CN113957457A - Graphene material and preparation method thereof - Google Patents
Graphene material and preparation method thereof Download PDFInfo
- Publication number
- CN113957457A CN113957457A CN202111304446.XA CN202111304446A CN113957457A CN 113957457 A CN113957457 A CN 113957457A CN 202111304446 A CN202111304446 A CN 202111304446A CN 113957457 A CN113957457 A CN 113957457A
- Authority
- CN
- China
- Prior art keywords
- graphene material
- anolyte
- electrolyzing
- ethylene
- electrolysis
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 62
- 239000000463 material Substances 0.000 title claims abstract description 44
- 238000002360 preparation method Methods 0.000 title description 9
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims abstract description 35
- 239000005977 Ethylene Substances 0.000 claims abstract description 35
- 238000000034 method Methods 0.000 claims abstract description 32
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 28
- LQZZUXJYWNFBMV-UHFFFAOYSA-N dodecan-1-ol Chemical compound CCCCCCCCCCCCO LQZZUXJYWNFBMV-UHFFFAOYSA-N 0.000 claims abstract description 17
- 239000002608 ionic liquid Substances 0.000 claims abstract description 14
- 229910052697 platinum Inorganic materials 0.000 claims abstract description 14
- 229910001220 stainless steel Inorganic materials 0.000 claims abstract description 13
- 239000010935 stainless steel Substances 0.000 claims abstract description 13
- 229940051841 polyoxyethylene ether Drugs 0.000 claims abstract description 10
- 229920000056 polyoxyethylene ether Polymers 0.000 claims abstract description 10
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 238000005868 electrolysis reaction Methods 0.000 claims description 29
- -1 hexylidene hexafluorophosphate Chemical compound 0.000 claims description 18
- KGWVFQAPOGAVRF-UHFFFAOYSA-N 1-hexylimidazole Chemical compound CCCCCCN1C=CN=C1 KGWVFQAPOGAVRF-UHFFFAOYSA-N 0.000 claims description 16
- 239000012528 membrane Substances 0.000 claims description 14
- 238000005341 cation exchange Methods 0.000 claims description 12
- JGTNAGYHADQMCM-UHFFFAOYSA-N perfluorobutanesulfonic acid Chemical compound OS(=O)(=O)C(F)(F)C(F)(F)C(F)(F)C(F)(F)F JGTNAGYHADQMCM-UHFFFAOYSA-N 0.000 claims description 10
- KAIPKTYOBMEXRR-UHFFFAOYSA-N 1-butyl-3-methyl-2h-imidazole Chemical compound CCCCN1CN(C)C=C1 KAIPKTYOBMEXRR-UHFFFAOYSA-N 0.000 claims description 9
- QOHANVRCHGWPNG-UHFFFAOYSA-N 1-ethyl-3-methyl-2h-imidazole;sulfuric acid Chemical compound OS(O)(=O)=O.CCN1CN(C)C=C1 QOHANVRCHGWPNG-UHFFFAOYSA-N 0.000 claims description 9
- 238000000746 purification Methods 0.000 claims description 4
- 239000011261 inert gas Substances 0.000 claims description 2
- 238000000527 sonication Methods 0.000 claims description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 20
- 238000004140 cleaning Methods 0.000 description 20
- 238000002156 mixing Methods 0.000 description 12
- 229910052786 argon Inorganic materials 0.000 description 10
- 238000010438 heat treatment Methods 0.000 description 10
- 238000005406 washing Methods 0.000 description 8
- 239000007788 liquid Substances 0.000 description 7
- 238000001035 drying Methods 0.000 description 6
- 238000000926 separation method Methods 0.000 description 6
- 238000009210 therapy by ultrasound Methods 0.000 description 6
- 230000003213 activating effect Effects 0.000 description 5
- 238000000861 blow drying Methods 0.000 description 5
- 238000001816 cooling Methods 0.000 description 5
- 239000003960 organic solvent Substances 0.000 description 5
- 238000003756 stirring Methods 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- 229910052799 carbon Inorganic materials 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 125000004432 carbon atom Chemical group C* 0.000 description 3
- 239000003575 carbonaceous material Substances 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- IQQRAVYLUAZUGX-UHFFFAOYSA-N 1-butyl-3-methylimidazolium Chemical compound CCCCN1C=C[N+](C)=C1 IQQRAVYLUAZUGX-UHFFFAOYSA-N 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 2
- 230000002776 aggregation Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000001000 micrograph Methods 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000004299 exfoliation Methods 0.000 description 1
- 238000009396 hybridization Methods 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 239000003014 ion exchange membrane Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Images
Classifications
-
- 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
- C25B1/135—Carbon
-
- 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
- C25B1/50—Processes
Abstract
The invention discloses a method for preparing a graphene material by electrolyzing ethylene, which comprises the following steps: putting a cathode into catholyte, putting an anode into anolyte, separating the catholyte and the anolyte by a diaphragm, introducing ethylene into the anolyte, and electrolyzing to obtain a graphene material; wherein the cathode is a stainless steel electrode, the anode is a platinum electrode, and the anolyte is a mixture of ionic liquid and dodecyl alcohol polyoxyethylene ether; the catholyte is ionic liquid. The invention also discloses a graphene material prepared by the method for preparing the graphene material by electrolyzing ethylene. The method is simple to operate and environment-friendly.
Description
Technical Field
The invention relates to the technical field of graphene, in particular to a graphene material and a preparation method thereof.
Background
Carbon atoms are bonded in an sp2 hybridization mode and are connected with each other to form a two-dimensional lattice plane similar to a honeycomb shape, the two-dimensional carbon material is called graphene, the structure of the graphene endows the graphene with unique properties in the aspects of electricity, mechanics, optics, heat and the like, and the graphene becomes a current research hotspot and simultaneously shows attractive application prospects in the fields of nano devices, sensors, solar cells, transistors, environments and the like.
For the research and application of graphene, the key point is the low-cost large-scale preparation of graphene. To date, there are many methods for preparing graphene, such as mechanical exfoliation, cutting carbon nanotube, epitaxial growth, chemical vapor deposition, thermal reduction, and reduced graphite oxide, which are mostly synthesized from top to bottom, and the obvious defect is that large-scale preparation cannot be achieved. Among these methods, the reduced-oxidized graphite method, which has the characteristics of high yield, readily available raw materials, simple steps, and the like, is most promising for large-scale preparation of graphene, but the method also has the problems of insufficient reduction, easy product re-stacking and agglomeration during reduction and post-treatment, poor environmental friendliness, and the like. Therefore, how to prepare graphene materials with high specific surface area by a simple chemical method is still a very worthy research work.
Disclosure of Invention
Based on the technical problems in the background art, the invention provides the graphene material and the preparation method thereof, the operation is simple, the environment is friendly, and the graphene carbon material can be effectively controlled and prepared by controlling the gas flow and the electrolysis parameters of the gaseous carbon source ethylene.
The invention provides a method for preparing a graphene material by electrolyzing ethylene, which comprises the following steps: putting a cathode into catholyte, putting an anode into anolyte, separating the catholyte and the anolyte by a diaphragm, introducing ethylene into the anolyte, and electrolyzing to obtain a graphene material;
wherein the cathode is a stainless steel electrode, the anode is a platinum electrode, and the anolyte is a mixture of ionic liquid and dodecyl alcohol polyoxyethylene ether; the catholyte is ionic liquid.
The electrolysis principle of the invention is as follows: ethylene generates active carbon atoms (or carbon-containing active groups) and hydrogen ions through electrocatalytic reaction at the anode; the active carbon atoms form a graphene material in the anode chamber, and hydrogen ions enter the cathode chamber through ion exchange to obtain electron separationHydrogen is discharged; the reaction formula is as follows: c2H4→graphene+H2↑。
According to the invention, a platinum electrode is taken as an anode and combined with an appropriate ionic liquid, so that the catalyst has strong catalytic capability on ethylene electrolysis, the ethylene electrolysis is catalyzed to generate graphene in the anode, and hydrogen is generated at the cathode; then purifying the anolyte to obtain a graphene material; the ionic liquid can be circularly recycled and is environment-friendly.
Preferably, in the anolyte, the ionic liquid is a mixture of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, 1-ethyl-3-methylimidazole hydrogensulfate and 1-butyl-3-methylimidazole perfluorobutylsulfonate.
Preferably, the volume ratio of the 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate to the 1-ethyl-3-methylimidazole bisulfate to the 1-butyl-3-methylimidazole perfluorobutyl sulfonate in the anolyte is 100:1 to 3:2 to 6.
Preferably, the volume ratio of the ionic liquid to the lauryl alcohol polyoxyethylene ether in the anolyte is 103-109: 0.1-0.5.
Preferably, in the catholyte, the ionic liquid is 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate.
Preferably, the membrane is a cation exchange membrane; preferably a homogeneous ion exchange membrane.
Preferably, the voltage of electrolysis is 4-8V; preferably, the electrolysis time is 0.5-2 h; preferably, the temperature of the electrolysis is 200-.
Preferably, the gas flow of ethylene is from 10 to 50 mL/h.
Preferably, the distance between the cathode and the anode is 0.5-1.5 cm.
Preferably, the volumes of the anolyte and catholyte are the same.
Preferably, the electrolysis is carried out in an inert gas atmosphere.
Preferably, sonication is continued during electrolysis.
Preferably, after electrolysis, purification treatment is performed to obtain the graphene material.
The purification treatment may comprise the following specific steps: and washing the electrolyzed anode, uniformly mixing the washing solution and the electrolyzed anode solution, performing solid-liquid separation, washing, and drying to obtain the graphene material.
The invention also provides a graphene material prepared by the method for preparing the graphene material by electrolyzing ethylene.
Has the advantages that:
according to the method, toxic and harmful dangerous chemicals such as strong acid and strong base are not used in the graphene preparation process, so that the waste liquid treatment process after the graphene is prepared by a liquid phase method is omitted; the graphene is prepared by electrolyzing gaseous carbon source ethylene, so that the process difficulty in the graphene preparation process is reduced; the catholyte and the anolyte are separated by the diaphragm, so that side reaction can be avoided, and the difficulty of purification treatment in the later period can be reduced; in addition, the method can effectively control and prepare the graphene carbonaceous material by controlling the gas flow and the electrolysis parameters of the gaseous carbon source ethylene.
Drawings
Fig. 1 is a scanning electron microscope image of the graphene material prepared in example 1.
Detailed Description
The technical solution of the present invention will be described in detail below with reference to specific examples.
Example 1
A method for preparing a graphene material by electrolyzing ethylene comprises the following steps:
respectively putting a stainless steel electrode and a platinum electrode into water at 40-100 ℃ for cleaning, then cleaning with an organic solvent, activating, and blow-drying for later use;
to 100mL of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate (HDHImPF for short)6) Adding 0.2mL of lauryl alcohol polyoxyethylene ether (POE 6 for short) and 2mL of 1-ethyl-3-methylimidazole hydrogen sulfate (Bmim for short)][HSO4]) And 4mL of 1-butyl-3-methylimidazol perfluorobutylsulfonate ([ Bmim ] for short)][PFBS]) Stirring and uniformly mixing by ultrasonic to obtain anolyte;
taking an electrolytic cell with a cation exchange membrane, wherein the electrolytic cell is divided into a cathode chamber and an anode chamber by the cation exchange membrane; placing the electrolytic cell in a heater, then placing a stainless steel electrode in a cathode chamber, placing a platinum electrode in an anode chamber, keeping the distance between the two electrodes at 1cm, then introducing argon into the heater and the electrolytic cell at the flow rate of 100mL/min to remove air in the heater and the electrolytic cell, then heating to 250 ℃ at the speed of 7.5 ℃/min and preserving heat; turning on an ultrasonic instrument, adjusting the ultrasonic power to 350W, switching on a stabilized voltage power supply, pouring 20mL of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate into a cathode chamber to serve as catholyte, pouring 20mL of anolyte into an anode chamber, adjusting the voltage of an electrolytic cell to be 5V, then introducing ethylene into the anolyte at the flow rate of 35mL/h, continuing ultrasonic treatment, maintaining constant temperature and constant pressure for electrolysis for 1h, stopping electrolysis and heating, cooling to room temperature, closing an argon valve, taking out the electrolytic cell, cleaning the electrolyzed anode, uniformly mixing a cleaning solution and the electrolyzed anolyte, performing solid-liquid separation, washing and drying to obtain the graphene material.
The graphene material prepared in example 1 was used for detection, and the result is shown in fig. 1. Fig. 1 is an electron microscope image of the graphene material prepared in example 1.
As can be seen from fig. 1, the graphene material is successfully prepared by the method of the present invention.
The continuous ultrasonic treatment in the electrolysis process can promote the uniform mixing of all substances, promote the electrolysis and avoid the agglomeration of graphene.
Example 2
A method for preparing a graphene material by electrolyzing ethylene comprises the following steps:
respectively putting a stainless steel electrode and a platinum electrode into water at 40-100 ℃ for cleaning, then cleaning with an organic solvent, activating, and blow-drying for later use;
adding 0.1mL of dodecyl alcohol polyoxyethylene ether, 1mL of 1-ethyl-3-methylimidazole hydrogen sulfate and 2mL of 1-butyl-3-methylimidazole perfluorobutyl sulfonate into 100mL of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, stirring and ultrasonically mixing uniformly to obtain an anolyte;
taking an electrolytic cell with a cation exchange membrane, wherein the electrolytic cell is divided into a cathode chamber and an anode chamber by the cation exchange membrane; placing the electrolytic cell in a heater, then placing a stainless steel electrode in a cathode chamber, placing a platinum electrode in an anode chamber, keeping the distance between the two electrodes at 0.5cm, then introducing argon into the heater and the electrolytic cell at a flow rate of 50mL/min to remove air in the heater and the electrolytic cell, then heating to 200 ℃ at a speed of 10 ℃/min and preserving heat; turning on an ultrasonic instrument, adjusting the ultrasonic power to 350W, switching on a stabilized voltage power supply, pouring 20mL of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate into a cathode chamber as catholyte, pouring 20mL of anolyte into an anode chamber, adjusting the voltage of an electrolytic cell to 8V, then introducing ethylene into the anolyte at a gas flow rate of 10mL/h, continuously performing ultrasonic treatment and maintaining constant temperature and constant voltage for electrolysis for 0.5h, stopping electrolysis and heating, cooling to room temperature, closing an argon valve, taking out the electrolytic cell, cleaning the electrolyzed anode, uniformly mixing a cleaning solution and the electrolyzed anolyte, performing solid-liquid separation, washing and drying to obtain the graphene material.
Example 3
A method for preparing a graphene material by electrolyzing ethylene comprises the following steps:
respectively putting a stainless steel electrode and a platinum electrode into water at 40-100 ℃ for cleaning, then cleaning with an organic solvent, activating, and blow-drying for later use;
adding 0.5mL of dodecyl alcohol polyoxyethylene ether, 3mL of 1-ethyl-3-methylimidazole hydrogen sulfate and 6mL of 1-butyl-3-methylimidazole perfluorobutyl sulfonate into 100mL of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, stirring and ultrasonically mixing uniformly to obtain an anolyte;
taking an electrolytic cell with a cation exchange membrane, wherein the electrolytic cell is divided into a cathode chamber and an anode chamber by the cation exchange membrane; placing the electrolytic cell in a heater, then placing a stainless steel electrode in a cathode chamber, placing a platinum electrode in an anode chamber, keeping the distance between the two electrodes at 1.5cm, then introducing argon into the heater and the electrolytic cell at a flow rate of 200mL/min to remove air in the heater and the electrolytic cell, then heating to 300 ℃ at a speed of 5 ℃/min and preserving heat; turning on an ultrasonic instrument, adjusting the ultrasonic power to 350W, switching on a stabilized voltage power supply, pouring 20mL of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate into a cathode chamber as catholyte, pouring 20mL of anolyte into an anode chamber, adjusting the voltage of an electrolytic cell to 4V, then introducing ethylene into the anolyte at a flow rate of 50mL/h, continuously performing ultrasonic treatment and maintaining constant temperature and constant voltage for electrolysis for 2h, stopping electrolysis and heating, cooling to room temperature, closing an argon valve, taking out the electrolytic cell, cleaning the electrolyzed anode, uniformly mixing a cleaning solution and the electrolyzed anolyte, performing solid-liquid separation, washing and drying to obtain the graphene material.
Example 4
A method for preparing a graphene material by electrolyzing ethylene comprises the following steps:
respectively putting a stainless steel electrode and a platinum electrode into water at 40-100 ℃ for cleaning, then cleaning with an organic solvent, activating, and blow-drying for later use;
adding 0.4mL of dodecyl alcohol polyoxyethylene ether, 2.5mL of 1-ethyl-3-methylimidazole hydrogen sulfate and 5mL of 1-butyl-3-methylimidazole perfluorobutyl sulfonate into 100mL of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, stirring and uniformly mixing by ultrasonic waves to obtain an anolyte;
taking an electrolytic cell with a cation exchange membrane, wherein the electrolytic cell is divided into a cathode chamber and an anode chamber by the cation exchange membrane; placing the electrolytic cell in a heater, then placing a stainless steel electrode in a cathode chamber, placing a platinum electrode in an anode chamber, keeping the distance between the two electrodes at 1.2cm, then introducing argon into the heater and the electrolytic cell at the flow rate of 80mL/min to remove air in the heater and the electrolytic cell, then heating to 220 ℃ at the speed of 8 ℃/min and preserving heat; turning on an ultrasonic instrument, adjusting the ultrasonic power to 350W, switching on a stabilized voltage power supply, pouring 20mL of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate into a cathode chamber as catholyte, pouring 20mL of anolyte into an anode chamber, adjusting the voltage of an electrolytic cell to 7V, then introducing ethylene into the anolyte at a flow rate of 25mL/h, continuing ultrasonic treatment and maintaining constant temperature and constant voltage for electrolysis for 1h, stopping electrolysis and heating, cooling to room temperature, closing an argon valve, taking out the electrolytic cell, cleaning the electrolyzed anode, uniformly mixing a cleaning solution and the electrolyzed anolyte, performing solid-liquid separation, washing and drying to obtain the graphene material.
Example 5
A method for preparing a graphene material by electrolyzing ethylene comprises the following steps:
respectively putting a stainless steel electrode and a platinum electrode into water at 40-100 ℃ for cleaning, then cleaning with an organic solvent, activating, and blow-drying for later use;
adding 0.3mL of dodecyl alcohol polyoxyethylene ether, 1.5mL of 1-ethyl-3-methylimidazole hydrogen sulfate and 3mL of 1-butyl-3-methylimidazole perfluorobutyl sulfonate into 100mL of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, stirring and uniformly mixing by ultrasonic waves to obtain an anolyte;
taking an electrolytic cell with a cation exchange membrane, wherein the electrolytic cell is divided into a cathode chamber and an anode chamber by the cation exchange membrane; placing the electrolytic cell in a heater, then placing a stainless steel electrode in a cathode chamber, placing a platinum electrode in an anode chamber, keeping the distance between the two electrodes at 0.8cm, then introducing argon into the heater and the electrolytic cell at a flow rate of 150mL/min to remove air in the heater and the electrolytic cell, then heating to 280 ℃ at a speed of 6 ℃/min and preserving heat; turning on an ultrasonic instrument, adjusting the ultrasonic power to 350W, switching on a stabilized voltage power supply, pouring 20mL of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate into a cathode chamber as catholyte, pouring 20mL of anolyte into an anode chamber, adjusting the voltage of an electrolytic cell to 5V, then introducing ethylene into the anolyte at a flow rate of 40mL/h, continuing ultrasonic treatment and maintaining constant temperature and constant voltage for electrolysis for 1.5h, stopping electrolysis and heating, cooling to room temperature, closing an argon valve, taking out the electrolytic cell, cleaning the electrolyzed anode, uniformly mixing a cleaning solution and the electrolyzed anolyte, performing solid-liquid separation, washing and drying to obtain the graphene material.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art should be considered to be within the technical scope of the present invention, and the technical solutions and the inventive concepts thereof according to the present invention should be equivalent or changed within the scope of the present invention.
Claims (10)
1. A method for preparing a graphene material by electrolyzing ethylene is characterized by comprising the following steps: putting a cathode into catholyte, putting an anode into anolyte, separating the catholyte and the anolyte by a diaphragm, introducing ethylene into the anolyte, and electrolyzing to obtain a graphene material;
wherein the cathode is a stainless steel electrode, the anode is a platinum electrode, and the anolyte is a mixture of ionic liquid and dodecyl alcohol polyoxyethylene ether; the catholyte is ionic liquid.
2. The method for preparing graphene material by electrolyzing ethylene according to claim 1, wherein the ionic liquid in the anolyte is a mixture of 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate, 1-ethyl-3-methylimidazole bisulfate and 1-butyl-3-methylimidazole perfluorobutyl sulfonate; preferably, in the anolyte, the volume ratio of 1, 6-di (3-hexylimidazole) hexylidene hexafluorophosphate to 1-ethyl-3-methylimidazole hydrogen sulfate to 1-butyl-3-methylimidazole perfluorobutyl sulfonate is 100:1-3: 2-6; preferably, the volume ratio of the ionic liquid to the lauryl alcohol polyoxyethylene ether in the anolyte is 103-109: 0.1-0.5.
3. The method for preparing graphene material by electrolyzing ethylene according to claim 1 or 2, wherein the ionic liquid in the catholyte is 1, 6-bis (3-hexylimidazole) hexylidene hexafluorophosphate.
4. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 3, wherein the membrane is a cation exchange membrane.
5. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 4, wherein the voltage of electrolysis is 4 to 8V; preferably, the electrolysis time is 0.5-2 h; preferably, the temperature of the electrolysis is 200-.
6. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 5, wherein the flow rate of ethylene is 10 to 50 mL/h.
7. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 6, wherein the distance between the cathode and the anode is 0.5 to 1.5 cm.
8. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 7, wherein the volumes of the anolyte and the catholyte are the same; preferably, the electrolysis is carried out in an inert gas atmosphere; preferably, sonication is continued during electrolysis.
9. The method for preparing graphene material by electrolyzing ethylene according to any one of claims 1 to 8, wherein the graphene material is prepared by performing purification treatment after the electrolysis.
10. A graphene material, characterized in that it is prepared by a method for preparing a graphene material by electrolyzing ethylene according to any one of claims 1 to 9.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN202111304446.XA CN113957457A (en) | 2021-11-05 | 2021-11-05 | Graphene material and preparation method thereof |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN202111304446.XA CN113957457A (en) | 2021-11-05 | 2021-11-05 | Graphene material and preparation method thereof |
Publications (1)
Publication Number | Publication Date |
---|---|
CN113957457A true CN113957457A (en) | 2022-01-21 |
Family
ID=79469197
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
CN202111304446.XA Pending CN113957457A (en) | 2021-11-05 | 2021-11-05 | Graphene material and preparation method thereof |
Country Status (1)
Country | Link |
---|---|
CN (1) | CN113957457A (en) |
Citations (14)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101634032A (en) * | 2009-08-14 | 2010-01-27 | 南京大学 | Green and fast electrochemical preparation method for graphene |
CN102465309A (en) * | 2010-11-10 | 2012-05-23 | 海洋王照明科技股份有限公司 | Preparation method of graphene |
GB201314084D0 (en) * | 2013-08-06 | 2013-09-18 | Univ Manchester | Production of graphene |
CN103407998A (en) * | 2013-07-19 | 2013-11-27 | 华侨大学 | Preparation method of high concentration and small flake diameter graphene dispersion |
CN104003373A (en) * | 2013-02-21 | 2014-08-27 | 海洋王照明科技股份有限公司 | Graphene material and preparation method thereof |
WO2016011180A1 (en) * | 2014-07-17 | 2016-01-21 | Santhanam Kalathur S V | Electrochemical process for producing graphene, graphene oxide, metal composites and coated substrates |
CN105452533A (en) * | 2013-05-30 | 2016-03-30 | 曼彻斯特大学 | Electrochemical process for production of graphene |
CN105624722A (en) * | 2016-01-05 | 2016-06-01 | 北京金吕能源科技有限公司 | Method for preparing graphene or carbon nanotubes by electrolyzing carbon dioxide |
US20170233255A1 (en) * | 2016-02-17 | 2017-08-17 | Aruna Zhamu | Electrochemical Method Of Producing Single-Layer Or Few-Layer Graphene Sheets |
RU2017105460A3 (en) * | 2017-02-21 | 2018-08-21 | ||
CN109072457A (en) * | 2016-02-17 | 2018-12-21 | 金属电解有限公司 | The method for preparing grapheme material |
CN109321932A (en) * | 2018-10-30 | 2019-02-12 | 深圳大学 | Graphene and the preparation method and application thereof |
JP2020050577A (en) * | 2018-09-28 | 2020-04-02 | 国立大学法人宇都宮大学 | Manufacturing method of graphene dispersion |
CN111575725A (en) * | 2020-05-18 | 2020-08-25 | 中国华能集团清洁能源技术研究院有限公司 | CO (carbon monoxide)2Method for preparing graphene through electrochemical conversion |
-
2021
- 2021-11-05 CN CN202111304446.XA patent/CN113957457A/en active Pending
Patent Citations (14)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101634032A (en) * | 2009-08-14 | 2010-01-27 | 南京大学 | Green and fast electrochemical preparation method for graphene |
CN102465309A (en) * | 2010-11-10 | 2012-05-23 | 海洋王照明科技股份有限公司 | Preparation method of graphene |
CN104003373A (en) * | 2013-02-21 | 2014-08-27 | 海洋王照明科技股份有限公司 | Graphene material and preparation method thereof |
CN105452533A (en) * | 2013-05-30 | 2016-03-30 | 曼彻斯特大学 | Electrochemical process for production of graphene |
CN103407998A (en) * | 2013-07-19 | 2013-11-27 | 华侨大学 | Preparation method of high concentration and small flake diameter graphene dispersion |
GB201314084D0 (en) * | 2013-08-06 | 2013-09-18 | Univ Manchester | Production of graphene |
WO2016011180A1 (en) * | 2014-07-17 | 2016-01-21 | Santhanam Kalathur S V | Electrochemical process for producing graphene, graphene oxide, metal composites and coated substrates |
CN105624722A (en) * | 2016-01-05 | 2016-06-01 | 北京金吕能源科技有限公司 | Method for preparing graphene or carbon nanotubes by electrolyzing carbon dioxide |
US20170233255A1 (en) * | 2016-02-17 | 2017-08-17 | Aruna Zhamu | Electrochemical Method Of Producing Single-Layer Or Few-Layer Graphene Sheets |
CN109072457A (en) * | 2016-02-17 | 2018-12-21 | 金属电解有限公司 | The method for preparing grapheme material |
RU2017105460A3 (en) * | 2017-02-21 | 2018-08-21 | ||
JP2020050577A (en) * | 2018-09-28 | 2020-04-02 | 国立大学法人宇都宮大学 | Manufacturing method of graphene dispersion |
CN109321932A (en) * | 2018-10-30 | 2019-02-12 | 深圳大学 | Graphene and the preparation method and application thereof |
CN111575725A (en) * | 2020-05-18 | 2020-08-25 | 中国华能集团清洁能源技术研究院有限公司 | CO (carbon monoxide)2Method for preparing graphene through electrochemical conversion |
Non-Patent Citations (1)
Title |
---|
高亚辉;尹国杰;张少文;王璐;孟巧静;李欣栋;: "电化学法制备石墨烯的研究进展", 材料工程, vol. 48, no. 8, pages 84 - 100 * |
Similar Documents
Publication | Publication Date | Title |
---|---|---|
US10702857B2 (en) | Monatomic metal-doped few-layer molybdenum disulfide electrocatalytic material, preparing method thereof, and method for electrocatalytic nitrogen fixation | |
Wu et al. | An electrocatalytic route for transformation of biomass-derived furfural into 5-hydroxy-2 (5 H)-furanone | |
US8961774B2 (en) | Electrochemical production of butanol from carbon dioxide and water | |
JP5752237B2 (en) | Electrochemical synthesis of arylalkyl surfactant precursors | |
JP4811844B2 (en) | Method for producing percarbonate | |
CN108588748A (en) | A kind of method that Carbon dioxide electrochemical reduction prepares methane and ethylene | |
Das et al. | Value added product recovery and carbon dioxide sequestration from biogas using microbial electrosynthesis | |
CN112076791A (en) | Ni-MOF film photocatalyst growing on surface of foamed nickel in situ, and preparation method and application thereof | |
CN111097402B (en) | Nano beta-lead dioxide catalyst, preparation method and application thereof | |
CN112430830B (en) | Preparation method and application of electrocatalytic reduction carbon dioxide electrode | |
CA3085243A1 (en) | Catalyst system for catalyzed electrochemical reactions and preparation thereof, applications and uses thereof | |
CN110965076A (en) | Preparation method of electrolytic water electrode with double-function three-dimensional layered core-shell structure | |
CN109136973A (en) | A kind of base metal doping molybdenum carbide hydrogen-precipitating electrode and its preparation method and application | |
CN109371418B (en) | method for improving biological reduction of CO by using graphene-foamy copper composite cathode2Method for electrosynthesizing acetic acid | |
Lekshmi et al. | Microbial electrosynthesis: carbonaceous electrode materials for CO 2 conversion | |
Yang et al. | Selective CO2 Electroreduction with enhanced oxygen evolution efficiency in affordable borate-mediated molten electrolyte | |
Wang et al. | Electrochemical synthesis of ferrate (VI) by regular anodic replacement | |
CN113957457A (en) | Graphene material and preparation method thereof | |
CN115537865B (en) | Application and preparation method of nanocrystallized foam silver electrode | |
Du et al. | Catalysts and electrolyzers for the electrochemical CO 2 reduction reaction: from laboratory to industrial applications | |
CN116216633A (en) | System and method for realizing pure water decomposition by photocatalysis-electrocatalytic coupling iodine circulation | |
CN110965071B (en) | Metal catalyst for electrochemical reduction of carbon dioxide and preparation and application thereof | |
CN114032561A (en) | Graphene and method for preparing graphene by electrolyzing ethanol in ionic liquid | |
CN111071999A (en) | Synthesis method of mesoporous graphite-like carbon nitride nanosheet with low metal content | |
CN112779558A (en) | Method for cathodic electrosynthesis of hydrogen peroxide by using PTFE (polytetrafluoroethylene) partially-hydrophobic modified graphite felt |
Legal Events
Date | Code | Title | Description |
---|---|---|---|
PB01 | Publication | ||
PB01 | Publication | ||
SE01 | Entry into force of request for substantive examination | ||
SE01 | Entry into force of request for substantive examination |