KR101816358B1 - Nanoparticles and nanofluids comprising the same - Google Patents
Nanoparticles and nanofluids comprising the same Download PDFInfo
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- KR101816358B1 KR101816358B1 KR1020150171757A KR20150171757A KR101816358B1 KR 101816358 B1 KR101816358 B1 KR 101816358B1 KR 1020150171757 A KR1020150171757 A KR 1020150171757A KR 20150171757 A KR20150171757 A KR 20150171757A KR 101816358 B1 KR101816358 B1 KR 101816358B1
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Abstract
The present invention relates to a nanoparticle comprising at least one functional group bonded to one surface or both surfaces of a surface of a carbon-based nano sheet, wherein the functional group has a length of 4 Å to 10 Å.
The nanoparticles according to an embodiment of the present invention include functional groups having a specific range of length to further improve the dispersibility upon contact with the solvent and the polymer material.
Description
The present invention relates to nanoparticles comprising functional groups having a certain range of lengths and nanofluids comprising them.
Thermal management in heat transfer equipment is one of the important factors in determining energy efficiency. In automobiles, various working fluids such as water, ethylene glycol (EG), propylene glycol, engine oil, mineral oil, kerosene oil, silicone oil, fluids play an important role for efficient thermal management.
In nanofluids, nanofluids are a fluid that has enhanced its inherent properties by adding nanoparticles. The most important point in nanofluids is whether the properties of nanoparticles are improved by the amount of nanoparticles. For this purpose, it is important that the nanoparticles are uniformly dispersed as they do not cling to each other.
Recent researches on graphene or carbon nanotubes based on carbon-based materials as nanoparticles have been carried out. These materials are excellent in electrical, thermal and mechanical properties, and can be applied to various fields such as sensors, batteries or hydrogen storage .
However, these nanoparticles of carbon-based materials are difficult to stably disperse and maintain in a fluid due to strong Van der Waals forces (induced dipole forces).
In order to solve this problem, various studies have been conducted to modify nanoparticles by dispersing various functional groups on the surface of the carbon-based particles and dispersing them in a solvent or a polymer. However, nanoparticles having various functional groups show dispersibility within a solvent or polymer for a certain period of time, but there may be a problem of coagulation due to interactions between particles with time and gradually precipitating.
Therefore, development of nanoparticles capable of minimizing aggregation between nanoparticles and improving dispersibility has been urgently required by investigating the influence on improvement of dispersibility of nanoparticles.
Disclosure of Invention Technical Problem [8] The present invention provides a nanoparticle and a nanofluid containing the nanoparticle which can further improve dispersibility upon contact with a solvent and a polymer substance.
According to an aspect of the present invention, there is provided a method of fabricating a nano-sized nano-sheet, comprising the steps of: Lt; / RTI >
Also provided is a nanofluid comprising the nanoparticles and the solvent.
The nanoparticles according to an embodiment of the present invention include functional groups having a specific range of length to further improve the dispersibility upon contact with the solvent and the polymer material.
BRIEF DESCRIPTION OF THE DRAWINGS The accompanying drawings, which are incorporated in and constitute a part of the specification, illustrate exemplary embodiments of the invention and, together with the description of the invention, It should not be construed as limited.
Fig. 1 shows a carbon-based nanosheet in a two-dimensional (2D) plate shape.
2 (A) to 2 (D) show the shape and length of a functional group according to the number of carbon atoms contained in a functional group, respectively, in the form of carbon nanoparticles having a functional group according to an embodiment of the present invention will be.
3 is a schematic diagram showing an example of the area of two-dimensional (2D) nanoparticles.
4 illustrates a method of evaluating the degree of dispersion of a nanofluid according to an embodiment of the present invention.
FIG. 5 illustrates a nanofluid of a time frame according to an embodiment of the present invention.
FIG. 6 illustrates a nanoparticle after removing a solvent of the nanofluid according to an embodiment of the present invention.
FIG. 7 is a graph showing a change in length of a functional group according to the number of carbon atoms contained in a functional group of a nanoparticle according to an embodiment of the present invention. FIG.
FIG. 8 is a graph illustrating dispersion of nanoparticles according to length of a functional group according to an embodiment of the present invention.
Fig. 9 shows the shape of the nanoparticles of Comparative Example 2. Fig.
FIG. 10 shows the shape of the nanoparticles of Example 1 according to an embodiment of the present invention.
Fig. 11 shows the shape of the nanoparticles of Comparative Example 3. Fig.
Hereinafter, the present invention will be described in detail in order to facilitate understanding of the present invention.
The terms and words used in the present specification and claims should not be construed as limited to ordinary or dictionary terms and the inventor may appropriately define the concept of the term in order to best describe its invention It should be construed as meaning and concept consistent with the technical idea of the present invention.
The nanoparticles of the present invention include at least one functional group bonded to one surface or both surfaces of a surface of a carbon-based nano sheet, and the functional group has a length of 4 Å to 10 Å.
The nanoparticles according to an embodiment of the present invention include functional groups having a specific range of length to further improve the dispersibility upon contact with the solvent and the polymer material.
In the nanoparticles according to an embodiment of the present invention, the carbon nanosheets are preferably two-dimensional carbon nanosheets, for example, graphene or graphene oxide.
The graphene refers to a single layer which is peeled off from graphite, and graphene oxide refers to a plate-like nanoparticle prepared by chemically oxidizing a graphite powder. Preferably, graphene oxide can be prepared by oxidizing graphite under strong acid and strong oxidizing agents.
The nanoparticles may be surface-modified with functional groups in the plane of the graphene or graphene oxide, wherein the functional group may be an epoxy group, an alcohol group, a carbonyl group, or a carboxyl group.
While graphene has a stable plate-like structure, graphene oxide can form irregular and various-shaped plate-like structures compared to graphene. Particularly, in the case of graphene oxide, the distance between the plate surface and the plate surface is maintained larger than that of graphene by surface modification through functional groups such as an epoxy group, an alcohol group, a carbonyl group, or a carboxyl group, It is possible to further improve the compatibility with the solvent and the polymer substance.
Particularly, since the alcohol group and the carboxyl group mentioned above have hydrophilicity, when they are modified with such a functional group, they can exhibit excellent dispersibility in water or a polar solvent.
Therefore, in the present invention, in order to suppress the aggregation phenomenon by the plate-like structure to improve dispersibility, a functional group is provided on the surface of the carbon-based nanosheet on the two-dimensional (2D) plate of FIG. 1, The length of the functional group was controlled by changing the number of carbon atoms in the modification process of the functional group on the sheet surface, and the effect of the functional group length on the improvement of dispersibility was confirmed. Thus, it has been confirmed that nanoparticles having a specific length range of from 4 Å to 10 Å can effectively improve the physical properties of the nanofluid, thereby completing the present invention.
Specifically, FIG. 2 shows changes in length and shape of functional groups according to the number of carbon atoms contained in functional groups (A) to (D), respectively.
In the nanoparticle according to one embodiment of the present invention, the functional group may be at least one functional group selected from an epoxy group, an alcohol group, a carbonyl group, and a carboxyl group, Lt; / RTI > This may be an optimal position for improving the dispersibility around the functional group and may be the position where the effect of the sterical hindrance can be seen most.
For example, in the case of graphene oxide, it is most preferable that the functional group is located at the center of the surface of the plate. If the functional group is on the end of the graphene oxide plate, the opposite edge of the nanoparticle can flocculate.
Thus, it may be desirable to couple the functional units to a minimum number of centers efficiently, rather than attaching them to the edges.
At this time, the length of the functional group may mean a straight line distance from the carbon starting from the functional group on the surface of the carbon-based nanosheet to the carbon atoms farthest from the functional carbon. For example, when the functional group is an epoxide group, it may be a straight line distance from the carbon contained in the epoxide group to the carbon atom farthest from the epoxide group.
According to an embodiment of the present invention, there is a probability that the two-dimensional nanoparticles are aggregated on both sides. Therefore, by having functional groups on both sides of the plate, the distance between the plate and the plate can be widened, Can be suppressed.
If the length of the functional group becomes longer than a certain length, the functional group tends to bend like a curved line rather than a straight line due to structural stability. In such a case, the functional group may have a problem of decreasing the dispersibility.
According to an embodiment of the present invention, it is preferable that the number of carbon atoms contained in one functional group is 4 to 7. If the number of carbon atoms contained in one functional group is less than 4, the length of the functional group may be short and the dispersing effect may be insufficient. When the number of carbon atoms exceeds 7, the length of the functional group becomes longer, So that it is not preferable from the viewpoint of dispersion efficiency.
According to an embodiment of the present invention, the ratio of the length of the nanoparticles to the length of the functional group (that is, the length of the functional group / length of the nanoparticles (length of the shortest side of the nanoparticles)) is preferably 0.4 to 1 can do.
When the length ratio is less than 0.4, the length of the functional group versus the length of the nanoparticles is short and the aggregation phenomenon between the plate and the plate is increased, so that the dispersion effect may be insignificant. When the ratio of the length is more than 1, It can be bent like a shape, so that the dispersibility can be rather reduced.
According to one embodiment of the present invention, the number of functional groups of the nanoparticles may be 2 to 10 (when present on both sides) per 100 Å 2 of nanoparticles.
That is, when a functional group is present on both sides of a nanoparticle, assuming that the length of one side is at least 10 Å,
Number of required functional groups = (area of nanoparticles / area where one functional group can cover dispersion)
Specifically, for example, when the lengths of the two-dimensional carbon nanoparticles are 50 Å and 80 Å, respectively, as shown in FIG. 3, and the area in which one functional group covers the dispersion is 100 Å 2 In the case where the functional group exists on both sides of the nanoparticle, assuming that the length of the nanoparticles is at least 10 angstroms, or a rectangular nanoparticle having a length of at least 10 angstroms).
Therefore, the number of necessary functional groups may be 80 or more, that is, 80 or more, preferably 80 to 400, per 4000 Å 2 of nanoparticle area.
The present invention also provides a nanofluid comprising the nanoparticles and the solvent.
The solvent may be any solvent selected from the group consisting of water, ethylene glycol (EG), and propylene glycol, or two of the solvents selected from the group consisting of water, ethylene glycol (EG), and propylene glycol A mixed solvent of a mixture of water and ethylene, more preferably a mixed solvent of water and ethylene glycol.
In the nanofluid according to an embodiment of the present invention, the weight ratio of the nanoparticles to the solvent may be 2 to 30:70 to 98, preferably 5 to 20:80 to 95.
The degree of dispersion of the nanofluid including nanoparticles according to an embodiment of the present invention may be 0.9 or more, preferably 0.92 or more.
The degree of dispersion can be evaluated by comparing the transmittance using optical instruments such as naked eyes, UV-Vis-IR equipment and Zeta potential, but it is preferable to use a quantitative evaluation method of dispersion, that is, based on Newton's equation By calculating the position of nanoparticles in a nanofluid in a time frame calculated by a molecular dynamics simulation, it is possible to quantitatively evaluate the coagulation of nanoparticles in the nanofluid.
For example, as the quantitative evaluation method described above, a dispersion degree evaluation apparatus implemented by a computer system may be used, and the dispersion degree evaluation method of the nanofluid of FIG. 4 may be used. The apparatus may include a processor, a memory, an input device, an output device, a storage, and a network interface, which are connected via a bus (B) (refer to Korean Patent Application No. 10-2015-0155999).
Specifically, the processor calculates the positional information of the nanoparticles present in the nanofluid in units of time frames through molecular dynamics simulation (S110). The processor computes the position of the nanoparticles in each time frame through molecular dynamics simulation and delivers them to the nanoparticle identification module.
In other words, as shown in FIG. 5, the processor computes the position of nanoparticles in the fluid according to a time frame by performing a molecular dynamics simulation with a predetermined amount of nanoparticles added to a unit volume of solvent.
The processor identifies nanoparticles dispersed in the nanofluid of the corresponding time frame (S120). For example, the processor identifies nanoparticles present in the nanofluid as shown in FIG. 6 when a nanofluid of a particular time frame as shown in FIG. 5 is input.
The processor calculates the centroid of the identified nanoparticles (S130). The processor computes the center coordinates of the nanoparticles using the coordinates of the atoms that make up the identified nanoparticles.
The processor assigns an identification number to the center of the calculated nanoparticle (S140). In other words, the processor assigns an identification number to each of the identified nanoparticles.
The processor calculates the center distance between the nanoparticles and determines whether the distance is less than the reference cohesion distance (S150). Here, the reference cohesion distance is 3.5 σ c -c (where σ c -c is 3.37 Å), which is 11.795 Å.
If the center distance between the nanoparticles is less than the reference cohesion distance, the processor determines cohesion between the nanoparticles (S160). For example, if the center distance between the nanoparticles is 7.694 ANGSTROM, which is smaller than the reference aggregation distance of 11.795 ANGSTROM, the processor judges that aggregation occurs between the nanoparticles.
Meanwhile, the processor determines that the dispersion phenomenon of the nanoparticles occurs when the center distance between the nanoparticles is greater than the reference aggregation distance (S165). That is, when the center distance between the nanoparticles is 17.781 ANGSTROM, which is larger than the reference aggregation distance of 11.795 ANGSTROM, the dispersion among the nanoparticles is determined.
The processor calculates the degree of dispersion of the nanoparticles in the nanofluid by reflecting the determination results in S160 and S165 (S170). In other words, the processor calculates the degree of dispersion of the nanoparticles in the nanofluid, reflecting the cohesion between the nanoparticles.
The processor confirms whether the calculation of the dispersion of the nanoparticles by time frame is completed (S180). In the present embodiment, the degree of dispersion of the nanofluid can be calculated in units of one time frame. When the processor has completed the calculation of the variance of the nanoparticles by time frame, the processor calculates an average of the variances calculated for each time frame (S190).
Based on the quantitative evaluation method of the degree of dispersion, it is possible to observe the variation of the dispersion according to the structure of each functional group of the nanoparticles, and the relationship between the length of the functional group and the dispersion stability of the nanoparticles can be identified. That is, when the length of the functional group for improving the dispersibility is 4 Å to 10 Å, the dispersibility is 0.9 or more, which can contribute to the improvement of the physical properties of the nanofluid efficiently.
BEST MODE FOR CARRYING OUT THE INVENTION Hereinafter, the present invention will be described in detail with reference to examples. However, the embodiments according to the present invention can be modified into various other forms, and the scope of the present invention should not be construed as being limited to the embodiments described below. The embodiments of the present invention are provided to enable those skilled in the art to more fully understand the present invention.
Example
EXAMPLES The present invention will be further illustrated by the following examples and experimental examples, but the present invention is not limited by these examples and experimental examples.
Example One
≪ Preparation of nanoparticles >
Modified graphene oxide nanoparticles (graphene oxide-thin film type, ACS Materials) having an average carbon atom number of 4 in the epoxide group located at the center of the graphene oxide produced by the Hummer's method were obtained.
≪ Preparation of nanofluids >
The nanofluids were prepared by mixing 10% by weight of the nanoparticles with a solvent of water and ethylene glycol in a weight ratio of 1: 1 with respect to the entire nanofluid.
Example 2
Except that modified graphene oxide nanoparticles (graphene oxide-thin film type, ACS Materials) having an atom number of carbon atoms of 7 in the epoxy group located at the center of graphene oxide were used. To obtain nanoparticles and nanofluids.
Comparative Example One
The nanoparticles (graphene oxide-thin film type, ACS Materials) and nanofluids were obtained in the same manner as in Example 1, except that graphene having no functional groups was used as the nanoparticles.
Comparative Example 2
Except that modified graphene oxide nanoparticles (graphene oxide-thin film type, ACS Materials) having an epoxy group having 1 carbon atom number located at the center of graphene oxide were used, and the same procedure as in Example 1 was carried out To obtain nanoparticles and nanofluids.
Comparative Example 3
Except that modified graphene oxide nanoparticles (graphene oxide-thin film type, ACS Materials) having a number of carbon atoms of 10 in the epoxide located at the center of graphene oxide were used, and the same procedure as in Example 1 was carried out To obtain nanoparticles and nanofluids.
Experimental Example One
<Measurement of Functional Length and Dispersion Diagram According to Number of Carbon Atoms>
The length and the degree of dispersion of the functional groups of the nanofluids of Examples 1 and 2 and Comparative Examples 1 to 3 were measured. The length and the degree of dispersion of the functional group can be calculated by calculating the position of the nanoparticles in the nanofluid in the time frame calculated through the molecular dynamics simulation based on the Newton equation, which is a detailed description of the present invention and the method described in FIG. We quantitatively evaluated the coagulation of nanoparticles in nanofluids. The lengths of the functional groups of each nanoparticle were determined by randomly selecting nanoparticles within the nanofluid system (density: 1 g / cm 3 , number of molecules (N) / volume (V) / temperature (T: 298 K) It calculates the length between about 50ps.
Fig. 7 shows changes in the lengths of the functional groups in the nanoparticles of Examples 1 and 2 and Comparative Examples 1 to 3 according to the number of carbon atoms, and the results of dispersion according to changes in the length of functional groups are shown in Fig. 8 and Table 1 .
(Length, A)
(Deg.of Dispersion)
As shown in FIG. 7, as the number of carbon atoms increases, the length of the functional group is relatively increased, confirming the correlation of the length of functional groups with the number of carbon atoms.
As can be seen from FIG. 8 and Table 1, in Comparative Example 1 which did not include a functional group, the degree of dispersion remarkably decreased. In Comparative Example 1 in which the number of carbon atoms was 1 and the functional group had a length of 2.462 +/- 0.044
In addition, as is clear from the results of Comparative Example 3, it was confirmed that the larger the length of the functional group, the greater the dispersion was. In other words, when Examples 1 and 2 and Comparative Example 3 were compared, in Examples 2 and 3, when the length of the functional group was in the range of 4 Å to 10 Å, the dispersion degree was 0.925 or more. As a result of the dispersion measurement of Comparative Example 3 having a length of 12.143 +/- 0.869 ANGSTROM, it was found that the dispersion degree was decreased due to the long agglomeration distance (within 11.9 A in the cut-off distance), and compared with Examples 1 and 2 It was confirmed that the dispersion degree decreased by about 20%.
9 to 11 illustrate the effect of the length of the functional group on the behavior of the nanoparticles. In order to investigate the effect of the length of the functional group on the behavior of the nanoparticles, the condensed-phase optimized molecular potentials for atomistic simulation studies (COMPASS) BIOVIA Software Inc., San Diego, Calif., USA).
Specifically, FIG. 9 shows the shape of the nanoparticles of Comparative Example 2 having a carbon atom number of 1 and a functional group length of 2.462 ± 0.044 Å. As can be seen from FIG. 9, in Comparative Example 2, the length of the functional group was so short that the shape of the functional group was not observed to be deformed (bent), and the structure control (steric hindrance) The dispersion effect is very small, but the dispersion effect is very small.
10 shows the shape of the nanoparticles of Example 1 with the number of carbon atoms being 1 and the length of the functional group being 4.786 +/- 0.623 angstroms. As can be seen from Fig. 10, the functional group of the silver nanoparticles of Example 1 has little bending, and the shape is maintained even when approaching in the lateral direction, so that the dispersibility is maintained. In addition, the effect of dispersibility through the structure control is remarkably increased, and it is confirmed that the two-dimensional nanoparticles exhibit excellent dispersibility due to less influence on each other even in the vertical direction.
11 shows the shape of the nanoparticles of Comparative Example 3 in which the number of carbon atoms is 10 and the length of the functional group is 12.143 ± 0.869 Å. As can be seen from FIG. 11, in Comparative Example 3, as the length of the functional group of the nanoparticles became longer, a straight (straight) shape was not maintained and bending was observed. In addition, the phenomenon of trapping by the functional group of nanoparticles occurs, and it can be confirmed that the dispersibility is reduced.
Claims (13)
Wherein the ratio of the length of the nanoparticles to the length of the functional group is from 0.4 to 1.
Wherein the length of the functional group is the length of the functional group located at the center of the nanoparticle.
Wherein the length of the functional group is the length of the epoxide group.
Wherein the solvent is any one selected from the group consisting of water, ethylene glycol (EG) and propylene glycol, or a mixed solvent of two or more thereof.
Wherein the weight ratio of the nanoparticles to the solvent is from 2 to 30:70 to 98 by weight.
Wherein the nanofluid has a degree of dispersion of 0.9 or more.
Wherein the degree of dispersion is calculated by calculating the position of the nanoparticles in the nanofluid in a time frame calculated through molecular dynamics simulation.
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| KR101159754B1 (en) | 2010-04-27 | 2012-06-28 | 국립대학법인 울산과학기술대학교 산학협력단 | Method of graphene synthesis via edge-functionalization of graphite |
| KR101325530B1 (en) | 2011-10-06 | 2013-11-07 | 주식회사 케이씨씨 | Functionalized methods of high quality graphene using conjugated system |
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| KR101159754B1 (en) | 2010-04-27 | 2012-06-28 | 국립대학법인 울산과학기술대학교 산학협력단 | Method of graphene synthesis via edge-functionalization of graphite |
| KR101325530B1 (en) | 2011-10-06 | 2013-11-07 | 주식회사 케이씨씨 | Functionalized methods of high quality graphene using conjugated system |
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