CN107159178A - A kind of TiO of graphene modified2The preparation method of membranaceous compound and its application in photocatalysis degradation organic contaminant - Google Patents
A kind of TiO of graphene modified2The preparation method of membranaceous compound and its application in photocatalysis degradation organic contaminant Download PDFInfo
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- CN107159178A CN107159178A CN201611174951.6A CN201611174951A CN107159178A CN 107159178 A CN107159178 A CN 107159178A CN 201611174951 A CN201611174951 A CN 201611174951A CN 107159178 A CN107159178 A CN 107159178A
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- 150000001875 compounds Chemical class 0.000 title claims abstract description 41
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 36
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 36
- 238000002360 preparation method Methods 0.000 title claims abstract description 26
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 15
- 238000007146 photocatalysis Methods 0.000 title claims abstract description 12
- 230000015556 catabolic process Effects 0.000 title claims abstract description 8
- 238000006731 degradation reaction Methods 0.000 title claims abstract description 8
- 239000000356 contaminant Substances 0.000 title claims abstract description 7
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 59
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims abstract description 23
- 239000011521 glass Substances 0.000 claims abstract description 22
- 238000004528 spin coating Methods 0.000 claims abstract description 12
- 238000000034 method Methods 0.000 claims abstract description 11
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 22
- 239000008367 deionised water Substances 0.000 claims description 17
- 229910021641 deionized water Inorganic materials 0.000 claims description 17
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 10
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 10
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 7
- -1 polytetrafluoroethylene Polymers 0.000 claims description 7
- 238000013019 agitation Methods 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 claims description 5
- 238000001035 drying Methods 0.000 claims description 5
- 239000002114 nanocomposite Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 4
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 4
- FPCJKVGGYOAWIZ-UHFFFAOYSA-N butan-1-ol;titanium Chemical compound [Ti].CCCCO.CCCCO.CCCCO.CCCCO FPCJKVGGYOAWIZ-UHFFFAOYSA-N 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 2
- 239000002253 acid Substances 0.000 claims 1
- DCKVNWZUADLDEH-UHFFFAOYSA-N sec-butyl acetate Chemical compound CCC(C)OC(C)=O DCKVNWZUADLDEH-UHFFFAOYSA-N 0.000 claims 1
- 238000010521 absorption reaction Methods 0.000 abstract description 5
- 238000012360 testing method Methods 0.000 abstract description 3
- 230000007613 environmental effect Effects 0.000 abstract 1
- 238000012986 modification Methods 0.000 abstract 1
- 239000000463 material Substances 0.000 description 7
- 239000006185 dispersion Substances 0.000 description 4
- 235000011167 hydrochloric acid Nutrition 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 239000003643 water by type Substances 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 238000003795 desorption Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 150000001721 carbon Chemical group 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002389 environmental scanning electron microscopy Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 1
- 238000000103 photoluminescence spectrum Methods 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004153 renaturation Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 description 1
- 229940043267 rhodamine b Drugs 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/18—Carbon
-
- B01J35/39—
-
- B01J35/59—
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
Abstract
The invention discloses a kind of TiO of graphene (GR) modification2Membranaceous compound (GR TiO2) preparation method and its application in photocatalysis degradation organic contaminant.The preparation method, which is mainly, to be first passed through hydro-thermal method and prepares TiO on FTO electro-conductive glass2Nanometer stick array；Then using spin-coating method in prepared TiO2GR is loaded on nanometer stick array, so as to obtain GR TiO2Membranaceous compound.Test result shows, the GR TiO prepared using the inventive method2Absorption of the membranaceous compound to light is stronger, excellent photocatalysis performance is shown during photocatalysis degradation organic contaminant, it is easy to separate, and repeats and utilizes, this has great application prospect in field of environmental improvement.
Description
Technical field
The invention belongs to field of nanometer material technology, and in particular to a kind of GR-TiO2The preparation method of membranaceous compound and in light
Application in catalytic degradation organic pollution.
Background technology
Titanium dioxide (TiO2) metal oxide semiconductor as photochemical catalyst has become the crowds such as material, the energy, environment
Multi-field study hotspot.Work as TiO2When the energy of absorption is more than its energy gap, under the exciting of photon, it can make in molecular orbit
Electronics leaves valence band and transits to conduction band, so that in valence band formation photohole (h+), in conduction band formation light induced electron (e-), photoproduction
Electron-hole pair is transferred to material surface and occurs oxidation reaction and reduction instead so that material has photocatalytic activity, but is turning
Move on to before material surface, electron-hole pair is easily reconfigured, causing the photocatalytic activity of material reduces.
Graphene (GR) be it is a kind of by carbon atom with sp2 hybridized orbits constitute hexangle type in honeycomb lattice new carbonaceous it is thin
Membrane material, it has huge surface area, and excellent adsorption capacity is good electron acceptor and transmits body, can be effective
Suppress the restructuring of photo-generate electron-hole pair, by TiO2With the compound absorption that can increase the absorption intensity of light, expand light of graphene
Scope.At present for graphene and TiO2The research of composite, focuses primarily upon graphene and nanometer grade powder TiO2Particle
It is compound, although to have expanded TiO2Light abstraction width, but the surface area of composite is still little, and nano particle is using ring
Be easy to inactivate and condense in border, not free settling, cause it to be difficult separation, reclaim and reuse.
The content of the invention
It is an object of the invention to provide the easily separated recovery of one kind and the enhanced GR-TiO of photocatalysis performance2It is membranaceous compound
Thing.
It is another object of the present invention to provide a kind of GR-TiO2The preparation method of membranaceous compound.
In order to realize the above object the technical solution adopted in the present invention is：
A kind of GR-TiO2The preparation method of membranaceous compound, comprises the following steps：
A, TiO prepared on FTO electro-conductive glass by hydro-thermal method2Nanometer stick array：
(1) FTO electro-conductive glass is cleaned by ultrasonic 20-30min with acetone, absolute ethyl alcohol, deionized water successively, dried standby
With；
(2) by deionized water and concentrated hydrochloric acid by volume 1:1 mixing, is added dropwise butyl titanate thereto while stirring, wherein
The volume ratio of butyl titanate and above-mentioned mixed liquor is 0.5-0.8:50, then the mixed liquor is poured into and is placed with FTO electro-conductive glass
In autoclave (100ml), baking oven is put into, react 15-20h at 140-160 DEG C；
(3) after reaction terminates, take out autoclave and rinsed with running water and be down to room temperature, take out with TiO2Nanometer rods
The FTO electro-conductive glass of array, with deionized water rinse for several times, product is dried naturally, that is, obtains TiO2Nanometer stick array.
B, using spin-coating method in TiO2GR is loaded on nanometer stick array, GR-TiO is obtained2Membranaceous compound：
(1) weigh a certain amount of graphene (GR) to be dissolved in absolute ethyl alcohol, ultrasonic agitation 60min obtains graphene dispersion
Liquid；
(2) graphene dispersing solution low speed is spun to the TiO of above-mentioned preparation with refiner2Nanometer stick array surface, is drying
Dried in case；
(3) deionized water rinse 3 times, dry naturally, so as to obtain GR-TiO2Membranaceous nano composite structure.
It is preferred that, the specification of the FTO electro-conductive glass is 25mm × 25mm.
It is preferred that, the FTO electro-conductive glass leans to polytetrafluoroethylene (PTFE) inwall with 60 ° of inclination angle, and conductive face-down.
It is preferred that, the concentration of the graphene dispersing solution is 0.5-1.5mg/ml.
The spin coating method is specifically, graphene dispersing solution is added dropwise in dry TiO2On nanometer stick array, 500rpm-
Spin coating 50-80s under 1000rpm low speed.
The drying temperature is 80 DEG C, and drying time is 6-8h.
It is above-mentioned in TiO2That prepared on nanometer stick array is the GR-TiO2Membranaceous compound.
The invention provides a kind of selectable application process, step is as follows：
A, rhodamine B (Rh B) solution for preparing 5mg/L；
B, by GR-TiO2Membranaceous compound is put into the self-control reactor equipped with Rh B solutions, is first inhaled in dark surrounds
Then attached 30-60min is irradiated the corresponding time with reaching the attached balance of absorption-desorption with simulated solar light source, and with Japan's Shimadzu
The UV-2550 types ultraviolet-uisible spectrophotometer test of company.
The present invention draws above-mentioned GR-TiO by substantial amounts of exploratory development2The preparation method of membranaceous compound, this method behaviour
Make simple, mild condition, all raw material is common to be easy to get.There are two committed steps in preparation process：TiO2Nanometer stick array
Prepare the spin coating with graphene.TiO2The preparation process of nanometer stick array need to be carried out in strict accordance with above-mentioned steps, and graphene
Spin coating directly affects prepared GR-TiO2The photocatalysis performance of membranaceous compound.
The beneficial effects of the present invention are there is provided a kind of GR-TiO2The preparation method of membranaceous compound, utilizes this method
Preparation-obtained membranaceous compound activity during photocatalysis degradation organic contaminant is high, easily separated to reclaim, it is to avoid pass
System nutty structure is easy to inactivate and condense in photocatalytic process, not caused by free settling difficult separation defect, preparation can weigh
Renaturation is good.
Preparation method technique of the present invention is simple, and easy to operate, without large-scale instrument and equipment, cost is low, with fine
Practical extending application value.
Brief description of the drawings
Fig. 1 is TiO2Nanometer stick array and GR-TiO2The scanning electron microscope diagram of membranaceous compound.
Fig. 2 is TiO2Nanometer stick array and GR-TiO2The UV-Vis DRS spectrogram of membranaceous compound.
Fig. 3 is TiO2Nanometer stick array and GR-TiO2The photoluminescence spectra comparison diagram of membranaceous compound.
Embodiment
The present invention is further illustrated below in conjunction with Figure of description and specific embodiment, but embodiment is not to the present invention
Technical scheme limit in any form.
Agents useful for same is purchased in market in following examples.
Embodiment 1：
Prepare GR-TiO2Membranaceous compound, step is as follows：
A, by FTO electro-conductive glass successively with acetone, absolute ethyl alcohol, deionized water be cleaned by ultrasonic 20min, dry standby；
B, 30ml deionized waters and 30ml concentrated hydrochloric acids mixed, 0..9ml butyl titanates are added dropwise thereto while stirring, so
The mixed liquor is poured into afterwards and is placed with the autoclave of FTO electro-conductive glass (100ml), baking oven is put into, reacted at 150 DEG C
18h；
After C, reaction terminate, take out autoclave and rinsed with running water and be down to room temperature, take out with TiO2Nanometer rods
The FTO electro-conductive glass of array, with deionized water rinse for several times, product is dried naturally, that is, obtains TiO2Nanometer stick array.
D, weigh a certain amount of graphene (GR) and be dissolved in absolute ethyl alcohol, ultrasonic agitation 60min obtains 1mg/ml graphite
Alkene dispersion liquid；
E, with refiner by graphene dispersing solution with 500rpm rotating speed spin coating 60s to above-mentioned preparation TiO2Nanometer rods battle array
List face, dries 4h in 80 DEG C of baking ovens；
F, deionized water rinse 3 times, dry naturally, so as to obtain GR-TiO2Membranaceous nano composite structure.
Embodiment 2：
Prepare GR-TiO2Membranaceous compound, step is as follows：
A, by FTO electro-conductive glass successively with acetone, absolute ethyl alcohol, deionized water be cleaned by ultrasonic 20min, dry standby；
B, 30ml deionized waters and 30ml concentrated hydrochloric acids mixed, 1.0ml butyl titanates are added dropwise thereto while stirring, then
The mixed liquor is poured into and is placed with the autoclave of FTO electro-conductive glass (100ml), baking oven is put into, 20h is reacted at 150 DEG C；
After C, reaction terminate, take out autoclave and rinsed with running water and be down to room temperature, take out with TiO2Nanometer rods
The FTO electro-conductive glass of array, with deionized water rinse for several times, product is dried naturally, that is, obtains TiO2Nanometer stick array.
D, weigh a certain amount of graphene (GR) and be dissolved in absolute ethyl alcohol, ultrasonic agitation 60min obtains 1mg/ml graphite
Alkene dispersion liquid；
E, with refiner by graphene dispersing solution with 800rpm rotating speed spin coating 60s to above-mentioned preparation TiO2Nanometer rods battle array
List face, dries 4h in 80 DEG C of baking ovens；
F, deionized water rinse 3 times, dry naturally, so as to obtain GR-TiO2Membranaceous nano composite structure.
Embodiment 3：
Prepare GR-TiO2Membranaceous compound, step is as follows：
A, by FTO electro-conductive glass successively with acetone, absolute ethyl alcohol, deionized water be cleaned by ultrasonic 20min, dry standby；
B, 30ml deionized waters and 30ml concentrated hydrochloric acids mixed, 1.0ml butyl titanates are added dropwise thereto while stirring, then
The mixed liquor is poured into and is placed with the autoclave of FTO electro-conductive glass (100ml), baking oven is put into, 20h is reacted at 150 DEG C；
After C, reaction terminate, take out autoclave and rinsed with running water and be down to room temperature, take out with TiO2Nanometer rods
The FTO electro-conductive glass of array, with deionized water rinse for several times, product is dried naturally, that is, obtains TiO2Nanometer stick array.
D, weigh a certain amount of graphene (GR) and be dissolved in absolute ethyl alcohol, ultrasonic agitation 60min obtains 1mg/ml graphite
Alkene dispersion liquid；
E, with refiner by graphene dispersing solution with 1000rpm rotating speed spin coating 60s to above-mentioned preparation TiO2Nanometer rods
Array surface, dries 6h in 80 DEG C of baking ovens；
F, deionized water rinse 3 times, dry naturally, so as to obtain GR-TiO2Membranaceous nano composite structure.
The present invention is with the GR-TiO prepared by embodiment 22Membranaceous compound carries out photocatalysis degradation organic contaminant experiment.
Table 1 is the concentration ratio of the t Rh B under simulated solar light irradiation.
GR-TiO2Application of the membranaceous compound in photocatalysis degradation organic contaminant, step is as follows：
A, prepare 5mg/L Rh B solutions it is standby；
B, the GR-TiO by preparation2Membranaceous compound is put into the self-control reactor equipped with 8ml Rh B solutions, first black
30min is adsorbed in dark situation to reach the attached balance of absorption-desorption, simulated solar light irradiation is then used；
C, the UV-2550 types ultraviolet-uisible spectrophotometer test not suction of Rh B solutions in the same time with Japanese Shimadzu Corporation
Luminosity.
The microscopic appearance of product is obtained by ESEM result, TiO2The microscopic appearance of nanometer stick array such as Fig. 1 (a) institutes
Show, GR-TiO2Shown in the microscopic appearance of membranaceous compound such as Fig. 1 (b), it can be seen that bar-shaped TiO2Surface covers one layer thoroughly
Bright GR films
In addition, the optical property of product is as shown in Figures 2 and 3, as a result show GR-TiO2Absorption of the membranaceous compound to light
Than pure TiO2By force.
Meanwhile, Rh B photocatalytic degradation situation is as shown in table 1 under simulated solar light irradiation, synchronization, GR-TiO2
Membranaceous compound can degrade more Rh B, illustrate GR-TiO2The photocatalysis performance of membranaceous compound is than pure TiO2By force.
Table 1
Claims (8)
1. a kind of TiO of graphene modified2The preparation method of membranaceous compound, it is characterised in that comprise the following steps：
A, TiO prepared on FTO electro-conductive glass by hydro-thermal method2Nanometer stick array：
(1) FTO electro-conductive glass is cleaned by ultrasonic 20-30min with acetone, absolute ethyl alcohol, deionized water successively, dried standby；
(2) by deionized water and concentrated hydrochloric acid by volume 1:1 mixing, is added dropwise butyl titanate, wherein metatitanic acid thereto while stirring
The volume ratio of butyl ester and above-mentioned mixed liquor is 0.5-0.8:50, then the mixed liquor is poured into the high pressure for being placed with FTO electro-conductive glass
In reactor (100ml), baking oven is put into, react 15-20h at 140-160 DEG C；
(3) after reaction terminates, take out autoclave and rinsed with running water and be down to room temperature, take out with TiO2Nanometer stick array
FTO electro-conductive glass, with deionized water rinse for several times, product is dried naturally, that is, obtains TiO2Nanometer stick array.
B, using spin-coating method in TiO2GR is loaded on nanometer stick array, GR-TiO is obtained2Membranaceous compound：
(1) weigh a certain amount of graphene (GR) to be dissolved in absolute ethyl alcohol, ultrasonic agitation 60min obtains graphene dispersing solution；
(2) graphene dispersing solution low speed is spun to the TiO of above-mentioned preparation with refiner2Nanometer stick array surface, does in an oven
It is dry；
(3) deionized water rinse 3 times, dry naturally, so as to obtain GR-TiO2Membranaceous nano composite structure.
2. GR-TiO according to claim 12The preparation method of membranaceous compound, it is characterised in that the FTO electro-conductive glass
Specification be 25mm × 25mm.
3. GR-TiO according to claim 12The preparation method of membranaceous compound, it is characterised in that FTO electro-conductive glass is with 0-
60 ° of inclination angle leans to polytetrafluoroethylene (PTFE) inwall, and conductive face-down.
4. GR-TiO according to claim 12The preparation method of membranaceous compound, it is characterised in that the graphene dispersing solution
Concentration be 0.5-1.5mg/ml.
5. GR-TiO according to claim 12The preparation method of membranaceous compound, it is characterised in that the spin coating method is specific
For graphene dispersing solution is added dropwise in dry TiO2On nanometer stick array, spin coating 50-80s under 500rpm-1000rpm low speed.
6. GR-TiO according to claim 12The preparation method of membranaceous compound, it is characterised in that the drying temperature is 80
DEG C, drying time is 6-8h.
7. GR-TiO as claimed in claim 12The GR-TiO that the preparation method of membranaceous compound is prepared2Membranaceous compound.
8. GR-TiO as claimed in claim 72Application of the membranaceous compound in photocatalysis degradation organic contaminant.
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| CN109887646A (en) * | 2019-03-08 | 2019-06-14 | 宁波石墨烯创新中心有限公司 | A kind of electrode and preparation method thereof |
| CN110465280A (en) * | 2019-09-11 | 2019-11-19 | 华北理工大学 | A kind of graphene-titanic oxide nanorod array composite material and preparation method and application |
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