CN114130216A - Pressure-resistant polysulfone-based membrane and preparation method thereof - Google Patents

Pressure-resistant polysulfone-based membrane and preparation method thereof Download PDF

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Publication number
CN114130216A
CN114130216A CN202111509263.1A CN202111509263A CN114130216A CN 114130216 A CN114130216 A CN 114130216A CN 202111509263 A CN202111509263 A CN 202111509263A CN 114130216 A CN114130216 A CN 114130216A
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polysulfone
pressure
resistant
pore
membrane
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张倩茹
赵岳轩
王乐译
朱娜娜
王新艳
王志勇
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SHANDONG ZHAOJIN MOTIAN CO Ltd
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SHANDONG ZHAOJIN MOTIAN CO Ltd
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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
    • B01D67/0002—Organic membrane manufacture
    • B01D67/0009—Organic membrane manufacture by phase separation, sol-gel transition, evaporation or solvent quenching
    • B01D67/0016—Coagulation
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/02—Reverse osmosis; Hyperfiltration ; Nanofiltration
    • B01D61/025—Reverse osmosis; Hyperfiltration
    • 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
    • B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
    • 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
    • B01D71/06—Organic material
    • B01D71/66—Polymers having sulfur in the main chain, with or without nitrogen, oxygen or carbon only
    • B01D71/68—Polysulfones; Polyethersulfones
    • 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
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/08—Seawater, e.g. for desalination
    • 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)
  • Chemical Kinetics & Catalysis (AREA)
  • Water Supply & Treatment (AREA)
  • Dispersion Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Environmental & Geological Engineering (AREA)
  • Organic Chemistry (AREA)
  • Nanotechnology (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)

Abstract

The invention relates to a pressure-resistant polysulfone base membrane, which comprises a non-woven fabric layer and a polysulfone base layer prepared by coating polysulfone solution on the non-woven fabric, wherein the polysulfone solution comprises the following components in percentage by weight: 15-25% of polysulfone, 4-18% of pore-forming agent, 0.04-0.2% of surfactant and the balance of solvent. The invention also relates to a preparation method of the pressure-resistant polysulfone based membrane, which comprises the following steps: 1) preparing polysulfone solution according to weight percentage, dissolving uniformly under certain dissolving condition, 2) coating the dissolved polysulfone solution on non-woven fabrics, and placing the non-woven fabrics in a coagulating bath for phase change solidification to form the pressure-resistant polysulfone base membrane. The polysulfone base membrane has uniform pores, the pore diameter is 10-50 nanometers, the water yield is 800-1200L/square meter/h, the cross section structure of the base membrane is a three-dimensional network frame structure, the pressure resistance is improved, the polysulfone base membrane is difficult to deform when running under the pressure of 5MPa, and the polysulfone base membrane is suitable for being used as a base membrane of a brackish water reverse osmosis membrane, a reverse osmosis membrane for high-salinity wastewater treatment and a sea water desalination reverse osmosis membrane.

Description

Pressure-resistant polysulfone-based membrane and preparation method thereof
Technical Field
The invention relates to the technical field of reverse osmosis membranes, in particular to a pressure-resistant polysulfone base membrane and a preparation method thereof.
Background
The reverse osmosis technology is a filtration technology for separating water and solutes in water by pressure drive, and is widely applied to the fields of high-purity water preparation, medical water preparation, seawater desalination, brackish water desalination, sewage recycling and the like in the electronic industry. With the shortage of fresh water resources and the increasing water pollution, reverse osmosis technology plays an increasingly important role in water purification.
The reverse osmosis membrane is a thin-layer medium for providing separation in the reverse osmosis technology and is a core component of the reverse osmosis technology. The currently mainstream reverse osmosis membrane is a thin semipermeable membrane with a three-layer structure manufactured by adopting an interfacial polymerization process, wherein the three-layer structure comprises a non-woven fabric layer, a polysulfone base layer and a polyamide desalting layer (separation layer). Wherein the non-woven fabric provides basic mechanical strength; the desalting layer is arranged on the uppermost layer and plays a role in separating ions; the polysulfone base layer is positioned in the middle of the non-woven fabric and the desalting layer, plays a role in porosity transition, provides porosity mechanical support for the desalting layer, and prevents the ultrathin polyamide layer from cracking under pressure. As the transition layer, the polysulfone base layer has good supporting effect, proper surface aperture size and good water permeability.
At present, the production technology of the reverse osmosis membrane in China is mature day by day, and particularly in the preparation of the low-pressure reverse osmosis membrane, the existing low-pressure reverse osmosis membrane has higher water yield and salt rejection rate and is widely applied to the field of water purification on a large scale. However, in a high-salt and high-pressure operation environment, the performance of the reverse osmosis membrane is still unstable, and the reverse osmosis membrane is particularly applied to the field of seawater desalination.
As is well known in the art, in the filtration of water and solutes in water, the pressure applied to the body of water is higher than the osmotic pressure of water that spontaneously permeates through the membrane due to concentration differences, and we generally refer to the higher difference as the transmembrane pressure difference. The higher the solute concentration of the water body to be separated, the larger the transmembrane pressure difference. When the transmembrane pressure difference exceeds the limit value of the mechanical strength of the reverse osmosis membrane, the polysulfone base layer is flattened, and pores among layers are tightly attached together, so that the membrane loses a flow channel of water, and the water yield is reduced.
The polysulfone infrastructure determines the pressure resistance. According to the order of pressure resistance from small to large, the common structure of the polysulfone base layer is a large bottom hole structure shown in fig. 1, a sponge chamber-shaped structure shown in fig. 2 and a three-dimensional network framework structure shown in fig. 3. Currently, the existing commercial reverse osmosis membrane basic structure is basically the first two structures.
Disclosure of Invention
Therefore, the invention provides a pressure-resistant polysulfone based membrane with a three-dimensional network framework structure and strong pressure resistance and a preparation method thereof.
In order to achieve the above objects, according to one aspect of the present invention, there is provided a pressure-resistant polysulfone based film, characterized by comprising a nonwoven fabric layer, and a polysulfone base layer prepared by coating a polysulfone solution on the nonwoven fabric layer, wherein the polysulfone solution comprises, in weight percent:
15-25% of polysulfone, 4-18% of pore-forming agent, 0.04-0.2% of surfactant and the balance of solvent.
Further, the polysulfone is bisphenol a type polysulfone, polyethersulfone or polyarylsulfone. The polysulfone content is related to the pore density and affects the strength of the membrane skeleton. Less than 15% of the base film layer has larger pores, and a large bottom hole structure is easy to form; and more than 25 percent of the pores of the base film layer are too small, so that a cavity structure is easily formed.
Furthermore, the pore-forming agent is one or a mixture of a small molecular pore-forming agent and a high molecular pore-forming agent, or a mixture of the small molecular pore-forming agent and the high molecular pore-forming agent;
the surfactant is sodium dodecyl benzene sulfonate, sodium dodecyl sulfate, tween, span, alkyl ether phosphate or phenol ether phosphate; the addition of the surfactant can adjust the stable state of the polymer component and the pore-forming agent component dissolved in the solvent, so as to achieve microphase uniformity. Addition levels below 0.04% have no significant effect; the addition amount is more than 0.2 percent, and the surfactant is difficult to remove completely after the base membrane is formed, thus having adverse effect on the preparation of the reverse osmosis membrane by interfacial polymerization.
The solvent is one or a mixture of N, N-dimethylformamide, N-dimethylacetamide and N-methyl-2-pyrrolidone.
Still further, the small molecule pore-forming agent is small molecule alcohol, ether, ketone, ester compound, such as ethanol, propanol (including n-propanol and isopropanol), ethylene glycol, glycerol, diethyl ether, ethylene glycol methyl ether, acetone, butanone or ethyl acetate; the polymer pore-forming agent is polyethylene glycol, polyvinyl alcohol or polyvinylpyrrolidone, etc. The pore-forming agent is added to adjust the open pore state of the surface during the molding of the base film. When the addition amount is less than 4%, the pore size distribution of the surface is wide, and macropores are easily generated, so that the internal structure is influenced; when the addition amount is more than 18%, the dissolving capacity of the solvent for polysulfone is reduced, the solution is not easy to be dissolved uniformly, and the strength of the base film is poor.
According to another aspect of the present invention, there is provided a method for preparing a pressure-resistant polysulfone-based film, comprising the steps of:
1) preparing polysulfone solution, and dissolving uniformly under certain dissolving condition,
the polysulfone solution comprises the following components in percentage by weight: 15-25% of polysulfone, 4-18% of pore-forming agent, 0.04-0.2% of surfactant and the balance of solvent;
2) and coating the dissolved polysulfone solution on non-woven fabrics, and placing the non-woven fabrics in a coagulating bath for phase change solidification to form the pressure-resistant polysulfone base membrane.
Further, in the step 1), the certain dissolution conditions are:
dissolution temperature: 40-90 ℃;
when the dissolving temperature is lower than 40 ℃, the dissolved polysulfone molecular chain cannot be well stretched, the polysulfone solution cannot achieve micro-phase uniformity, the solution has a turbidity phenomenon, and the prepared base membrane has poor mechanical strength; above 90 ℃, partial addition of substances generates denaturation, the solution color deepens, and the pore structure of the basement membrane changes.
And (3) adding sequence: firstly adding the liquid materials in the components, then adding the solid additives in the components, and finally adding the polysulfone;
stirring speed: the stirring speed is determined according to the structure of the stirring paddle used in the dissolution.
And further, in the adding sequence, firstly adding the liquid material, dissolving for 15-30 min, then adding the solid additive, dissolving for 30-60 min, and finally adding polysulfone.
Furthermore, in the stirring speed, if an inclined blade type stirring paddle is used, the stirring speed is 120-200 r/min; if a disk-type stirring paddle is used, the stirring speed is 1000-3000 r/min.
According to the adding sequence, materials in the solution after the polysulfone is dissolved can be uniformly mixed at a molecular level; if the stirring speed is lower than the lower limit value, the solution is not easy to be uniformly dissolved, and a turbid phenomenon exists; if the molecular weight is higher than the upper limit value, the molecular chain is partially broken under the shearing force, and the mechanical strength of the film is influenced.
Still further, in the step 2), the thickness of the polysulfone solution coating is 15-50 microns.
If the coating thickness is less than 15 micrometers, the coating control requirement is too high because the coating is too thin, and the operation is not easy; if the thickness of the coating is more than 50 μm, pores of the lower layer of the polysulfone layer become sparse and the strength becomes poor.
Still further, in the step 2), the temperature of the coagulation bath is set to be 5 to 25 ℃.
The coagulation bath temperature affects the structure of the basement membrane and the surface pore size. If the temperature is lower than 5 ℃, the surface open pore is too small, and the water yield is low; if the temperature is higher than 25 ℃, the surface rapid forming hinders the solvent replacement in the polysulfone solution, and the formed base membrane has a big bottom hole structure.
Still further, in the above step 1):
the polysulfone is bisphenol A type polysulfone, polyether sulfone or polyarylsulfone;
the pore-forming agent is one or a mixture of a plurality of micromolecule pore-forming agents or macromolecule pore-forming agents, or a mixture of the micromolecule pore-forming agents and the macromolecule pore-forming agents;
the surfactant is sodium dodecyl benzene sulfonate, sodium dodecyl sulfate, tween, span, alkyl ether phosphate or phenol ether phosphate;
the solvent is one or a mixture of N, N-dimethylformamide, N-dimethylacetamide and N-methyl-2-pyrrolidone.
Compared with the prior art, the invention has the following beneficial effects:
the polysulfone base membrane prepared by the method has uniform pores, the pore diameter range is 10-50 nanometers, the water yield is 800-1200L/square meter/h, the cross section structure of the base membrane is a three-dimensional network frame structure, the pressure resistance is improved, the base membrane is not easy to deform when the base membrane is operated under the pressure of 5MPa, and the base membrane is particularly suitable for being used as a bitter saline water reverse osmosis membrane, a reverse osmosis membrane for high-salinity wastewater treatment and a sea water desalination reverse osmosis membrane.
These and other aspects of the invention are apparent from and will be elucidated with reference to the embodiments described hereinafter.
Description of the drawings:
the structure and further objects and advantages of the present invention will be better understood by the following description taken in conjunction with the accompanying drawings, in which like reference characters identify like elements, and in which:
FIG. 1 is a schematic view showing the microstructure of a conventional polysulfone substrate having a large-bottomed pore structure;
FIG. 2 is a schematic view showing the microstructure of a polysulfone base layer of a conventional sponge chamber-like structure;
fig. 3 is a schematic view showing the microstructure of a polysulfone base layer of a conventional three-dimensional network framework structure.
Detailed Description
The pressure-resistant polysulfone-based film and the process for producing the same according to the present invention will be described in detail with reference to the following examples:
example 1
Step 1): preparing polysulfone solution, and dissolving uniformly under certain dissolving condition,
the polysulfone solution comprises the following components in percentage by weight: 17% of bisphenol A polysulfone, 8% of ethanol as a pore-forming agent, 0.05% of sodium dodecylbenzenesulfonate as a surfactant, and 74.95% of N, N-dimethylformamide as a solvent
The certain dissolution conditions were carried out as follows:
dissolution temperature: 40 ℃;
and (3) adding sequence: firstly adding the liquid materials (namely N, N-dimethylformamide and ethanol) in the components, dissolving for 15min, then adding the solid additive (namely sodium dodecyl benzene sulfonate) in the components, dissolving for 30min, and finally adding polysulfone;
stirring speed: an inclined blade type stirring paddle is used, and the stirring speed is 150 r/min.
Step 2): coating the dissolved polysulfone solution on non-woven fabric, placing the non-woven fabric in a coagulating bath for phase change solidification to form a pressure-resistant polysulfone basal membrane, wherein,
the thickness of the polysulfone solution coating is 30 microns;
the coagulation bath temperature was set at 15 ℃.
The respective solution compositions and the relevant process parameters for all examples 1 to 5, including example 1, are given in table 1 below.
TABLE 1 polysulfone solutions of examples 1-5 each composition and related Process parameters
Example 1 Example 2 Example 3 Example 4 Example 5
Polysulfone Bisphenol A polysulfone 17% 20 percent of polyether sulfone Polyarylsulfone and other polymers 15% Bisphenol A polysulfone 17% Polyether sulfone 25%
Pore-forming agent 8 percent of ethanol N-propanol 18% Ethylene glycol 6% 4 percent of glycerol 10 percent of polyethylene glycol
Surface active agent Sodium dodecyl benzene sulfonate 0.05% Sodium dodecyl sulfate 0.04% Tween 0.2% 0.06 percent of span Alkyl ether phosphate 0.1%
Solvent(s) 74.95 percent of N, N-dimethylformamide N, N-dimethylacetamide 61.96 78.8 percent of N-methyl-2-pyrrolidone 78.94% of N, N-dimethylacetamide N, N-dimethylformamide 64.9%
Dissolution temperature 40℃ 60℃ 80℃ 90℃ 50℃
Polysulfone solution coating thickness 30 micron 40 micron 50 micron 20 micron 15 micron
Temperature of coagulation bath 15℃ 20℃ 10℃ 5℃ 25℃
Pore size of polysulfone-based membrane 28 nm 23 nm 51 nm 46 nm 12 nm
Water yield 950L/㎡/h 832L/㎡/h 1207L/㎡/h 1048L/㎡/h 810L/㎡/h
Withstand pressure 3.5MPa 4MPa 2.5MPa 3.5MPa 5MPa
As can be seen from the examples 1-5 listed in the table 1 above, the polysulfone base membrane prepared by the method disclosed by the invention can be used for preparing the polysulfone base membrane with uniform pores, the pore diameter range is 10-50 nanometers, the water yield is 800-1200L/square meter/h, the cross section structure of the base membrane is a three-dimensional network frame structure, the pressure resistance is improved, the polysulfone base membrane is not easy to deform when the polysulfone base membrane is operated under the pressure of 2.5-5 MPa, and the polysulfone base membrane is particularly suitable for being used as a brackish water reverse osmosis membrane, a reverse osmosis membrane for high-salinity wastewater treatment and a base membrane for sea water desalination.
While the invention has been described with respect to the foregoing technical disclosure and features, it will be understood that various changes and modifications in the above structure, including combinations of features disclosed herein either individually or as claimed, and obviously including other combinations of such features, may be resorted to by those skilled in the art, without departing from the spirit of the invention. Such variations and/or combinations are within the skill of the art to which the invention pertains and are within the scope of the following claims.

Claims (10)

1. The pressure-resistant polysulfone base film is characterized by comprising a non-woven fabric layer and a polysulfone base layer prepared by coating polysulfone solution on the non-woven fabric layer, wherein the polysulfone solution comprises the following components in percentage by weight:
15-25% of polysulfone, 4-18% of pore-forming agent, 0.04-0.2% of surfactant and the balance of solvent.
2. The pressure resistant polysulfone based membrane according to claim 1, wherein the polysulfone is bisphenol a polysulfone, polyethersulfone or polyarylsulfone.
3. The pressure resistant polysulfone based membrane according to claim 2, wherein the pore former is one or a mixture of small molecule pore former and high molecule pore former, or a mixture of small molecule pore former and high molecule pore former; the surfactant is sodium dodecyl benzene sulfonate, sodium dodecyl sulfate, tween, span, alkyl ether phosphate or phenol ether phosphate; the solvent is one or a mixture of N, N-dimethylformamide, N-dimethylacetamide and N-methyl-2-pyrrolidone.
4. A preparation method of a pressure-resistant polysulfone based membrane is characterized by comprising the following steps:
1) preparing polysulfone solution, and dissolving uniformly under certain dissolving condition,
the polysulfone solution comprises the following components in percentage by weight: 15-25% of polysulfone, 4-18% of pore-forming agent, 0.04-0.2% of surfactant and the balance of solvent;
2) and coating the dissolved polysulfone solution on non-woven fabrics, and placing the non-woven fabrics in a coagulating bath for phase change solidification to form the pressure-resistant polysulfone base membrane.
5. The method for producing a pressure-resistant polysulfone based membrane according to claim 4, wherein in step 1), the certain dissolution conditions are:
dissolution temperature: 40-90 ℃;
and (3) adding sequence: firstly adding the liquid materials in the components, then adding the solid additives in the components, and finally adding the polysulfone;
stirring speed: the stirring speed is determined according to the structure of the stirring paddle used in the dissolution.
6. The method for preparing a pressure-resistant polysulfone-based membrane according to claim 5, wherein in the adding sequence, a liquid material is added first to dissolve for 15-30 min, then a solid additive is added to dissolve for 30-60 min, and finally polysulfone is added.
7. The method for producing a pressure-resistant polysulfone based membrane according to claim 5, wherein the stirring speed is 120 to 200r/min if a pitched blade type stirring blade is used; if a disk-type stirring paddle is used, the stirring speed is 1000-3000 r/min.
8. The method for preparing a pressure-resistant polysulfone based membrane according to any of claims 4-7, wherein in step 2), the thickness of polysulfone solution coating is 15-50 μm.
9. The method for preparing a pressure-resistant polysulfone based film as claimed in claim 8, wherein in the step 2), the coagulation bath temperature is set to 5-25 ℃.
10. The method for producing a pressure-resistant polysulfone-based film according to claim 4, wherein the polysulfone is bisphenol A-type polysulfone, polyethersulfone or polyarylsulfone; the pore-forming agent is one or a mixture of a plurality of micromolecule pore-forming agents or macromolecule pore-forming agents, or a mixture of the micromolecule pore-forming agents and the macromolecule pore-forming agents; the surfactant is sodium dodecyl benzene sulfonate, sodium dodecyl sulfate, tween, span, alkyl ether phosphate or phenol ether phosphate; the solvent is one or a mixture of N, N-dimethylformamide, N-dimethylacetamide and N-methyl-2-pyrrolidone.
CN202111509263.1A 2021-12-10 2021-12-10 Pressure-resistant polysulfone-based membrane and preparation method thereof Pending CN114130216A (en)

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Publication number Priority date Publication date Assignee Title
CN1883779A (en) * 2006-05-19 2006-12-27 广州美能材料科技有限公司 Process for preparing composite hollow fiber membrane
CN1899678A (en) * 2005-07-19 2007-01-24 天津工业大学 Method for producing hollow fiber film
CN1935338A (en) * 2006-09-22 2007-03-28 中国科学院长春应用化学研究所 Aromatic polyamide reverse osmose composite membrane
CN101733022A (en) * 2009-03-12 2010-06-16 北京碧水源膜科技有限公司 High-strength polyvinylidene fluoride hollow fiber membrane and production method thereof
US20200114317A1 (en) * 2015-11-24 2020-04-16 Oasys Water LLC Support layers for forward osmosis membranes

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1899678A (en) * 2005-07-19 2007-01-24 天津工业大学 Method for producing hollow fiber film
CN1883779A (en) * 2006-05-19 2006-12-27 广州美能材料科技有限公司 Process for preparing composite hollow fiber membrane
CN1935338A (en) * 2006-09-22 2007-03-28 中国科学院长春应用化学研究所 Aromatic polyamide reverse osmose composite membrane
CN101733022A (en) * 2009-03-12 2010-06-16 北京碧水源膜科技有限公司 High-strength polyvinylidene fluoride hollow fiber membrane and production method thereof
US20200114317A1 (en) * 2015-11-24 2020-04-16 Oasys Water LLC Support layers for forward osmosis membranes

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Application publication date: 20220304