regarded as an important process related to energy conversion application. Therefore, improving OER efficiency is a key step in the development of sustainable alternative energy. However, the energy barrier created by the multi-step reactions in anode kinetics allows the OER to have a higher reaction overpotential than the hydrogen evolution reaction, making the oxygen evolution half-reaction the rate-determining step in the water splitting reaction, greatly limiting the reaction efficiency of water electrolysis. Therefore, the development of an electrocatalyst with high catalytic activity, good stability and low cost is very important.
Similar to two-dimensional materials such as graphene, the two-dimensional metal graphene material is generally a metal nanosheet having a thickness of only an atomic layer (single layer or few layers), and has characteristics of high specific surface area, abundant defect sites, excellent conductivity and the like. More importantly, the metal alkene material can expose a large number of unsaturated metal sites, so that the metal alkene material is expected to show excellent catalytic performance in heterogeneous catalytic reactions. In recent years, in the thermocatalytic conversion of methane, small molecules (H) 2 O、CO 2 、N 2 、O 2 Etc.), researchers have shown the catalytic performance far superior to that of the conventional metal catalysts by regulating and controlling the components and structure of the metal alkene catalysts in heterogeneous catalytic reactions such as photo/electro-catalytic conversion, cathode/anode reaction of fuel cells, etc. Although in the preliminary stage, metallocene catalysts have emerged as a new avenue for driving the development of heterogeneous catalysis.
Ir and Ru, which are the most advanced acidic OER catalysts at present, have relatively low overpotential and Tafel slope, and particularly excellent stability. Ir is considered a more desirable catalyst candidate for OER than Ru because it is somewhat less active but more stable. It is well known that the performance of nanocatalysts is largely influenced by the morphology, but methods related to Ir nanostructure control are rarely reported. Most Ir nanostructures obtained so far are limited to nanoparticles with very limited OER activity, which severely hampers an in-depth study of the relationship between Ir nanomaterial structure and performance to achieve OER catalytic optimization.
The invention prepares the self-assembled two-dimensional Ir metallocene electrocatalyst by taking Ir nanocrystals with the particle size of less than 2 nanometers as assembly units through a gas/liquid interface self-assembly method by a one-pot method, and overcomes the defects of complex preparation method, non-uniform product components, high cost and the like of the existing Ir-based nanocrystal material. The ultra-thin two-dimensional metallocene self-assembled by the ultra-small Ir nanocrystal can be prepared in one reaction by a gas/liquid interface self-assembly method for the first time, and the electrocatalyst has an ultra-thin porous two-dimensional structure, has intrinsic catalytic activity and stability of the Ir-based material in acidic OER, and provides a wide prospect in electrocatalysis.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides a method for preparing a self-assembled two-dimensional Ir metallocene electrocatalyst by a one-pot method, and the two-dimensional ultrathin Ir metallocene electrocatalyst can be prepared by a one-pot reaction by adopting a gas/liquid interface self-assembly method. The preparation process is simple, rapid and efficient, and is suitable for large-scale industrial production.
The purpose of the invention is realized by the following technical scheme:
1) respectively weighing polyvinylpyrrolidone (-360000) and iridium chloride trihydrate in a beaker according to a certain molar ratio;
2) adding ethylene glycol into the beaker used in the step 1), and carrying out ultrasonic treatment to promote polyvinylpyrrolidone (-360000) and iridium chloride trihydrate to dissolve into the ethylene glycol to form a light green mixed solution;
3) adding ultrapure water into the beaker obtained in the step 2) and stirring to enable the ultrapure water and the original solution to be mutually soluble;
4) transferring the mixed solution obtained in the step 3) into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and placing the reaction kettle in a 220 o C, reacting for 2 hours in a constant-temperature air-blast drying box;
5) centrifuging the reaction mixture obtained in step 4), washing with ethanol 3-4 times, and then washing at 60 deg.C o And C, vacuum drying to obtain a final product.
The invention has the beneficial effects that:
(1) the invention provides a preparation method of a self-assembled two-dimensional Ir metallocene electrocatalyst, which is simple and easy to operate, does not need special equipment, is suitable for large-scale preparation, can prepare the two-dimensional Ir metallocene electrocatalyst by only one reaction, and can meet the requirements of practical application;
(2) the two-dimensional Ir metallocene electrocatalyst prepared by the invention has high preparation speed and high product purity, and improves the preparation efficiency;
(3) the two-dimensional Ir metalene electrocatalyst prepared by the invention has good catalytic effect on acidic electrocatalytic oxygen evolution reaction;
(4) the method of the invention is simple and easy to implement, and does not need special equipment.
Drawings
FIG. 1 is a two-dimensional Ir metalene electrocatalyst macroscopic TEM image;
FIG. 2 two-dimensional Ir metalene electrocatalyst high magnification TEM image;
FIG. 3 shows an X-ray diffraction (XRD) pattern of the two-dimensional Ir metallocene electrocatalyst prepared by the method of the present invention, wherein the diffraction peak positions and peak shapes in the experimental obtained spectrogram and the simulated spectrogram are well matched, which proves that the two structures are consistent, and the purity of the prepared sample is good;
FIG. 4A two-dimensional Ir metallocene electrocatalyst prepared by the method of the present invention at 0.5M H 2 SO 4 LSV diagram in (1), it can be seen that the overpotential is far lower than that of commercial IrO 2 Catalysts and conventional Ir nanoparticle catalysts.
Detailed Description
The present invention will be described in further detail with reference to the following embodiments, which are not intended to limit the scope of the present invention.
Example 1
Firstly, respectively weighing 0.9 mmol of polyvinylpyrrolidone (-40000) and 0.05 mmol of iridium chloride trihydrate to dissolve in 6 mL of ethylene glycol, adding 3 mL of ultrapure water into the mixed solution to dissolve mutually to form a light green mixed solution, transferring the solution into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and putting the high-pressure reaction kettle into a reaction kettle with a 220 mm polytetrafluoroethylene lining o C reacting in constant temperature air-blast drying oven for 2 hr, centrifuging, ultrasonic cleaning with ethanol for 3-4 times, and washing with water at 60 deg.C o And C, drying under vacuum drying to obtain the two-dimensional Ir metallocene electrocatalyst.
Example 2
Firstly, respectively weighing 9 mmol of polyvinylpyrrolidone (-40000) and 0.5 mmol of polyvinylpyrrolidoneDissolving mmol iridium chloride trihydrate into 60 mL ethylene glycol, adding 30 mL ultrapure water into the mixed solution to mutually dissolve the iridium chloride trihydrate and the ethylene glycol to form a light green mixed solution, transferring the solution into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and putting the high-pressure reaction kettle into a reactor with a 220-inch polytetrafluoroethylene lining o C reacting in constant temperature air-blast drying oven for 2 hr, centrifuging, ultrasonic cleaning with ethanol for 3-4 times, and washing with water at 60 deg.C o And C, drying under vacuum drying to obtain the two-dimensional Ir metallocene electrocatalyst.
Example 3
Firstly, respectively weighing 0.9 mmol of polyvinylpyrrolidone (-40000) and 0.05 mmol of iridium chloride trihydrate to dissolve in 6 mL of ethylene glycol, adding 3 mL of ultrapure water into the mixed solution to dissolve mutually to form a light green mixed solution, transferring the solution into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and putting the high-pressure reaction kettle into a reaction kettle with a 220 mm polytetrafluoroethylene lining o C reacting for 6 hours in a constant temperature air-blast drying oven, then centrifugally separating, ultrasonically cleaning for 3-4 times by using ethanol, and then cleaning at 60 degrees o And C, drying under vacuum drying to obtain the two-dimensional Ir metallocene electrocatalyst.
Example 4
Firstly, respectively weighing 0.9 mmol of polyvinylpyrrolidone (-40000) and 0.05 mmol of iridium chloride trihydrate to dissolve in 6 mL of ethylene glycol, adding 3 mL of formaldehyde to the mixed solution to dissolve mutually to form a light green mixed solution, transferring the solution to a high-pressure reaction kettle with a polytetrafluoroethylene lining, and putting the high-pressure reaction kettle into a reaction kettle with a 220. sup. th.e polytetrafluoroethylene lining o C reacting in constant temperature air-blast drying oven for 2 hr, centrifuging, ultrasonic cleaning with ethanol for 3-4 times, and washing with water at 60 deg.C o And C, drying under vacuum drying to obtain the two-dimensional Ir metallocene electrocatalyst.
Claims (4)
1. The self-assembled two-dimensional Ir metalene electrocatalyst is characterized in that the nano particles are formed by self-assembling Ir nanocrystals with the particle size of less than 2 nanometers as assembling units to form metalene with a two-dimensional ultrathin structure.
2. A preparation method of a self-assembled two-dimensional Ir metallocene electrocatalyst is characterized by comprising the following steps:
1) weighing polyvinylpyrrolidone (360000) and iridium chloride trihydrate in a certain molar ratio, and dissolving the polyvinylpyrrolidone and the iridium chloride trihydrate in ethylene glycol;
2) adding ultrapure water into the solution obtained in the step 1), mixing, transferring into a high-pressure reaction kettle with a polytetrafluoroethylene lining, and carrying out heating reaction in a constant-temperature air-blast drying oven;
3) centrifuging, washing and drying to obtain a black powdery product.
3. The self-assembled two-dimensional Ir metallocene electrocatalyst according to claim 2, wherein the solvent used is ethylene glycol and the iridium salt used is iridium chloride trihydrate.
4. The method of preparing a self-assembled two-dimensional Ir metallocene electrocatalyst according to claim 2, wherein the reaction temperature in step 2) is 220 ℃ o And C, the reaction time is 2 to 12 hours.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115400765A (en) * | 2022-09-30 | 2022-11-29 | 东南大学 | Pd-based double-layer metal alkene nano material, and preparation method and application thereof |
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| CN109126781A (en) * | 2018-09-20 | 2019-01-04 | 吉林大学 | A kind of ultra-thin RhPdH nanometer sheet material and the preparation method and application thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115400765A (en) * | 2022-09-30 | 2022-11-29 | 东南大学 | Pd-based double-layer metal alkene nano material, and preparation method and application thereof |
| CN115400765B (en) * | 2022-09-30 | 2023-12-26 | 东南大学 | Pd-based double-layer metal alkene nanomaterial, and preparation method and application thereof |
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