CN114318403B - Method for preparing platinum monoatomic material by adopting alkyl imidazole ionic liquid - Google Patents
Method for preparing platinum monoatomic material by adopting alkyl imidazole ionic liquid Download PDFInfo
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- CN114318403B CN114318403B CN202111669776.9A CN202111669776A CN114318403B CN 114318403 B CN114318403 B CN 114318403B CN 202111669776 A CN202111669776 A CN 202111669776A CN 114318403 B CN114318403 B CN 114318403B
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Abstract
The invention discloses a method for preparing platinum monoatomic material by cyclic voltammetry by taking alkyl imidazole ionic liquid as electrolyte. The method comprises the steps of adopting a three-electrode system, wherein a sample prepared by composite electrodeposition is used as a working electrode, a platinum sheet is used as a counter electrode, a non-mercury wire electrode is used as a reference electrode, an alkyl imidazole ionic liquid is used as an electrolyte, and loading platinum monoatoms through Cyclic Voltammetry (CV). The platinum single-atom-loaded composite electrode material prepared by adopting the alkyl imidazole ionic liquid as the electrolyte has good hydrogen evolution catalytic activity, and can be applied to the field of water electrolysis hydrogen production.
Description
Technical Field
The invention relates to the technical field of monoatomic catalysts, in particular to a method for preparing a platinum monoatomic material by adopting an alkyl imidazole ionic liquid.
Background
The increasing depletion and rise of fossil fuels have driven a number of environmental problems to seek new clean energy sources. The hydrogen energy has the advantages of high energy density, no pollution of combustion products, renewable energy and the like, is recognized as a green energy carrier, and is one of the most potential energy sources in the future. The development of hydrogen production technology is a primary problem to be solved by the generalization of hydrogen energy technology. Compared with the traditional hydrogen production method, the electrolytic water hydrogen production has the advantages of mature industrialization, no pollution, high purity of the produced hydrogen, and the like, and is widely concerned, but the energy consumption is still too high. Therefore, development of an electrode material having a low overpotential and a high catalytic activity is urgent.
Platinum-containing catalysts are considered to be the best electrode for hydrogen production by water electrolysis, but their high cost and scarcity have prevented their large-scale use. In recent years, researchers have focused on increasing the efficiency of platinum utilization by reducing the amount of platinum used, with single-atom catalysts (SACs) attracting extensive research interest due to their high atomic utilization and unique electronic properties for various reactions. However, the surface free energy of the monoatomic platinum is higher, agglomeration is easy to occur, the stability of the monoatomic platinum is further hindered, the preparation conditions of SACs are harsh, and the development of a novel method for controllably preparing the monoatomic platinum material has important significance.
The method for preparing the monoatomic platinum electrocatalyst by electrodeposition has simple and convenient operation and simple process, and the obtained material can be directly used as an electrode in the process of preparing hydrogen by electrolyzing water, does not need an adhesive or a conductive agent, and effectively improves the stability of the electrode. However, the preparation of the monoatomic platinum electrocatalyst in the traditional aqueous solution has some defects, such as too fast mass transfer of ions in the aqueous solution, narrow electrochemical window and the like, so that the problems of easy agglomeration of platinum monoatoms or too small load capacity and the like are caused, and finally the hydrogen evolution performance of the synthesized monoatomic platinum electrocatalyst can be influenced.
Disclosure of Invention
In view of the above-mentioned drawbacks of the prior art, the technical problem to be solved by the present invention is to use alkyl imidazole ionic liquid as electrolyte based on the dissolution mechanism of the platinum sheet counter electrode in the ionic liquid, and to realize the preparation of platinum monoatomic material by cyclic voltammetry.
In order to achieve the above purpose, the invention provides a method for preparing platinum monoatomic material by adopting alkyl imidazole ionic liquid, which comprises the following steps:
firstly, dissolving nickel chloride hexahydrate, cobalt chloride hexahydrate and graphene oxide serving as raw materials in a eutectic solution to form electrolyte, and performing constant potential composite electrodeposition in a standard three-electrode system to obtain a Ni-Co-GO composite electrode material; placing the Ni-Co-GO composite electrode material into a tube furnace for nitriding, wherein urea is used as a nitrogen source;
step two, taking the Ni-Co-GO-N composite electrode material subjected to nitriding in the step two as a working electrode to form a three-electrode system, adding alkyl imidazole ionic liquid into an electrolytic cell containing the three-electrode system, and anchoring monoatomic platinum by adopting a cyclic voltammetry;
and step three, taking the platinum single-atom-loaded composite electrode material prepared in the step two out of the electrolytic cell, cleaning, and finally drying.
Further, in the step one, the reference electrode in the standard three-electrode system is a non-mercury wire electrode, and the counter electrode is a nickel plate.
Further, in the step one, the working electrode in the standard three-electrode system is one of carbon cloth, foam nickel or carbon paper.
Further, in the second step, the alkyl imidazole ionic liquid is one of 1-ethyl-3-methylimidazole tetrafluoroborate ionic liquid or 1-butyl-3-methylimidazole tetrafluoroborate ionic liquid.
Further, the adding amount of the alkyl imidazole ionic liquid is 30mL.
Further, the condition of the cyclic voltammetry in the second step is that the sweeping speed is 60-100 mV/s, the voltage interval is-0.6 to-1.2V, and the cycle number is 4000-8000.
Further, in the first step, the eutectic solution is formed by dissolving choline chloride in ethylene glycol.
Further, in the step two, the platinum sheet electrode is used as a counter electrode, and the non-mercury wire electrode is used as a reference electrode.
Further, the nitriding temperature in the first step is 260-300 ℃.
And in the third step, the cleaning process is to clean with deionized water and then clean with absolute ethyl alcohol.
Compared with the prior art, the invention has the remarkable advantages that:
1. the alkyl imidazole ionic liquid adopted by the invention is nontoxic, has degradability, can be recycled, and has a wider electrochemical window and higher viscosity. The solvent is used as electrolyte, and the platinum monoatomic material is directly prepared by an electrochemical method, so that the method is a novel environment-friendly controllable synthesis process;
2. the method can effectively reduce the dosage of platinum in the composite electrode material, and improve the utilization rate of platinum, thereby effectively reducing the cost;
3. compared with other processes for preparing platinum monoatomic materials, the preparation technology provided by the invention is simpler, the process is greatly shortened, the process is controllable, and the requirements on equipment conditions are lower, so that the cost is greatly reduced.
The conception, specific structure, and technical effects of the present invention will be further described with reference to the accompanying drawings to fully understand the objects, features, and effects of the present invention.
Drawings
FIG. 1 is a process flow diagram of the preparation of platinum monoatomic material using an alkyl imidazole ionic liquid according to the invention;
FIG. 2 shows Pt prepared according to example one of the present invention SA Transmission electron microscopy images and spherical electron microscopy HAADF-STEM images of the Ni-Co-GO-N composite material, wherein circles are marked as monoatomic platinum;
FIG. 3 shows Pt obtained in example II of the present invention SA Transmission electron microscopy and spherical electron microscopy HAADF-STEM of the Ni-Co-GO-N composite, with circles marked as monoatomic platinum.
Detailed Description
The following description of the preferred embodiments of the present invention refers to the accompanying drawings, which make the technical contents thereof more clear and easy to understand. The present invention may be embodied in many different forms of embodiments and the scope of the present invention is not limited to only the embodiments described herein.
Example 1
In this embodiment, a method for preparing Pt monoatomic material by using 1-ethyl-3-methylimidazole tetrafluoroborate ionic liquid is mainly described, and the process flow is shown in fig. 1, and the specific operation steps are as follows:
dissolving 2.38g of nickel chloride hexahydrate, 1.19g of cobalt chloride hexahydrate and 0.3g of Graphene Oxide (GO) solid particles in a eutectic solution, wherein the eutectic solution is formed by dissolving choline chloride in ethylene glycol, performing constant potential composite electrodeposition in a standard three-electrode system consisting of a nickel sheet serving as a counter electrode, a Carbon Cloth (CC) serving as a working electrode and a non-mercury wire electrode serving as a reference electrode, wherein the voltage is-0.6V, and obtaining a Ni-Co-GO composite electrode material; and (3) placing the Ni-Co-GO composite electrode material into a tube furnace for nitriding, wherein 0.3g of urea is used as a nitrogen source, the temperature is 300 ℃, and the nitrided Ni-Co-GO-N composite electrode material is obtained.
Step two, taking the Ni-Co-GO-N composite electrode subjected to nitriding in the step two as a working electrode, a platinum sheet electrode as a counter electrode and a non-mercury wire electrode as a reference electrode, adding 30mL of 1-ethyl-3-methylimidazole tetrafluoroborate ionic liquid into an electrolytic cell containing three electrodes, anchoring monoatomic platinum by adopting a cyclic voltammetry, wherein the sweeping speed is 100mV/s, the voltage interval is-0.6 to-1.2V, and the cycle number is 4000.
Step three, the platinum single-atom loaded composite electrode material Pt prepared in the step two is subjected to the preparation SA Taking out the Ni-Co-GO-N from the electrolytic cell, washing with deionized water for multiple times, washing with absolute ethyl alcohol for multiple times, and finally drying.
And step four, material characterization: and (3) shooting an HAADF image of the sample prepared in the step (III) in a STEM mode, wherein the bright points are platinum atoms, so that the monoatomic platinum is uniformly distributed on the carrier. This is described with 1-ethyl-3-methylimidazole tetrafluoroborate ([ EMIm)]BF 4 ) The solution is electrolyte and can be used for preparing platinum monoatomic materialAnd (5) material. Compared with other process preparation technologies, the method has the advantages of simplicity, low requirement on equipment conditions, great shortening of the process, controllable process and effective reduction of cost.
Example two
In this embodiment, a method for preparing Pt monoatomic material by using 1-butyl-3-methylimidazole tetrafluoroborate ionic liquid is mainly described, and the process flow is shown in fig. 1, and the specific operation steps are as follows:
dissolving 4.96g of nickel chloride hexahydrate, 2.38g of cobalt chloride hexahydrate and 0.3g of Graphene Oxide (GO) solid particles in a eutectic solution, wherein the eutectic solution is formed by dissolving choline chloride in ethylene glycol, performing constant potential composite electrodeposition in a standard three-electrode system consisting of a nickel sheet serving as a counter electrode, a Carbon Cloth (CC) serving as a working electrode and a non-mercury wire electrode serving as a reference electrode, wherein the voltage is-0.7V, and obtaining a Ni-Co-GO composite electrode material; and (3) placing the Ni-Co-GO composite electrode material into a tube furnace for nitriding, wherein 0.3g of urea is used as a nitrogen source, the temperature is 300 ℃, and the nitrided Ni-Co-GO-N composite electrode material is obtained.
Step two, taking the Ni-Co-GO-N composite electrode subjected to nitriding in the step two as a working electrode, a platinum sheet electrode as a counter electrode and a non-mercury wire electrode as a reference electrode, adding 30mL of 1-butyl-3-methylimidazole tetrafluoroborate ionic liquid into an electrolytic cell containing three electrodes, anchoring monoatomic platinum by adopting a cyclic voltammetry, wherein the scanning speed is 100mV/s, the voltage interval is-0.6 to-1.2V, and the cycle number is 6000.
Step three, the same as in the first embodiment;
and step four, material characterization: and (3) shooting an HAADF image of the sample prepared in the step (III) in a STEM mode, wherein the bright points are platinum atoms, so that the monoatomic platinum is uniformly distributed on the carrier. This is described with 1-butyl-3-methylimidazole tetrafluoroborate ([ BMIm ]]BF 4 ) The solution is electrolyte, and can prepare platinum monoatomic material. Compared with other process preparation technologies, the method has the advantages of simplicity, low requirement on equipment conditions, great shortening of the process, controllable process and effective reduction of cost.
The foregoing describes in detail preferred embodiments of the present invention. It should be understood that numerous modifications and variations can be made in accordance with the concepts of the invention without requiring creative effort by one of ordinary skill in the art. Therefore, all technical solutions which can be obtained by logic analysis, reasoning or limited experiments based on the prior art by the person skilled in the art according to the inventive concept shall be within the scope of protection defined by the claims.
Claims (8)
1. The method for preparing the platinum monoatomic material by adopting the alkyl imidazole ionic liquid is characterized by comprising the following steps of:
firstly, dissolving nickel chloride hexahydrate, cobalt chloride hexahydrate and graphene oxide serving as raw materials in a eutectic solution to form electrolyte, and performing constant potential composite electrodeposition in a standard three-electrode system to obtain a Ni-Co-GO composite electrode material; placing the Ni-Co-GO composite electrode material into a tube furnace for nitriding, wherein urea is used as a nitrogen source;
step two, taking the Ni-Co-GO-N composite electrode material subjected to nitriding in the step two as a working electrode to form a three-electrode system, adding alkyl imidazole ionic liquid into an electrolytic cell containing the three-electrode system, and anchoring monoatomic platinum by adopting a cyclic voltammetry;
step three, taking the platinum single-atom-loaded composite electrode material prepared in the step two out of the electrolytic cell, cleaning, and finally drying;
the alkyl imidazole ionic liquid in the second step is one of 1-ethyl-3-methylimidazole tetrafluoroborate ionic liquid or 1-butyl-3-methylimidazole tetrafluoroborate ionic liquid;
the adding amount of the alkyl imidazole ionic liquid is 30mL.
2. The method for preparing platinum monoatomic material by using alkyl imidazole ionic liquid according to claim 1, wherein in the step one, the reference electrode is a non-mercury wire electrode, and the counter electrode is a nickel sheet.
3. The method for preparing platinum monoatomic material by using alkyl imidazole ionic liquid according to claim 1, wherein the working electrode in the standard three-electrode system in the step one is one of carbon cloth, foam nickel or carbon paper.
4. The method for preparing platinum monoatomic material by adopting the alkyl imidazole ionic liquid according to claim 1, wherein the cyclic voltammetry in the second step is performed at a sweeping speed of 60-100 mV/s, a voltage interval of-0.6 to-1.2V and a cycle number of 4000-8000.
5. The method for preparing platinum monoatomic material using an alkylimidazole ionic liquid according to claim 1, wherein the eutectic solution in step one is formed by dissolving choline chloride in ethylene glycol.
6. The method for preparing platinum monoatomic material by using alkyl imidazole ionic liquid according to claim 1, wherein in the second step, a platinum sheet electrode is used as a counter electrode, and a non-mercury wire electrode is used as a reference electrode.
7. The method for preparing platinum monoatomic material by using an alkyl imidazole ionic liquid according to claim 1, wherein the nitriding temperature in the first step is 260-300 ℃.
8. The method for preparing platinum monoatomic material by using an alkyl imidazole ionic liquid according to claim 1, wherein in the third step, the cleaning process is to clean with deionized water and then clean with absolute ethyl alcohol.
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