CN112851215B - Preparation method and application of low-cost silicomanganese slag-based geopolymer film - Google Patents
Preparation method and application of low-cost silicomanganese slag-based geopolymer film Download PDFInfo
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Abstract
The invention discloses a preparation method and application of a low-cost silicomanganese slag-based geopolymer film for oil-water separation. The preparation method comprises the steps of putting the silicomanganese slag, sodium hydroxide and water into a stirring device, violently stirring to obtain uniform slurry, filling and covering the slurry on the pores and the surface of a stainless steel screen mesh through dip-coating, and performing thermal curing to obtain the silicomanganese slag-based geopolymer film with the super-hydrophilic/underwater super-oleophobic property, wherein the mass ratio of the water to the silicomanganese slag is 0.5-0.9, and H is2The ratio of O to Na is 5: 2. Compared with the traditional inorganic ceramic oil-water separation membrane method, the method has the advantages of simple process and low synthesis temperature, greatly reduces the preparation cost of the inorganic oil-water separation membrane, and in addition, the geopolymer membrane taking the stainless steel screen mesh as the matrix well improves the problem of poor toughness of the geopolymer. When the prepared silicomanganese slag geopolymer film is used for oil-water separation, the prepared silicomanganese slag geopolymer film has the characteristics of high flux and high separation efficiency, and has potential application prospects.
Description
Technical Field
The invention belongs to the field of inorganic membrane preparation and solid waste resource utilization, and particularly relates to a preparation method and application of a low-cost silicomanganese slag-based geopolymer membrane.
Background
With the vigorous development of offshore oil exploitation and transportation, accidents of crude oil leakage frequently occur in the process, a large amount of oily wastewater is generated, and serious environmental pollution and ecological damage are caused. The membrane separation method has the characteristics of high efficiency, low energy consumption, easy operation and the like, has obvious advantages in the field of oil-water separation, and the main problems of limiting the application of the membrane in the oil-water separation are that the membrane is easy to pollute and poor in stability[1]. In recent years, the fish scale biomimetic-based super-hydrophilic/underwater super-oleophobic membrane can protect the membrane material from being polluted by oil stains, and fundamentally solves the problem of membrane pollution, thereby arousing the extensive attention of researchers[2]。
Currently, the super-hydrophilic/underwater super-oleophobic membranes mainly comprise organic polymer membranes, metal screens or inorganic ceramic membranesAnd the like. The preparation of the super-hydrophilic/underwater super-oleophobic membrane based on organic polymer generally comprises the hydrophilic modification of a membrane material, and can be divided into matrix modification and surface modification according to a modification method[3]. The matrix modification is to modify the membrane material by methods such as graft copolymerization or blending hydrophilic components and the like, and then use the modified membrane material for the preparation of the membrane; the surface modification is to directly graft hydrophilic monomers on the surface of a commercial membrane. Organic polymer films have the disadvantages of poor mechanical properties, poor chemical resistance and easy deformation. The metal screen does not have obvious super-hydrophilic/super-oleophobic characteristics, so a micro-nano secondary coarse structure is usually constructed on the surface of the metal screen, or a compound coating with high surface energy is prepared in the modes of surface coating, electrochemical deposition and the like to regulate and control the super-wetting property of the net film, thereby improving the hydrophilicity of the film[4]. However, hydrophilic coatings generally suffer from poor mechanical stability and abrasion resistance, resulting in a short membrane life. The inorganic ceramic membrane has excellent mechanical, chemical and thermal stability, and can work under some harsh conditions such as corrosive and high-temperature environments[5]. However, the ceramic film preparation must adopt a high-temperature sintering process, which results in high production cost and limits the industrial application thereof. Therefore, the development and preparation of the oil-water separation membrane which is simple, low in cost, high in strength and high in stability is the key research point in the field.
The geopolymer is an inorganic aluminosilicate cementing material generated by reacting a silicon-aluminum natural mineral or solid waste with an alkali solution at a certain temperature, and has an amorphous to semi-crystalline three-dimensional network structure[6]. Currently, researchers' research on geopolymerization is mainly focused on micro-mechanisms and their mechanics and durability as building materials. In addition, there are geopolymers used in catalysts[7]Adsorbent, and process for producing the same[8]pH buffer[9]And related reports in high-added-value fields. Notably, geopolymers are prepared under strongly alkaline conditions, and their surfaces contain abundant terminal hydroxyl groups, thus exhibiting strong hydrophilicity.
The inorganic oil-water separation membrane reported in the literature at present needs to be subjected to a high-temperature sintering process, so that the production cost and the energy consumption are high; a large amount of domestic patents and literature data are consulted through the system, and no relevant report about the silicomanganese slag-based geopolymer oil-water separation membrane is found.
The following are relevant references given by the inventors:
[1] popsician, wangjian, liufu, development of oil-water separation membrane research [ J ], membrane science and technology, 2019, 39 (03): 132-141.
[2] Xulanfang, wanfeng, hero, duckweed; super-hydrophilic/underwater super-oleophobic membrane functional material and research progress [ J ], material report, 2020, 34 (17): 17105-17114.
[3] Yuan Jing, Liao Fangfang, Guo Yani, Liyuan; preparation of a superhydrophilic superoleophobic oil-water separation membrane and its properties [ J ], chemical evolution, 2019, 31 (01): 144-155.
[4]Zhang F，Zhang W B，Shi Z，et al.Nanowire-haired inorganic membranes with superhydrophilicity and underwater ultralow adhesive superoleophobicity for high-efficiency oil/water separation[J].Advanced Materials，2013，25(30)：4192-4198。
[5] Morning xi, zhuli, king forest, quarterly family friends, perennial, five dream universities, Zhang hong liang, and xu slowly; use of inorganic ceramic membranes in the treatment of oily wastewater [ J ], proceedings of wuhan university of engineering, 2020, 42 (05): 511-517.
[6] The research progress of a novel alkali-activated cementing material catalyst of Zuanjun, Yang Meng Yang, Kangle, tension, Zhang Ke [ J ]; inorganic materials bulletin, 2016, 31 (03): 225-233.
[7]Zhang Y J，Han Z C，He P Y，Chen H.Geopolymer-based catalysts for cost-effective environmental governance：A review based on source control and end-of-pipe treatment[J].Journal of Cleaner Production，2020：121556。
[8]Rasaki S A，Bingxue Z，Guarecuco R，Thomas T，Yang M H，Geopolymer for use in heavy metals adsorption，and advanced oxidative processes：A critical review[J].Journal of Cleaner Production，2019，213：42-58。
[9]Novais R M，Carvalheiras J，Seabra M P，Pullar R C.Labrincha J A，Innovative application for bauxite residue:Red mud-based inorganic polymer spheres as pH regulators[J].Journal of hazardous materials，2018，358：69-81。
Disclosure of Invention
The invention aims to provide a preparation method of a low-cost silicomanganese slag-based geopolymer film for oil-water separation.
In order to realize the task, the invention adopts the following technical solution:
the preparation method of the low-cost silicomanganese slag-based geopolymer film for oil-water separation is characterized in that silicomanganese slag, sodium hydroxide and deionized water are placed into a stirring device, wherein the mass ratio of the deionized water to the silicomanganese slag is 0.5-0.9, and H is2O/Na is 5: 2; and stirring to obtain uniform slurry, filling and covering the slurry on the pores and the surface of the stainless steel screen by dip-coating, and performing thermal curing to obtain the silicomanganese slag-based geopolymer film with the super-hydrophilic/underwater super-oleophobic characteristic.
The method is implemented by the following steps:
(1) weighing silicomanganese slag according to the formula amount;
(2) weighing sodium hydroxide according to the formula ratio, and placing the sodium hydroxide into a beaker;
(3) weighing deionized water according to the formula amount, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution obtained in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) cutting a 40-mesh square-hole stainless steel screen into a round shape with the diameter of 50mm, sequentially cleaning with a cleaning agent, deionized water and absolute ethyl alcohol, and drying for later use;
(7) uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
The experimental result of the applicant shows that the silicomanganese slag-based geopolymer film prepared by the method can be applied to separation of oil-water mixtures, and the specific implementation steps are as follows:
(1) the separation device for the self-made oil-water mixture comprises two sand core cups with the inner diameter of 40mm, 2 silica gel sealing rings with the inner diameter of 40mm and the outer diameter of 50mm and a clamp, and the prepared silicomanganese slag geopolymer film is wetted for 5min, clamped between the sealing rings and fixed by the clamp.
(2) Respectively dyeing oil and water by using Sudan III and indigo dyes, respectively mixing 50g of dyed oil and water, pouring an oil-water mixture into an upper sand core cup, carrying out oil-water separation under the driving of gravity, pouring liquid on the upper side of a membrane into the beaker and measuring the mass of the liquid when no water drops on the lower side of the membrane, wherein the oil-water separation efficiency can be calculated by the following formula:
efficiency of oil-water separation (m)0/50)×100％。
The oil is petroleum ether, hexane or petroleum diesel.
The preparation method of the low-cost silicomanganese slag-based geopolymer film has the innovation points that the solid waste silicomanganese slag is used as the raw material, the geopolymer inorganic film for oil-water separation is prepared at low cost, and compared with the traditional preparation process of the inorganic ceramic film, the preparation method has the advantages of simple process, low synthesis temperature and capability of greatly reducing the preparation cost of the inorganic oil-water separation film. When the prepared silicomanganese slag geopolymer film is used for oil-water separation, the silicomanganese slag geopolymer film has the characteristics of high flux and high separation efficiency, and has potential application prospects.
Drawings
FIG. 1 is a diagram of a homemade oil-water separator;
FIG. 2 is a scanning electron microscope photograph of a silicomanganese slag geopolymer film obtained in a preparation example;
FIG. 3 is the underwater oil contact angle of the silicomanganese slag geopolymer film obtained in the preparation example.
The present invention will be described in further detail with reference to the following drawings and examples.
Detailed Description
It should be noted that the following examples are only for better illustrating the present invention and the present invention is not limited to these examples.
The embodiment provides a preparation method of a low-cost silicomanganese slag-based polymer film, which comprises the steps of putting silicomanganese slag, sodium hydroxide and deionized water into a stirring device, wherein the mass ratio of the deionized water to the silicomanganese slag is 0.5-0.9, and H is2O/Na is 5: 2; and stirring to obtain uniform slurry, filling and covering the slurry on the pores and the surface of the stainless steel screen by dip-coating, and performing thermal curing to obtain the silicomanganese slag-based geopolymer film with the super-hydrophilic/underwater super-oleophobic characteristic.
The specific experimental raw materials and reagents are as follows:
(1) silicon manganese slag from steel company in Diety county in Han Shaanxi, ball milled for 2 hours for later use, and the density of the silicon manganese slag is 2.87g/cm3Specific surface area of 532m2/kg。
(2) Solid sodium hydroxide, available from national chemical reagents, Inc., analytical grade reagent, molecular weight 40.00 g/mol.
(3) Deionized water is self-made in a laboratory.
(4) Petroleum ether is purchased from chemical reagents of national medicine group, Inc., and is a colorless liquid with analytically pure reagents.
(5) N-hexane was purchased from national pharmaceutical group chemical reagent, Inc., analytical pure reagent, colorless liquid, molecular weight 86.18 g/mol.
(6) Petroleum diesel is purchased from medium petroleum group ltd as a yellowish liquid.
Preparation example 1:
(1) weighing 10g of silicomanganese slag;
(2) weighing 2g of sodium hydroxide, and placing the sodium hydroxide into a beaker;
(3) weighing 5g of deionized water, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution obtained in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) a 40-mesh square-hole stainless steel screen mesh is cut into a circular shape with a diameter of 50mm, washed with a detergent, deionized water and absolute ethanol in sequence, and then dried for later use, and fig. 2(a) shows a scanning electron microscope photograph of the stainless steel screen mesh.
(7) Uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) by using a brush to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
FIG. 2(b) is a scanning electron micrograph of the resulting silicomanganese slag geopolymer film. FIG. 3(a) is the underwater petroleum ether contact angle of the prepared silicomanganese slag geopolymer film.
Preparation example 2:
(1) weighing 10g of silicomanganese slag;
(2) weighing 2.4g of sodium hydroxide, and placing the sodium hydroxide into a beaker;
(3) weighing 6g of deionized water, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) cutting a 40-mesh square-hole stainless steel screen into a circle with the diameter of 50mm, sequentially cleaning with a cleaning agent, deionized water and absolute ethyl alcohol, and drying for later use.
(7) Uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) by using a brush to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
FIG. 2(c) is a scanning electron micrograph of the resulting silicomanganese slag geopolymer film. FIG. 3(b) is the underwater petroleum ether contact angle of the prepared silicomanganese slag geopolymer film.
Preparation example 3:
(1) weighing 10g of silicomanganese slag;
(2) weighing 2.8g of sodium hydroxide, and placing the sodium hydroxide into a beaker;
(3) weighing 7g of deionized water, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) a 40-mesh square-hole stainless steel screen mesh was cut into a circular shape having a diameter of 50mm, washed with a detergent, deionized water, and absolute ethanol in this order, and dried for use, and fig. 2(a) is a scanning electron microscope photograph of the stainless steel screen mesh.
(7) Uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) by using a brush to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
FIG. 2(d) is a scanning electron micrograph of the resulting silicomanganese slag geopolymer film. FIG. 3(c) is the underwater petroleum ether contact angle of the prepared silicomanganese slag geopolymer film.
Preparation example 4:
(1) weighing 10g of silicomanganese slag;
(2) weighing 3.2g of sodium hydroxide, and placing the sodium hydroxide into a beaker;
(3) weighing 8g of deionized water, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) a 40-mesh square-hole stainless steel screen mesh was cut into a circular shape having a diameter of 50mm, washed with a detergent, deionized water, and absolute ethanol in this order, and dried for use, and fig. 2(a) is a scanning electron microscope photograph of the stainless steel screen mesh.
(7) Uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) by using a brush to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
FIG. 2(e) is a scanning electron micrograph of the resulting silicomanganese slag geopolymer film. Fig. 3(d) is the underwater petroleum ether contact angle of the prepared silicomanganese slag geopolymer film, and fig. 3(e) and (f) are the underwater hexane and petrochemical diesel contact angles of the prepared silicomanganese slag geopolymer film, respectively.
Comparative example 5:
(1) weighing 10g of silicomanganese slag;
(2) weighing 3.6g of sodium hydroxide, and placing the sodium hydroxide into a beaker;
(3) weighing 9g of deionized water, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform slurry;
(6) a 40-mesh square-hole stainless steel screen mesh was cut into a circular shape having a diameter of 50mm, washed with a detergent, deionized water, and absolute ethanol in this order, and dried for use, and fig. 2(a) is a scanning electron microscope photograph of the stainless steel screen mesh.
(7) Uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) by using a brush to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
FIG. 2(f) is a scanning electron micrograph of the resulting silicomanganese slag geopolymer film. It can be known from the figure that when the mass ratio of the deionized water to the silicomanganese slag reaches 0.9, the geopolymer slurry cannot fully cover the surface and the pore passages of the stainless steel screen mesh, and therefore, the silicomanganese slag-based geopolymer film cannot be successfully prepared in the comparative example.
The following are examples of applicants' use for oil-water separation via silicomanganese slag geopolymer membranes.
Application example 1:
(1) wetting the silicomanganese slag geopolymer film prepared in preparation example 1 for 5min, and fixing the film in an oil-water separation device shown in figure 1; the oil-water separation device comprises two sand core cups with the inner diameter of 40mm, 2 silica gel sealing rings with the inner diameter of 40mm and the outer diameter of 50mm and a clamp.
(2) Respectively dyeing petroleum ether and water by using Sudan III and indigo dyes, respectively mixing 50g of dyed petroleum ether and 50g of dyed water, pouring the mixture into an upper sand core cup, carrying out oil-water separation under the driving of gravity, pouring liquid on the upper side of a membrane into the beaker and measuring the mass of the liquid when no water drops on the lower side of the membrane, wherein the oil-water separation efficiency can be calculated by the following formula:
efficiency of oil-water separation (m)0/50)×100％
Namely, the separation efficiency of the silicomanganese slag geopolymer membrane on the mixture of petroleum ether and water is 98.4%.
Application example 2:
(1) the silicomanganese slag geopolymer film prepared in preparation example 2 was wetted for 5min and fixed in an oil-water separation device shown in fig. 1. The oil-water separator had the same structure as in application example 1.
(2) Dyeing by using indigo dye water, mixing 50g of dyed water, 50g of petrochemical diesel oil and water, pouring the mixture into an upper sand core cup, carrying out oil-water separation under the driving of gravity, pouring liquid on the upper side of a membrane into a beaker and measuring the mass of the liquid when no water drops on the lower side of the membrane, wherein the oil-water separation efficiency can be calculated by the following formula:
efficiency of oil-water separation (m)0/50)×100％
Namely, the separation efficiency of the silicomanganese slag geopolymer membrane on the mixture of petroleum diesel and water is 99.0%.
Application example 3:
(1) the silicomanganese slag geopolymer film prepared in preparation example 4 was wetted for 5min and fixed in an oil-water separation device shown in fig. 1. The oil-water separator had the same structure as in application example 1.
(2) Respectively dyeing n-hexane and water by using Sudan III and indigo dyes, respectively mixing 50g of dyed n-hexane and water, pouring the mixture into an upper sand core cup, carrying out oil-water separation under the driving of gravity, pouring liquid on the upper side of a membrane into a beaker and measuring the mass of the liquid when no water drops on the lower side of the membrane, wherein the oil-water separation efficiency can be calculated by the following formula:
efficiency of oil-water separation (m)0/50)×100％
Namely, the separation efficiency of the silicomanganese slag geopolymer film on a mixture of n-hexane and water is 98.2%.
Claims (4)
1. A preparation method of a low-cost silicomanganese slag-based polymer film is characterized by placing silicomanganese slag, sodium hydroxide and deionized water into a stirring device, wherein the mass ratio of the deionized water to the silicomanganese slag is 0.5-0.9, and H is2O/Na is 5: 2; stirring to obtain uniform slurry, filling and covering the slurry on the pores and the surface of a stainless steel screen by dip-coating, and performing thermal curing to obtain the silicomanganese slag-based geopolymer film with super-hydrophilic/underwater super-oleophobic characteristics;
the method is implemented by the following steps:
(1) weighing silicomanganese slag according to the formula amount;
(2) weighing sodium hydroxide according to the formula ratio, and placing the sodium hydroxide into a beaker;
(3) weighing deionized water according to the formula amount, and placing the deionized water into a beaker;
(4) dissolving the sodium hydroxide weighed in the step (2) into the deionized water weighed in the step (3), stirring and cooling to room temperature;
(5) placing the mixed solution obtained in the step (4) into a stirrer, placing the silicomanganese slag weighed in the step (1) into the stirrer, and stirring to obtain uniform silicomanganese slag geopolymer slurry;
(6) cutting a 40-mesh square-hole stainless steel screen into a round shape with the diameter of 50mm, sequentially cleaning with a cleaning agent, deionized water and absolute ethyl alcohol, and drying for later use;
(7) uniformly coating the silicomanganese slag geopolymer slurry obtained in the step (5) on the pore passages and the surface of the stainless steel screen cleaned in the step (6) to obtain a geopolymer film precursor;
(8) and (4) filling the geopolymer film precursor obtained in the step (7) into a plastic package bag, and curing for 24 hours in a thermostat at 80 ℃ to obtain the silicomanganese slag-based geopolymer film.
2. Use of a silicomanganese slag-based geopolymer membrane prepared according to the method of claim 1 for separating oil-water mixtures.
3. The application of claim 2, comprising the following steps:
(1) the separation device for the self-made oil-water mixture comprises two sand core cups with the inner diameter of 40mm, 2 silica gel sealing rings with the inner diameter of 40mm and the outer diameter of 50mm and a clamp, wherein the prepared silicon-manganese slag geopolymer film is wetted for 5min, clamped between the sealing rings and fixed by the clamp;
(2) respectively dyeing oil and water by using Sudan III and indigo dyes, respectively mixing the oil and the water which are dyed in equal amount, pouring an oil-water mixture into an upper sand core cup, carrying out oil-water separation under the driving of gravity, pouring liquid on the upper side of a membrane into a beaker and measuring the mass of the liquid when no water drops on the lower side of the membrane, wherein the oil-water separation efficiency can be calculated by the following formula:
efficiency of oil-water separation (m)0/50)×100％。
4. The use according to claim 3, wherein the oil is petroleum ether, hexane or petroleum diesel.
Priority Applications (1)
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| CN102961974A (en) * | 2012-11-15 | 2013-03-13 | 广西大学 | Geopolymer inorganic membrane and preparation method thereof |
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| CN102961974A (en) * | 2012-11-15 | 2013-03-13 | 广西大学 | Geopolymer inorganic membrane and preparation method thereof |
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