CN114849485A - Universal self-cleaning anti-membrane pollution method based on pulse water pressure response - Google Patents
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D65/00—Accessories or auxiliary operations, in general, for separation processes or apparatus using semi-permeable membranes
- B01D65/02—Membrane cleaning or sterilisation ; Membrane regeneration
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
- C02F1/441—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by reverse osmosis
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
- C02F1/442—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by nanofiltration
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
- C02F1/444—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by ultrafiltration or microfiltration
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2321/00—Details relating to membrane cleaning, regeneration, sterilization or to the prevention of fouling
- B01D2321/22—Electrical effects
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A20/00—Water conservation; Efficient water supply; Efficient water use
- Y02A20/124—Water desalination
- Y02A20/131—Reverse-osmosis
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Nanotechnology (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
Abstract
The invention discloses a universal autonomous membrane fouling resistant method for pulse water pressure response. The technical scheme of the invention integrates membrane pollution prevention and control into a whole, does not use other power supply equipment (particularly different from the conventional method of stimulating the piezoelectric filter membrane material to resist membrane pollution by in-situ vibration through external voltage), does not use water treatment agents and a conventional backwashing membrane pollution resisting means, only depends on periodically changed transmembrane pressure difference in the wastewater membrane separation process to stimulate the piezoelectric filter membrane material to generate charges, and can prevent multiple membrane pollution through multiple actions of in-situ generated oxidation free radicals, electrostatic repulsion and dielectrophoresis force. Under the periodic pressure-variable operation mode, the membrane pollution is remarkably controlled, the membrane flux is remarkably improved compared with a constant-pressure operation mode, and the technical scheme has a good universal application prospect in the field of wastewater membrane separation and pollution resistance.
Description
Technical Field
The invention belongs to the technical field of water treatment membranes, and particularly relates to a universal self-cleaning membrane pollution resistance method based on pulse water pressure response.
Background
The membrane separation technology has the characteristics of high efficiency, environmental protection and the like, and is widely applied to environmental wastewater treatment. However, membrane fouling as a bottleneck problem restricting the development of membrane technology can lead to a sudden increase in membrane filtration pressure drop and energy consumption, and significantly reduce membrane flux and separation efficiency. The current membrane pollution treatment methods comprise physical backwashing, chemical cleaning, membrane material modification and the like. For example, chinese patent application CN 110921777 a discloses a method for preventing and treating water treatment membrane pollution, which combines chemical and physical cleaning processes, including three steps of permeation stripping, pre-oxidation, and rinsing cleaning. The methods relieve the membrane pollution problem to a certain extent, but still have the problems of additional equipment and chemical reagents, easy corrosion and damage of membrane materials, production influence caused by shutdown and cleaning, and the like.
The piezoelectric material is widely used in the electronic information industry in the early stage, and the piezoelectric material subjected to high-voltage electric field polarization treatment has a positive piezoelectric effect and a reverse piezoelectric effect at the same time. Under the action of external force, dipoles inside the piezoelectric material are separated and generate piezoelectric potential, namely positive piezoelectric effect. On the contrary, by applying an electric field to the polarization direction of the piezoelectric material, the piezoelectric material generates mechanical deformation or mechanical pressure in a certain direction, i.e., inverse piezoelectric effect. Piezoelectric materials can generate oxygen-containing radicals under external mechanical force stimulation such as ultrasound, and are increasingly receiving wide attention as piezoelectric catalytic materials in the aspects of degradation of dye wastewater and the like (Nano Energy, 2019, 66, 104083). Through retrieval, related applications have been disclosed in the field of water treatment membrane separation in the prior art, for example, chinese patent applications CN 106925140 a and CN 106853340 a disclose a method for resisting membrane pollution by organic and inorganic piezoelectric filter membranes, respectively, but both are based on the inverse piezoelectric effect, that is, the membrane pollution is inhibited by applying voltage by external power equipment and stimulating the piezoelectric filter membrane to generate vibration in situ, which undoubtedly increases unnecessary energy consumption, and the operation modes of the membrane separation process are also constant voltage operation modes. Piezoelectric ceramics, which is one of inorganic materials, have the characteristics of stable physicochemical properties and high mechanical strength. It can also be embodied as a water treatment ceramic filter membrane in the related prior application (CN 106608668A). However, the membrane process in this application is operated in a constant pressure operation mode, and the core of the membrane process is only piezoelectric ceramics, which can be used as a sewage treatment filtering membrane, and only the wastewater treatment effect based on membrane effluent COD is emphasized, and the membrane pollution problem is difficult to avoid. The anti-pollution requirement of the piezoelectric filter membrane in wastewater treatment needs to be further discussed and solved.
Based on the defects of the prior art, a novel membrane pollution prevention and control technology which does not depend on external auxiliary membrane pollution resistant equipment and cleaning reagents and has the diversity of separation membranes, the universality of wastewater treatment objects and the long-term effect of membrane pollution resistance is urgently needed to be invented.
Disclosure of Invention
1. Problems to be solved
The invention aims to solve the problem of providing a self-cleaning, environment-friendly and energy-saving long-acting anti-membrane pollution method with strong universality and pulse water pressure response.
2. Technical scheme
In order to solve the problems, the technical scheme adopted by the invention is as follows:
(1) the membrane material with impulse water pressure response comprises one or more than two of inorganic piezoelectric materials, organic piezoelectric materials and inorganic-organic composite piezoelectric materials. The inorganic piezoelectric filter membrane material comprises barium titanate, lead zirconate titanate, lead meta-niobate, lead barium lithium niobate, lithium gallate, lithium germanate, titanium germanate, lithium niobate, lithium tantalate, zinc oxide, quartz, modified doped membrane material thereof and the like; the organic piezoelectric filter membrane material comprises polyvinylidene fluoride, polytetrafluoroethylene, polyamide, polypropylene and modified doped membrane materials thereof and the like;
(2) as a further improvement of the invention, the piezoelectric filter membrane for water treatment comprises a microfiltration membrane, an ultrafiltration membrane, a nanofiltration membrane and a reverse osmosis membrane;
(3) as a further development of the invention, the membrane separation operation is a dead-end or cross-flow operation of a periodic pressure swing operation;
(4) as a further improvement of the invention, a complete periodic variable voltage operation comprises a constant voltage operation stage, a voltage reduction operation stage and a voltage boosting operation stage in sequence. The running time of the constant-pressure running stage is 10-86400 s, and the constant-pressure running pressure range is 1-10000 kPa; the operation time of the pressure reduction operation stage is 1-1000 s, and the pressure reduction target pressure range is 0-9999 kPa. The operation time of the boosting operation stage is 1-1000 s, and the range of the boosting target pressure is 1-10000 kPa.
(5) As a further improvement of the invention, the piezoelectric filter membrane material is used for membrane pollution control in the membrane separation process of one or more mixed wastewater of organic wastewater, inorganic wastewater, microbial wastewater, salt-containing wastewater and heavy metal wastewater.
3. Advantageous effects
Compared with the prior art, the invention has the beneficial effects that:
(1) the invention provides a universal self-cleaning anti-membrane pollution method with pulse water pressure response, which is characterized in that a piezoelectric filter membrane material with a positive piezoelectric effect is used as a water treatment filter membrane, only a periodic variable-pressure operation mode is needed in the membrane separation process, pulse piezoelectric potential and clean oxidation free radicals are continuously generated in situ on the membrane through the positive piezoelectric effect, and membrane pollution is resisted in cooperation with multiple action modes such as electrostatic repulsion, dielectrophoresis force and the like. The method can prevent and control membrane pollution for a long time without external anti-pollution equipment and chemical cleaning reagents;
(2) the universal self-cleaning anti-membrane pollution method with the pulse water pressure response is suitable for all micro-filtration membranes, ultra-filtration membranes, nano-filtration membranes and reverse osmosis membranes which are prepared from materials with the positive piezoelectric effect and used for water treatment, and the treated wastewater objects comprise one or more mixed wastewater of organic wastewater, inorganic wastewater, microbial wastewater, salt-containing wastewater and heavy metal wastewater, and have the characteristic of broad-spectrum anti-membrane pollution for water treatment;
(3) the universal self-cleaning anti-membrane pollution method for the pulse water pressure response can solve the problem of membrane pollution of water treatment for a long time under the conditions of no work and no influence on production, and the membrane flux can be increased by several times to tens of times compared with that under the condition of constant pressure operation.
Drawings
FIG. 1A shows the in-situ piezoelectric potential of a piezoelectric and non-piezoelectric manganese-doped barium titanate ceramic membrane measured during the periodic pressure-swing or constant-pressure membrane separation process;
FIG. 1B shows the actually measured in-situ generated radicals of a manganese-doped barium titanate piezoelectric ceramic membrane during the separation of 9 periodic pressure-change membranes;
FIG. 2A is a comparison of membrane flux for treating different wastewaters during periodic pressure-variable membrane separation of piezoelectric and non-piezoelectric manganese-doped barium titanate ceramic membranes;
FIG. 2B shows the flux of different mixed wastewater treated by the piezoelectric manganese doped barium titanate ceramic membrane during the separation process of periodic pressure change membrane;
FIG. 2C shows the flux of the piezoelectric and non-piezoelectric manganese-doped barium titanate ceramic membrane in the process of periodic pressure-swing membrane separation for treating the actual landfill leachate;
fig. 2D is a film contamination electron microscope photograph of a piezoelectric and non-piezoelectric manganese doped barium titanate ceramic film after different waste waters are treated in a periodic pressure-variable film separation process.
Detailed Description
The present invention will be further explained with reference to examples. The following examples are provided only for illustrating the present invention and are not intended to limit the scope of the present invention.
Example 1
The manganese-doped barium titanate micro-filtration ceramic membrane (the average pore diameter is about 5 mu m) after electric field polarization is used as a water treatment piezoelectric filtration membrane, the pressure of the membrane separation operation is quickly increased to 1kPa within 1s, and then the pressure is quickly reduced to 0kPa within 1s after the operation pressure is kept constant for 10s under 1 kPa. And taking the variable pressure program as a variable pressure membrane separation operation cycle, and repeatedly executing the variable pressure program to finish the dead-end membrane separation process. The membrane separation operation is applied to the treatment of oily wastewater, the pulse water pressure which is repeatedly changed in a lifting way is used for inducing to generate a positive piezoelectric effect, and the pulse piezoelectric potential is continuously generated in the membrane in situ to generate a free radical oxidation membrane oil drop pollutant, electrostatic repulsion, dielectrophoresis force and other multiple action modes to resist membrane pollution, the membrane pollution is well prevented and controlled, and the membrane flux is basically stable for a long time.
Comparative example 1
The manganese-doped barium titanate microfiltration ceramic membrane (with the average pore diameter of about 5 mu m) is used as a water treatment non-piezoelectric filter membrane, and the dead-end membrane separation process is completed by using the constant transmembrane pressure difference of 1 kPa. The membrane separation operation is applied to the treatment of oily wastewater, and due to the adoption of a constant-pressure operation mode, the membrane cannot be induced repeatedly to generate an effective positive piezoelectric effect, the piezoelectric potential and free radicals formed in situ of the membrane are limited, membrane pollution cannot be prevented and controlled effectively in time, and the membrane flux can be subjected to continuous irreversible attenuation in a very short time.
Example 2
The polytetrafluoroethylene ultrafiltration membrane (with average pore diameter of about 50nm) after electric field polarization is used as a water treatment piezoelectric filtration membrane, the membrane separation operation is firstly carried out for rapidly increasing the pressure to 100kPa within 10s, then the operation pressure of 100kPa is kept constant for 50s, and then the pressure is rapidly reduced to below 10kPa within 10 s. And taking the pressure-changing program as a pressure-changing membrane separation operation cycle, and repeatedly executing the pressure-changing program to complete the cross-flow membrane separation process. The membrane separation operation is applied to the treatment of medical pathogenic bacteria wastewater, the piezoelectric effect is generated by the induction of repeatedly-lifting-changing pulse water pressure, the piezoelectric potential is continuously generated in the membrane in-situ, so that the membrane pollution is resisted in multiple action modes of generating free radicals to oxidize and remove pathogenic bacteria membrane pollutants, electrostatic repulsion, dielectrophoresis force and the like, the membrane flux can be maintained basically stable for a long time, and the membrane pollution is well prevented and controlled.
Comparative example 2
The polytetrafluoroethylene ultrafiltration non-piezoelectric membrane (average pore diameter about 50nm) is used as a water treatment non-piezoelectric membrane, and the cross-flow membrane separation process is completed by constant transmembrane pressure difference of 100 kPa. The membrane separation operation is applied to the treatment of medical pathogenic bacteria wastewater, and due to the adoption of a constant-pressure operation mode, an effective direct piezoelectric effect cannot be generated by repeated induction, the piezoelectric potential and the oxidation free radical formed in situ of the membrane are limited, the electrostatic repulsion and dielectrophoresis effects are weak, membrane pollution cannot be effectively prevented and controlled in time, and the membrane flux can be continuously and irreversibly attenuated in a short time.
Example 3
The polyvinylidene fluoride nanofiltration membrane (the average aperture is about 1nm) polarized by an electric field is used as a water treatment piezoelectric filtration membrane, the pressure of the membrane separation operation is quickly increased to 1000kPa within 100s, the pressure is continuously kept constant for 1000kPa for 100s, and then the pressure is quickly reduced to below 100kPa within 100 s. And taking the variable pressure program as a variable pressure membrane separation operation cycle, and repeatedly executing the variable pressure program to finish the dead-end membrane separation process. The membrane separation operation is applied to the treatment of bovine serum albumin wastewater containing nano silicon oxide particles, the piezoelectric effect is generated by the induction of repeatedly-lifting-changing pulse water pressure, the piezoelectric potential is continuously generated in the membrane in situ, membrane pollution is resisted in multiple action modes such as free radical oxidation bovine serum albumin membrane pollutants, electrostatic repulsion, dielectrophoresis force and the like, the membrane flux can be maintained to be basically stable for a long time, and the membrane pollution is well prevented and controlled.
Comparative example 3
And (3) taking a polyvinylidene fluoride nanofiltration membrane (the average pore diameter is about 1nm) as a water treatment non-piezoelectric filter membrane, and finishing the separation process of the dead-end membrane by using a constant transmembrane pressure difference of 1000 kPa. The membrane separation operation is applied to the treatment of bovine serum albumin wastewater containing nano silicon oxide particles, and a constant-pressure operation mode is adopted, so that an effective direct piezoelectric effect cannot be generated by repeated induction, the piezoelectric potential formed in situ of the membrane is limited, membrane pollution cannot be effectively prevented and controlled in time, and the membrane flux can be continuously and irreversibly attenuated in a short time.
Example 4
The polarized polyvinylidene fluoride/lead titanate composite reverse osmosis ceramic membrane (the average pore diameter is about 0.1nm) is used as a water treatment piezoelectric filter membrane, the pressure of the membrane separation operation is quickly increased to 10000kPa within 1000s, and then the pressure is quickly reduced to below 500kPa within 1000s after the operation pressure of 10000kPa is kept constant for 1000 s. And taking the pressure-changing program as a pressure-changing membrane separation operation cycle, and repeatedly executing the pressure-changing program to complete the cross-flow membrane separation process. The membrane separation operation is applied to the treatment of the lead-containing sodium chloride wastewater, the positive piezoelectric effect is generated by the induction of the repeatedly-changed pulse water pressure, the piezoelectric potential is continuously generated in the membrane in situ, the membrane flux can be maintained to be basically stable for a long time, and the membrane pollution is well prevented and controlled.
Comparative example 4
Polyvinylidene fluoride/lead titanate composite reverse osmosis ceramic membrane (average pore diameter is about 0.1nm) is used as a water treatment non-piezoelectric filter membrane, and cross flow membrane separation process is completed by 10000kPa constant transmembrane pressure difference. The membrane separation operation is applied to the treatment of the lead-containing sodium chloride wastewater, and due to the adoption of a constant-pressure operation mode, the effective positive piezoelectric effect cannot be generated by repeated induction, the piezoelectric potential formed by the in-situ membrane is limited, the membrane pollution cannot be effectively prevented and controlled in time, and the continuous irreversible attenuation can be generated in a short time.
The invention and its embodiments have been described above schematically, without limitation, and the figures shown in the drawings are only one of the embodiments of the invention, to which the practical result is not limited. Therefore, without departing from the spirit of the present invention, a person skilled in the art shall not be able to devise the similar structural modes and embodiments without inventively designing them, but shall fall within the scope of the present patent.
Claims (5)
1. A pulse water pressure response universal self-cleaning anti-membrane pollution method is characterized in that:
(1) the piezoelectric filter membrane material comprises at least one of an inorganic piezoelectric material, an organic piezoelectric material and an inorganic-organic composite piezoelectric material;
(2) the inorganic piezoelectric filter membrane material comprises barium titanate, lead zirconate titanate, lead meta-niobate, lead barium lithium niobate, lithium gallate, lithium germanate, titanium germanate, lithium niobate, lithium tantalate, zinc oxide, quartz and modified doped membrane materials thereof;
(3) the organic piezoelectric filter membrane material comprises polyvinylidene fluoride, polytetrafluoroethylene, polyamide, polypropylene and modified doped membrane materials thereof.
2. The piezoelectric filter material of claim 1, wherein: the piezoelectric filter membrane for water treatment comprises a microfiltration membrane, an ultrafiltration membrane, a nanofiltration membrane and a reverse osmosis membrane.
3. The universal self-cleaning membrane fouling resistant method of the impulse water pressure response as claimed in claim 1, wherein: the membrane separation operation is a dead-end or cross-flow operation with periodic pressure swing operation.
4. The periodic voltage varying operation of claim 3, wherein: a complete periodic variable voltage operation sequentially comprises a constant voltage operation stage, a voltage reduction operation stage and a voltage boosting operation stage. The running time of the constant-pressure running stage is 10-86400 s, and the constant-pressure running pressure range is 1-10000 kPa; the operation time of the pressure reduction operation stage is 1-1000 s, and the pressure reduction target pressure range is 0-9999 kPa. The running time of the boosting operation stage is 1-1000 s, and the range of the boosting target pressure is 1-10000 kPa.
5. Use of the method for membrane fouling resistance based on the direct piezoelectric effect according to claim 1, characterized in that:
the piezoelectric filter membrane material is used for membrane pollution control in the membrane separation process of one or more mixed wastewater of organic wastewater, inorganic wastewater, microbial wastewater, salt-containing wastewater and heavy metal wastewater.
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