CN105618085A - Method for preparing rGO-loaded petal-shaped MoS2 heterostructure - Google Patents
Method for preparing rGO-loaded petal-shaped MoS2 heterostructure Download PDFInfo
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- CN105618085A CN105618085A CN201510961222.4A CN201510961222A CN105618085A CN 105618085 A CN105618085 A CN 105618085A CN 201510961222 A CN201510961222 A CN 201510961222A CN 105618085 A CN105618085 A CN 105618085A
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/02—Sulfur, selenium or tellurium; Compounds thereof
- B01J27/04—Sulfides
- B01J27/047—Sulfides with chromium, molybdenum, tungsten or polonium
- B01J27/051—Molybdenum
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/18—Carbon
Abstract
The invention discloses a method for preparing rGO-loaded petal-shaped MoS2 heterostructure, and aims to improve the efficiency of photocatalytic degradation of organic dye. The method is a treatment method for increasing the crystallization degree through one-step hydrothermal reaction synthesis and annealing treatment, a heterogeneous composite structure that petal-shaped MoS2 clusters and rGO clusters are twined mutually can be formed, adsorption of organic pollutants can be remarkably improved due to the large specific surface area of a two-dimensional material, photo-induced electrons can be prompted to be rapidly transferred to a graphene lamella due to a heterogeneous interface of the two-dimensional material, photo-induced holes with oxidability in an MoS2 valence band is engaged in organic pollutant degradation, and thus the photocatalysis property of the material can be greatly improved. Moreover, the MoS2/rGO heterostructure plays a prompting role in improving the response of the material within a visible light range. The method is simple and clear in technical idea, and the degradation efficiency of the composite material to the organic dye is remarkably improved. The invention further discloses the technical idea for preparing semiconductor heterostructure by using a hydrothermal method and improving the efficiency of photocatalytic degradation of the organic dye.
Description
[technical field]
The invention belongs to conductor photocatalysis degradating organic dye field, relate to a kind of rGO load petal-shaped MoS2The preparation method of heterojunction structure.
[background technology]
Environmental pollution and energy crisis become the key issue that restriction current social is fast-developing. Conductor photocatalysis degradation of organic substances both can effectively utilize sunlight, it is also possible to administers the problem of environmental pollution being on the rise, and becomes current academia and the focus of industrial quarters concern. As semiconductor light-catalyst, most basic requirement has three: one, selected semi-conducting material to have suitable band gap, improves the absorbance to visible ray as far as possible; Two, material itself to have big specific surface area, in order to can fully be combined with Organic substance to be degraded and adsorb; Three, photo-generate electron-hole separates in time, it is to avoid compound again.
Since Graphene finds for 2004, start people's research boom to two-dimensional material. Molybdenum bisuphide (MoS2) as the Typical Representative of transient metal sulfide, there is the stratiform sandwich structure of uniqueness. Its interlayer is combined by van der Waals interaction power. It is similar to Graphene, MoS2Can also grow into the ultra-thin two-dimension structure of several layers, and to change its band gap variable at 1.3eV��1.8eV along with the number of plies, namely can realize fully absorbing visible ray in a big way. And, two-dimensional slice MoS2Having that specific surface area is big, edge dangling bonds abundant, surface activity high, the realization for high-performance optical catalyst provides possibility.
But single MoS2Can not effectively suppressing the compound in light induced electron and hole, to promoting, photocatalysis efficiency is unfavorable. How to promote the separation in light induced electron and hole, become the bottleneck problem restricting its photocatalysis characteristic. If by MoS2With other two-dimensional material compound, utilize its strong heterogeneous interface effect entirely possible reach light induced electron and hole efficiently separate. Graphene has high electric conductivity and optical transmittance, if by Graphene and MoS2Compound, neither affects MoS2Absorption to light, it is possible to promote that light induced electron is quickly transferred to Graphene, and hole remains in MoS2On, significant increase photocatalysis characteristic.
[summary of the invention]
It is an object of the invention to the shortcoming overcoming above-mentioned prior art, it is provided that a kind of rGO load petal-shaped MoS2The preparation method of heterojunction structure, the method is to prepare MoS by one step hydro thermal method2/ rGO heterogeneous material compound, forms a kind of petal-shaped MoS2Cluster and graphene sheet layer compact winding and have the heterojunction structure of bigger serface, light induced electron for producing under light illumination provides effective transmission channel, realize efficiently separating of light induced electron and hole, significantly improve the usefulness of the photocatalytically degradating organic dye of material.
For reaching above-mentioned purpose, the present invention is achieved by the following technical solutions:
A kind of rGO load petal-shaped MoS2The preparation method of heterojunction structure, comprises the following steps:
1) selecting two molybdic acid hydrate sodium and thiourea is reactant, and graphene oxide is presoma, is sufficiently mixed, and obtains homodisperse suspended mixed solution;
2) with autoclave for holding vessel, mixed solution, as reactant, adopts hydro-thermal method, prepares rGO load petal-shaped MoS2The mixed solution of composite construction;
3) mixed solution it is carried out and dries, obtaining MoS2/ rGO composite construction powder.
The present invention is further improved by:
Further comprising the steps of:
4) by making annealing treatment raising MoS2The degree of crystallinity of/rGO composite construction powder and interface state.
Described step 4) in, it being annealed processing under vacuum or argon gas atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
Described step 1) in, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5; In parts by weight, the addition of graphene oxide is the 0%��10% of two molybdic acid hydrate sodium.
Described step 1) in, suspended mixed solution is obtained by stirring and ultrasonic Treatment.
Described step 2) in, reaction vessels is that Teflon still lining is equipped with rustless steel still set, and volume is 100mL.
Described step 2) in, autoclave is positioned in baking oven, reaction temperature is 210 DEG C, and the response time is 3��30h, furnace cooling or after water-cooled take out product, stand-by.
Described step 3) in, cleaning treatment is successively in acetone, deionized water and dehydrated alcohol, with the centrifugation 3 times of 8000r/min, and each 5min, the mixed solution after being processed, stand-by.
Described step 3) in, cleaned mixed solution is placed in vacuum drying oven, at the temperature of 80 DEG C, dries 12h, obtain MoS2/ rGO composite construction powder, stand-by.
Compared with prior art, the method have the advantages that
MoS prepared by the present invention2/ rGO composite is petal-shaped MoS2Cluster is dispersed on graphene sheet layer, is mutually wound around, and interface cohesion is good. After this composite mixes with organic dyestuff, the specific surface area relatively large due to two-dimensional material and all atoms are all exposed to the such intrinsic attribute in top layer, and material contacts fully with organic dyestuff, considerably increases catalytic site. The present invention utilizes MoS2And the heterogeneous interface formed between Graphene, the separation in light induced electron and hole can be effectively facilitated, the light of reinforced composite absorbs and photocatalysis performance. The present invention is with two molybdic acid hydrate sodium for molybdenum source, with thiourea for sulfur source, in hydrothermal reaction process, and forming core under the promotion of graphite oxide functional group, and in water-heat process, realize the reduction to graphite oxide, thus forming MoS2The heterojunction structure that cluster and Graphene are combined closely, along with the prolongation in response time presents MoS2The growing up of cluster, decentralized, the crystallization degree of hetero-junctions is improve by follow-up annealing.
[accompanying drawing explanation]
Fig. 1 is the MoS of preparation2Cluster scanning electron microscope (SEM) photograph;
Fig. 2 is the MoS of preparation2/ rGO composite construction scanning electron microscope (SEM) photograph;
Fig. 3 is MoS2Cluster and MoS2/ rGO composite construction degraded RhB degradation efficiency comparison diagram.
[detailed description of the invention]
Below in conjunction with specific embodiment, the present invention is described in further detail:
The present invention utilizes one step hydro thermal method to prepare rGO load petal-shaped MoS2Composite construction; To MoS under vacuum or argon gas atmosphere2/ rGO composite construction powder is annealed processing, and promotes its degree of crystallinity further; Adjust presoma kind in course of reaction, the addition of graphene oxide and response time, it is achieved to MoS2The change of cluster geometric properties and control. MoS of the present invention2The preparation method of/rGO heterojunction structure, comprises the following steps:
(1) selecting two molybdic acid hydrate sodium and thiourea is reactant, and graphene oxide is presoma, is sufficiently mixed, dispersed suspended mixed solution.
The mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, the addition of graphene oxide controls in 0%��10% scope of two molybdic acid hydrate sodium, above-mentioned reactant is joined in 60mL deionized water and obtains mixed solution, mixed solution is to obtain homodisperse suspension by stirring and ultrasonic Treatment, stand-by.
(2) with autoclave for holding vessel, mixed solution, as reactant, adopts hydro-thermal method, prepares rGO load petal-shaped MoS2The mixed solution of composite construction.
Autoclave adopts Teflon still lining to be equipped with rustless steel still set, specification is 100mL, pour scattered mixing suspension into still lining, loading to screw in rustless steel still set is positioned in a conventional oven, reaction temperature is 210 DEG C, response time is 3��30h, furnace cooling or after water-cooled take out product, stand-by.
(3) mixed solution it is carried out and dries, obtaining MoS2/ rGO composite construction powder.
By the MoS that hydro-thermal reaction obtains2/ rGO composite construction mixed solution, respectively in acetone, deionized water and dehydrated alcohol, is centrifuged 3 times with the rotating speed of 8000r/min, each 5min, obtain cleaned mixed solution, subsequently cleaned mixed solution is placed in vacuum drying oven, dries 12h, obtain MoS for 80 DEG C2/ rGO composite construction powder, stand-by.
(4) MoS is improved further by annealing2The degree of crystallinity of/rGO composite construction powder and interface state.
Being annealed processing under vacuum or argon gas atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
Embodiment 1
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, without graphene oxide, hydro-thermal reaction synthesis MoS2Cluster. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Being annealed processing under Ar atmospheric condition, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
As it is shown in figure 1, MoS prepared by this example2The diameter of cluster is 2.34 ��m, the high-visible some MoS in cluster surface2Lamella, cluster bad dispersibility.
Embodiment 2
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 1% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 1.31 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 3
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 2.5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 1.22 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 4
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
As in figure 2 it is shown, MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 1.06 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely, and cluster dispersibility is better.
Embodiment 5
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 7.5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.83 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 6
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 10% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO hetero-junctions2The diameter of cluster is 0.68 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely, cluster good dispersion.
Embodiment 7
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 1.5h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
There is not petal-shaped MoS in material prepared by this example2Cluster.
Embodiment 8
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 3h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.45 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 9
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 6h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.54 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 10
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 12h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.76 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 11
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 18h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.88 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 12
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 24h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 0.93 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Embodiment 13
With two molybdic acid hydrate sodium and thiourea for reactant, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5, and graphene oxide is presoma, and the addition of graphene oxide is the 5% of two molybdic acid hydrate sodium, hydro-thermal reaction synthesis MoS2/ rGO composite. Hydrothermal temperature is 210 DEG C, and the response time is 30h. Making annealing treatment under an ar atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
MoS prepared by this example2Petal-shaped MoS in/rGO composite2The diameter of cluster is 1.93 ��m, the high-visible MoS in cluster surface2Lamella, cluster and graphene sheet layer are combined closely.
Fig. 3 chooses embodiment 1 (MoS2)��4(MoS2/rGO-5)��6(MoS2/ rGO-10) MoS for preparing2/ rGO composite carries out the degradation experiment of rhdamine B, dark reaction reacts 150min after terminating under illumination effect, takes out appropriate mixed liquor every 30min and tests, as seen from the figure, the degradation efficiency of embodiment 4 and 6 is above embodiment 1, it was shown that MoS prepared by the present invention2/ rGO composite is significantly increased for the degradation efficiency of organic dyestuff.
The technical characteristic of the present invention: 1) design of the present invention is clear, and principle is understandable; 2) preparation method of the present invention is simple, a step can prepare rGO load petal-shaped MoS by hydro-thermal reaction2Cluster composite construction; 3) the composite heterogeneous interface that prepared by the present invention can promote efficiently separating of light induced electron and hole, significantly improves its photocatalysis performance; 4) the invention provides a kind of technical thought utilizing two-dimensional material interlayer coupling to realize light absorption and photocatalysis performance enhancing and method.
Above content is only the technological thought that the present invention is described; protection scope of the present invention can not be limited with this; every technological thought proposed according to the present invention, any change done on technical scheme basis, each fall within the protection domain of claims of the present invention.
Claims (9)
1. a rGO load petal-shaped MoS2The preparation method of heterojunction structure, it is characterised in that comprise the following steps:
1) selecting two molybdic acid hydrate sodium and thiourea is reactant, and graphene oxide is presoma, is sufficiently mixed, and obtains homodisperse suspended mixed solution;
2) with autoclave for holding vessel, mixed solution, as reactant, adopts hydro-thermal method, prepares rGO load petal-shaped MoS2The mixed solution of composite construction;
3) mixed solution it is carried out and dries, obtaining MoS2/ rGO composite construction powder.
2. rGO load petal-shaped MoS according to claim 12The preparation method of heterojunction structure, it is characterised in that further comprising the steps of:
4) by making annealing treatment raising MoS2The degree of crystallinity of/rGO composite construction powder and interface state.
3. rGO load petal-shaped MoS according to claim 22The preparation method of heterojunction structure, it is characterised in that described step 4) in, it being annealed processing under vacuum or argon gas atmosphere, annealing temperature is 450 DEG C, and heating rate is 5 DEG C/min, and temperature retention time is 2h, furnace cooling.
4. rGO load petal-shaped MoS according to claim 12The preparation method of heterojunction structure, it is characterised in that described step 1) in, the mol ratio of two molybdic acid hydrate sodium and thiourea is 1:5; In parts by weight, the addition of graphene oxide is the 0%��10% of two molybdic acid hydrate sodium.
5. the rGO load petal-shaped MoS according to claim 1 or 42The preparation method of heterojunction structure, it is characterised in that described step 1) in, suspended mixed solution is obtained by stirring and ultrasonic Treatment.
6. rGO load petal-shaped MoS according to claim 12The preparation method of heterojunction structure, it is characterised in that described step 2) in, reaction vessels is that Teflon still lining is equipped with rustless steel still set, and volume is 100mL.
7. the rGO load petal-shaped MoS according to claim 1 or 62The preparation method of heterojunction structure, it is characterised in that described step 2) in, autoclave is positioned in baking oven, reaction temperature is 210 DEG C, and the response time is 3��30h, furnace cooling or after water-cooled take out product, stand-by.
8. rGO load petal-shaped MoS according to claim 12The preparation method of heterojunction structure, it is characterised in that described step 3) in, cleaning treatment is successively in acetone, deionized water and dehydrated alcohol, with the centrifugation 3 times of 8000r/min, and each 5min, the mixed solution after being processed, stand-by.
9. the rGO load petal-shaped MoS according to claim 1 or 82The preparation method of heterojunction structure, it is characterised in that described step 3) in, cleaned mixed solution is placed in vacuum drying oven, at the temperature of 80 DEG C, dries 12h, obtain MoS2/ rGO composite construction powder, stand-by.
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| CN110252346B (en) * | 2019-05-29 | 2022-03-18 | 江苏大学 | MoS2/SnS2Preparation method and application of/r-GO composite photocatalyst |
| CN111111729A (en) * | 2019-12-18 | 2020-05-08 | 西安交通大学 | Molybdenum disulfide-based nanocomposite material with hollow sandwich laminated structure and preparation method thereof |
| CN111111729B (en) * | 2019-12-18 | 2021-08-13 | 西安交通大学 | Molybdenum disulfide-based nanocomposite material with hollow sandwich laminated structure and preparation method thereof |
| CN111167502A (en) * | 2020-02-14 | 2020-05-19 | 山西大学 | Chemically-connected non-noble metal heterostructure composite material and preparation method and application thereof |
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