CN108046238A - A kind of regulation and control method of the pore structure of carbon nanotubes membrane material - Google Patents
A kind of regulation and control method of the pore structure of carbon nanotubes membrane material Download PDFInfo
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- CN108046238A CN108046238A CN201711323448.7A CN201711323448A CN108046238A CN 108046238 A CN108046238 A CN 108046238A CN 201711323448 A CN201711323448 A CN 201711323448A CN 108046238 A CN108046238 A CN 108046238A
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- 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
- B01J13/00—Colloid chemistry, e.g. the production of colloidal materials or their solutions, not otherwise provided for; Making microcapsules or microballoons
- B01J13/0091—Preparation of aerogels, e.g. xerogels
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
- C09C1/00—Treatment of specific inorganic materials other than fibrous fillers; Preparation of carbon black
- C09C1/44—Carbon
Abstract
The present invention provides a kind of regulation and control methods of the pore structure of carbon nanotubes membrane material, are put into carbon nano-tube film in the mixed solution of leavening agent and compatilizer first, stand；After mixed solution penetrates into carbon nano-tube film inside, leavening agent, which decomposes, generates microbubble, generates micro-explosion effect so that the structure of carbon nano-tube film is gradually loose；At this point, the pore structure inside carbon nano-tube film can be adjusted；Then the carbon nano-tube film after the completion of regulation and control is freeze-dried, the carbon nano tube membrane structure after regulation and control is made to be maintained.The present invention can realize the regulation and control of carbon nano-tube film pore structure, 100 nanometers 10 microns of carbon nano-tube film average pore size modification scope.The carbon nano-tube film aggregate of the different pore size obtained, can be as nano particle and the framework material of fluoropolymer resin, can also be separately as multi-functional packing material or aerogel material.The method of the present invention is simple and practicable, at low cost, suitable for industrialization promotion.
Description
Technical field
The present invention relates to a kind of regulation and control methods of the pore structure of carbon nanotubes membrane material.
Background technology
Carbon nanotubes also known as Baji-tube, are a kind of One-dimensional Quantum materials with special carbon six-membered ring structure, radial dimension
For nanometer scale, axial dimension is micron dimension, has excellent mechanics, electrically and thermally performance.With nanometer technology
Development, the means such as applied chemistry vapour deposition process, by by carbon nano tube growth into aerogel structure, after being densified by solution
Obtain the carbon nanotubes Buckie paper or carbon nano-tube film of self-supporting.Carbon nano-tube film has self-supporting holey as a kind of
The carbon nanotube aggregate of structure not only inherits the superior function of single-root carbon nano-tube, but also with good electric property.
Carbon nano-tube film has macro-size, the processing being more suitable in follow-up use, in smart sensing material, artificial muscle and multi-functional
Field of compound material has application prospect.
But due to the hole inside carbon nano-tube film be nanoscale (100-400 nanometers), inorganic nanoparticles, graphite
Alkene and macromolecule resin can be hardly entered inside carbon nano-tube film, can not be realized effective functionalized design, be made carbon nano-tube film
Application obtained great limitation.Therefore, a kind of method for inventing pore structure for controlling carbon nano-tube film and porosity is non-
It is often necessary.
At present, scholar carries out the suspension prepared by carbon nanotube powder mostly by the way of sonic oscillation scattered tune
Control.However, the violent effect of sonic oscillation can make to have the carbon nano-tube film of self supporting structure to disintegrate, it can also make carbon nanometer in film
Pipe is damaged and hydraulic performance decline, so the method for traditional sonic oscillation can not be suitable for carbon nano-tube film internal void knot
The regulation and control of structure.
The content of the invention
The technical problem to be solved by the present invention is to how the pore structure of carbon nanotubes membrane material be regulated and controled.
In order to solve the above-mentioned technical problem, the technical scheme is that providing a kind of hole knot of carbon nanotubes membrane material
The regulation and control method of structure, it is characterised in that：, include the following steps：
Step 1：Carbon nano-tube film is put into the mixed solution of leavening agent and compatilizer, stood；When mixed solution penetrates into
Behind carbon nano-tube film inside, leavening agent, which decomposes, generates microbubble, generates micro-explosion effect so that the structure of carbon nano-tube film is gradual
It is loose；At this point, the pore structure inside carbon nano-tube film can be adjusted；
Step 2：Carbon nano-tube film after the completion of regulation and control is freeze-dried, avoids wicking-power in solvent evaporation process by carbon
The fluff structure of nanotube films destroys, and the carbon nano tube membrane structure after regulation and control is made to be maintained.
Preferably, in the step 1, the form of carbon nano-tube film is single-walled carbon nanotube, multi-walled carbon nanotube or list
The combination of wall carbon nano tube and multi-walled carbon nanotube；Carbon nano-tube film is the combination of conductor, semiconductor or conductor and semiconductor
Body.
Preferably, the preparation method of the carbon nano-tube film is floating catalytic chemical gas phase growth methods or carbon nano pipe array
Direct membrane method.
Preferably, in the step 1, compatilizer is the solution to dissolve each other with carbon nano-tube film；It is described mutual with carbon nano-tube film
Molten solution is ethanol solution, acetone soln or dichloromethane solution.
Preferably, in the step 1, leavening agent for mass percent concentration 10%~60% hydrogenperoxide steam generator or
The dilution heat of sulfuric acid of mass percent concentration 10% and the mixed liquor of metallic zinc powder；Or dilute nitre of mass percent concentration 10%
The mixed liquor of acid solution and sodium sulfite.
Preferably, in the step 1, after the short texture of carbon nano-tube film, the regulation and control model in aperture inside carbon nano-tube film
It encloses for 100 nanometers~10 microns.
Preferably, in the step 1, by being matched to mixed solution, the adjusting of concentration, action time and temperature, realize
Regulation and control to the pore structure inside carbon nano-tube film.
Preferably, in the step 1, compatilizer contributes into inside carbon nano-tube film；Leavening agent is used to generate micro- gas
Bubble；Therefore the mixed solution of compatilizer and leavening agent can enter inside carbon nano-tube film and generate microbubble, realize carbon nanometer
The hole regulation and control of periosteum, Neither of the two can be dispensed for compatilizer and leavening agent.
Preferably, in the step 2, the specific method of freeze-drying is：Carbon nano-tube film after the completion of regulation and control is put into
In glacial acetic acid or dimethyl sulfoxide (DMSO), when freezing 3~12 is small under -10 DEG C~-80 DEG C environment, freeze drying box is subsequently placed into
It is interior, -10 DEG C~-40 DEG C of temperature setting range, when drying 12~72 is small.
Preferably, in the step 2, by freeze-drying effectively keep regulation and control after the completion of carbon nano-tube film it is loose
Structure makes it not cave in, shrink and destroy due to during drying because the wicking-power effect that solution evaporation generates.
Compared with prior art, the present invention has the advantages that：
1st, the present invention can realize the regulation and control of carbon nanotubes membrane material pore structure, carbon nano-tube film average pore size regulation and control model
Enclose 100 nanometers -10 microns.
2nd, the carbon nano-tube film aggregate of different pore size produced by the present invention can be used as multi-functional packing material or gas
Gel rubber material.
3rd, the carbon nanometer film produced by the present invention with different pore size can be compound with nano particle or fluoropolymer resin, makees
For nano particle and the framework material of fluoropolymer resin, the Functional Design of carbon nano-tube film is realized.
4th, the method for the present invention is simple and practicable, at low cost, suitable for industrialization promotion.
Specific embodiment
With reference to specific embodiment, the present invention is further explained.It is as described below, it is only presently preferred embodiments of the present invention,
Not to the present invention in any form with substantial limitation, it is noted that for those skilled in the art,
On the premise of not departing from the method for the present invention, several improvement and supplement can be also made, these are improved and supplement also should be regarded as this
The protection domain of invention.All those skilled in the art, without departing from the spirit and scope of the present invention, when can
The equivalent variations for a little variation, modification and evolution made using disclosed above technology contents, be the present invention etc.
Imitate embodiment；Meanwhile change, the modification of any equivalent variations that all substantial technologicals according to the invention make above-described embodiment
With differentiation, in the range of still falling within technical scheme.
Embodiment 1
Prepare carbon nanotube aerogel material
(1) selection Length x Width is 5 centimetres, (victory enlightening nano material in Suzhou is limited for the carbon nano-tube film of 15 microns of thickness
Company), the average pore in carbon nano-tube film is 200 nanometers -400 nanometers.
(2) hydrogenperoxide steam generator that 300 milliliters of concentration are 50% is mixed with the ethanol solution of 300 milliliters of concentration 99%,
It pours into glass dish.
(3) carbon nano-tube film is put into the mixed solution that step 2 configures, is impregnated in the environment for being 45 degrees Celsius in temperature
24 it is small when, obtain containing a large amount of holes carbon nanotube aerogel (about 3 centimetres of thickness).
(4) by the carbon nanotube aerogel obtained in step 3, carefully film taking-up is put into 400 milliliters of ice from plastic disc
In acetic acid, be put under -80 degrees Celsius of low temperature environment freezing 3 it is small when, treat that solution is completely solidified into solid-state.
(5) using freeze-drying, when vacuum drying 72 is small under -10 degrees Celsius, the gap structure of carbon nano-tube yarn is made
It is maintained, is prepared into the carbon nanotube aerogel material that thickness is 3 centimetres or so, hole is micro- for 6-10 in the aerogel material
Rice, can be used for multi-functional conductive filling material.
The present embodiment by using the mixed solution of hydrogen peroxide processing method, using generating micro-molecular gas in solution
Micro-explosion effect, make carbon nano tube membrane structure gradually loose, internal voids become larger.By freeze-drying by carbon nano-tube film
Dry at low ambient temperatures, make it is fluffy after structure be maintained, so as to fulfill the tune of the pore structure to kind of carbon nano-tube film
Control.
Embodiment 2
Prepare the carbon nano-tube film that average pore is 2 microns
(1) it is 5 centimetres that selection is long and wide, (victory enlightening nano material in Suzhou is limited for the carbon nano-tube film of about 15 microns of thickness
Company), it is 200 nanometers -400 nanometers to measure the average pore between carbon nanotubes.
(2) prepare the dilute nitric acid solution of 200 milliliters of weight ratios 10% and the mixed liquor of sodium sulfite, and with 100 milliliter third
Ketone solution mixes, and pours into glass dish.
(3) carbon nano-tube film is put into the mixed solution that step 2 configures, is soaked in the environment for being 35 degrees Celsius in temperature
Bubble, 32 it is small when, obtain the fluffy carbon nano-tube film of macroporous structure.
(4) carbon nano-tube film obtained in step 3 taking-up is put into 300 milliliters of glacial acetic acid, is put into -25 degrees Celsius
When freezing 6 is small under low temperature environment, treat that solution is completely solidified into solid-state.
(5) using freeze-drying, when vacuum drying 36 is small under -40 degrees Celsius, the gap structure of carbon nano-tube yarn is made
It is maintained, realizes the hole regulation and control inside carbon nano-tube film.
After tested to treated 1.8-2.4 micron of carbon nano-tube film internal void, average pore is 2.1 microns, this
Carbon nano-tube film can be used for the framework material of inorganic nanoparticles doping.
Embodiment 3
The fast preparation method of the carbon nanotubes membrane material of 1 micron of average pore
(1) selection Length x Width is 5 centimetres, (victory enlightening nano material in Suzhou is limited for the carbon nano-tube film of 15 microns of thickness
Company), it is 200 nanometers -400 nanometers to measure the average pore between carbon nanotubes.
(2) prepare the mixed liquor of 200 milliliter 10% of dilution heat of sulfuric acid and metallic zinc powder, and with 150 milliliters of dichloromethanes
Alkane solution mixes, and pours into glass dish.
(3) carbon nano-tube film is put into the mixed solution that step 2 configures, is impregnated in the environment for being 55 degrees Celsius in temperature
3 it is small when, obtain the fluffy carbon nano-tube film of macroporous structure.
(4) carbon nano-tube film obtained in step 3 taking-up is put into 300 milliliters of glacial acetic acid, is put into -80 degrees Celsius
When freezing 3 is small under low temperature environment, treat that solution is completely solidified into solid-state.
(5) using freeze-drying, when vacuum drying 12 is small under -10 degrees Celsius, the gap structure of carbon nano-tube yarn is made
It is maintained, realizes the hole regulation and control inside carbon nano-tube film.
After tested to treated 0.8-1.5 micron of carbon nano-tube film internal void, which can be used for high
The reinforcement material of performance composite material.
Claims (10)
- A kind of 1. regulation and control method of the pore structure of carbon nanotubes membrane material, which is characterized in that include the following steps：Step 1：Carbon nano-tube film is put into the mixed solution of leavening agent and compatilizer, stood；It is received when mixed solution penetrates into carbon Behind mitron film inside, leavening agent, which decomposes, generates microbubble, generates micro-explosion effect so that the structure of carbon nano-tube film is gradually dredged Pine；At this point, the pore structure inside carbon nano-tube film can be adjusted；Step 2：Carbon nano-tube film after the completion of regulation and control is freeze-dried, the carbon nano tube membrane structure after regulation and control is made to be maintained.
- 2. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, the form of carbon nano-tube film is received for single-walled carbon nanotube, multi-walled carbon nanotube or single-walled carbon nanotube and multi wall carbon The combination of mitron；Carbon nano-tube film is conductor, semiconductor or conductor and the assembly of semiconductor.
- 3. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described The preparation method of carbon nano-tube film is floating catalytic chemical gas phase growth methods or the direct membrane method of carbon nano pipe array.
- 4. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, compatilizer is the solution to dissolve each other with carbon nano-tube film；The solution to dissolve each other with carbon nano-tube film is ethanol solution, Acetone soln or dichloromethane solution.
- 5. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, leavening agent is the hydrogenperoxide steam generator of mass percent concentration 10%~60% or mass percent concentration 10% The mixed liquor of dilution heat of sulfuric acid and metallic zinc powder；Or mass percent concentration 10% dilute nitric acid solution and sodium sulfite it is mixed Close liquid.
- 6. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, after the short texture of carbon nano-tube film, the modification scope in aperture is 100 nanometers~10 microns inside carbon nano-tube film.
- 7. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, by being matched to mixed solution, the adjusting of concentration, action time and temperature, realize to the hole inside carbon nano-tube film The regulation and control of gap structure.
- 8. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 1, compatilizer contributes into inside carbon nano-tube film；Leavening agent is used to generate microbubble；Therefore compatilizer and bulk The mixed solution of agent can enter inside carbon nano-tube film and generate microbubble, realize the hole regulation and control of carbon nano-tube film, compatible Neither of the two can be dispensed for agent and leavening agent.
- 9. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：It is described In step 2, the specific method of freeze-drying is：Carbon nano-tube film after the completion of regulation and control is put into glacial acetic acid or dimethyl sulfoxide (DMSO) In, when freezing 3~12 is small under -10 DEG C~-80 DEG C environment, it is subsequently placed into freeze drying box, -10 DEG C of temperature setting range ~-40 DEG C, when drying 12~72 is small.
- 10. a kind of regulation and control method of the pore structure of carbon nanotubes membrane material as described in claim 1, it is characterised in that：Institute It states in step 2, the open structure of the carbon nano-tube film after the completion of effectively keeping by freeze-drying, makes it will not be dry It caves in, shrink and destroys due to the wicking-power effect that solution evaporation generates in dry process.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109810499A (en) * | 2019-01-29 | 2019-05-28 | 上海交通大学 | A kind of preparation method of nylon/carbon nanotube aerogel |
| CN110635135A (en) * | 2019-09-11 | 2019-12-31 | 北京航空航天大学 | Conductive paste and preparation method thereof |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101271079A (en) * | 2008-05-07 | 2008-09-24 | 天津大学 | Glass carbon electrode decorated by carbon nano tube-DNA complex and its production method and application |
| CN101417257A (en) * | 2007-10-26 | 2009-04-29 | 中国科学院沈阳自动化研究所 | Single-wall carbon nano tube and multi-wall carbon nano tube separation method |
| CN101760806A (en) * | 2008-12-26 | 2010-06-30 | 黑龙江大学 | Polymer/carbon nano tube nano fiber material and preparation method and application thereof |
| CN104418316A (en) * | 2013-08-27 | 2015-03-18 | 清华大学 | Carbon nanotube sponge body and preparation method thereof |
-
2017
- 2017-12-12 CN CN201711323448.7A patent/CN108046238A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101417257A (en) * | 2007-10-26 | 2009-04-29 | 中国科学院沈阳自动化研究所 | Single-wall carbon nano tube and multi-wall carbon nano tube separation method |
| CN101271079A (en) * | 2008-05-07 | 2008-09-24 | 天津大学 | Glass carbon electrode decorated by carbon nano tube-DNA complex and its production method and application |
| CN101760806A (en) * | 2008-12-26 | 2010-06-30 | 黑龙江大学 | Polymer/carbon nano tube nano fiber material and preparation method and application thereof |
| CN104418316A (en) * | 2013-08-27 | 2015-03-18 | 清华大学 | Carbon nanotube sponge body and preparation method thereof |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109810499A (en) * | 2019-01-29 | 2019-05-28 | 上海交通大学 | A kind of preparation method of nylon/carbon nanotube aerogel |
| CN109810499B (en) * | 2019-01-29 | 2021-11-09 | 上海交通大学 | Preparation method of nylon/carbon nanotube aerogel |
| CN110635135A (en) * | 2019-09-11 | 2019-12-31 | 北京航空航天大学 | Conductive paste and preparation method thereof |
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Application publication date: 20180518 |