CN112707566A - Functionalized carbon-based salt difference power generation permeable membrane and preparation method and application thereof - Google Patents
Functionalized carbon-based salt difference power generation permeable membrane and preparation method and application thereof Download PDFInfo
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Abstract
The invention discloses a functionalized carbon-based salt difference power generation permeable membrane and a preparation method and application thereof. First of all. The method comprises the steps of firstly preparing a composite film with functional groups, wherein the film not only has ion selectivity, but also has a photo-thermal conversion effect, applying the film to seawater desalination, carrying out seawater desalination by utilizing solar heat, utilizing capillary force as a driving force, utilizing salinity difference on two sides of the film to carry out salinity difference power generation, and synergistically converting clean and sustainable solar energy and salinity difference energy into electric energy which can be directly utilized by human beings, thereby achieving the purpose of effectively utilizing resources.
Description
Technical Field
The invention relates to the technical field of salt difference energy power generation, in particular to a functionalized carbon-based salt difference power generation permeable membrane and a preparation method and application thereof.
Background
With the increasing exhaustion of fossil energy, the energy crisis is becoming more serious. The strategic development plan of clean and renewable energy is made by countries in the world to solve the problems of fossil energy exhaustion, environmental pollution and the like in the future. The salt difference energy is a renewable energy source with large storage capacity and no pollution, and is a 'blue' energy source which converts gibbs free energy into electric energy, so that the salt difference energy has attracted wide attention. The power generation by utilizing the salt difference energy is an energy conversion mode with application prospect. However, the conventional commercial ion exchange membrane has high manufacturing cost and complicated manufacturing process, and thus development of a novel salt-difference power generation is imminent.
Desalination of sea water is one of the most serious global challenges of the current era. Currently, various measures have been taken by medical researchers worldwide to meet the increasing demand for water resources, wherein desalination of sea water is considered as a major and promising measure to address the water shortage due to the abundant sea water reserves. The adoption of the traditional fossil energy for seawater desalination not only wastes energy but also causes environmental pollution. Further aggravating the fossil energy shortage problem.
Disclosure of Invention
One of the purposes of the invention is to provide a preparation method of a functionalized carbon-based salt difference power generation permeable membrane.
The invention also aims to provide the functionalized carbon-based salt difference power generation permeable membrane prepared by the preparation method.
The invention also aims to provide the application of the functionalized carbon-based salt difference power generation permeable membrane in seawater desalination.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows: a preparation method of a functionalized carbon-based salt difference power generation permeable membrane comprises the following steps:
the method comprises the following steps: adding carbon nanotubes with certain mass into water at room temperature to prepare a base solution A; adding a certain amount of bacterial cellulose into the base solution A to serve as a framework structure, and then adding a proper amount of polar solvent to serve as a dissolving agent to obtain a base solution B; adding a certain amount of acetic acid into the base solution B to obtain a solution C;
step two: performing ultrasonic dispersion on the solution C prepared in the step one to obtain a uniformly mixed solution D;
step three: pumping a certain amount of the solution D prepared in the second step into a vacuum pumping filtration device for pumping filtration to obtain a filter membrane E;
step four: and (4) freeze-drying the filter membrane E prepared in the third step to obtain the salt difference power generation permeable membrane.
Preferably, in the first step, the carbon nanotubes are multi-walled carbon nanotubes with a particle size of 0.5-2.5 μm, and the concentration of the carbon nanotubes in the base liquid a is 0.025-0.033 g/mL.
Preferably, in the first step, the polar solvent is N-methyl pyrrolidone, and the volume ratio of the bacterial cellulose, the N-methyl pyrrolidone and the acetic acid is 4-6: 12.5-20: 3-5.
Preferably, in the second step, the ultrasonic power of the ultrasonic dispersion is 500W, and the ultrasonic time is 50-80 min.
Preferably, in the fourth step, the freezing temperature of the freeze drying is-50 ℃, and the freezing time is 20-30 min.
The invention also provides a functionalized carbon-based salt difference power generation permeable membrane prepared by the preparation method.
The thickness of the salt difference power generation permeable membrane is 0.1-2.0 mm.
The invention also provides application of the functionalized carbon-based salt difference power generation permeable membrane in seawater desalination, namely provides a salt difference power generation-seawater desalination coupling device based on the functionalized carbon-based salt difference power generation permeable membrane, which comprises a seawater supply layer and the salt difference power generation permeable membrane, wherein a hole with the depth of 0.005-1.0mm is formed in the upper surface of the seawater supply layer, the salt difference power generation permeable membrane is arranged in the hole, a heat insulation layer is further arranged around the salt difference power generation permeable membrane, and the upper surface and the lower surface of the salt difference power generation permeable membrane are externally connected with a load through a double-guide copper foil adhesive tape.
Preferably, the heat insulation layer is silica aerogel felt, the porosity is 80% -90%, and the density is 3-250kg/m3The heat conductivity coefficient is 0.013-0.025W/m.k, and the thickness is 4-6 mm.
Preferably, the seawater supply layer is a cellulose sponge.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention introduces a salt tolerance power generation concept on the basis of the traditional solar seawater desalination, utilizes solar heat to desalinate seawater, utilizes capillary force as driving force, and utilizes the salinity difference at two sides of the film to generate salt tolerance power.
2. The film prepared by the invention has simple preparation process, low cost and higher ion selectivity.
3. The film prepared by the invention not only has ion selectivity, but also has a photo-thermal conversion effect, and can fully utilize solar energy to desalt seawater and simultaneously carry out salt tolerance power generation.
4. The salt difference power generation-seawater desalination coupling device provided by the invention has the advantages of simple structure, cleanness, no pollution, higher cost performance and market application value. And provides a new solution and idea for future engineering application.
Drawings
FIG. 1 is an SEM scanning electron micrograph of a salt-difference power generation permeable membrane prepared in example 1 of the present invention.
FIG. 2 is an FTIR spectrum of a salt-difference power-generating permeable membrane prepared in example 1 of the present invention.
FIG. 3 is a Zeta potential diagram of a salt difference power generation permeable membrane prepared in example 1 of the present invention.
FIG. 4 is a light absorption spectrum of a salt-difference power generation permeable membrane prepared in example 1 of the present invention in a visible light band.
Fig. 5 is a schematic diagram of the operation of the coupling device for salt-difference power generation and seawater desalination of the present invention, wherein 1, a salt-difference power generation permeable membrane, 2, a heat insulation layer, 3, a seawater supply layer, 4, a double copper foil tape, 5, a lead, 6 and a load.
FIG. 6 is an electrical property of the salt-poor power generating permeable membrane prepared in example 1 of the present invention in different solutions.
FIG. 7 is the electrochemical performance of the salt-difference power generation permeable membrane prepared in example 1 of the present invention in NaCl solutions of different concentrations.
Detailed Description
The invention is described in further detail below with reference to the figures and specific examples.
Example 1
The method comprises the following steps: under the condition of room temperature, 0.5g of multi-walled carbon nanotubes with the particle size of 0.5 mu m are added into 20mL of deionized water to prepare a base solution A; adding 8mL of bacterial cellulose as a framework structure into the base solution A, and adding 25mL of polar solvent N-methyl pyrrolidone as a dissolving agent to obtain a base solution B; adding 6mL of acetic acid into the base solution B to obtain a solution C;
step two: placing the solution C prepared in the first step into an ultrasonic dispersion machine, and performing ultrasonic dispersion for 50min at the power of 500W to obtain a uniformly mixed solution D;
step three: extracting a certain amount of the solution D prepared in the third step by a liquid transfer gun, and performing suction filtration for 5min by a vacuum suction filtration device to obtain a filter membrane E;
step four: and (3) placing the filter membrane E prepared in the third step in a freeze drying oven at-50 ℃ for freeze drying for 20min to obtain the salt difference power generation permeable membrane. The thickness of the salt difference power generation permeable membrane is 0.095mm measured by a screw micrometer.
Fig. 1 is an SEM (scanning electron microscope) image of the salt difference power generation permeable membrane prepared in this example, and the microstructure of the thin film shows that the surface of the thin film is rough, and the carbon nanotubes are well attached to the bacterial cellulose.
FIG. 2 is an FTIR spectrum of the salt difference generating permeable membrane prepared in this example, in which 3339cm is shown-12891cm as the O-H stretching vibration peak-1Is C-H stretching vibration peak, 1627cm-1The C ═ O stretching vibration peak indicates that the film successfully introduced carboxyl functionality.
FIG. 3 is a Zeta potential diagram of the salt difference power generation permeable membrane prepared in this example, showing that the membrane has strong selectivity for cations.
Fig. 4 is a light absorption spectrum of the salt-difference power generation permeable membrane prepared in this embodiment in the visible light band, which shows that the membrane has strong light absorption in the visible light band and can perform sufficient photo-thermal conversion.
The salt difference power generation permeable membrane prepared by the embodiment is a composite membrane with functional groups, wherein the composite membrane comprises a carbon nano tube, N-methyl pyrrolidone, acetic acid and bacterial cellulose, the functional groups are carboxyl groups, and the introduction of the carboxyl groups can improve the surface charge of the membrane and improve the ion selectivity.
Example 2
The method comprises the following steps: under the condition of room temperature, 0.8g of multi-walled carbon nanotubes with the particle size of 1.5 mu m are added into 25mL of deionized water to prepare a base solution A; adding 10mL of bacterial cellulose serving as a framework structure into the base solution A, and adding 30mL of polar solvent N-methyl pyrrolidone serving as a dissolving agent to obtain a base solution B; adding 8mL of acetic acid into the base solution B to obtain a solution C;
step two: placing the solution C prepared in the first step into an ultrasonic dispersion machine, and performing ultrasonic dispersion for 60min at the power of 500W to obtain a uniformly mixed solution D;
step three: extracting a certain amount of the solution D prepared in the third step by a liquid transfer gun, and performing suction filtration for 7min by a vacuum suction filtration device to obtain a filter membrane E;
step four: and (3) placing the filter membrane E prepared in the third step in a freeze drying oven at-50 ℃ for freeze drying for 25min to obtain the salt tolerance power generation permeable membrane. The thickness of the salt difference power generation permeable membrane is 0.422mm measured by a micrometer screw.
Example 3
The method comprises the following steps: under the condition of room temperature, 1.0g of multi-walled carbon nanotubes with the particle size of 2.5 microns are added into 30mL of deionized water to prepare a base solution A; adding 12mL of bacterial cellulose as a framework structure into the base solution A, and adding 40mL of polar solvent N-methyl pyrrolidone as a dissolving agent to obtain a base solution B; adding 10mL of acetic acid into the base solution B to obtain a solution C;
step two: placing the solution C prepared in the first step into an ultrasonic dispersion machine, and performing ultrasonic dispersion for 80min at the power of 500W to obtain a uniformly mixed solution D;
step three: extracting a certain amount of the solution D prepared in the third step by a liquid transfer gun, and performing suction filtration for 10min by a vacuum suction filtration device to obtain a filter membrane E;
step four: and (3) placing the filter membrane E prepared in the third step in a freeze drying oven at-50 ℃ for freeze drying for 30min to obtain the salt tolerance power generation permeable membrane. The thickness of the salt difference power generation permeable membrane is 1.025mm measured by a screw micrometer.
Example 4
And (3) utilizing the prepared salt difference power generation osmotic membrane to manufacture a coupling device of salt difference power generation and seawater desalination. As shown in fig. 5, the device comprises a seawater supply layer 3 and a salt difference power generation permeable membrane 1, wherein a hole with the depth of 0.005-1.0mm is formed in the upper surface of the seawater supply layer 3, the salt difference power generation permeable membrane 1 is arranged in the hole, a heat insulation layer 2 is further arranged around the salt difference power generation permeable membrane 1, and the upper surface and the lower surface of the salt difference power generation permeable membrane 1 are externally connected with two leads 5 led out from a load 6 through a double-lead copper foil adhesive tape 4.
The seawater supply layer 3 is a strip-shaped cellulose sponge, the length is 3-6cm, and the width is 0.3-0.5 cm. The cellulose sponge has high water absorption rate, can float on the surface of seawater on one hand, and can fully absorb seawater on the other hand.
The heat insulating layer 2 is made of silicon dioxide aerogel felt, the porosity is 80% -90%, and the density is 3-250kg/m3The heat conductivity coefficient is 0.013-0.025W/m.k, and the thickness is 4-6 mm. The silica aerogel felt has light weight, good heat insulation effect and low heat conductivity coefficient. Therefore, the silica aerogel felt is tightly wrapped around the salt-difference power generation permeable membrane 1, and plays a role in preventing heat from being dissipated to the surrounding environment.
The mechanical assembly between the salt-difference power generating permeable membrane 1, the seawater supply layer 3 and the heat insulating layer 2, it being understood that the photothermal conversion is performed by photothermal conversion of a solar heat absorbing material, where the electrons in the photothermal material will be excited to a higher energy state, i.e. photoexcitation, when the energy of the incident photons matches the energy required to achieve the electronic transition. But since the high energy state is unstable, the electrons of the high energy state will self-return to the low energy state. This return will generate hot carriers that redistribute energy through electron-electron, electron-phonon, phonon-phonon interactions, thereby releasing heat and increasing the temperature of the photothermal material. To improve solar thermal conversion efficiency, the photothermal material should have a broad absorption spectrum that covers the entire solar irradiance. The sunlight incident to the earth surface can be divided into three bands, namely ultraviolet (300-. And the carbon-based material is used as a common photo-thermal conversion material and has better coverage in solar irradiance.
It is understood that ion-selective refers to a channel having a high permeability to one or a concentrated ion, and a lesser or non-permeability to other ions. Example (b)Such as potassium channel pair K+And Na+Has a permeability ratio of about 100: 1. acetylcholine receptor cation channels for small cations, e.g. Na+、K+Are highly permeable to Cl-Is not permeable. In the nano-porous material, when the double electric layers of the pore walls are close to each other, based on the selectivity of the nano-pore channels to ions, the ions in the pore channels can generate directional movement under the action of concentration difference, so that the concentration difference can be converted into electric energy, namely, salt difference power generation. The salt tolerance power generation can be carried out due to the salt tolerance caused by water evaporation in the seawater desalination.
The whole apparatus was placed in a 500mL beaker and placed under sunlight for the experiment. The data acquisition instrument is used for acquiring electric signals, and in order to research the performance of the device in different salt solutions with different concentrations, the concentrations (0.2mM, 0.5mM, 1.0mM and 1.5mM) of the solutions in the beaker and the types (CuCl) of the electrolytes are respectively changed2NaCl, and KCl), the results are shown in fig. 6 and 7.
FIG. 6 shows the salt difference power generation permeable membranes prepared in example 1 respectively containing 1mM NaCl and CuCl2And electrical properties in KCl solution. It can be seen that, although the NaCl and KCl solutions are single compounds, the electrical properties of the NaCl solution are much better than those of KCl. During the 1000s measurement time, the voltage first increased slightly in the NaCl solution, peaked at around 300s (-31 mV), and still 22mV at 1000s, but in the KCl solution, the voltage gradually dropped, approaching 5mV at 1000 s. From the zeta potential diagram in FIG. 3, it can be concluded that the saline difference power generating permeable membrane has cation selectivity to Na+The selectivity of the ion is better than K+Ions. Binary compound CuCl2The electrical performance of the compound is superior to that of a monobasic compound, reaches a peak value at 700s (-33 mv), and can be kept stable for a long time. In CuCl2In solution, since the copper ion is a divalent ion, the charge per ion is larger than that of a monovalent ion such as Na+、K+High, and therefore, its electrical signal is higher than that of NaCl and KCl solutions of the same concentration.
FIG. 7 is a graph showing the electrochemical performance of the salt-difference power-generating permeable membrane prepared in example 1 in NaCl solutions of different concentrations (0.2mM, 0.5mM, 1.0mM, 1.5 mM). It can be seen that the electrical properties do not increase linearly with increasing concentration. This experimental phenomenon is in accordance with the debye length theory, and as the electrolyte concentration increases, the thickness of the debye length decreases and the ion transport is less affected by electrostatic interactions. At high ion concentrations, the Electric Double Layer (EDL) is negligible compared to the channel size, and shielding of the EDL occurs near the charged nanochannels. Thus, the conductivity of the overall solution is dominant. At a concentration of 0.5mM, the maximum voltage was obtained.
In summary, in the device, the salt difference power generation permeable membrane is used as a photo-thermal conversion material, sunlight is almost completely absorbed due to the rough structure of the surface of the membrane, photo-thermal conversion is carried out, meanwhile, the capillary force of solar evaporation is used as a driving force, the concentration of the solution on the two sides of the permeable membrane is different due to the evaporation of water, concentration difference is generated under the action of the permeable membrane, salt difference power generation is carried out by utilizing the concentration difference between the concentrated solution and the dilute solution, and the generated electric energy is applied to an external load. The solar energy and salt difference energy cooperative conversion device utilizes solar energy and heat conversion drive and salt difference power generation in a coupling mode, clean and sustainable solar energy and salt difference energy are converted into electric energy which can be directly utilized by human beings, and the purpose of effectively utilizing resources is achieved.
Claims (10)
1. A preparation method of a functionalized carbon-based salt difference power generation permeable membrane is characterized by comprising the following steps:
the method comprises the following steps: adding carbon nanotubes with certain mass into water at room temperature to prepare a base solution A; adding a certain amount of bacterial cellulose into the base solution A to serve as a framework structure, and then adding a proper amount of polar solvent to serve as a dissolving agent to obtain a base solution B; adding a certain amount of acetic acid into the base solution B to obtain a solution C;
step two: performing ultrasonic dispersion on the solution C prepared in the step one to obtain a uniformly mixed solution D;
step three: pumping a certain amount of the solution D prepared in the second step into a vacuum pumping filtration device for pumping filtration to obtain a filter membrane E;
step four: and (4) freeze-drying the filter membrane E prepared in the third step to obtain the salt difference power generation permeable membrane.
2. The method as claimed in claim 1, wherein in the step one, the carbon nanotubes are multi-walled carbon nanotubes with a particle size of 0.5-2.5 μm, and the concentration of the carbon nanotubes in the base fluid a is 0.025-0.033 g/mL.
3. The method for preparing a functionalized carbon-based salt difference power generation permeable membrane according to claim 1, wherein in the first step, the polar solvent is N-methyl pyrrolidone, and the volume ratio of the bacterial cellulose, the N-methyl pyrrolidone and the acetic acid is 4-6: 12.5-20: 3-5.
4. The preparation method of the functionalized carbon-based salt difference power generation permeable membrane according to claim 1, wherein in the second step, the ultrasonic power of the ultrasonic dispersion is 500W, and the ultrasonic time is 50-80 min.
5. The method for preparing a functionalized carbon-based salt difference power generation permeable membrane according to claim 1, wherein in the fourth step, the freeze drying is carried out at a freezing temperature of-50 ℃ for 20-30 min.
6. The functionalized carbon-based salt differential power generation permeable membrane prepared by the preparation method of claim 1.
7. The application of the functionalized carbon-based salt difference power generation permeable membrane in seawater desalination is characterized by comprising a seawater supply layer and the salt difference power generation permeable membrane, wherein a hole with the depth of 0.005-1.0mm is formed in the upper surface of the seawater supply layer, the salt difference power generation permeable membrane is arranged in the hole, a heat insulation layer is further arranged around the salt difference power generation permeable membrane, and the upper surface and the lower surface of the salt difference power generation permeable membrane are externally connected with a load through a double-guide copper foil adhesive tape.
8. The use of a functionalized carbon-based salt difference power generating permeable membrane according to claim 7 for desalination of sea water, wherein the thickness of the salt difference power generating permeable membrane is 0.1-2.0 mm.
9. The use of a functionalized carbon-based salt-difference power generation permeable membrane in seawater desalination as claimed in claim 7, wherein the thermal insulation layer is silica aerogel felt, the porosity is 80% -90%, and the density is 3-250kg/m3The heat conductivity coefficient is 0.013-0.025W/m.k, and the thickness is 4-6 mm.
10. The use of a functionalized carbon-based salt difference power generating permeable membrane according to claim 7 for desalination of sea water, wherein the sea water supply layer is a cellulose sponge.
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