CN112892230A - High-desalination polyamide composite reverse osmosis membrane for seawater desalination and preparation method thereof - Google Patents
High-desalination polyamide composite reverse osmosis membrane for seawater desalination and preparation method thereof Download PDFInfo
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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
- B01D69/125—In situ manufacturing by polymerisation, polycondensation, cross-linking or chemical reaction
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- 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
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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
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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
- B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
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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
- B01D71/06—Organic material
- B01D71/56—Polyamides, e.g. polyester-amides
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2325/00—Details relating to properties of membranes
- B01D2325/36—Hydrophilic membranes
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- 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
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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
Abstract
The invention provides a high-desalination polyamide composite reverse osmosis membrane for seawater desalination and a preparation method thereof. Because the micelle network structure has the function of a surfactant, the micelle network structure can be remained at the outermost layer of the aqueous solution and plays a role in regulating the migration behavior of the diamine monomer in the aqueous phase. The mixed micelle is easy to prepare, can obviously influence the diffusion of diamine monomers in a water phase, so that the nodule and protrusion structures on the surface of the membrane are adjusted, the surface structure of the reverse osmosis membrane is better and smoother, the defects on the surface of the membrane are further reduced, the desalination rate of the membrane is over 99.5 percent under the feed liquid of 32000ppm NaCl, and the water flux is only slightly reduced. The invention provides a novel method for preparing a high-desalination polyamide reverse osmosis membrane with complete structure and few defects, and provides a novel idea for regulating and controlling the membrane preparation process of the polyamide reverse osmosis membrane.
Description
Technical Field
The invention relates to a preparation method of a high-desalination composite polyamide reverse osmosis membrane.
Background
By 2025, reported by the united nations, approximately 52 hundred million people worldwide will have no safe drinking water and 18 hundred million people will face serious water shortage problems. Seawater accounts for 96.53 percent of the total water of the earth, seawater desalination is one of effective means for supplying supplementary water resources, wherein membrane seawater desalination is a mainstream method in the field of seawater desalination due to high water production efficiency. At present, the reverse osmosis seawater desalination technology is one of the best means for solving the growing demand of clean water production. However, the separation performance of Reverse Osmosis (RO) membranes for desalination of sea water is still to be further improved to reduce the cost of water production, but there is a "trade-off" effect between separation permeability and selectivity, which makes the improvement of the separation performance of membranes more challenging. Theoretically, in the preparation process of the RO membrane, the amine monomer in the water phase and the acyl chloride monomer in the oil phase have good interfacial reaction capability, so that the polyamide separation layer of the membrane has good crosslinking degree. However, conventional Interfacial Polymerization (IP) reactions are very rapid, and thus the MPD concentration and distribution of the interfacial reaction zone directly affects the degree of crosslinking, structural uniformity, and surface morphology of the polyamide layer, ultimately affecting the separation performance of the membrane. Because the concentration and distribution of MPD in the interfacial reaction zone mainly depend on the diffusion behavior of MPD, including migration direction and speed, the conventional interfacial polymerization process is difficult to accurately adjust the diffusion of MPD, so that the conventional interfacial polymerization process is difficult to avoid local generation of some micro defects in the polymerization process, and some incompletely reacted crosslinking areas are formed, so that the structure of the membrane is not uniform, and the separation performance of the membrane is difficult to achieve the best. Therefore, it is important that reverse osmosis membranes have a highly uniform pore size or fewer defects.
A surfactant is a molecule commonly used to modify the surface tension of a solution, which has a hydrophilic group at one end and a hydrophobic group at the other end, and which aligns at the surface energy of the solution, thus having a built-in solventDissolving, dispersing and reducing interfacial tension, and corresponding practical application. In recent years, attempts have been made to modify the IP process by surfactants, changing the degree of crosslinking and the pore structure of the polyamide to improve the separation performance of the membrane. For example, Jin et al (Liang, y.; Zhu, y.; Liu, c.; Lee, k. -r.; Hung, w. -s.; Wang, z.; Li, y.; Elimelech, m.; Jin, j.; Lin, s., Polyamide nanofiltraction membrane with high hly unit-nanometer positions for)
precision separation[J]Nature communications,2020,11(1),2015.) uses small molecule Sodium Dodecyl Sulfate (SDS) to modulate the diffusion of Piperazine (PI), thereby changing the degree of cross-linking of the membrane and the pore size of the membrane, and improving the separation performance of the membrane. Zhang et al (Tan, z.; Chen, s.; Peng, x.; Zhang, l.; Gao, c., Polyamide membranes with nanoscale bending structures for water purification [ J. ]]Science,2018,360(6388), 518-521) regulates the diffusion of Piperazine (PI) by means of macromolecular polyvinyl alcohol (PVA), and a parylene-type polyamide film having a nodular or rhomboid structure can be produced, exhibiting high water permeability. However, these are used in nanofiltration membrane (NF) modification, are not used in Reverse Osmosis (RO) membranes, and are only a single species effect. In addition, Shen et al (Q.Jia, H.Han, L.Wang, B.Liu, H.Yang, J.Shen, Effects of CTAC microorganisms on the molecular structures and separation properties of thin-film composites (TFC) membranes in formed emulsions processes [ J.]Desalinization, 2014,340(1), 30-41) modifies the membrane polyamide crosslinking by modulating the interfacial polymerization process of m-phenylenediamine (MPD) through cetyltrimethylammonium chloride (CTAC) micelles, thereby increasing the membrane selectivity to salts, in particular for divalent salts (MgCl)2) Has good separation effect.
Disclosure of Invention
The invention aims to provide a high-desalination polyamide composite reverse osmosis membrane and a preparation method thereof, aiming at the defects of the existing reverse osmosis membrane for seawater desalination. By selecting a three-dimensional network-like micelle structure which is composed of triblock ether polymer ((PEO)100-(PPO)65-(PEO)100PF127) and dodecaneSodium Dodecyl Sulfate (SDS) self-assembles in aqueous solution to form mixed micelles. Amine monomers in aqueous solutions are readily adsorbed near the surface of the aqueous solution by the micellar network prior to the interfacial polymerization process. When an organic phase solution is added, the micelle network space is utilized to selectively regulate and control the diffusion of m-phenylenediamine (MPD), and the polyamide composite reverse osmosis membrane with high desalination degree is prepared.
In order to achieve the purpose, the invention adopts the following technical scheme: a preparation method of a high-desalting polyamide composite reverse osmosis membrane comprises the steps of firstly preparing a mixed aqueous solution with a three-dimensional network micelle structure and polyamine, and utilizing the network micelle structure to adjust the diffusion path and the diffusion rate of a polyamine monomer in an aqueous phase, so that the preparation of the polyamide composite reverse osmosis membrane with a uniform structure and few defects is realized, and the specific steps are as follows:
(1) pluronic F127(PF127) and Sodium Dodecyl Sulfate (SDS) are mixed in an aqueous phase solution according to a certain proportion to form a micelle solution, wherein the concentration of the PF127 is 0.05-0.2 wt%, and the concentration of the SDS is 0.05 wt%; and then adding a polyamine monomer, an acid-binding agent and a pH regulator, wherein the concentration of the polyamine monomer is 1-3 wt%, and the concentrations of the acid-binding agent and the pH regulator are both 0-5 wt%.
(2) Pouring the solution prepared in the step (1) on a polysulfone membrane for 1-8 minutes, and then placing the membrane in a ventilated place to dry in the shade.
(3) Pouring 0.05-0.3 wt% of polyacyl chloride monomer solution onto the polysulfone membrane dried in the shade in the step (2), reacting for 40-100 seconds, removing the redundant solution on the surface of the porous support membrane, and then drying the membrane in the shade in a ventilated place.
(4) And (4) drying the membrane obtained in the step (3) at the temperature of 60-100 ℃ for 5-20 minutes to obtain the high-desalination polyamide composite reverse osmosis membrane.
Further, in the step (1), the concentration of Pluronic F127 and the concentration of sodium lauryl sulfate are both 0.05 wt%, the concentration of m-phenylenediamine is 2 wt%, and the film dipping time is 5 minutes.
Further, in the step (1), the acid-binding agent is triethylamine, sodium hydroxide, potassium hydroxide, lithium hydroxide, or the like, and the pH adjusting agent is camphorsulfonic acid, hydrochloric acid, sodium hydroxide, tertiary sodium phosphate, or the like.
Further, in the step (1), the polyamine monomer is prepared by mixing any one or more of m-phenylenediamine, p-phenylenediamine, sym-phenylenediamine, 5-methyl-m-phenylenediamine, 2-hydroxy-propane diamine and the like in any proportion.
Further, in the step (2), the drying time in the shade is 5-10 minutes, wherein the higher the concentration of Pluronic F127 and sodium dodecyl sulfate is, the longer the drying time in the shade of the film is required.
Further, in the step (3), the polybasic acyl chloride monomer is one or more of trimesoyl chloride, terephthaloyl chloride, m-benzoyl chloride and the like which are mixed according to any proportion.
Further, in the step (3), the organic solvent for dissolving the polybasic acyl chloride monomer is formed by mixing one or more of Isopar G, n-hexane, n-heptane or n-decane according to any proportion.
Further, in the step (3), the reaction time in the polyacyl chloride monomer solution is 1 minute.
Further, in the step (4), the drying temperature of the oven is 80 ℃ and the time is 10 minutes.
Further, the high-desalination polyamide composite reverse osmosis membrane prepared by the method is applied to seawater desalination.
The invention has the beneficial effects that: utilizes the combination of hydrophobic block parts (PPO) in an amphiphilic block polymer (PF127) and hydrophobic chains between alkyl groups on SDS, and hydrophilic ends (SO) of the SDS4-head-outward property, thereby self-assembling in aqueous solution to form a micelle; the micelle has longer tentacles (PEO), so that a three-dimensional network-like micelle structure can be formed. In addition, the network structure has good hydrophilicity (-C-O-C-), certain gaps and a good regulating effect on the diffusion of polyamine monomers such as m-phenylenediamine (MPD). Due to the structural action, the polyamine monomer can enter the oil phase from the aqueous phase solution to react with the polybasic acyl chloride monomer such as trimesoyl chloride (TMC) more quickly and uniformly, so that the two monomers (MPD and TMC) react more completely, the crosslinking degree is higher, the film defects are fewer, and the film surface is more uniform and smooth. Thereby further reducingThe defect of the membrane surface improves the desalination rate of the membrane.
Drawings
FIG. 1 is an atomic force microscope image of the three-dimensional network-like micelles (d, e) formed in example 3 of the present invention and the other network structures (a, b) formed in example 2, and c, f are the widths of the other network structures and micelle gaps measured, respectively.
FIG. 2 is a flow chart of a polyamide composite reverse osmosis membrane according to an embodiment of the present invention, which is a flow chart of preparation of example 3.
FIG. 3 is an electron microscope image of a polyamide composite reverse osmosis membrane provided in an embodiment of the present invention, wherein a-d and e-h are respectively a scanning electron microscope and a transmission electron microscope image of the reverse osmosis membrane, and the membrane preparation is specifically examples 1 to 4.
Detailed Description
FIG. 2 is a flow diagram of a process for preparing a polyamide composite reverse osmosis membrane according to the present invention. First, micelles of a network structure were formed by adjusting the ratio between Pluronic F127 and sodium lauryl sulfate, and then combined with a diamine monomer such as m-phenylenediamine to prepare an aqueous solution. Because the network structure has the function of a surfactant, the network structure can remain in the outermost layer of the aqueous solution and play a role in regulating the signing behavior of the diamine monomer in the aqueous phase, thereby obviously improving the diffusion path and the diffusion rate of the polyamine monomer in the aqueous phase.
The following detailed description will be given to make the invention more clear in conjunction with specific examples, but the invention and the scope of the patent are not limited to the following examples, and all the normal modifications thereof should fall within the scope of the invention.
Example 1:
4g of camphorsulfonic acid and 2g of m-phenylenediamine were dissolved in 98ml of deionized water in this order, and finally 2g of triethylamine was used to adjust the pH. Pouring the solution into the upper surface of a prepared polysulfone porous supporting layer for 5 minutes, pouring out the redundant solution, and placing the solution under an ultraclean workbench for 6 minutes and the like for drying in the shade; then 0.15G of Isopar G solution of trimesoyl chloride 100ml is poured into the reactor to carry out interfacial polymerization, the reactor is placed under a clean bench for 10 minutes and dried in the shade, and then the reactor is placed in an air drying oven at 80 ℃ for 10 minutes to obtain the polyamide composite reverse osmosis membrane which is marked as M0 membrane.
Example 2:
0.05g of Sodium Dodecyl Sulfate (SDS) is firstly put into 98ml of deionized water, after the sodium dodecyl sulfate is fully dissolved, 4g of camphorsulfonic acid and 2g of m-phenylenediamine are fully dissolved in turn, and finally 2g of triethylamine is used for adjusting the pH value. Pouring the solution into the upper surface of a prepared polysulfone porous supporting layer for 5 minutes, pouring out the redundant solution, and placing the solution under an ultraclean workbench for 6 minutes and the like for drying in the shade; then 0.15G of Isopar G solution of trimesoyl chloride 100ml is poured into the reactor to carry out interfacial polymerization, the reactor is placed under a clean bench for 10 minutes and dried in the shade, and then the reactor is placed in an air drying oven at 80 ℃ for 10 minutes to obtain the polyamide composite reverse osmosis membrane which is marked as M1 membrane.
Example 3:
0.05g of Pluronic F-127(PF127) was placed in 98ml of deionized water, and after the solution was sufficiently dissolved, 4g of camphorsulfonic acid and 2g of m-phenylenediamine were dissolved in this order, and finally 2g of triethylamine was used to adjust the pH. Pouring the solution into the upper surface of a prepared polysulfone porous supporting layer for 5 minutes, pouring out the redundant solution, and placing the solution under an ultraclean workbench for 6 minutes and the like for drying in the shade; then 0.15G of Isopar G solution of trimesoyl chloride 100ml is poured into the reactor to carry out interfacial polymerization, the reactor is placed under a clean bench for 10 minutes and dried in the shade, and then the reactor is placed in an air drying oven at 80 ℃ for 10 minutes to obtain the polyamide composite reverse osmosis membrane which is marked as M2 membrane.
Example 4:
0.05g of Pluronic F-127(PF127) and 0.05g of Sodium Dodecyl Sulfate (SDS) were initially placed in 98ml of deionized water and allowed to dissolve sufficiently to form a micellar network; then, 4g of camphorsulfonic acid and 2g of m-phenylenediamine were dissolved sufficiently in this order, and finally, 2g of triethylamine was used to adjust the pH. Pouring the solution into the upper surface of a prepared polysulfone porous supporting layer for 5 minutes, pouring out the redundant solution, and placing the solution under an ultraclean workbench for 6 minutes and the like for drying in the shade; then 0.15G of Isopar G solution of trimesoyl chloride 100ml is poured into the reactor to carry out interfacial polymerization, the reactor is placed under a clean bench for 10 minutes and dried in the shade, and then the reactor is placed in an air drying oven at 80 ℃ for 10 minutes to obtain the polyamide composite reverse osmosis membrane which is marked as M3 membrane.
Example 5:
in addition to the above-mentioned proportion of Pluronic F-127(PF127) at a concentration of 0.1g to 0.25g and Sodium Dodecyl Sulfate (SDS), the other conditions were consistent with those of example 4 and were designated as M4, M5, M6 and M7 membranes.
Membrane characterization and Performance testing
FIG. 1(a) is a figure of PF127 in an aqueous solution in example 3, which has a dense layer on the surface layer and no micelle formation; the enlarged view of FIG. 1(b) shows a larger gap spacing, about 150 nm. FIG. 1(d) is the appearance of the micelle formed by self-assembly of PF127 and SDS in aqueous solution in example 4, and it can be seen that the mixed micelle network has multiple layers, the micelle is uniformly dispersed, and PEO chains are stretched; it can be seen from the enlarged view of FIG. 1(e) that the micelle is regular in shape, like a sphere, and the PEO interchain gap is narrow at about 60 nm.
FIGS. 3a-h are scanning and transmission electron microscope images of films prepared in examples 1-4, respectively, from which it can be seen that the film surface structure varied more, the M3 film thickness decreased, and the film surface nodular pattern was greater and more uniform.
The separation performance of the membranes was evaluated by a cross-flow filtration test system. Installing a membrane to be tested in a membrane pool of a flat plate membrane device, and pre-pressing the membrane for 1h by using 32000ppm and 20L NaCl solution under the pressure of 5.5MPa and at the temperature of 25 ℃; after the water flux reached a steady state, the permeability of the membrane was tested and the results are shown in table 1. According to the test results, PF127/SDS regulation can obviously improve the desalination of the membrane, the membrane separation is optimal when the concentration is 0.05 wt%/0.05 wt%, the desalination rate is more than 99.5%, and the flux also reaches 34.3 L.m-2·h-1And can be widely applied to seawater treatment.
The membrane separation performance was measured at 25 ℃ under 5.5MPa using 32000ppm, 20L NaCl solution, as shown in the following table:
| types of membranes (PF127/SDS) | Water flux (L.m)-2·h-1) | Salt rejection (%) |
| M0(0wt％/0wt％) | 36.48 | 99.33 |
| M1(0wt％/0.05wt％) | 38.38 | 99.44 |
| M2(0.05wt％/0wt％) | 27.14 | 99.02 |
| M3(0.05wt％/0.05wt％) | 34.30 | 99.54 |
| M4(0.10wt％/0.05wt％) | 31.31 | 99.45 |
| M5(0.15wt％/0.05wt％) | 30.13 | 99.36 |
| M6(0.20wt％/0.05wt％) | 28.99 | 99.55 |
| M7(0.25wt％/0.05wt％) | 22.61 | 99.43 |
Claims (9)
1. A preparation method of a high-desalting polyamide composite reverse osmosis membrane specifically comprises the following steps:
(1) pluronic F127(PF127) and Sodium Dodecyl Sulfate (SDS) are mixed in an aqueous phase solution according to a certain proportion to form a micelle solution, wherein the concentration of the PF127 is 0.05-0.2 wt%, and the concentration of the SDS is 0.05 wt%; and then adding a polyamine monomer, an acid-binding agent and a pH regulator, wherein the concentration of the polyamine monomer is 1-3 wt%, and the concentrations of the acid-binding agent and the pH regulator are both 0-5 wt%.
(2) Pouring the solution prepared in the step (1) on a polysulfone membrane for 1-8 minutes, and then drying in the shade.
(3) Pouring 0.05-0.3 wt% of polyacyl chloride monomer solution on the polysulfone membrane dried in the shade in the step (2), reacting for 40-100 seconds, and then drying in the shade.
(4) And (4) drying the membrane obtained in the step (3) at the temperature of 60-100 ℃ for 5-20 minutes to obtain the high-desalination polyamide composite reverse osmosis membrane.
2. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (1), the concentration of Pluronic F127 and the concentration of sodium dodecyl sulfate are both 0.05 wt%, the concentration of m-phenylenediamine is 2 wt%, and the film immersion time is 5 minutes.
3. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (1), the acid-binding agent is triethylamine, sodium hydroxide, potassium hydroxide, lithium hydroxide and the like, and the pH regulator is camphorsulfonic acid, hydrochloric acid, sodium hydroxide, tertiary sodium phosphate and the like.
4. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (1), the polyamine monomer is prepared by mixing one or more of m-phenylenediamine, p-phenylenediamine, trimesamine, 5-methyl-m-phenylenediamine, 2-hydroxy-propane diamine and the like according to any proportion.
5. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (2), the drying time in the shade is 5-10 minutes, wherein the higher the concentration of Pluronic F127 and sodium dodecyl sulfate is, the longer the drying time in the shade of the film is required.
6. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (3), the polybasic acyl chloride monomer is one or more of trimesoyl chloride, paraphenyl chloride, m-benzoyl chloride and the like which are mixed according to any proportion.
7. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (3), the organic solvent for dissolving the polyacyl chloride monomer is formed by mixing one or more of Isopar G, n-hexane, n-heptane or n-decane according to any proportion.
8. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (3), the reaction time in the polyacyl chloride monomer solution is 1 minute.
9. The highly desalinated polyamide composite reverse osmosis membrane according to claim 1, wherein: in the step (4), the temperature is 80 ℃ and the time is 10 minutes.
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| US11502322B1 (en) | 2022-05-09 | 2022-11-15 | Rahul S Nana | Reverse electrodialysis cell with heat pump |
| US11855324B1 (en) | 2022-11-15 | 2023-12-26 | Rahul S. Nana | Reverse electrodialysis or pressure-retarded osmosis cell with heat pump |
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