CN102432088A - Method for preparing carbon nanometer tube/graphene three-dimensional nanometer structure capacitance desalination electrode - Google Patents
Method for preparing carbon nanometer tube/graphene three-dimensional nanometer structure capacitance desalination electrode Download PDFInfo
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- CN102432088A CN102432088A CN2011102576040A CN201110257604A CN102432088A CN 102432088 A CN102432088 A CN 102432088A CN 2011102576040 A CN2011102576040 A CN 2011102576040A CN 201110257604 A CN201110257604 A CN 201110257604A CN 102432088 A CN102432088 A CN 102432088A
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 161
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 57
- 238000010612 desalination reaction Methods 0.000 title claims abstract description 32
- 238000000034 method Methods 0.000 title abstract description 14
- 229910052799 carbon Inorganic materials 0.000 title abstract description 11
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 43
- 239000010439 graphite Substances 0.000 claims abstract description 43
- 238000002360 preparation method Methods 0.000 claims abstract description 17
- 239000000839 emulsion Substances 0.000 claims abstract description 6
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims abstract description 6
- 239000002041 carbon nanotube Substances 0.000 claims description 53
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 53
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 17
- 239000003990 capacitor Substances 0.000 claims description 11
- 238000001035 drying Methods 0.000 claims description 10
- 239000012286 potassium permanganate Substances 0.000 claims description 10
- 238000003756 stirring Methods 0.000 claims description 10
- 238000005406 washing Methods 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 8
- 238000009413 insulation Methods 0.000 claims description 7
- 238000013019 agitation Methods 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 claims description 5
- 238000010790 dilution Methods 0.000 claims description 5
- 239000012895 dilution Substances 0.000 claims description 5
- 239000012065 filter cake Substances 0.000 claims description 5
- 238000001914 filtration Methods 0.000 claims description 5
- 239000005457 ice water Substances 0.000 claims description 5
- 239000011159 matrix material Substances 0.000 claims description 5
- 238000002156 mixing Methods 0.000 claims description 5
- 230000007935 neutral effect Effects 0.000 claims description 5
- 239000008367 deionised water Substances 0.000 claims description 4
- 229910021641 deionized water Inorganic materials 0.000 claims description 4
- 239000002048 multi walled nanotube Substances 0.000 claims description 4
- 239000007772 electrode material Substances 0.000 claims description 2
- 238000002791 soaking Methods 0.000 claims description 2
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims 1
- 150000001875 compounds Chemical class 0.000 abstract description 10
- 239000007788 liquid Substances 0.000 abstract description 3
- 239000000463 material Substances 0.000 abstract 2
- -1 polytetrafluoroethylene Polymers 0.000 abstract 1
- 239000004810 polytetrafluoroethylene Substances 0.000 abstract 1
- 238000011033 desalting Methods 0.000 description 23
- 238000005265 energy consumption Methods 0.000 description 7
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 6
- 239000008151 electrolyte solution Substances 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 239000002071 nanotube Substances 0.000 description 3
- 239000012266 salt solution Substances 0.000 description 3
- 239000013535 sea water Substances 0.000 description 3
- 239000011780 sodium chloride Substances 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 239000003643 water by type Substances 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 2
- 230000002776 aggregation Effects 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 238000002242 deionisation method Methods 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 238000004821 distillation Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 241000446313 Lamella Species 0.000 description 1
- 240000007594 Oryza sativa Species 0.000 description 1
- 235000007164 Oryza sativa Nutrition 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 235000005770 birds nest Nutrition 0.000 description 1
- 230000001413 cellular effect Effects 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000021615 conjugation Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 230000002068 genetic effect Effects 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000009335 monocropping Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 238000001223 reverse osmosis Methods 0.000 description 1
- 235000009566 rice Nutrition 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000002109 single walled nanotube Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 235000005765 wild carrot Nutrition 0.000 description 1
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- Carbon And Carbon Compounds (AREA)
Abstract
The invention relates to a method for preparing a carbon nanometer tube/graphene three-dimensional nanometer structure capacitance desalination electrode, which belongs to the field of the capacitance desalination electrode preparation. The method comprises the following steps that: firstly, graphite oxide/carbon nanometer tube high-stability dispersing liquid is obtained, and the graphite oxide/carbon nanometer tube compounds are fast peeled at a low temperature to obtain carbon nanometer tube/graphene three-dimensional nanometer compound materials. The carbon nanometer tube/graphene three-dimensional nanometer compound materials and polytetrafluoroethylene emulsion are uniformly mixed and coated on graphite paper, the carbon nanometer tube/graphene three-dimensional nanometer structure capacitance desalination electrode is prepared after being baked. The method has the advantages that the temperature is low, simplicity is realized, and the operation is easy. The obtained carbon nanometer tube/graphene three-dimensional nanometer structure capacitance desalination electrode has good conductivity and better desalination performance, and potential prospects are realized in the capacitance desalination aspect.
Description
Technical field
The present invention relates to the preparation method of a kind of carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode, the desalination electrode of the present invention's preparation has efficiently, the desalting performance of less energy-consumption.Belong to electric desalting electrode manufacturing process technical field.The present invention can be used to can be applicable to the desalination of seawater and bitter alkali water, worker, agriculture prodn and domestic water (underground water) softening.
Background technology
Water resources crisis is one of maximum resource crisis that this century, the whole world faced, and seawater and brackish water desalting are the important channels that solves this crisis.Existing desalting method mainly contains distillation method and embrane method.The distillation method service temperature is high, and energy consumption is bigger; Bird nest harm and seriously corroded; Embrane method is strict to film properties, film spoilage height and expensive.In addition, all there is the high shortcoming of energy consumption in these desalting method, even if consume energy minimum reverse osmosis membrane, its energy consumption also is about ten times of theoretical value.Therefore, the research and development desalting technology application prospect that energy consumption is low, cost is low is very bright.The capacitor type desalination process be a kind of based on electric double layer capacitance away from brand-new desalting technology.This method energy consumption is low, desalting efficiency is high, and is environmentally friendly.Can be applicable to the aspect such as softening of desalination and worker, agriculture prodn and the domestic water of seawater and brackish water, its development space with have a extensive future.
Graphene is the elementary cell that constitutes graphite as a kind of carbon material of emerging bi-dimensional cellular shape structure.It has the electrochemical window of good electrical conductivity, broad, high chemical stability, and bigger specific surface area.Though the theoretical specific surface area of Graphene is very big, because stronger Van der Waals force between sheet and the sheet, phenomenons such as lamination between easy genetic horizon and the layer and reunion make the Graphene specific surface area reduce greatly, thereby have reduced desalting performance.People such as Pan (L i H.B; Zou L.D. Lu T A comparative study on electrosorptive behavior of carbon nanotubes and graphene for capacitive deionization Journal of Electroanalytical Chemistry 653 (2011) 40 – 44) prepared Graphene desalination electrode; Its Graphene serious agglomeration, specific surface area has only 77 m
2/ g, desalting performance is relatively poor.People such as Zou (L i H.B; Zou L.D. Pan L.K. Novel Graphene-Like Electrodes for Capacitive Deionization Environ. Sci. Technol. 2010; 44; 8692 – 8697) prepare Graphene desalination electrode and reunited more seriously, reduced its desalting performance.Therefore, how solving the reunion of Graphene, improve its effective ratio area, increase nano pore, strengthen its desalting performance, is a challenging job.
Summary of the invention
The objective of the invention is to overcome the shortcoming of Graphene electrodes; The carbon nanotube of high-specific surface area, high conductivity is inserted between graphene layer; Make carbon nanotube be grafted on the Graphene surface; Make to be separated from each other out between graphene layer and the layer, prevent the Graphene reunion, to reach the purpose that improves the Graphene specific surface area.Can play bridge linking effect in the middle of carbon nanotube embeds Graphene separated from one another is coupled together, form three-dimensional conductive network structure, can introduce more Donna rice duct simultaneously, help ion diffusion, can improve desalting performance greatly.The carbon nanotube of special hollow structure, satisfactory electrical conductivity, low-resistivity is introduced preparation a kind of novel carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode between graphene layer, have good electrical conductivity and desalting performance preferably.
The objective of the invention is to reach through following technique means and measure.
The present invention also provides a kind of carbon nanotube/Graphene three-dimensional manometer complex capacitance type desalination electrode and preparation method thereof, may further comprise the steps:
(1) preparation of electrode materials: under the ice-water bath condition, graphite is under agitation slowly joined in the vitriol oil of massfraction 98%, slowly add potassium permanganate again, its graphite: the vitriol oil: the mass ratio of potassium permanganate is 1:40～100:2 ~ 8, at 32-38
oIn the C water bath with thermostatic control, stir insulation 1-6 h down, after reaction finishes, slowly add the deionized water dilution, stir several minutes, press graphite: H
2O
2Mass ratio be the H that 1:7 ~ 10 adds massfractions 30%
2O
2, leave standstill after-filtration, the thorough washing filter cake, washing is to neutral, and drying obtains graphite oxide under the room temperature; By graphite oxide: the mass ratio of carbon nanotube is 99:1～4:1, and graphite oxide and carbon nanotube ultra-sonic dispersion in deionized water, after being uniformly dispersed, are detached drying; The mixture of above-mentioned gained is placed pre-warmed tube furnace, and insulation for some time can obtain carbon nanotube/Graphene three-dimensional manometer matrix material.
(2) preparation of carbon nanotube/Graphene three-dimensional manometer complex capacitance type desalination electrode: the adding massfraction is that the ptfe emulsion of 5-15% is a sticker in the carbon nanotube/Graphene of step (1) gained; Be applied to after mixing on the Graphite Electrodes paper, subsequently at 100-110
oThe C oven dry is spent the night, and finally makes the compound desalination electrode of carbon nanotube/Graphene.
Above-mentioned graphite oxide Graphene/even carbon nanotube dispersion liquid; This dispersion liquid can be stablized more than the week; Explain that carbon nanotube fully is inserted in the graphite oxide, graphite oxide and carbon nanotube combine through П-П conjugation, and graphite oxide and nanotube can reach nano level to be disperseed; Increase the dispersiveness of carbon nanotube in water, helped the preparation of electrode.
Above-mentioned pre-warmed silica tube is 200-500
oC, soaking time is 5-20 min, low temperature of the present invention can make carbon nanotube/graphite oxide body volume rapid expansion peel off.The oxidized burning of carbon material when the too high inert-free gas of temperature is protected is crossed to hang down and can not be played the effect of peeling off fast.
Above-mentioned carbon nanotube is many walls nanotube, and diameter is 5-50 nm.Agglomeration is stronger between the single-walled nanotube, and the reactive force between nanotube and the Graphene is more weak can't to be disperseed it, and SWCN can not be separated the Graphene lamella.
Above-mentioned graphite oxide: when the mass ratio of carbon nanotube was 99:1～4:1, the gained Graphene was separated from each other, and contacting between carbon nanotube and the Graphene is better; Playing the conducting bridge continuous cropping uses; The electrode nano pore structure increases, and make salt ion can pass in and out electrode interior more fast, and internal resistance is less; Electroconductibility is better, and desalting performance is preferable; Along with the increase of content of carbon nanotubes, the sheet structure of Graphene is easy to surrounded by carbon nanotube, has caused the internal resistance of electrode to begin to increase, and reduces its desalting performance.
It is simple that the present invention prepares process, and energy consumption is little, easy handling.The prepared carbon nanotube of the inventive method/Graphene three-dimensional manometer combined electrode has good electrical conductivity and desalting performance preferably, is having the potential application prospect aspect the capacitor type desalination.
Embodiment
After specific embodiment of the present invention being described at present.
Embodiment 1
Under the ice-water bath condition, 3 g graphite are under agitation slowly joined in the vitriol oil of 120 mL massfractions 98%, slowly add 14 g potassium permanganate again, its graphite: the vitriol oil: the mass ratio of potassium permanganate is 1:40:4.7,35
oIn the C water bath with thermostatic control, stir insulation 2 h down, after reaction finishes, slowly add the dilution of 500 mL deionized waters, stir several minutes, press graphite: H
2O
2Mass ratio be the H that 1:7.5 adds 22.5 mL massfractions 30%
2O
2, leave standstill after-filtration, the thorough washing filter cake, washing is to neutral, and drying obtains graphite oxide under the room temperature.With the multi-walled carbon nano-tubes of about 10 ~ 30 nm of diameter, press graphite oxide: carbon nanotube mass ratio 9:1, mix ultrasonic 2 h, after being uniformly dispersed, detach drying.The mixture of above-mentioned gained placed preheat to 300
oIn the tube furnace of C, be incubated 10 min, can obtain carbon nanotube/Graphene three-dimensional manometer matrix material.With adding massfraction in the carbon nanotube/Graphene of gained is that 10% ptfe emulsion is a sticker, is applied to after mixing on the Graphite Electrodes paper, subsequently at 100-110
oThe C oven dry is spent the night.Finally make the compound desalination electrode of carbon nanotube/Graphene.
Test the ratio electric capacity of the compound desalination electrode of above-mentioned carbon nanotube/Graphene.Use CHI 660D type electrochemical workstation, electrolytic solution is 0.5 M NaCl solution, and scanning speed is 5 mv; Voltage range is-0.4-0.6 V; The specific capacitance that records this electrode is 216.6 F/g.Its desalting performance of the electrode test of above-mentioned preparation, in the salt solution of 1000 mg/L, two ends apply the voltage of 2.0 V, and its desalting efficiency is greater than 80%.
Embodiment 2
Under the ice-water bath condition, 3 g graphite are under agitation slowly joined in the vitriol oil of 150 mL massfractions 98%, slowly add 21 g potassium permanganate again, its graphite: the vitriol oil: the mass ratio of potassium permanganate is 1:50:7,35
oIn the C water bath with thermostatic control, stir insulation 3 h down, after reaction finishes, slowly add the dilution of 500 mL deionized waters, stir several minutes, press graphite: H
2O
2Mass ratio be the H that 1:8.3 adds 25 mL massfractions 30%
2O
2, leave standstill after-filtration, the thorough washing filter cake, washing is to neutral, and drying obtains graphite oxide under the room temperature.Diameter is about the multi-walled carbon nano-tubes of 20 ~ 40 nm, presses graphite oxide: carbon nanotube mass ratio 17:3, mix ultrasonic 1.5 h, after being uniformly dispersed, detach drying.The mixture of above-mentioned gained placed preheat to 200
oIn the tube furnace of C, be incubated 8 min, can obtain carbon nanotube/Graphene three-dimensional manometer matrix material.With adding massfraction in the carbon nanotube/Graphene of gained is that 8% ptfe emulsion is a sticker, is applied to after mixing on the Graphite Electrodes paper, subsequently at 100-110
oThe C oven dry is spent the night.Finally make the compound desalination electrode of carbon nanotube/Graphene.
Test the ratio electric capacity of the compound desalination electrode of above-mentioned carbon nanotube/Graphene.Use CHI 660D type electrochemical workstation, electrolytic solution is 0.5 M NaCl solution, and scanning speed is 10 mv; Voltage range is-0.4-0.6 V; The specific capacitance that records this electrode is 100 F/g.Its desalting performance of the electrode test of above-mentioned preparation, in the salt solution of 1200 mg/L, two ends apply the voltage of 2.0 V, and its desalting efficiency is greater than 70%.
Embodiment 3
Under the ice-water bath condition, 4 g graphite are under agitation slowly joined in the vitriol oil of 240 mL massfractions 98%, slowly add 24g potassium permanganate again, its graphite: the vitriol oil: the mass ratio of potassium permanganate is 1:60:6,35
oIn the C water bath with thermostatic control, stir insulation 2 h down, after reaction finishes, slowly add the dilution of 500 mL deionized waters, stir several minutes, press graphite: H
2O
2Mass ratio be the H that 1:9 adds 36 mL massfractions 30%
2O
2, leave standstill after-filtration, the thorough washing filter cake, washing is to neutral, and drying obtains graphite oxide under the room temperature.Diameter is about the multi-walled carbon nano-tubes of 30 ~ 50 nm, presses graphite oxide: carbon nanotube mass ratio 19:1, mix ultrasonic 1.5 h, after being uniformly dispersed, detach drying.The mixture of above-mentioned gained placed preheat to 300
oIn the tube furnace of C, be incubated 10 min, can obtain carbon nanotube/Graphene three-dimensional manometer matrix material.With adding massfraction in the carbon nanotube/Graphene of gained is that 12% ptfe emulsion is a sticker, is applied to after mixing on the Graphite Electrodes paper, subsequently at 100-110
oThe C oven dry is spent the night.Finally make the compound desalination electrode of carbon nanotube/Graphene.
Test the ratio electric capacity of the compound desalination electrode of above-mentioned carbon nanotube/Graphene.Use CHI 660D type electrochemical workstation, electrolytic solution is 0.5 M NaCl solution, and scanning speed is 10 mv; Voltage range is-0.4-0.6V; The specific capacitance that records this electrode is 114.6 F/g.Its desalting performance of the electrode test of above-mentioned preparation, in the salt solution of 500 mg/L, two ends apply the voltage of 2.0 V, and its desalting efficiency is greater than 90%.
Claims (3)
1. the preparation method of carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode is characterized in that may further comprise the steps:
(1) preparation of electrode materials: under the ice-water bath condition, graphite is under agitation slowly joined in massfraction 98% vitriol oil, slowly add potassium permanganate, wherein graphite again: the vitriol oil: the mass ratio of potassium permanganate is 1:40～100:2 ~ 8, at 32-38
oIn the C water bath with thermostatic control, stir insulation 1-6 h down, after reaction finishes, slowly add the deionized water dilution, stir several minutes, press graphite: H
2O
2Mass ratio be the H that 1:7 ~ 10 adds massfractions 30%
2O
2, leave standstill after-filtration, the thorough washing filter cake, washing is to neutral, and drying obtains graphite oxide under the room temperature; By graphite oxide: the mass ratio of carbon nanotube is 99:1～4:1, and graphite oxide and carbon nanotube ultra-sonic dispersion in deionized water, after being uniformly dispersed, are detached drying; The mixture of above-mentioned gained is placed pre-warmed tube furnace, and insulation for some time can obtain carbon nanotube/Graphene three-dimensional manometer matrix material;
(2) preparation of carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode: the adding massfraction is that the ptfe emulsion of 5-15% is a sticker in the carbon nanotube/Graphene of step (1) gained; Be applied to after mixing on the Graphite Electrodes paper, subsequently at 100-110
oThe C oven dry is spent the night, and makes carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode.
2. the preparation method of carbon nanotube according to claim 1/Graphene 3-D nano, structure capacitor type desalination electrode is characterized in that carbon nanotube/graphite oxide pre-heating temperature is 200-500
oC, soaking time is 5-20 min.
3. the preparation method of carbon nanotube according to claim 1/Graphene 3-D nano, structure capacitor type desalination electrode; It is characterized in that carbon nanotube is a multi-walled carbon nano-tubes in this carbon nanotube/Graphene 3-D nano, structure capacitor type desalination electrode, diameter is 5-50 nm.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103626172A (en) * | 2013-11-29 | 2014-03-12 | 上海利物盛企业集团有限公司 | Method for preparing graphite paper with high thermal conductivity |
| CN103794379A (en) * | 2012-11-02 | 2014-05-14 | 海洋王照明科技股份有限公司 | Graphene/carbon nano-tube composite material, and preparation method and application thereof |
| CN104140144A (en) * | 2014-08-03 | 2014-11-12 | 大连理工大学 | Preparation method and application of graphene oxide liquid crystal emulsion |
| CN105129927A (en) * | 2015-09-10 | 2015-12-09 | 上海大学 | Preparing method of graphene/carbon nanotube aerogel composite capacitive type desalting electrode |
| CN105461022A (en) * | 2014-09-12 | 2016-04-06 | 南京大学 | Flake graphite doped binary carbon material composite electrode, and preparation thereof, and applications of flake graphite doped binary carbon material composite electrode in electroadsorption desalination |
| CN107089707A (en) * | 2017-03-20 | 2017-08-25 | 上海大学 | Structure capacitance desalination electrode core shell structure three-dimensional graphene composite material and preparation method thereof |
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| US20050026012A1 (en) * | 2003-07-28 | 2005-02-03 | O'hara Jeanette E. | Diffusion media tailored to account for variations in operating humidity and devices incorporating the same |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103794379A (en) * | 2012-11-02 | 2014-05-14 | 海洋王照明科技股份有限公司 | Graphene/carbon nano-tube composite material, and preparation method and application thereof |
| CN103626172A (en) * | 2013-11-29 | 2014-03-12 | 上海利物盛企业集团有限公司 | Method for preparing graphite paper with high thermal conductivity |
| CN104140144A (en) * | 2014-08-03 | 2014-11-12 | 大连理工大学 | Preparation method and application of graphene oxide liquid crystal emulsion |
| CN104140144B (en) * | 2014-08-03 | 2015-10-28 | 大连理工大学 | A kind of preparation method of the desalination graphene oxide crystalline emulsion that flows |
| CN105461022A (en) * | 2014-09-12 | 2016-04-06 | 南京大学 | Flake graphite doped binary carbon material composite electrode, and preparation thereof, and applications of flake graphite doped binary carbon material composite electrode in electroadsorption desalination |
| CN105129927A (en) * | 2015-09-10 | 2015-12-09 | 上海大学 | Preparing method of graphene/carbon nanotube aerogel composite capacitive type desalting electrode |
| CN105129927B (en) * | 2015-09-10 | 2017-08-11 | 上海大学 | The preparation method of graphene/carbon nano-tube aeroge composite capacitance-type desalting electrode |
| CN107089707A (en) * | 2017-03-20 | 2017-08-25 | 上海大学 | Structure capacitance desalination electrode core shell structure three-dimensional graphene composite material and preparation method thereof |
| CN107089707B (en) * | 2017-03-20 | 2021-08-10 | 上海大学 | Core-shell structure three-dimensional graphene composite material for capacitive desalination electrode and preparation method thereof |
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| CN102432088B (en) | 2013-03-06 |
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