CN115367838A - Novel membrane contactor system for recovering dissolved methane in anaerobic effluent - Google Patents
Novel membrane contactor system for recovering dissolved methane in anaerobic effluent Download PDFInfo
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- 230000010412 perfusion Effects 0.000 claims abstract description 57
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- 239000007789 gas Substances 0.000 claims abstract description 26
- 239000012159 carrier gas Substances 0.000 claims abstract description 17
- 230000002572 peristaltic effect Effects 0.000 claims abstract description 8
- 238000003860 storage Methods 0.000 claims abstract description 6
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- 210000004379 membrane Anatomy 0.000 claims description 89
- 239000002351 wastewater Substances 0.000 claims description 23
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- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 11
- 210000002469 basement membrane Anatomy 0.000 claims description 3
- -1 polytetrafluoroethylene Polymers 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 2
- 239000000741 silica gel Substances 0.000 claims description 2
- 229910002027 silica gel Inorganic materials 0.000 claims description 2
- 239000004205 dimethyl polysiloxane Substances 0.000 claims 1
- 229920001600 hydrophobic polymer Polymers 0.000 claims 1
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- 238000011084 recovery Methods 0.000 abstract description 8
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- 239000003463 adsorbent Substances 0.000 abstract description 2
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- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
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- 238000000034 method Methods 0.000 description 6
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- 239000013557 residual solvent Substances 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- 239000010802 sludge Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229910021642 ultra pure water Inorganic materials 0.000 description 1
- 239000012498 ultrapure water Substances 0.000 description 1
- 238000009280 upflow anaerobic sludge blanket technology Methods 0.000 description 1
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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
-
- 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
-
- 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
- B01D67/0081—After-treatment of organic or inorganic membranes
- B01D67/0088—Physical treatment with compounds, e.g. swelling, coating or impregnation
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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
- B01D67/0081—After-treatment of organic or inorganic membranes
- B01D67/0095—Drying
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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
-
- 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
- B01D71/30—Polyalkenyl halides
- B01D71/32—Polyalkenyl halides containing fluorine atoms
- B01D71/34—Polyvinylidene fluoride
-
- 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
- C02F1/20—Treatment of water, waste water, or sewage by degassing, i.e. liberation of dissolved gases
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2323/00—Details relating to membrane preparation
- B01D2323/39—Electrospinning
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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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
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- Environmental & Geological Engineering (AREA)
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Abstract
The invention discloses a novel membrane contactor system for recovering dissolved methane in anaerobic effluent, and belongs to the technical field of wastewater treatment, chemical engineering and environmental protection. The device comprises a water inlet tank, a peristaltic pump, an air pump, a buffer container, a liquid perfusion membrane contactor module, an air storage tank, a pressure meter, a flowmeter and the like, wherein the liquid perfusion membrane contactor module mainly comprises a two-side clamping device and a liquid perfusion membrane, and a cavity passage at two sides is formed by isolating a groove of the clamping device through the membrane, so that water flow and air flow reversely flow at two sides of the liquid perfusion membrane respectively. The system can fully utilize the gas-gas pressure difference and the chemical potential difference of three phases of anaerobic effluent, the perfusion liquid membrane and the carrier gas, and the difference of intermolecular forces (such as solubility) of perfusion liquid and methane molecules or water molecules to selectively drive methane mass transfer, remarkably improve the recovery efficiency and purity of dissolved methane, does not relate to the use of a large amount of adsorbents and secondary degassing treatment, is environment-friendly and low in cost, and has important practical significance and long-term strategic significance for improving the recycling and sustainable development capacity of anaerobic biological treatment.
Description
Technical Field
The invention belongs to the technical field of wastewater treatment, chemical engineering and environmental protection, and relates to a resource recovery system for treating dissolved methane in anaerobic wastewater based on a liquid perfusion membrane contactor.
Background
Anaerobic biotechnology can convert waste water into clean water and methane energy, is widely applied to sewage treatment plants in various regions of the world, and becomes an important means for relieving global water crisis and energy shortage. Nevertheless, due to the advection limitation of an anaerobic reactor (such as upflow anaerobic sludge blanket UASB) system, the generated methane accounts for about 11-100% of the dissolved methane and is discharged into the environment along with anaerobic effluent, which not only causes great loss of energy, but also generates secondary problems such as greenhouse effect (the greenhouse effect is 25 times of carbon dioxide), explosion (the explosion limit is 1.4 mg/L) and the like, and seriously restricts the high-efficiency resource utilization and sustainable development of the anaerobic biotechnology. Therefore, the recovery of dissolved methane in anaerobic effluent is of great practical significance.
Currently, techniques available for separating dissolved methane from anaerobic effluent include stripping, spray aeration, packed towers, membrane contactors, and the like. However, the steam stripping, spray aeration and packed tower carry out methane mass transfer by directly contacting anaerobic waste water with carrier gas, and the operation problems such as water bubbles or flooding are easy to occur. The membrane contactor uses a hydrophobic membrane as a barrier for separating a gas phase and a liquid phase, and is driven by a gas-partial pressure difference provided by vacuum or scavenging, methane is firstly transferred to a wastewater/membrane phase interface from an anaerobic wastewater body, then enters the membrane phase and is diffused and transferred to the membrane phase/gas phase interface, and finally reaches the gas phase body, so that the methane is effectively recovered. Therefore, the membrane contactor has independently controllable gas and liquid operating parameters, can effectively avoid the problems, has the advantages of large specific surface area per unit volume, low energy consumption, small occupied area and the like, and has great potential in the aspect of recovering anaerobic effluent and dissolving methane. However, the process of recovering methane by using a membrane contactor not only involves gas-liquid (liquid water/methane) separation, and partial anaerobic effluent is also changed into gas (water vapor) from liquid under the drive of vacuum or scavenging, while the wastewater/membrane interface of the traditional membrane contactor has low selectivity to methane and water vapor, and high water vapor flux is usually accompanied in the process of dissolving methane by recovering anaerobic effluent, which accelerates the condensation of water vapor in the membrane, reduces the mass transfer flux of methane, and causes the recovered mixed gas to contain a large amount of water vapor, so that the low-concentration methane needs to be separated from the generated gas mixture before recovery and reuse, and even if cogeneration is carried out, energy-intensive secondary dehydration treatment is also needed.
Disclosure of Invention
The invention aims to solve the problems of low recovery efficiency and selectivity and the like in the process of recovering anaerobic effluent and dissolving methane by using a traditional membrane contactor system, adopts a novel membrane contactor system for recovering methane in an anaerobic effluent dissolved state, can fully utilize the gas-gas partial pressure difference and chemical potential difference of three phases of anaerobic effluent, perfusion liquid membrane and carrier gas, and the difference of intermolecular forces (such as solubility) of perfusion liquid and methane molecules or water molecules, and selectively drives the mass transfer of methane, wherein the mass transfer process is different from the traditional membrane contactor system (figure 2), and the methane molecule transfer step comprises the following steps: (1) Methane molecules are transferred from the wastewater phase to the wastewater phase/liquid perfusion membrane interface; (2) The methane molecules are bound-solvated (water molecules are trapped) at the interface with the perfusion liquid by intermolecular forces; (3) Methane molecules enter the liquid perfusion film and are transferred to a liquid perfusion film/carrier gas phase interface; (4) The methane molecules desorb at the interface and pass to the bulk of the carrier gas phase. The system can obviously improve the recovery efficiency and purity of dissolved methane, does not involve the use of a large amount of adsorbents and secondary degassing treatment, is environment-friendly and low in cost, and has important significance for ensuring public safety, reducing greenhouse effect and optimizing energy structures.
Therefore, the technical scheme of the invention is as follows:
a novel membrane contactor system (figure 1) for recovering dissolved methane in anaerobic effluent comprises a water inlet tank, a peristaltic pump, an air pump, a buffer container, a membrane contactor module, an air storage tank, a pressure gauge, a flowmeter and the like; the membrane contactor module mainly comprises two clamping devices and a liquid perfusion membrane; the middle part of the inner side of the clamping device is a cubic groove, the outer side of the clamping device is respectively provided with two threaded round holes communicated with the two ends of the groove, and the threaded round holes are externally connected with quick plugs and serve as water (gas) inlet and water (gas) outlet ports; the liquid perfusion membrane comprises a porous base membrane and perfusion liquid, and the perfusion liquid is limited in the porous base membrane; the multi- (micro) porous base film has a high porosity; the perfusion liquid is a liquid with high methane solubility, low water solubility (immiscible with water), low volatility, affinity with the basement membrane and higher affinity than water; the liquid perfusion film is fixed between the two clamping devices through screws and silica gel gaskets, and the liquid perfusion film and the inner walls of the grooves of the two clamping devices can form an anaerobic wastewater channel and a carrier gas channel respectively. Anaerobic wastewater to be treated is pumped into a buffer container through a peristaltic pump, then enters a wastewater channel of a liquid perfusion membrane contactor at a relatively stable flow and pressure for treatment, meanwhile, air is pumped into a carrier gas channel of the liquid perfusion membrane contactor through an air pump in a direction opposite to water flow, the pressure and the flow of inlet and outlet water and inlet and outlet air are monitored through a pressure gauge and a flow meter, finally, dissolved methane in the wastewater permeates to a gas phase (carrier gas channel) through a liquid perfusion diffusion membrane under the common driving of a chemical head provided by perfusion liquid and a gas-divided pressure head provided by carrier gas, and is collected by a gas storage tank, and the circulation of water molecules is blocked.
Preferably: the porous base membrane is a polyvinylidene fluoride fiber membrane; the aperture of the porous basement membrane is 0.1-0.2 μm; the porosity of the porous base membrane is 80-90%.
Preferably: the perfusion liquid is silicone oil with the viscosity of 20-500 cts.
Preferably: the liquid perfusion film is formed by combining a porous base film with perfusion liquid through a spin coater, wherein the rotating speed of the spin coater is 2000-4000 rpm.
Preferably: the system operates at a transmembrane pressure of 5-50kpa.
Preferably: the system operates with a gas to liquid ratio of 0.5 to 1.
Drawings
FIG. 1 is a schematic diagram of the novel membrane contactor system for recovering dissolved methane from anaerobic effluent according to the present invention.
Fig. 2 is a schematic structural diagram of a conventional membrane contactor and a liquid-filled membrane contactor module.
Fig. 3 is a graph comparing the methane and water vapor flux of a conventional membrane contactor with a liquid-flooded membrane contactor.
Fig. 4 is a physical diagram of a conventional membrane contactor module and a liquid-filled membrane contactor module at different operating stages.
The specific implementation mode is as follows:
the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings, and it is to be understood that the described embodiments are only some embodiments of the present invention, but not all embodiments, and in no way limit the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments of the present invention without making any creative effort, shall fall within the protection scope of the present invention.
The utility model provides a retrieve novel membrane contactor system of anaerobism play water dissolved methane, includes into water pitcher 1, peristaltic pump 2, air pump 3, buffer container 4, membrane contactor module 7, gas holder 8, manometer 9 and flowmeter 10 etc. and the membrane contactor module mainly includes clamping device 6 and liquid perfusion membrane 12. Anaerobic effluent to be treated in the water inlet tank 1 is pumped into a buffer container 4 through a peristaltic pump 2, then enters a wastewater channel of a liquid perfusion membrane contactor module 7 at relatively stable flow and pressure for treatment, meanwhile, air is pumped into a carrier gas channel of the liquid perfusion membrane contactor module 7 through an air pump 3 in a direction opposite to water flow, the pressure and the flow of the inlet water and the outlet water are monitored through a pressure gauge 9 and a flow meter 10, and finally dissolved methane in the wastewater permeates through a liquid perfusion membrane 12 to reach a gas phase (carrier gas channel) under the common driving of chemical potential difference provided by perfusion liquid and gas-partial pressure difference provided by carrier gas and is collected by a gas storage tank 8.
Example 1
The method for treating the anaerobic wastewater containing dissolved methane by using the liquid perfusion membrane contactor system with the resource recovery function comprises the following steps:
the treated object is artificially synthesized dissolved methane wastewater, and the preparation method comprises the following steps:
injecting 16L of ultrapure water into a 20L water distribution tank, opening methane gas inlet, adjusting the gas inlet pressure to 1bar, adjusting the gas inlet pressure to 2bar, and keeping the pressure at 50cm 3/ Introducing methane gas at the speed of min until the internal pressure of the tank body is stabilized to 2bar, and closing the gas inletAnd (3) starting a constant-temperature magnetic stirrer, setting the constant temperature to be 25, regulating the rotation speed of a rotor to be 2000rpm, stirring for 12 hours, and preparing the synthetic wastewater with the dissolved methane concentration of 25 +/-5 mg/L.
The liquid infusion membrane was prepared as follows:
weighing a certain mass of polyvinylidene fluoride (PVDF) powder, and placing the PVDF powder in a vacuum drying oven at 80 ℃ for drying for more than 4 hours. Weighing dried PVDF powder, dissolving the PVDF powder in a Dimethylformamide (DMF) solvent to prepare a 15wt% mixed solution, and continuously stirring the mixed solution for 12 hours at the temperature of 45 ℃ to obtain a uniform and stable spinning solution. And standing and defoaming for a certain time in a vacuum drying oven until no bubbles appear. Setting spinning technological parameters: the jet speed is 0.2mm/min; a positive voltage of 13V; a negative voltage of 2V; humidity is 40%; the temperature is 30 ℃; the receiving distance is 15cm at DEG C; receiving the rotating speed of a rotary drum of 100rpm; the translation distance is 10mm left and right; the translation speed is 150mm/min; and starting the electrostatic spinning machine to spin for 10 hours. And after the membrane spinning is finished, taking down the spun PVDF electrostatic spinning nanofiber hydrophobic membrane, putting the membrane into a vacuum drying oven at 30 ℃ for drying for more than 0.5h so as to be beneficial to volatilizing residual solvent or water, and finally pressing the membrane flatly by using a glass plate. Shearing the porous membrane into a proper size, fixing the porous membrane on a disc of a spin coater, regulating the rotation speed to 4000rpm, selecting silicone oil which has higher methane solubility than water, low volatility, water insolubility, affinity with a PVDF membrane and affinity greater than water as perfusion liquid, injecting the perfusion liquid into the spin coater, closing the spin coater after 1min, and taking out the liquid perfusion membrane.
Constructing a novel liquid perfusion membrane contactor module:
the porous PVDF fiber membrane and the liquid perfusion membrane (silicone oil perfusion porous PVDF membrane) are respectively sealed in a gas-liquid separation cavity through a clamping device to construct a traditional membrane contactor module and a novel liquid perfusion membrane contactor module, wherein the membrane and the inner walls of the grooves of the clamping devices on the two sides form an anaerobic wastewater channel and a carrier gas channel. Connecting the contactor module to the system in a vertical direction, enabling the separation process to be independent of gravity action, starting the system in a circulating convection operation mode (schematic diagram 1), and stably pumping synthetic wastewater into the gas-liquid membrane contactor at a flow rate of 5L/h through a peristaltic pump and a buffer container to enable the synthetic wastewater to circulate at one side of a membraneFlowing the nitrogen gas at the other side by 60 cm 3 The flow rate/min was used as purge gas to the membrane, the gas-liquid ratio was about 0.72 and the transmembrane pressure difference was 20Kpa.
The comparative results are shown in FIG. 3, where the mass transfer flux of methane in the liquid-filled membrane contactor system is 3.435 mol/m 2 H, significantly higher than 0.869mol/m of a conventional membrane contactor 2 H is used as the reference value. Moreover, the liquid-perfused membrane contactor has high water vapor/methane selectivity, water vapor flux of almost 0, and recovered methane with higher purity, compared to porous membrane water vapor flux of 1.233mol/m 2 H is used as the reference value. In addition, as shown in fig. 4, a significant capillary condensation phenomenon can also be found at the air outlet of the conventional membrane contactor, compared to a liquid-filled membrane contactor. Therefore, the novel membrane contactor system for recovering dissolved methane in anaerobic effluent disclosed by the invention can obviously improve the recovery efficiency and purity of dissolved methane.
Claims (6)
1. A novel membrane contactor system for recovering dissolved methane in anaerobic effluent is characterized in that: the system comprises a water inlet tank, a peristaltic pump, an air pump, a buffer container, a liquid perfusion membrane contactor module, an air storage tank, a pressure meter, a flowmeter and the like, anaerobic effluent to be treated is pumped into the buffer container through the peristaltic pump and then flows into a wastewater channel of the liquid perfusion membrane contactor module at a stable flow and pressure, meanwhile, air is pumped into a carrier gas channel of the liquid perfusion membrane contactor module through the air pump in a direction opposite to water flow, the pressure and the flow of the inlet and outlet air and the inlet and outlet water of the liquid perfusion membrane contactor module are monitored through the pressure meter and the flowmeter, and finally, dissolved methane in the wastewater reaches a gas phase (carrier gas channel) through membrane permeation under the common driving of a chemical potential difference provided by perfusion liquid and a gas-partial pressure difference provided by the carrier gas and is collected by the air storage tank.
2. The membrane contactor system as claimed in claim 1, wherein the membrane contactor system is adapted to recover methane in a dissolved state from anaerobic effluent, and comprises: the liquid perfusion membrane contactor module comprises a two-side clamping device and a novel liquid perfusion membrane; the middle part of the inner side of the clamping device is a cubic groove, the outer side of the clamping device is respectively provided with two threaded circular holes communicated with the two ends of the groove, and the threaded circular holes are externally connected with quick plugs and serve as water (gas) inlet and water (gas) outlet ports; the liquid perfusion film comprises a porous base film and perfusion liquid, and the perfusion liquid is limited in the porous base film; the liquid pouring film is fixed between the two clamping devices through screws and silica gel gaskets, and the liquid pouring film and the inner walls of the grooves of the two clamping devices form an anaerobic wastewater channel and a carrier gas channel respectively.
3. The porous membrane according to claim 2, wherein: the porous base membrane is made of hydrophobic polymers such as polytetrafluoroethylene, polyvinylidene fluoride and polydimethylsiloxane; the aperture of the porous basement membrane is 0.05-0.5 μm; the porosity of the porous base membrane is 65-95%.
4. Perfusion liquid according to claim 2, wherein: the perfusion liquid is immiscible with water; the solubility of methane in the perfusion liquid is higher than the solubility of methane in water; the perfusion liquid is not volatilized at normal temperature and normal pressure; the perfusion liquid is compatible with the porous base membrane; the affinity of the perfusion liquid with the porous base membrane is greater than the affinity of water with the porous base membrane.
5. The membrane contactor system as claimed in claim 1, wherein the membrane contactor system is adapted to recover methane in a dissolved state from anaerobic effluent, and comprises: the transmembrane pressure of the operation of the system is less than the critical opening pressure of the liquid in the liquid perfusion membrane pores.
6. The novel membrane contactor system for recovering dissolved methane from an anaerobic effluent as claimed in claim 1, wherein: the system operates with a gas-to-liquid flow ratio greater than 0.48.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5236474A (en) * | 1991-09-13 | 1993-08-17 | Bend Research, Inc. | Membrane-based removal of condensable vapors |
| US20160206993A1 (en) * | 2015-01-21 | 2016-07-21 | Liyuan DENG | Closed cycle continuous membrane ionic liquids absorption/desorption process for co2 capture |
| CN112194250A (en) * | 2020-11-06 | 2021-01-08 | 天津城建大学 | System and method for recycling biogas energy in organic wastewater anaerobic membrane biological treatment |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5236474A (en) * | 1991-09-13 | 1993-08-17 | Bend Research, Inc. | Membrane-based removal of condensable vapors |
| US20160206993A1 (en) * | 2015-01-21 | 2016-07-21 | Liyuan DENG | Closed cycle continuous membrane ionic liquids absorption/desorption process for co2 capture |
| CN112194250A (en) * | 2020-11-06 | 2021-01-08 | 天津城建大学 | System and method for recycling biogas energy in organic wastewater anaerobic membrane biological treatment |
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