CN111268732A - Method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma and product thereof - Google Patents
Method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma and product thereof Download PDFInfo
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Abstract
The invention discloses a method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma, which comprises the following steps: mixing water and graphite powder, stirring, and performing low-temperature plasma irradiation while stirring to obtain graphene slurry; dripping sulfuric acid into the graphene slurry to obtain acidic graphene slurry; adding molybdenum trioxide into the acidic graphene slurry, stirring and simultaneously carrying out low-temperature plasma irradiation to obtain molybdenum disulfide graphene slurry; and centrifuging the molybdenum disulfide graphene slurry, carrying out solid-liquid separation, and then freeze-drying the solid part to obtain the molybdenum disulfide graphene aerogel. The invention also discloses molybdenum disulfide graphene aerogel. According to the invention, the molybdenum disulfide and the graphene are uniformly dispersed and mixed based on ultraviolet radiation and microwave radiation generated in a low-temperature plasma system, and additional ultrasonic dispersion is not required. The adsorption performance and the hydrogen evolution performance of the molybdenum disulfide graphene aerogel prepared by the method are higher than those of the molybdenum disulfide graphene aerogel prepared by the traditional method.
Description
Technical Field
The invention relates to the field of material preparation method research and development, in particular to a method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma and a product thereof.
Background
Currently, molybdenum disulfide graphene aerogel is mainly prepared by a hydrothermal method, a chemical vapor deposition method, a solvothermal-thermal treatment method, a physical doping method and the like. The chemical vapor deposition method is to form a composite coating nanomaterial by vaporizing a target material and sequentially depositing on a base material. The preparation process is complex, target materials need to be purchased in advance, and large-scale popularization is difficult in practical industrial application.
In the hydrothermal method and the solvothermal-thermal treatment method for preparing the molybdenum disulfide graphene aerogel, a reducing agent is additionally added to reduce graphene oxide, and a low-valence sulfur source is subsequently added to reduce high-valence molybdenum so as to generate molybdenum disulfide particles on graphene particles. The physical doping method is to introduce nitride, carbide and phosphide into a molybdenum disulfide or graphene system, and the overall preparation process still adopts a solvothermal heat treatment method as a main body. In general, the molybdenum disulfide graphene aerogel prepared by the technology has the problems of complex preparation process, high dependence on a reducing agent and a low-valence sulfur source, poor adsorption performance of the prepared composite material and the like.
In the prior art, in preparation of graphene-based nano molybdenum disulfide composite aerogel, high-valence molybdenum salt and graphene oxide are generally mixed to preload or cover high-valence titanium molybdenum on the surface of the graphene oxide, and then reduction of the high-valence titanium molybdenum and the graphene oxide is realized by additionally adding a thiocyanide reducing agent. In general, graphene oxide and a thiocyanide reducing agent are directly used as a carbon source and a sulfur source, so that the preparation cost is relatively high. The thiocyanide reducing agent is a highly toxic substance, so that the operator is easily poisoned, and the synthetic residual liquid still needs to be deeply disposed. Meanwhile, the molybdenum disulfide in the prepared graphene-based nano molybdenum sulfide composite aerogel is not uniformly distributed, and the adsorption and hydrogen evolution performance of the composite aerogel is poor.
Therefore, based on the above discussion, it is a key to solve the bottleneck problem of the molybdenum disulfide graphene aerogel that research and development of a preparation technology with simple process, no need of additionally adding a reducing agent and a low-valence sulfur source in the process, and better performance of the finished product is achieved.
Disclosure of Invention
The purpose of the invention is as follows: the invention aims to solve the technical problem of providing a method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma.
The invention also aims to solve the technical problem of providing the molybdenum disulfide graphene aerogel.
In order to solve the technical problems, the technical scheme adopted by the invention is as follows: the invention provides a method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma, which comprises the following steps:
1) mixing water and graphite powder, stirring at the rotating speed of 60-180 rpm, and performing low-temperature plasma irradiation for 0.5-1.5 hours while stirring to obtain graphene slurry;
2) dripping sulfuric acid into the graphene slurry to obtain acidic graphene slurry;
3) adding molybdenum trioxide into the acidic graphene slurry, stirring at the rotating speed of 60-180 rpm, and simultaneously performing low-temperature plasma irradiation for 0.5-1.5 hours to obtain molybdenum disulfide graphene slurry;
4) and centrifuging the molybdenum disulfide graphene slurry, carrying out solid-liquid separation, and then carrying out vacuum freeze drying on the solid part to obtain the molybdenum disulfide graphene aerogel.
Wherein the liquid-solid ratio of the water to the graphite powder in the step 1) is 1-3: 1 mL/mg.
Wherein the action voltage of the low-temperature plasma irradiation in the step 1) is 20-50 KV, and the action atmosphere is oxygen.
Wherein the concentration of sulfuric acid in the step 2) is 1-2M.
Wherein the mass ratio of the molybdenum trioxide to the acidic graphene slurry in the step 3) is 5-15: 100.
Wherein, the action voltage of the low-temperature plasma irradiation in the step 3) is 20-50 KV, and the action atmosphere is argon.
Wherein the vacuum freeze drying temperature in the step 4) is-90 to-10 ℃, and the vacuum freeze drying time is 6 to 18 hours.
The invention further discloses the molybdenum disulfide graphene aerogel obtained by the preparation method.
The reaction mechanism is as follows: in the low-temperature plasma action process, high-energy electrons released by the high-voltage electrode end collide with oxygen to generate oxygen radicals, and the oxygen radicals and water molecules react to generate hydrogen radicals, hydroxyl radicals and hydrated electrons. Meanwhile, ultraviolet radiation and microwave radiation are generated along with the transition of excited particle energy level in the process of low-temperature plasma action. Oxygen and hydroxyl radicals may convert graphite to graphene oxide. While hydrogen radicals, ultraviolet radiation, and microwave radiation can convert graphene oxide to reduced graphene through a thermal reduction mechanism. Molybdenum trioxide is mixed into acidic graphene slurry and then stirred, and low-temperature plasma irradiation is carried out simultaneously, because the acting atmosphere is argon gas and the acting slurry is strong in acidity, hydrated electrons are combined with hydrogen ions in the slurry to generate hydrogen radicals, and the hydrogen radicals become dominant radicals in the slurry. The hydrogen radicals react with sulfate radicals to produce hydrogen sulfide. The hydrogen sulfide combines with the molybdenum trioxide to produce molybdenum disulfide and hydrogen ions. Under the stirring action and the ultraviolet radiation and microwave radiation action, the molybdenum disulfide and the graphene are uniformly mixed together to form the molybdenum disulfide graphene. Under the action of freeze drying, molybdenum disulfide graphene is converted into molybdenum disulfide graphene aerogel.
Has the advantages that: according to the invention, graphite powder is directly adopted as a raw material, the price is low, the graphene preparation process is directly realized through low-temperature plasma, the use of a traditional thiocyanide toxic reducing agent is avoided, only a freeze drying part of a traditional graphene aerogel preparation method is reserved, and the formation and mixing processes of the graphene and molybdenum disulfide are carried out in a low-temperature plasma environment at the early stage. According to the method, the graphene and the molybdenum disulfide are prepared only by taking the graphite powder and the sulfuric acid as the carbon source and the sulfur source, the production and reduction processes of the traditional graphene oxide are simplified, and the production of the reduced graphene is realized only in one system. According to the invention, the molybdenum disulfide and the graphene are uniformly dispersed and mixed based on ultraviolet radiation and microwave radiation generated in a low-temperature plasma system, and additional ultrasonic dispersion is not required. The adsorption performance and the hydrogen evolution performance of the molybdenum disulfide graphene aerogel prepared by the method are higher than those of the molybdenum disulfide graphene aerogel prepared by the traditional method.
Drawings
FIG. 1 is a flow chart of the treatment method of the present invention.
Detailed Description
The invention is further described below with reference to the figures and examples.
Example 1 influence of sulfuric acid concentration added to graphene slurry on adsorption and hydrogen evolution performance of prepared molybdenum disulfide graphene aerogel
Mixing water and graphite powder according to the liquid-solid ratio of 1: 1mL/mg, stirring at the rotating speed of 60rpm, and simultaneously carrying out low-temperature plasma irradiation for 0.5 hour to obtain graphene slurry, wherein the action voltage of the low-temperature plasma irradiation is 20KV, and the action atmosphere is oxygen. Sulfuric acid is dripped into the graphene slurry to ensure that the concentration of the sulfuric acid in the slurry is respectively 0.5M, 0.7M, 0.9M, 1M, 1.5M, 2M, 2.1M, 2.3M and 2.5M, thereby obtaining nine groups of acid graphene slurries. Respectively adding molybdenum trioxide into nine groups of acidic graphene slurries according to the mass ratio of the molybdenum trioxide to the acidic graphene slurries of 5:100, stirring at the rotating speed of 60rpm, and simultaneously carrying out low-temperature plasma irradiation for 0.5 hour to obtain nine groups of molybdenum disulfide graphene slurries, wherein the action voltage of the low-temperature plasma irradiation is 20KV, and the action atmosphere is argon. And centrifuging nine groups of molybdenum disulfide graphene slurry, performing solid-liquid separation, and then keeping the solid part at-10 ℃ for vacuum freeze drying for 6 hours to obtain nine groups of molybdenum disulfide graphene aerogel.
Adsorption test and adsorption capacity calculation: adding 40mg of molybdenum disulfide graphene aerogel into 80mL of methylene blue organic solution with the concentration of 250mg/L, stirring for 30 minutes at 360rpm, standing, and taking supernatant for detection. The methylene blue concentration in the liquid is measured according to the standard "determination of methylene blue adsorption value by test method of woody activated carbon" (GB-T12496.10-1999). The adsorption capacity of the molybdenum disulfide graphene aerogel on methylene blue is calculated according to a formula (1), wherein QtIs the adsorption capacity (mg/g) of molybdenum disulfide graphene aerogel on methylene blue, c0And ctThe concentration (mg/L) of methylene blue in the liquid before and after the adsorption test, m is the mass (g) of the added molybdenum disulfide graphene aerogel, and V is the volume (L) of the test solution.
Current density and electric double layer capacitance calculation: current density (268.5 mA/cm)2) And electric double layer capacitance (mF/cm)2) The calculation (the overpotential is 300mV) is detected and calculated according to the method in the graphene-based nano molybdenum sulfide composite aerogel construction and adsorption and hydrogen evolution performance research.
The test results of this example are shown in Table 1.
Table 1 influence of sulfuric acid concentration added to graphene slurry on adsorption performance and hydrogen evolution performance of prepared molybdenum disulfide graphene aerogel
As can be seen from table 1, when the concentration of the sulfuric acid added to the graphene slurry is less than 1M (as in table 1, when the concentration of the sulfuric acid added to the graphene slurry is 0.9, 0.7, 0.5 and lower values not listed in table 1), the amount of sulfuric acid is less, the amount of hydrogen radicals and hydrogen sulfide generated correspondingly decreases, the amount of molybdenum disulfide sequentially generated after the hydrogen sulfide is combined with molybdenum trioxide decreases, and the molybdenum disulfide and the graphene are insufficiently mixed, so that the active area, defect structure and active site density of the composite aerogel are increasedThe condition is worsened, the adsorption capacity of the prepared composite aerogel is lower than 282mg/g, and the current density is lower than 264mA/cm2The electric double layer capacitance is lower than 203mF/cm2. When the concentration of sulfuric acid added to the graphene slurry is equal to 1-2M (as shown in table 1, when the concentration of sulfuric acid added to the graphene slurry is 1, 1.5, or 2), since the acting atmosphere is argon gas and the acting slurry is strongly acidic, hydrated electrons combine with hydrogen ions to generate hydrogen radicals, and the hydrogen radicals become dominant radicals in the slurry. The hydrogen radicals react with sulfate radicals to produce hydrogen sulfide. The hydrogen sulfide combines with the molybdenum trioxide to produce molybdenum disulfide and hydrogen ions. Under the stirring action and the ultraviolet radiation and microwave radiation action, the molybdenum disulfide and the graphene are uniformly mixed together to form the molybdenum disulfide graphene. The finally formed composite aerogel has better conditions of active area, defect structure and active site density, the adsorption capacity of the prepared composite aerogel is more than 292mg/g, and the current density is more than 271mA/cm2The electric double layer capacitance is more than 211mF/cm2. When the concentration of sulfuric acid added to the graphene slurry is greater than 2M (as shown in table 1, when the concentration of sulfuric acid added to the graphene slurry is 2.1, 2.3, 2.5 and higher values not listed in table 1), the generated hydrogen sulfide is excessive, and the hydrogen sulfide is loaded on the surfaces of molybdenum disulfide and graphene, so that the mixing uniformity of molybdenum disulfide and graphene is poor, the formation conditions of the active area, defect structure and active site density of the composite aerogel are poor, and the adsorption capacity, current density and electric double layer capacitance of the composite aerogel are all significantly reduced along with the further increase of the concentration of sulfuric acid added to the graphene slurry. Therefore, in an integrated manner, the benefit and the cost are combined, and when the concentration of sulfuric acid added into the graphene slurry is equal to 1-2M, the adsorption performance and the hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel can be improved most.
Example 2 the mass ratio of molybdenum trioxide and acidic graphene slurry has an influence on the adsorption performance and hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel
Mixing water and graphite powder according to the liquid-solid ratio of 2: 1mL/mg, stirring at the rotating speed of 120rpm, and simultaneously carrying out low-temperature plasma irradiation for 1 hour to obtain graphene slurry, wherein the action voltage of the low-temperature plasma irradiation is 35KV, and the action atmosphere is oxygen. And (3) dripping sulfuric acid into the graphene slurry to enable the concentration of the sulfuric acid in the slurry to be 2M, so as to obtain the acidic graphene slurry. Adding molybdenum trioxide into the acidic graphene slurry according to the mass ratio of the molybdenum trioxide to the acidic graphene slurry of 2.5: 100, 3.5: 100, 4.5: 100, 5:100, 10: 100, 15:100, 15.5: 100, 16.5: 100 and 17.5: 100 respectively, stirring at the rotating speed of 120rpm, and simultaneously carrying out low-temperature plasma irradiation for 1 hour to obtain nine groups of molybdenum disulfide graphene slurries, wherein the action voltage of the low-temperature plasma irradiation is 35KV, and the action atmosphere is argon. And centrifuging nine groups of molybdenum disulfide graphene slurry, performing solid-liquid separation, and then keeping the solid part at-50 ℃ for vacuum freeze drying for 12 hours to obtain nine groups of molybdenum disulfide graphene aerogel.
The adsorption test and calculation of adsorption capacity, current density and electric double layer capacitance were the same as in example 1.
The test results of this example are shown in Table 2.
Table 2 the mass ratio of molybdenum trioxide and acidic graphene slurry has influence on the adsorption performance and hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel
As can be seen from Table 2, when the mass ratio of the molybdenum trioxide to the acidic graphene slurry is less than 5:100 (as shown in Table 2, when the mass ratio of the molybdenum trioxide to the acidic graphene slurry is 4.5: 100, 3.5: 100, 2.5: 100 and lower values not listed in Table 2), less molybdenum disulfide is generated by combining hydrogen sulfide and molybdenum trioxide, and the molybdenum disulfide and graphene are mixed uniformly and less, so that the active area, defect structure and active site density formation condition of the composite aerogel are all deteriorated, and the adsorption capacity of the prepared composite aerogel is lower than 292mg/g, and the current density is lower than 265 mA/cm/g2The electric double layer capacitance is lower than 207mF/cm2. Molybdenum trioxide and acid stoneWhen the mass ratio of the graphene slurry is 5-15: 100 (as shown in table 2, when the mass ratio of the molybdenum trioxide to the acidic graphene slurry is 5:100, 10: 100, or 15: 100), the hydrogen sulfide is combined with the molybdenum trioxide to generate a proper amount of molybdenum disulfide. Under the stirring action and the ultraviolet radiation and microwave radiation action, the molybdenum disulfide and the graphene are uniformly mixed together to form the molybdenum disulfide graphene. The finally formed composite aerogel has better conditions of active area, defect structure and active site density, the adsorption capacity of the prepared composite aerogel is larger than 304mg/g, and the current density is larger than 279mA/cm2The electric double layer capacitance is more than 215mF/cm2. When the mass ratio of the molybdenum trioxide to the acidic graphene slurry is greater than 15:100 (as shown in table 2, when the mass ratio of the molybdenum trioxide to the acidic graphene slurry is 15.5: 100, 16.5: 100, 17.5: 100, and higher values not listed in table 2), the amount of molybdenum disulfide generated by combining hydrogen sulfide and molybdenum trioxide is excessive, so that the mixing uniformity of molybdenum disulfide and graphene is poor, the formation conditions of the active area, the defect structure, and the active site density of the composite aerogel are poor, and the adsorption capacity, the current density, and the electric double layer capacitance of the composite aerogel are all significantly reduced as the mass ratio of the molybdenum trioxide to the acidic graphene slurry is further increased. Therefore, in an overall aspect, the benefit and the cost are combined, and when the mass ratio of the molybdenum trioxide to the acidic graphene slurry is equal to 5-15: 100, the adsorption performance and the hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel can be improved.
Example 3 Effect of action Voltage of Low temperature plasma irradiation on adsorption Performance and Hydrogen evolution Performance of prepared molybdenum disulfide graphene aerogel
Mixing water and graphite powder according to the liquid-solid ratio of 3:1mL/mg, stirring at the rotating speed of 180rpm, and simultaneously carrying out low-temperature plasma irradiation for 1.5 hours to obtain graphene slurry, wherein the action voltage of the low-temperature plasma irradiation is 50KV, and the action atmosphere is oxygen. And (3) dripping sulfuric acid into the graphene slurry to enable the concentration of the sulfuric acid in the slurry to be 2M, so as to obtain the acidic graphene slurry. Adding molybdenum trioxide into the acidic graphene slurry according to the mass ratio of the molybdenum trioxide to the acidic graphene slurry of 15:100, stirring at the rotating speed of 180rpm, and simultaneously carrying out low-temperature plasma irradiation for 1.5 hours while stirring to obtain the molybdenum disulfide graphene slurry, wherein the action voltages of the low-temperature plasma irradiation are respectively 10KV, 15KV, 18KV, 20KV, 35KV, 50KV, 52KV, 55KV and 60KV, and the action atmosphere is argon. And centrifuging the molybdenum disulfide graphene slurry, performing solid-liquid separation, and then keeping the solid part at-90 ℃ for vacuum freeze drying for 18 hours to obtain nine groups of molybdenum disulfide graphene aerogel.
The adsorption test and calculation of adsorption capacity, current density and electric double layer capacitance were the same as in example 1.
The test results of this example are shown in Table 3.
Table 3 influence of the action voltage of low-temperature plasma irradiation on the adsorption performance and hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel
As can be seen from table 3, when the action voltage of the low-temperature plasma irradiation is lower than 20KV (as shown in table 3, the action voltage of the low-temperature plasma irradiation is 18KV, 15KV, 10KV and lower values not listed in table 3), the yield and action effect of hydrated electrons are deteriorated, the amount of generated hydrogen radicals and hydrogen sulfide are correspondingly reduced, the amount of molybdenum disulfide formed by combining hydrogen sulfide with molybdenum trioxide is reduced, the mixing uniformity of molybdenum disulfide and graphene is reduced, so that the active area, defect structure and active site density of the composite aerogel are deteriorated, the adsorption capacity of the prepared composite aerogel is lower than 293mg/g, and the current density is lower than 276mA/cm2The electric double layer capacitance is less than 213mF/cm2. When the action voltage of the low-temperature plasma irradiation is equal to 20-50 KV (as shown in table 3, the action voltage of the low-temperature plasma irradiation is equal to 20KV, 35KV, and 50 KV), the hydrated electrons combine with the hydrogen ions to generate hydrogen radicals, and the hydrogen radicals become dominant radicals in the slurry. The hydrogen radicals react with sulfate radicals to produce hydrogen sulfide. The hydrogen sulfide combines with the molybdenum trioxide to produce molybdenum disulfide and hydrogen ions. Under the stirring action and the ultraviolet radiation and microwave radiation action, the molybdenum disulfide and the graphene are uniformly mixed together to form the molybdenum disulfide graphene. The final composite aerogel active surfaceThe formation conditions of product, defect structure and active site density are all good, so that the adsorption capacity of the prepared composite aerogel is larger than 316mg/g, and the current density is larger than 286mA/cm2The electric double layer capacitance is more than 221mF/cm2. When the operating voltage of the low-temperature plasma irradiation is higher than 50KV (as shown in table 3, when the operating voltage of the low-temperature plasma irradiation is 52KV, 55KV, 60KV and higher values not listed in table 3), the generated hydrogen radicals and hydrogen sulfide are excessive, so that the molybdenum disulfide generated by combining the hydrogen sulfide and molybdenum trioxide is excessive, the mixing uniformity of the molybdenum disulfide and graphene is poor, the active area, defect structure, and active site density of the composite aerogel are not good, and the adsorption capacity, current density, and electric double layer capacitance of the composite aerogel are all significantly reduced as the operating voltage of the low-temperature plasma irradiation is further increased. Therefore, in summary, the benefit and the cost are combined, and when the action voltage of low-temperature plasma irradiation is equal to 20-50 KV, the adsorption performance and the hydrogen evolution performance of the prepared molybdenum disulfide graphene aerogel are favorably improved.
Comparative example molybdenum disulfide graphene aerogel prepared by the invention is compared with the existing composite gas in gelling adsorption performance and hydrogen evolution performance
The preparation method of the molybdenum disulfide graphene aerogel comprises the following steps: mixing water and graphite powder according to the liquid-solid ratio of 3:1mL/mg, stirring at the rotating speed of 180rpm, and simultaneously carrying out low-temperature plasma irradiation for 1.5 hours to obtain graphene slurry, wherein the action voltage of the low-temperature plasma irradiation is 50KV, and the action atmosphere is oxygen. And (3) dripping sulfuric acid into the graphene slurry to enable the concentration of the sulfuric acid in the slurry to be 2M, so as to obtain the acidic graphene slurry. Adding molybdenum trioxide into the acidic graphene slurry according to the mass ratio of the molybdenum trioxide to the acidic graphene slurry of 15:100, stirring at the rotating speed of 180rpm, and simultaneously performing low-temperature plasma irradiation for 1.5 hours while stirring to obtain the molybdenum disulfide graphene slurry, wherein the action voltage of the low-temperature plasma irradiation is 50KV, and the action atmosphere is argon. And centrifuging the molybdenum disulfide graphene slurry, carrying out solid-liquid separation, and then keeping the solid part at-50 ℃ for vacuum freeze drying for 12 hours to obtain the molybdenum disulfide graphene aerogel.
Existing compositesPreparing aerogel: the composite aerogel is prepared according to a preparation method of graphene-based nano molybdenum sulfide composite aerogel construction and adsorption and hydrogen evolution performance research. The specific method comprises the following steps: (1) first, 3mmol of MoO was taken3Adding 30mL of deionized water into a certain mass of Graphene Oxide (GO), uniformly dispersing for 10 minutes by magnetic stirring, and performing ultrasonic treatment for 1 hour to obtain a uniformly dispersed suspension; (2) dissolving 8mmol of KSCN in 10mL of deionized water, and slowly adding the solution dropwise into MoO under the condition of magnetic stirring3Continuing magnetic stirring for 30 minutes in the mixed suspension of GO and GO, and further performing ultrasonic dispersion for 30 minutes; (3) keeping magnetic stirring, and gradually adding ammonia water into the mixed suspension solution obtained in the step (2) dropwise to adjust the pH value to 10 so as to ensure uniform dispersion of the suspension; (4) finally, transferring the mixed suspension with the adjusted pH value into a 50mL polytetrafluoroethylene high-pressure reaction kettle, and placing the reaction kettle into an air-blast drying oven to heat for 24 hours at a constant temperature; (5) after the autoclave was taken out and naturally cooled to room temperature, the sample was taken out from the autoclave and washed with deionized water (3 cycles). And then placing the sample in liquid nitrogen solution for quick freezing and keeping for 5 minutes, and keeping at-54 ℃ for vacuum freeze drying for 24 hours to obtain the graphene-based molybdenum disulfide composite aerogel.
The adsorption test and calculation of adsorption capacity, current density and electric double layer capacitance were the same as in example 1.
The test results of this example are shown in Table 4.
Table 4 comparison of the gelling adsorption performance and hydrogen evolution performance of the molybdenum disulfide graphene aerogel prepared by the present invention and the existing composite gas
As can be seen from table 4, the adsorption capacity, current density, and electric double layer capacitance of the molybdenum disulfide graphene aerogel prepared by the present invention are all higher than those of the currently reported composite gas gelation. According to the invention, no additional reducing agent is required to be added in the preparation process of the molybdenum disulfide graphene aerogel, and the adsorption performance and the hydrogen evolution performance of the prepared aerogel are superior to those of the reported composite gas gelation.
Claims (8)
1. A method for preparing molybdenum disulfide graphene aerogel by using low-temperature plasma is characterized by comprising the following steps:
1) mixing water and graphite powder, stirring at the rotating speed of 60-180 rpm, and performing low-temperature plasma irradiation for 0.5-1.5 hours while stirring to obtain graphene slurry;
2) dripping sulfuric acid into the graphene slurry to obtain acidic graphene slurry;
3) adding molybdenum trioxide into the acidic graphene slurry, stirring at the rotating speed of 60-180 rpm, and simultaneously performing low-temperature plasma irradiation for 0.5-1.5 hours to obtain molybdenum disulfide graphene slurry;
4) and centrifuging the molybdenum disulfide graphene slurry, carrying out solid-liquid separation, and then carrying out vacuum freeze drying on the solid part to obtain the molybdenum disulfide graphene aerogel.
2. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the liquid-solid ratio of water to graphite powder in the step 1) is 1-3: 1 mL/mg.
3. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the action voltage of the irradiation of the low-temperature plasma in the step 1) is 20-50 KV, and the action atmosphere is oxygen.
4. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the sulfuric acid concentration in the step 2) is 1-2M.
5. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the mass ratio of the molybdenum trioxide to the acidic graphene slurry in the step 3) is 5-15: 100.
6. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the action voltage of the low-temperature plasma irradiation in the step 3) is 20-50 KV, and the action atmosphere is argon.
7. The method for preparing the molybdenum disulfide graphene aerogel by using the low-temperature plasma according to claim 1, wherein the vacuum freeze-drying temperature in the step 4) is-90 to-10 ℃, and the vacuum freeze-drying time is 6 to 18 hours.
8. Molybdenum disulfide graphene aerogel obtained by the production method according to any one of claims 1 to 7.
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| CN104773725A (en) * | 2015-04-09 | 2015-07-15 | 厦门大学 | Method for preparing graphene by using low-temperature plasmas |
| CN107394127A (en) * | 2017-06-13 | 2017-11-24 | 陕西科技大学 | A kind of molybdenum disulfide graphene aerogel electrode material preparation method |
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| CN112569914A (en) * | 2020-12-11 | 2021-03-30 | 常熟理工学院 | Method for preparing uranium adsorbent by using ammonia water and acrylonitrile wastewater of coking plant |
| CN112569914B (en) * | 2020-12-11 | 2023-02-28 | 常熟理工学院 | Method for preparing uranium adsorbent by using ammonia water and acrylonitrile wastewater of coking plant |
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