CN107879759A - A kind of preparation method of alundum (Al2O3)/tin ash composite ceramic film - Google Patents
A kind of preparation method of alundum (Al2O3)/tin ash composite ceramic film Download PDFInfo
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- CN107879759A CN107879759A CN201610866982.1A CN201610866982A CN107879759A CN 107879759 A CN107879759 A CN 107879759A CN 201610866982 A CN201610866982 A CN 201610866982A CN 107879759 A CN107879759 A CN 107879759A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D67/00—Processes specially adapted for manufacturing semi-permeable membranes for separation processes or apparatus
- B01D67/0039—Inorganic membrane manufacture
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/12—Composite membranes; Ultra-thin membranes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/02—Inorganic material
- B01D71/024—Oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/02—Inorganic material
- B01D71/024—Oxides
- B01D71/025—Aluminium oxide
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/10—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on aluminium oxide
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/453—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zinc, tin, or bismuth oxides or solid solutions thereof with other oxides, e.g. zincates, stannates or bismuthates
- C04B35/457—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zinc, tin, or bismuth oxides or solid solutions thereof with other oxides, e.g. zincates, stannates or bismuthates based on tin oxides or stannates
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B38/00—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof
- C04B38/0045—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof by a process involving the formation of a sol or a gel, e.g. sol-gel or precipitation processes
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3293—Tin oxides, stannates or oxide forming salts thereof, e.g. indium tin oxide [ITO]
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- Engineering & Computer Science (AREA)
- Ceramic Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Inorganic Chemistry (AREA)
- Manufacturing & Machinery (AREA)
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Abstract
The invention discloses a kind of preparation method of alundum (Al2O3)/tin ash composite ceramic film, boehmite sol is made it is characterized in that being dissolved in using alundum (Al2O3) predecessor in the solvent of certain volume, five water crystallization stannic chlorides, which are dissolved in the solvent of certain volume, is made tin ash colloidal sol, the polyvinyl alcohol of certain volume fraction is added after both mixing, it is well mixed to obtain after coating liquid the film on ceramic matrix, obtain composite ceramic film through drying, sintering.Composite ceramics membrane aperture prepared by the present invention is good, voidage is high, acid-alkali-corrosive-resisting, membrane flux are high, and actual desalting effect is notable.
Description
Technical field
The invention belongs to ceramic field of membrane preparation, the system of specifically a kind of alundum (Al2O3)/tin ash composite ceramic film
Preparation Method.
Background technology
In recent years, because the critical shortage of China's water resource stock, pollution are on the rise, desalinization, which is used as, solves this
The effective technology of problem is increasingly subject to the strong interest of domestic and international educational circles.The technical process is not substantially by season and weather shadow
Ring, and water supply quality, steady sources, by the use of desalinization water as urban life and industrial water, can a large amount of fresh-water-savings,
Desalinization simultaneously is that one kind is increased income measure, can make land freshwater resources total amount increase, be advantageous to the improvement of land water environment.
But the technology can inevitably produce a large amount of concentrated seawaters, i.e. high slat-containing wastewater while fresh water is obtained.If by its
It is untreated and directly discharge, ocean water body certainly will be caused to be polluted, or even destroy the marine eco-environment.Processing is high at present
The technology of brine waste mainly has Re Fa and embrane method, and due to hot normal plane, to face that energy consumption is big, efficiency is low, floor space is big etc. many lacks
Point, increasing scholar, enterprise turn one's attention to embrane method desalting technology field.The mainstream technology of embrane method such as counter-infiltration at present,
Membrane module is essentially organic high molecular layer used by the desalinating process such as nanofiltration, and in fact this kind of organic hybrid films can not be preferable
The industrial wastewater for being applied to current water quality extensively, while the greatest problem that embrane method faces, fouling membrane caused by concentration polarization and
Flux depression is also to restrict the key technology limitation that organic film further applies industrial wastewater.Inorganic ceramic membrane is high-strength with its
The good characteristics such as degree, acid and alkali-resistance, high temperature resistant, pore-size distribution be narrow, it is insufficient caused by effectively improving organic film material in itself, its
Metal oxide film surface can produce electrostatic interaction with the ion in treatment fluid and charging cpd with electric charge and increase it and disturb
Random degree, it not only can effectively mitigate the embrane method such as concentration polarization common fault and reduce fouling membrane, and can while holding membrane flux
Effectively to retain ion etc., so as to greatly remove the ion and charging cpd in brine waste, reach to being given up containing high salt
The good processing of water.
Ceramic membrane is mainly to be prepared by the commonplace inorganic material such as oxidized metal, kaolin.Beginning is in World War II
Atom bomb period is prepared, in order to separate UF6Isotope, scientist attempt to employ porous ceramic film material first and succeeded.
To the 1980s, with the rapidly development of industry, separation process proposes higher and higher requirement to membrane material,
Such as strong acid-base, the application of the membrane separation technique of strong corrosive environment, and organic film can not better meet industrial needs, further
Promote the great development of ceramic membrane and wide demand.Inorganic ceramic membrane material has the advantages of it is unique notable：(1) it is acidproof
Caustic corrosion, high chemical stability energy, available for extreme environment；(2) high mechanical properties, so as to carry out backsurging operation,
Advantageously reduce fouling membrane；(3) superpower anti-microbe ability, it is not easy to produce any effect with microorganism；(4) higher heat is steady
Qualitative, due to the high temperature sintering preparation process of ceramic membrane, its SC service ceiling temperature is up to more than 800 DEG C；(5) there is preferable hole
Footpath is distributed, and can more effectively control separation process, grasps the i.e. controllable microstructure of appropriate condition；(6) due to thereon
State feature so that cleaning and regeneration technology have more selectivity, strong acid-base reaction, and high-temperature steam, backwash can be used to
Clear up fouling membrane so that the recovery of ceramic membrane energy higher degree uses；(7) service life is grown, general reachable 3-5, even more
It is long；(8) producing will not threaten to ecological environment substantially in preparation process.
But because the preparation process of ceramic membrane is difficult to control, the film layer that possesses preferable aperture and porosity can not be obtained and
Can not be separately as high slat-containing wastewater desalinating process, its application in numerous desalination fields substantially as pretreatment, reduces
The inorganic and organic concentration of raw water reaches the water quality requirement of feed water by reverse osmosis, preferably to ensure the strainability of reverse osmosis membrane
And service life；Also there are some ceramic membranes by the modified effect for reaching hydrophobic filter, so as to be carried out using membrane distillation method
The desalinating process of seawater and bittern.The former has widely applied example and preferably can provide entering for high quality for reverse osmosis membrane
Water, but be but rarely reported (such as sea, bittern) using ceramic membrane as independent PROCESS FOR TREATMENT high slat-containing wastewater.The latter big many places now
Commercial Application is not realized really in laboratory stage.
The content of the invention
In view of the shortcomings of the prior art, the technical problem that the present invention intends to solve is to propose a kind of alundum (Al2O3)/titanium dioxide
The preparation method of tin composite ceramic film.
The technical scheme that the present invention solves the technical problem is to provide a kind of alundum (Al2O3)/tin ash composite ceramic
The preparation method of porcelain film, it is characterised in that the preparation method comprises the following steps：
(1) boehmite sol is prepared：At ambient pressure, boehmite sol is prepared with alundum (Al2O3) predecessor, it is described
Alundum (Al2O3) predecessor molar concentration is 0.2-0.6mol/L；
(2) tin ash colloidal sol is prepared：At ambient pressure, tin ash colloidal sol, nothing are prepared with five water crystallization stannic chlorides
Water crystallization stannic chloride molar concentration is 0.2-0.6mol/L；
(3) boehmite-tin ash coating liquid is prepared：By boehmite sol and tin ash colloidal sol using mol ratio as 1:5-
5:1 mixing, uniform stirring 1-30 minutes, then obtained so that 5%-25% volume fraction addition polyvinyl alcohol (PVA) is well mixed
Coating liquid；
(4) coat, dry and sinter：Film is carried out using dip-coating method, ceramic matrix is stood into 1- in coating liquid
10 minutes, taking-up was placed in 1-24 hours under room temperature condition；1-4 hours are sintered under conditions of 400-800 DEG C, obtain three oxidations two
Aluminium/tin ash composite ceramic film.
Compared with prior art, the beneficial effects of the present invention are：Ceramic film prepared by the present invention be alundum (Al2O3)/
Tin ash composite membrane, it is a kind of novel composite ceramic film layer；Prepared using sol-gal process, aperture is good, and porosity is moderate；
There are stronger hydrolysis properties in aqueous phase；There is stronger electrostatic repulsion to the salt ion in high level salt solution, in T=35
DEG C, under the conditions of pH=4-5, TMP=0.3Mpa, calcium ion, the clearance of magnesium ion have respectively reached 79% and 75%, are far above
Other removal efficiency similar to ceramic membrane to this kind of salt ion.
Brief description of the drawings
Fig. 1 is the surface scan electricity of the preparation method embodiment 1 of alundum (Al2O3) of the present invention/tin ash composite ceramic film
Mirror image.
Embodiment
Detailed statement is made to the present invention below by way of some embodiments, but the invention is not limited in these embodiments.
The invention provides the preparation method of alundum (Al2O3)/tin ash composite ceramic film, comprise the following steps：
(1) boehmite sol is prepared：At ambient pressure, boehmite sol is prepared with alundum (Al2O3) predecessor, it is described
Alundum (Al2O3) predecessor molar concentration is 0.2-0.6mol/L.
(2) tin ash colloidal sol is prepared：At ambient pressure, tin ash colloidal sol, nothing are prepared with five water crystallization stannic chlorides
Water crystallization stannic chloride molar concentration is 0.2-0.6mol/L.
(3) boehmite-tin ash coating liquid is prepared：By boehmite sol and tin ash colloidal sol using mol ratio as 1:5-
5:1 mixing, uniform stirring 1-30 minutes, then obtain coating liquid so that 5%-25% volume fraction addition PVA is well mixed.
(4) coat, dry and sinter：Film is carried out using dip-coating method, ceramic matrix is stood into 1- in coating liquid
10 minutes, taking-up was placed in 1-24 hours under room temperature condition.1-4 hours are sintered under conditions of 400-800 DEG C, obtain three oxidations two
Aluminium/tin ash composite ceramic film.
The alundum (Al2O3) predecessor is aluminium isopropoxide or aluminium secondary butylate；The tin ash predecessor is five water crystallizations
Stannic chloride.
Boehmite and tin ash the colloidal sol mol ratio is 1:1.
The volume fraction of the addition PVA is 15%.
Embodiment 1
(1) weigh 22.69g aluminium isopropoxides to be dissolved in 200ml distilled water, under agitation continuous heating, directly
80 DEG C or so are risen to temperature and keeps constant, are added magnetic agitation rotor and are started to continue stirring.The heating stirring duration 2
Hour, distilled water is during which added frequently to keep water.After heating stirring terminates, until solution is cooled to room temperature, it is left to add 1ml
Right nitric acid peptization, is then transferred to heating water bath in three mouthfuls of cucurbits by solution, is stirred at reflux under the conditions of 85 DEG C 16 hours
Aging is carried out, and then obtains the boehmite sol of 0.55mol/L water white transparency clarification.
(2) the water crystallization stannic chlorides of 38.556g five are weighed, being dissolved in heating stirring in 200ml distilled water makes it fully dissolve；So
Solution is transferred in three mouthfuls of cucurbits the heating water bath under the conditions of 95 DEG C afterwards, is stirred at reflux 2 hours, and then obtain 0.55mol/
The faint yellow tin ash colloidal sols of L.
(3) weigh a certain amount of PVA to be placed in beaker, add the solution that appropriate distilled water is formulated as 35g/L, swelling is about
After 10min, temperature setting is begun to warm up at 90 DEG C and continues to stir, obtain colourless, clarification, transparent viscous solution.
(4) boehmite sol and tin ash colloidal sol mol ratio are 1:1 is mixed, and stirring 5min is stand-by.By prepared by
35g/L PVA solution (volume fraction 15%) and complex sol be mixed to get coating liquid.
(6) dip-coating method film is used, ceramic matrix is stood 10 minutes in coating liquid, is spontaneously dried 24 hours,
It is placed in Muffle furnace and sinters, it is 1.5 DEG C/min of programming rate that Muffle furnace, which sets condition, and 2h is incubated after temperature rises to 700 DEG C.
The ceramic membrane prepared is characterized.
Prepared composite ceramic film surface SEM is surveyed using FDAC S-4800 cold field emissions SEM
Take temperature sign.
The pure water flux of the ceramic membrane is determined on homemade ceramic membrane evaluating apparatus, is calculated and obtained using formula (1)：
In formula, V is that pure water passes through total amount；A is the effective area of the film；T is filtration time.The present invention is using distillation
Water, 25 DEG C of operating pressure 0.2MPa, temperature conditions.
The porosity ε of the film is characterized, and is cut matrix surface dry film and is weighed weight W1Afterwards, by boiling and abundant in water
Wetting, weighs wet film weight W2, with the porosity ε of following formula calculating film：
In formula,For the density of water, 1g/m3；P is the hybrid density of aluminum oxide and tin oxide, 5.04g/m3, wherein W1
For 0.52g, W2For 0.57g.
The thickness h of the film determines, and before film claims that vehicle weight W must be dried3, film weight W is weighed after film4, with following formula meter
Calculate the average thickness h of UF membrane layer：
In formula, A be the film area, A=2 π rIt is interiorL(rIt is interiorFor the internal diameter of membrane tube, L is the length of membrane tube), wherein W4For
375.13g, W3For 374.35g, A 0.017m2。
The film acid-proof alkaline measure, it is respectively that 1mol/L hydrochloric acid is molten in concentration that table 1, which gives the composite ceramic film,
Liquid and 1mol/L sodium hydroxide solutions soak quality, the correction data of pure water permeation flux of film before and after 24h.
The quality of composite ceramic film, pure water permeation flux before and after the acid of table 1, alkali immersion
Composite ceramic film surfacing as seen from Figure 1 prepared by the present invention is smooth, free from flaw.
Formula (1) calculate prepared ceramic membrane pure water permeation flux of the invention is 367.06L/m2h。
The ceramic membrane porosity ε that formula (2) is calculated prepared by the present invention is 32.6%.
The ceramic membrane thickness h that formula (3) is calculated prepared by the present invention is 6.1 μm.
Larger change does not occur for composite ceramics film quality and pure water permeation flux of the present invention before and after the display immersion of table 1
Change.This illustrates that composite ceramic film prepared by this experiment has been internally formed close crystal structure, and chemical bonding is firm, be not easy by
The material damages such as acid, alkali.
Filtration treatment is carried out to high slat-containing wastewater using composite ceramic film prepared in embodiment 1.At T=35 DEG C, pH
Determined under the conditions of=4-5, TMP=0.3MPa：Alundum (Al2O3)/tin ash composite ceramic film pure water prepared by embodiment 1
Permeation flux is 240L/m2H, Mg2+And Ca2+The rejection of ion is respectively 75% and 79%.
The present invention does not address part and is applied to prior art.
Claims (5)
- A kind of 1. preparation method of alundum (Al2O3)/tin ash composite ceramic film, it is characterised in that the preparation method include with Lower step：（1）Boehmite sol is prepared：At ambient pressure, boehmite sol, three oxygen are prepared with alundum (Al2O3) predecessor It is 0.2-0.6mol/L to change two aluminium predecessor molar concentrations；（2）Tin ash colloidal sol is prepared：At ambient pressure, tin ash colloidal sol, anhydrous knot are prepared with five water crystallization stannic chlorides Brilliant stannic chloride molar concentration is 0.2-0.6 mol/L；（3）Boehmite-tin ash coating liquid is prepared：By boehmite sol and tin ash colloidal sol using mol ratio as 1:5-5:1 Mixing, uniform stirring 1-30 minutes, then polyvinyl alcohol is added with 5%-25% volume fraction（PVA）It is well mixed to obtain film Liquid；（4）Coating, dry and sinter：Film is carried out using dip-coating method, ceramic matrix is stood to 1-10 points in coating liquid Clock, taking-up are placed in 1-24 hours under room temperature condition；Under conditions of 400-800 DEG C sinter 1-4 hours, obtain alundum (Al2O3)/ Tin ash composite ceramic film.
- 2. the preparation method of alundum (Al2O3) according to claim 1/tin ash composite ceramic film, it is characterised in that three Al 2 O predecessor is aluminium isopropoxide or aluminium secondary butylate.
- 3. the preparation method of alundum (Al2O3) according to claim 1/tin ash composite ceramic film, it is characterised in that institute It is 1 to state boehmite and tin ash colloidal sol mol ratio:1.
- 4. the preparation method of alundum (Al2O3) according to claim 1/tin ash composite ceramic film, it is characterised in that institute The volume fraction for stating addition PVA in coating liquid is 15%.
- 5. the preparation method of alundum (Al2O3) according to claim 1/tin ash composite ceramic film, it is characterised in that institute It is five water crystallization stannic chlorides to state tin ash predecessor.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109293345A (en) * | 2018-11-23 | 2019-02-01 | 郑州中瓷科技有限公司 | High reflectance high-strength ceramic substrate and preparation method thereof |
| CN109569315A (en) * | 2018-10-29 | 2019-04-05 | 董林妤 | A kind of preparation and its application method of the inorganic ceramic membrane handling oily waste water |
| CN109650935A (en) * | 2019-02-15 | 2019-04-19 | 中国计量大学 | A kind of preparation method of the adjustable alumina porous ceramic film of hole shape |
| CN110898679A (en) * | 2019-11-29 | 2020-03-24 | 珠海大横琴科技发展有限公司 | Filter membrane preparation method and filter membrane |
| CN111437726A (en) * | 2020-04-24 | 2020-07-24 | 佛山市中国科学院上海硅酸盐研究所陶瓷研发中心 | Tin oxide ultrafiltration membrane and preparation method and application thereof |
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2016
- 2016-09-30 CN CN201610866982.1A patent/CN107879759A/en active Pending
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109569315A (en) * | 2018-10-29 | 2019-04-05 | 董林妤 | A kind of preparation and its application method of the inorganic ceramic membrane handling oily waste water |
| CN109569315B (en) * | 2018-10-29 | 2021-06-15 | 绍兴市柯桥区锦策智能科技有限公司 | Preparation and application method of inorganic ceramic membrane for treating oily wastewater |
| CN109293345A (en) * | 2018-11-23 | 2019-02-01 | 郑州中瓷科技有限公司 | High reflectance high-strength ceramic substrate and preparation method thereof |
| CN109293345B (en) * | 2018-11-23 | 2020-10-02 | 郑州中瓷科技有限公司 | High-reflectivity and high-strength ceramic substrate and preparation method thereof |
| CN109650935A (en) * | 2019-02-15 | 2019-04-19 | 中国计量大学 | A kind of preparation method of the adjustable alumina porous ceramic film of hole shape |
| CN109650935B (en) * | 2019-02-15 | 2022-03-22 | 中国计量大学 | Preparation method of porous alumina ceramic membrane with adjustable pore shape |
| CN110898679A (en) * | 2019-11-29 | 2020-03-24 | 珠海大横琴科技发展有限公司 | Filter membrane preparation method and filter membrane |
| CN111437726A (en) * | 2020-04-24 | 2020-07-24 | 佛山市中国科学院上海硅酸盐研究所陶瓷研发中心 | Tin oxide ultrafiltration membrane and preparation method and application thereof |
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