CN106348244B - A kind of graphene-based nanowire composite structures and preparation method thereof - Google Patents
A kind of graphene-based nanowire composite structures and preparation method thereof Download PDFInfo
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- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 106
- 239000002131 composite material Substances 0.000 title claims abstract description 35
- 238000002360 preparation method Methods 0.000 title abstract description 8
- 150000002736 metal compounds Chemical class 0.000 claims description 97
- 239000000758 substrate Substances 0.000 claims description 33
- 238000000034 method Methods 0.000 claims description 16
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- 229910001297 Zn alloy Inorganic materials 0.000 claims description 14
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- 238000006243 chemical reaction Methods 0.000 claims description 6
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- 230000008569 process Effects 0.000 claims description 4
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 3
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 3
- 239000011248 coating agent Substances 0.000 claims description 3
- 238000000576 coating method Methods 0.000 claims description 3
- 230000003247 decreasing effect Effects 0.000 claims description 3
- SOQBVABWOPYFQZ-UHFFFAOYSA-N oxygen(2-);titanium(4+) Chemical compound [O-2].[O-2].[Ti+4] SOQBVABWOPYFQZ-UHFFFAOYSA-N 0.000 claims description 3
- 230000035484 reaction time Effects 0.000 claims description 3
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 3
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 3
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- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
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- 238000007605 air drying Methods 0.000 description 1
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- 238000005229 chemical vapour deposition Methods 0.000 description 1
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- 229910052710 silicon Inorganic materials 0.000 description 1
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- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
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- 239000011701 zinc Substances 0.000 description 1
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Abstract
The present invention provides a kind of graphene-based nanowire composite structures and preparation method thereof, using the metallic compound nano line vertical-growth of at least two different main groups on graphene-based bottom, so that it is guaranteed that under the premise of graphene-based bottom performance, improve the specific surface area at graphene-based bottom, and combine the performance of the metallic compound nano line of at least two different main groups with the performance of graphene, be conducive to grapheme material applied in technical field of semiconductors；Simultaneously, the diameter of the metallic compound nano line of two kinds of different main groups is not identical, the surface area accounting of the big metallic compound nano line of diameter is greater than the surface area accounting of the small metallic compound nano line of diameter, at this time, the performance of the big metallic compound nano line of diameter is the main performance of graphene-based nanowire composite structures, to adjust the material and diameter of nano wire by selection, to realize the performance controllability and flexible and selectable of graphene-based nanowire composite structures.
Description
Technical Field
The invention relates to the technical field of semiconductors, in particular to a graphene-based nanowire composite structure and a preparation method thereof.
Background
With the development of semiconductor technology and the continuous reduction of technical nodes, the traditional silicon material has many limitations and defects, and graphene is the thinnest, the highest strength and the strongest novel nano material in the world at present, so that graphene becomes an ideal substitute of silicon.
Since the single-layer graphene film has a zero forbidden bandwidth and the semiconductor material is required to have a certain forbidden bandwidth, if the advantages of the graphene film can be utilized to be applied to the technical field of semiconductors, greater technical progress will be brought.
The application of graphene is generally widened by adopting a composite structure of a semiconductor nano material and graphene, however, the composite structure can only show one semiconductor nano material performance and is often not adjustable, which greatly limits the improvement of the device performance formed by the composite structure.
Disclosure of Invention
In order to overcome the above problems, the present invention aims to provide a graphene-based nanowire composite structure and a method for preparing the same.
In order to achieve the above object, the present invention provides a graphene-based nanowire composite structure, comprising: a graphene substrate; and at least two different main group metal compound nanowires vertically grown on the graphene substrate.
Preferably, the metal compound nanowires include at least titanium alloy nanowires and zinc alloy nanowires.
Preferably, the titanium alloy nanowire is a titanium dioxide nanowire, and the zinc alloy nanowire is a zinc oxide nanowire.
Preferably, the metal compound nanowires of different main groups are arranged alternately in one-dimensional direction.
Preferably, the diameters of the metal compound nanowires of different main groups are different, and the diameters of the metal compound nanowires of the same main group are the same.
Preferably, the metal compound nanowires of different main groups are arranged in order of decreasing diameter, and the metal compound nanowires of the same main group with the same diameter are located on the same straight line or the same circular line.
Preferably, when the metal compound nanowires of the same main group and the same diameter are located on the same ring wire, the metal compound nanowires of different main groups are arranged in concentric rings.
Preferably, the shape of the loop line is circular, oval, square, regular polygon, or pentagram.
Preferably, when the metal compound nanowires of the same main group and the same diameter are located on the same straight line, straight lines in which the metal compound nanowires of different main groups are arranged in a radial shape.
Preferably, the graphene substrate is a single-layer graphene film, a graphene oxide film and a reduced graphene oxide film.
In order to achieve the above object, the present invention further provides a preparation method of the graphene-based nanowire composite structure, including the following steps:
step 01: providing a graphene substrate;
step 02: coating a mask on the graphene substrate; dividing metal compound nanowire growth areas of different main groups on the graphene substrate, and preparing mask plates corresponding to the metal compound nanowire growth areas of the different main groups;
step 03: respectively growing corresponding metal compound nanowires in the metal compound nanowire growth areas of different main groups by adopting mask plates corresponding to the metal compound nanowire growth areas of different main groups; wherein,
step 031, for one of the main group metal compound nanowire growth regions, removing the mask of the one of the main group metal compound nanowire growth regions and exposing the graphene substrate of the one of the main group metal compound nanowire growth regions by using the one of the main group metal compound nanowire growth region mask through photolithography and/or etching;
032, vertically growing the metal compound nanowire of one main group on the exposed graphene substrate;
and 033, repeating the 031-.
Preferably, in step 032, the metal compound nanowires of different main groups have different diameters by setting the concentration of the reaction solution, the reaction temperature and the reaction time.
Preferably, the material of the mask is a photoresist, and then in step 031, the mask in the metal compound nanowire growth region of one of the main groups is removed through a photolithography process.
According to the graphene-based nanowire composite structure and the preparation method thereof, the metal compound nanowires of at least two different main groups vertically grow on the graphene substrate, so that the specific surface area of the graphene substrate is improved on the premise of ensuring the performance of the graphene substrate, and the performance of the metal compound nanowires of at least two different main groups is combined with the performance of graphene, so that the graphene material is favorably applied to the technical field of semiconductors; meanwhile, the diameters of the two metal compound nanowires of different main groups are different, the surface area ratio of the metal compound nanowire with the large diameter is larger than that of the metal compound nanowire with the small diameter, and at the moment, the performance of the metal compound nanowire with the large diameter is the main performance of the graphene-based nanowire composite structure, so that the performance adjustability and the flexible selectivity of the graphene-based nanowire composite structure are realized by selecting and adjusting the material and the diameter of the nanowire.
Drawings
Fig. 1 is a schematic cross-sectional view of a graphene-based nanowire composite structure according to a preferred embodiment of the present invention
Fig. 2 is a schematic top view of a graphene-based nanowire composite structure according to a preferred embodiment of the invention
Fig. 3 is a schematic top view of a graphene-based nanowire composite structure according to a preferred embodiment of the invention
Fig. 4 is a schematic top view of a graphene nanowire composite structure according to a preferred embodiment of the invention
Fig. 5 is a schematic flow chart of a method for preparing a graphene nanowire composite structure according to a preferred embodiment of the present invention
Detailed Description
In order to make the contents of the present invention more comprehensible, the present invention is further described below with reference to the accompanying drawings. The invention is of course not limited to this particular embodiment, and general alternatives known to those skilled in the art are also covered by the scope of the invention.
The invention is described in further detail below with reference to the accompanying figures 1-5 and specific examples. It should be noted that the drawings are in a simplified form and are not to precise scale, and are only used for conveniently and clearly achieving the purpose of assisting in describing the embodiment.
The graphene-based nanowire composite structure in this embodiment includes: a graphene substrate; and at least two different main group metal compound nanowires vertically grown on the graphene substrate. Since the nanowires are grown on the graphene substrate, the bottom of the nanowires is bonded to the graphene through a chemical bond, for example, a carbon bond of the graphene is bonded to a metal bond. The graphene substrate may be a single-layer graphene film, a graphene oxide film, and a reduced graphene oxide film.
Referring to fig. 1, in the present embodiment, the metal compound nanowires include titanium alloy nanowires 2 and zinc alloy nanowires 1, but the present invention is not limited to these two nanowires. Preferably, the titanium alloy nanowire 2 is a titanium dioxide nanowire, and the zinc alloy nanowire 1 is a zinc oxide nanowire. The metal compound nanowires of different main groups are arranged at intervals in the one-dimensional direction, the metal compound nanowires of different main groups have different diameters, and the metal compound nanowires of the same main group have the same diameter, please refer to fig. 1 again, the titanium alloy nanowires 2 and the zinc alloy nanowires 1 are arranged at intervals in the one-dimensional direction, the diameter of the titanium alloy nanowires 2 is larger than that of the zinc alloy nanowires 1, here, the diameters of the titanium alloy nanowires 2 can be similar or the same, and the diameters of the zinc alloy nanowires 1 can be similar or the same; in addition, the same meaning of the diameters of the metal compound nanowires of the same main group is: the metal compound nanowires of the same main group have the same diameter or have similar diameters, for example, the difference between the diameters of the metal compound nanowires of the same main group is not more than 10 nm.
Here, the metal compound nanowires of different main groups are arranged in order of decreasing diameter, and the metal compound nanowires of the same main group having the same diameter are located on the same straight line or the same circular line. Specifically, referring to fig. 2, the diameter of the titanium alloy nanowire 2 is greater than that of the zinc alloy nanowire 1, the titanium alloy nanowire 2 and the zinc alloy nanowire 1 are respectively arranged into a one-dimensional array, and the arrays are sequentially and alternately arranged into a rectangular array; referring to fig. 3, the titanium alloy nanowires 2 and the zinc alloy nanowires 1 are respectively arranged in a one-dimensional array and the arrays are radially arranged, referring to fig. 4, the titanium alloy nanowires 2 with the same diameter are arranged in a ring, the zinc alloy nanowires 1 with the same diameter are arranged in a ring, the ring formed by the metal compound nanowires with the smaller diameter is surrounded by the ring formed by the metal compound nanowires with the larger diameter, that is, the ring formed by the zinc alloy nanowires 1 is surrounded by the ring formed by the titanium alloy nanowires 2, and the two arrays are repeatedly stacked outwards to form a concentric ring.
Referring to fig. 5, in the present embodiment, the preparation method of the graphene-based nanowire composite structure includes the following steps:
step 01: providing a graphene substrate;
specifically, the graphene substrate may be a single-layer graphene film or a graphene oxide film or a reduced graphene oxide film. The single-layer graphene film can be prepared by adopting a high-temperature thermal decomposition method and a chemical vapor deposition method, and the methods can successfully prepare the high-quality single-layer graphene film. The graphene oxide film can be obtained by spin-coating, spin-coating and air-drying the graphene oxide film by adopting an aqueous solution method, but the graphene oxide film is basically multilayer, so that a single-layer graphene oxide film is difficult to obtain.
Step 02: coating a mask on the graphene substrate; dividing metal compound nanowire growth areas of different main groups on the graphene substrate, and preparing mask plates corresponding to the metal compound nanowire growth areas of the different main groups;
specifically, the growth regions of the metal compound nanowires of different main groups are divided according to actual needs, and a mask for the growth region of each corresponding metal compound nanowire of each main group is prepared. The mask may be made of an organic material or an inorganic material, the organic material may be but not limited to photoresist, an anti-reflection layer plus photoresist, or only an anti-reflection layer, and the inorganic material may be silicon nitride, silicon oxide, or the like, preferably silicon oxide, because the density of silicon nitride is higher, the obtained mask is harder, and the graphene substrate at the bottom of the mask is damaged due to more severe over-etching.
Step 03: respectively growing corresponding metal compound nanowires in the metal compound nanowire growth areas of different main groups by adopting mask plates corresponding to the metal compound nanowire growth areas of different main groups; wherein,
specifically, step 03 includes:
step 031, for one of the main group metal compound nanowire growth regions, removing the mask of the one of the main group metal compound nanowire growth regions and exposing the graphene substrate of the one of the main group metal compound nanowire growth regions by using the one of the main group metal compound nanowire growth region mask through photolithography and/or etching;
here, for example, when growing the metal compound nanowire of the first main group, the mask on the growth region of the metal compound nanowire corresponding to the first main group is removed, and the removal method may adopt photolithography, plasma dry etching or a combination of the two; if the material of the mask is selected from photoresist or an anti-reflection layer and photoresist, the mask can be removed by adopting a one-step photoetching process, and if the material of the mask is only selected from the anti-reflection layer, the mask can be removed by adopting a process of photoetching firstly and then chemical etching or plasma etching.
032, vertically growing the metal compound nanowire of one main group on the exposed graphene substrate;
for example, for the titanium alloy nanowire region, the titanium precursor solution can be prepared by a hydrothermal method at a temperature of 300-600 ℃, or by an electrochemical plating method; aiming at the zinc alloy nanowire area, a zinc precursor solution can be prepared by a hydrothermal method at the temperature of 100-500 ℃ or by methods such as electrochemical plating; the metal compound nanowires of different main groups have different diameters by setting the concentration of the reaction solution, the reaction temperature, and the reaction time.
And 033, repeating the 031-.
Specifically, after the metal compound nanowires of the first main group grow well, the mask of the growth region of the metal compound nanowires of the second main group is removed again in step 031, then the metal compound nanowires of the second main group are grown in step 032, and so on, thereby completing the preparation of all the metal compound nanowires.
It should be noted that, for a metal compound nanowire that has been grown before, when a metal compound nanowire of a different main group is grown subsequently, a subsequent metal precursor solution may adhere to the surface of the metal compound nanowire that has been grown before to continue growing, or may not adhere to the surface of the metal compound nanowire that has been grown before to continue growing, the former may cause the metal compound nanowire that has been grown before to continue to become thick, and the latter may cause the metal compound nanowire that has been grown before to slightly become thin, but this does not affect the quality and performance of the finally formed graphene-based nanowire composite structure.
It should be further noted that when graphene oxide is selected as the graphene substrate, after the metal compound nanowires of different main groups are grown in step 03, the graphene oxide may be reduced to a reduced graphene oxide thin film, and thus, in this case, the graphene in the finally formed composite structure may be a reduced graphene oxide thin film or a graphene oxide thin film.
In summary, the graphene-based nanowire composite structure provided by the invention adopts the metal compound nanowires of various different main groups to be compounded with the graphene film, so that the performance of the graphene substrate including single-layer graphene, graphene oxide or reduced graphene oxide and the performance of the metal compound nanowires of various different main groups are compatible, and the application field of graphene is widened. Furthermore, when the diameters of the metal compound nanowires of different main groups are different, the ratio of the specific surface area of the metal compound nanowire with the large diameter to the specific surface area of all the metal compound nanowires is large, so that the composite structure mainly shows the performance of the metal compound nanowire with the large diameter.
Although the present invention has been described with reference to preferred embodiments, which are illustrated for the purpose of illustration only and not for the purpose of limitation, it will be apparent to those skilled in the art that various changes and modifications can be made therein without departing from the spirit and scope of the invention as defined in the appended claims.
Claims (11)
1. A graphene-based nanowire composite structure, comprising: a graphene substrate; and at least two different main group metal compound nanowires vertically grown on the graphene substrate; the metal compound nanowires of different main groups are arranged at intervals in a one-dimensional direction; the diameters of the metal compound nanowires of different main groups are different, and the diameters of the metal compound nanowires of the same main group are the same; the metal compound nanowires of different main groups are arranged in the order of decreasing diameter, and the metal compound nanowires of the same main group with the same diameter are positioned on the same straight line or the same ring line.
2. The graphene-based nanowire composite structure of claim 1, wherein the metal compound nanowires comprise at least titanium alloy nanowires and zinc alloy nanowires.
3. The graphene-based nanowire composite structure of claim 1, wherein the metal compound nanowires are titanium dioxide nanowires and zinc oxide nanowires.
4. The graphene-based nanowire composite structure of claim 1, wherein the metal compound nanowires of different main groups are arranged in concentric rings when the metal compound nanowires of the same main group with the same diameter are located on the same ring.
5. The graphene-based nanowire composite structure of claim 4, wherein the loop wire is circular, elliptical, square, regular polygonal, or pentagon shaped.
6. The graphene-based nanowire composite structure according to claim 1, wherein when the metal compound nanowires of the same main group having the same diameter are positioned on the same straight line, straight lines formed by the metal compound nanowires of different main groups are arranged in a radial shape.
7. The graphene-based nanowire composite structure of any one of claims 1-6, wherein the graphene substrate is a single-layer graphene thin film.
8. The graphene-based nanowire composite structure according to any one of claims 1 to 6, wherein the graphene substrate is a graphene oxide thin film or a reduced graphene oxide thin film.
9. A method for preparing the graphene-based nanowire composite structure of claim 1, comprising the steps of:
step 01: providing a graphene substrate;
step 02: coating a mask on the graphene substrate; dividing metal compound nanowire growth areas of different main groups on the graphene substrate, and preparing mask plates corresponding to the metal compound nanowire growth areas of the different main groups;
step 03: respectively growing corresponding metal compound nanowires in the metal compound nanowire growth areas of different main groups by adopting mask plates corresponding to the metal compound nanowire growth areas of different main groups; wherein,
step 031, for one of the main group metal compound nanowire growth regions, removing the mask of the one of the main group metal compound nanowire growth regions and exposing the graphene substrate of the one of the main group metal compound nanowire growth regions by etching using the one of the main group metal compound nanowire growth region mask; wherein, the mask adopts silicon oxide or silicon nitride;
032, vertically growing the metal compound nanowire of one main group on the exposed graphene substrate;
and 033, repeating the 031-.
10. The method of claim 9, wherein the metal compound nanowires of different main groups have different diameters by setting the concentration of the reaction solution, the reaction temperature, and the reaction time in step 032.
11. The method of claim 9, wherein the mask is made of a photoresist, and in step 031, the mask in the growth region of the metal compound nanowire of one of the main groups is removed by a photolithography process.
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| CN104549363B (en) * | 2014-12-31 | 2018-04-17 | 江苏大学 | A kind of nano metal or metal alloy catalyst and preparation method thereof |
| CN106449133B (en) * | 2016-10-08 | 2020-03-31 | 全普半导体科技(深圳)有限公司 | Single-layer graphene film-based composite structure, preparation method and semiconductor device |
| CN206244402U (en) * | 2016-10-09 | 2017-06-13 | 全普光电科技(上海)有限公司 | A kind of graphene-based nanowire composite structures |
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