CN115260669B - Polymer power generation film, preparation method thereof and power generation device - Google Patents
Polymer power generation film, preparation method thereof and power generation device Download PDFInfo
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Abstract
The application discloses a polymer power generation film, a preparation method thereof and a power generation device, wherein the polymer power generation film comprises the following components: a hydrophilic polymer, a thermally responsive polymer, and a redox electrolyte, wherein the hydrophilic polymer has an oxygen-containing functional group. Therefore, the moisture and the heat can be utilized to jointly drive the power generation, and the power generation performance is improved.
Description
Technical Field
The application relates to the field of functional materials, in particular to a polymer power generation film, a preparation method thereof and a power generation device.
Background
In natural environments, moisture tends to coexist with heat, which is widely present in outdoor environments, in the production of organisms and in the agricultural industry. The research on a humidity and heat co-driven power generation film in the related art is still in a blank stage, and how to effectively utilize humidity and heat energy widely sourced in nature to realize energy conversion has great development potential.
Therefore, the current polymer power generation film, the preparation method thereof and the power generation device still need to be improved.
Disclosure of Invention
In one aspect of the present application, the present application provides a polymer power generating film comprising: a hydrophilic polymer, a thermally responsive polymer, and a redox electrolyte, wherein the hydrophilic polymer has an oxygen-containing functional group. Therefore, the moisture and the heat can be utilized to jointly drive the power generation, and the power generation performance is improved.
According to an embodiment of the application, the mass ratio of the hydrophilic polymer, the thermally responsive polymer and the redox electrolyte is (79-98.8): (1-18): (0.2-3). Therefore, the electricity generating performance can be further improved.
According to an embodiment of the present application, the hydrophilic polymer comprises at least one of polystyrene sulfonic acid, polyacrylic acid, and hydroxyethyl cellulose. Therefore, the electricity generating performance can be further improved.
According to an embodiment of the present application, the thermally responsive polymer comprises at least one of poly 3, 4-ethylenedioxythiophene, polystyrene sulfonate, polypyrrole, and cellulose. Therefore, the electricity generating performance can be further improved.
According to an embodiment of the application, the redox couple electrolyte comprises at least one of potassium iodide/potassium tri-iodide, potassium ferricyanide/potassium ferrocyanide and cobalt bipyridine bis-trifluoromethanesulfonyl imide/cobalt bipyridine bis-trifluoromethanesulfonyl imide. Therefore, the electricity generating performance can be further improved.
According to an embodiment of the present application, the thickness of the polymer conductive film is 0.3 to 1mm. Thus, the power generation assembly of the flexible wearable device can be conveniently manufactured.
In another aspect of the present application, the present application provides a method for preparing the aforementioned polymer power generating film, comprising: providing a mixed solution comprising a hydrophilic polymer, a thermally responsive polymer, and a redox couple electrolyte; and (3) carrying out film drying treatment on the mixed solution under the conditions that the relative humidity is 35-55% and the temperature is 20-55 ℃, wherein the film drying treatment time is 4-10h, so as to obtain the polymer power-generating film. Thus, the polymer film can be produced by a simple method, and the method has all the characteristics and advantages of the polymer film and is not described herein.
According to an embodiment of the present application, the providing a mixed solution includes: providing an aqueous hydrophilic polymer solution, an aqueous thermally responsive polymer solution, and the redox couple electrolyte; mixing the aqueous hydrophilic polymer solution, the aqueous thermally responsive polymer solution and the redox electrolyte in a mass ratio of (263-330): (3-60): (0.2-3) stirring and mixing to obtain the mixed solution, wherein the mass percentage concentration of the hydrophilic polymer aqueous solution and the mass percentage concentration of the thermally responsive polymer aqueous solution are respectively and independently 10-50%. Thus, a polymer power generation film having excellent power generation performance can be obtained.
In yet another aspect, the present application provides a power generating device, including at least one power generating structure, where the power generating structure includes a first electrode layer, a polymer power generating film, and a second electrode layer that are sequentially stacked, where the polymer power generating film is the aforementioned polymer power generating film, and the first electrode layer or the second electrode layer has a through hole thereon, and the through hole exposes a part of a main surface of the polymer power generating film. Thus, a portable wearable power generation device can be obtained.
According to an embodiment of the present application, the materials of the first electrode layer and the second electrode layer each independently include at least one of gold, silver, and graphite. Therefore, the method is applicable to various indoor and outdoor real scenes and realizes the power supply of small commercial appliances.
Drawings
The foregoing and/or additional aspects and advantages of the application will become apparent and may be better understood from the following description of embodiments taken in conjunction with the accompanying drawings in which:
FIG. 1 shows a schematic structure of a polymer power generating film according to an embodiment of the present application;
FIG. 2 shows a schematic structural view of a power generation device according to an embodiment of the present application;
FIG. 3 shows a top view photograph of a power generation device according to one embodiment of the present application;
FIG. 4 shows a schematic structural view of a power generation device according to still another embodiment of the present application;
FIG. 5 shows a graph of the current density produced by the power plant of example 6 at a temperature differential of 10℃at 70% relative humidity;
FIG. 6 shows a graph of the current density produced by the power plant of example 4 at a temperature differential of 10℃with 70% relative humidity;
fig. 7 shows a graph of the current density produced by the power plant of example 5 at a temperature difference of 10 c at 70% relative humidity.
Reference numerals illustrate:
1: a hydrophilic polymer; 2: thermally responsive polymer: 3: a redox couple electrolyte; 4: a polymer power generating film; 5: a first electrode layer; 6: a second electrode layer; 7: an electricity meter; 8: a power generation structure.
Detailed Description
Embodiments of the present application are described in detail below, examples of which are illustrated in the accompanying drawings, wherein like or similar reference numerals refer to like or similar elements or elements having like or similar functions throughout. The embodiments described below by referring to the drawings are illustrative only and are not to be construed as limiting the application.
In one aspect of the present application, the present application provides a polymer power generating film, referring to fig. 1, comprising: a hydrophilic polymer 1, a thermally responsive polymer 2, and a redox couple electrolyte 3, wherein the hydrophilic polymer 1 has an oxygen-containing functional group. The oxygen-containing functional groups in the hydrophilic polymer can adsorb water molecules and dissociate movable ions by utilizing the humidity and the temperature difference existing simultaneously under natural conditions; the heat-responsive polymer can enable the movable ions to spontaneously diffuse from the hot side of the polymer power generation film to the cold side of the polymer power generation film under the drive of temperature difference, so that the transmission of the ions is effectively improved, the two driving force directions are cooperated, the ion migration is more efficient, and the power generation performance of the polymer power generation film is further effectively improved.
For easy understanding, the principle of the polymer power generation film of the present application having the aforementioned advantageous effects will be briefly described as follows:
in the application, the inventor finds that the oxygen-containing functional groups in the hydrophilic polymer can efficiently adsorb water molecules and dissociate to form mobilizable hydrogen ions (hydronium ions), and the hydronium ions can be transmitted in a specific direction (from high concentration to low concentration) inside the material under the action of diffusion due to the difference of hydration degrees at two sides of the polymer power generation film, and negatively charged hydrophilic polymer chains serving as counter ions cannot migrate due to larger volume and fixation, so that positive and negative charge separation is realized, and potential difference is formed at two sides of the polymer composite film; further, under temperature differential conditions, the thermally responsive polymer promotes ion-directed migration such that water and hydrogen ions migrate to the low temperature side of the polymer composite membrane, while the hydrophilic polymer chains are located on a side near the high temperature side of the polymer composite, thereby effectively improving ion transport and thus changing the ionic conductance of the polymer composite membrane. Meanwhile, the directional transmission of the movable ions is also cooperated with the redox reaction of the redox couple electrolyte, so that the ionic conductivity of the polymer composite film is further improved, and the electricity generating performance of the polymer electric-generating film is further enhanced.
According to some embodiments of the present application, the proportions of the constituent components in the polymer electric-generating film are not particularly limited, for example, the mass ratio of the hydrophilic polymer, the thermally responsive polymer and the redox electricity to the electrolyte in the polymer electric-generating film is (79 to 98.8): (1-18): (0.2-3). When the mass ratio of the hydrophilic polymer, the thermally responsive polymer and the redox electrolyte in the polymer electric membrane is within the above range, it is possible to achieve improvement in the electric properties of the polymer electric membrane by forming a large amount of hydronium ions by adsorption of water molecules by the hydrophilic polymer, while promoting ion transport of the hydronium ions by a small amount of the thermally responsive polymer, and promoting ion conduction of water and hydrogen ions by a small amount of the redox electrolyte.
In the present application, all numbers disclosed herein are approximate, whether or not the word "about" or "about" is used. The numerical value of each number may vary by less than 10% or reasonably as considered by those skilled in the art, such as 1%, 2%, 3%, 4% or 5%.
According to some embodiments of the present application, the kind of the hydrophilic polymer is not particularly limited, and for example, the hydrophilic polymer may include at least one of polystyrene sulfonic acid, polyacrylic acid, and hydroxyethyl cellulose.
According to some embodiments of the present application, the kind of the thermally responsive polymer is not particularly limited, and for example, the thermally responsive polymer may include at least one of poly 3, 4-ethylenedioxythiophene, polystyrene sulfonate, polypyrrole, and cellulose.
According to some embodiments of the present application, the kind of hydrophilic polymer is not particularly limited, and for example, the redox couple electrolyte may include at least one of potassium iodide/potassium triiodide, potassium ferricyanide/potassium ferrocyanide, and cobalt bipyridine bis-trifluoromethanesulfonyl imide/cobalt bipyridine bis-trifluoromethanesulfonyl imide.
According to some embodiments of the present application, the thickness of the polymer power generation film is not particularly limited, and for example, the thickness of the polymer power generation film may be 0.3 to 1mm. When the thickness of the polymer generating film is within the above range, the thickness of the polymer generating film is moderate, and the electricity generating performance and the bending performance are good, so that the wearable device can be conveniently manufactured.
In another aspect of the present application, the present application provides a method for preparing the aforementioned polymer power generating film, comprising: providing a mixed solution comprising a hydrophilic polymer, a thermally responsive polymer, and a redox couple electrolyte; and (3) carrying out film drying treatment on the mixed solution at the relative humidity of 35-55% and the temperature of 20-55 ℃ for 4-10h to obtain the polymer conductive film. The polymer composite film with large area, mechanical flexibility, cutting capability, customization and strong power generation capacity can be obtained by simple casting and film airing methods.
According to one embodiment of the application, the environmental conditions of the film drying process may be: film drying and drying were carried out in an environment with a relative humidity of 45% and a temperature of 37 ℃.
According to some embodiments of the present application, the method of providing the mixed solution is not particularly limited, and for example, providing the mixed solution may include: providing an aqueous hydrophilic polymer solution, an aqueous thermally responsive polymer solution, and a redox electropair electrolyte; mixing an aqueous hydrophilic polymer solution, an aqueous thermally responsive polymer solution and a redox electrolyte in a mass ratio of 263-330: (3-60): (0.2-3) stirring and mixing to obtain a mixed solution, wherein the mass percent concentration of the aqueous hydrophilic polymer solution and the aqueous thermally responsive polymer solution is 10-50% respectively and independently, preferably, the mass percent concentration of the aqueous hydrophilic polymer solution and the aqueous thermally responsive polymer solution may be 18% or 30% respectively and independently.
In still another aspect of the present application, referring to fig. 2, 3 and 4, the present application proposes a power generation device, including at least one power generation structure 8, the power generation structure 8 including a first electrode layer 5, a polymer power generation film 4 and a second electrode layer 6 stacked in this order, wherein the polymer power generation film 4 is the aforementioned polymer power generation film, and the first electrode layer 5 or the second electrode layer 6 has a through hole through which a part of a main surface of the polymer power generation film 4 is exposed. The polymer power generation film is used as a power generation layer and is assembled with a pair of electrode layers to form a layered structure, so that the power generation device can generate voltage and current in a real outdoor environment (humidity 50% -80% and temperature difference 2-10 ℃), the power generation signal has excellent stability, the power generation device can be repeatedly used for multiple times, and the whole power generation process can not bring any environmental pollution. Specifically, in natural environment, the power generation device can be suitable for real scenes in various seasons, the application range can be 20-90% of relative humidity, and the temperature is 10-80 ℃, so that the power supply function of the miniaturized commercial electric appliance can be realized. In addition, in a real outdoor environment, the power generation device can be manufactured into a portable wearable power generation system after being integrated in series. Under the environment of real outdoor conditions in various seasons, sweat and heat of a human body are utilized to realize power supply for small-sized electric appliances in a complex environment, convenience is provided for daily travel, production and life, and great practical application value is achieved.
In order to facilitate understanding, the principle of the power generation device of the present application having the above advantageous effects will be briefly described as follows:
because the polymer power generation film has good hydrophilicity, water vapor molecules can be adsorbed from the environment continuously, so that the dissociation of functional groups in the material is induced. Wherein the oxygen-containing functional groups of the polymer material can dissociate electropositive hydrogen ions after adsorbing water molecules. Because one surface of the first electrode layer or the second electrode layer is of a multi-through hole structure, water molecules can pass through, and the other surface of the first electrode layer or the second electrode layer is of a whole-layer structure, water molecules can be blocked from passing through, and therefore a concentration gradient of hydrogen ions can be formed inside the polymer power generation film. Under the action of the concentration gradient, free hydrogen ions can diffuse from a high concentration region to a low concentration region, and the negatively charged functional group framework is fixed on a polymer chain and cannot move. Thus, the directional migration of ions causes positive and negative charges to separate, inducing the generation of an electrical signal. Meanwhile, the temperature difference between the first electrode layer and the second electrode layer further promotes dissociation and diffusion of ions, effective transmission of carriers is improved, and meanwhile, the temperature difference and the reversible redox couple react cooperatively, so that the electricity generating performance of the electricity generating device is effectively improved.
In the description of the application, a "first feature" or "second feature" may include one or more of such features.
According to some embodiments of the present application, materials of the first electrode layer and the second electrode layer are not particularly limited, for example, materials of the first electrode layer and the second electrode layer each independently include at least one of gold, silver, and graphite. The conductive material mature in the preparation and synthesis technology is used as the electrode layer forming material, so that mass production of the power generation device is facilitated, and the practicability and the economical efficiency of the power generation device are effectively improved.
According to some embodiments of the present application, referring to fig. 4, the power generation device may include a plurality of power generation structures, and the connection manner between the plurality of power generation structures is not particularly limited, for example, the plurality of power generation structures 8 may be connected in series and/or parallel with each other.
In the description of the present application, "plurality" means two or more.
In the description of the present application, "a and/or B" may include any of the cases of a alone, B alone, a and B, wherein A, B is merely for example, which may be any technical feature of the present application that uses "and/or" connection.
The following description of the present application is made by way of specific examples, which are given for illustration of the present application and should not be construed as limiting the scope of the application. The examples are not to be construed as limiting the specific techniques or conditions described in the literature in this field or as per the specifications of the product. The reagents or apparatus used were conventional products commercially available without the manufacturer's attention.
Example 1
(1) 13.4 g of polyacrylic acid with the mass percentage concentration of 30% is mixed with 3.1 g of polypyrrole with the mass percentage concentration of 30% and 0.15 g of potassium iodide/potassium tri-iodide, and the mixture is stirred for 10 minutes by ultrasonic waves;
(2) And (3) airing and drying the mixed solution prepared in the step (1) in an environment with the relative humidity of 45% and the temperature of 37 ℃ for 10 hours to obtain the polymer generating film.
Example 2
(1) 6.7 g of a polystyrene sulfonic acid aqueous solution with a mass percentage concentration of 30%, 0.5 g of poly 3, 4-ethylenedioxythiophene with a mass percentage concentration of 30%) are mixed: polystyrene sulfonate, and 0.02 g potassium ferricyanide/potassium ferrocyanide powder were mixed, and stirred ultrasonically for 10 minutes to form a mixed solution;
(2) And (3) airing and drying the mixed solution prepared in the step (1) in an environment with the relative humidity of 45% and the temperature of 37 ℃ for 6 hours to obtain the polymer generating film.
Example 3
(1) Mixing 4.5 g of a 30% by mass concentration aqueous solution of hydroxyethyl cellulose, 0.04 g of a 30% by mass concentration cellulose, and 0.003 g of cobalt bis (trifluoromethanesulfonyl) imide/cobalt bis (trifluoromethanesulfonyl) imide, and stirring ultrasonically for 10 minutes to form a mixed solution;
(2) And (3) airing and drying the mixed solution prepared in the step (1) in an environment with the relative humidity of 45% and the temperature of 37 ℃ for 4 hours to obtain the polymer generating film.
Example 4
(1) Taking two gold sheets with the size of 1X1 cm as electrode layers, wherein one gold sheet is taken as a first electrode layer, the other gold sheet is taken as a second electrode layer, and uniformly punching holes on the second electrode layer, wherein the aperture is 1.3 mm;
(2) The polymer power generation film prepared in example 1 was cut to obtain a polymer power generation film having a size of 1×1 cm, and the first electrode layer, the polymer power generation film after cutting, and the second electrode layer were laminated in this order to obtain a power generation device.
Example 5
(1) Taking two silver sheets with the size of 1X1 cm as electrode layers, wherein one silver sheet is taken as a first electrode layer, the other silver sheet is taken as a second electrode layer, and uniformly punching holes on the second electrode layer, wherein the aperture is 1.3 mm;
(2) The polymer power generation film prepared in example 3 was cut to obtain a polymer power generation film having a size of 1×1 cm, and the first electrode layer, the polymer power generation film after cutting, and the second electrode layer were laminated in this order to obtain a power generation device.
Example 6
(1) Taking two graphite sheets with the size of 1X1 cm as electrode layers, wherein one graphite sheet is taken as a first electrode layer, the other graphite sheet is taken as a second electrode layer, and uniformly punching holes on the second electrode layer, wherein the aperture is 1.3 mm;
(2) The polymer power generation film prepared in example 1 was cut to obtain a polymer power generation film having a size of 1×1 cm, and the first electrode layer, the polymer power generation film after cutting, and the second electrode layer were laminated in this order to obtain a power generation device.
The results show that: the polymer power generation film prepared in example 1 has good mechanical flexibility and a thickness of 1.0 mm. The polymer power generation film prepared in example 2 has good mechanical flexibility and thickness of 0.7 mm. The polymer power generation film prepared in example 3 has good mechanical flexibility and thickness of 0.3 mm.
The power generation devices prepared in example 4, example 5 and example 6 were placed in a humid and natural temperature differential environment (relative humidity 70%, upper and lower electrodes temperature differential 10 ℃), the first and second electrode layers of the power generation device were connected to a test instrument, respectively, and the instrument recorded the generated electrical signals in real time.
The test results show that: referring to fig. 6, the power generation device of example 4 can generate a short-circuit current density of 0.5 milliamp/square centimeter and can be operated continuously for about 24 hours, showing good stability. Referring to fig. 7, the power generation device of example 5 can generate a short-circuit current density of about 0.55 milliamp/square centimeter and can operate continuously for about 24 hours, showing good stability. Referring to fig. 5, the power generation device of example 6 can produce a short circuit current density of about 0.8 milliamp/square centimeter and can operate continuously for about 24 hours, showing good stability.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs. All patents and publications referred to herein are incorporated by reference in their entirety. The terms "comprising" or "including" are used in an open-ended fashion, i.e., including the teachings described herein, but not excluding additional aspects.
In the description of the present specification, reference to the term "one embodiment," "another embodiment," etc., means that a particular feature, structure, material, or characteristic described in connection with the embodiment is included in at least one embodiment of the application. In this specification, schematic representations of the above terms are not necessarily directed to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, the different embodiments or examples described in this specification and the features of the different embodiments or examples may be combined and combined by those skilled in the art without contradiction. In addition, it should be noted that, in this specification, the terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated.
While embodiments of the present application have been shown and described above, it will be understood that the above embodiments are illustrative and not to be construed as limiting the application, and that variations, modifications, alternatives and variations may be made to the above embodiments by one of ordinary skill in the art within the scope of the application.
Claims (6)
1. A polymer power generating film, comprising:
a hydrophilic polymer, a thermally responsive polymer, and a redox electrolyte, wherein the hydrophilic polymer has an oxygen-containing functional group, wherein the mass ratio of the hydrophilic polymer, the thermally responsive polymer, and the redox electrolyte is (79-98.8): (1-18): (0.2-3); the hydrophilic polymer is at least one of polystyrene sulfonic acid, polyacrylic acid and hydroxyethyl cellulose; the thermal response polymer is at least one of poly 3, 4-ethylenedioxythiophene, polystyrene sulfonate, polypyrrole and cellulose; the redox couple electrolyte is at least one of potassium iodide/potassium tri-iodide, potassium ferricyanide/potassium ferrocyanide and bipyridine bis-trifluoromethanesulfonyl imide cobalt/bipyridine bis-trifluoromethanesulfonyl imide cobalt.
2. The polymer power generating film according to claim 1, wherein the thickness of the polymer power generating film is 0.3mm to 1mm.
3. A method of producing the polymer power generating film according to claim 1 or 2, characterized by comprising:
providing a mixed solution comprising a hydrophilic polymer, a thermally responsive polymer, and a redox couple electrolyte;
and (3) carrying out film drying treatment on the mixed solution under the conditions of 35-55% of relative humidity and 20-55 ℃ for 4-10 hours to obtain the polymer power generation film.
4. A method according to claim 3, wherein said providing a mixed solution comprises:
providing an aqueous hydrophilic polymer solution, an aqueous thermally responsive polymer solution, and the redox couple electrolyte;
mixing the aqueous hydrophilic polymer solution, the aqueous thermally responsive polymer solution and the redox electrolyte in a mass ratio of (263-330): (3-60): (0.2-3) stirring and mixing to obtain the mixed solution,
wherein the mass percentage concentration of the hydrophilic polymer aqueous solution and the mass percentage concentration of the thermally responsive polymer aqueous solution are respectively 10-50% independently.
5. A power generation device, comprising at least one power generation structure, wherein the power generation structure comprises a first electrode layer, a polymer power generation film and a second electrode layer which are sequentially stacked, the polymer power generation film is the polymer power generation film according to claim 1 or 2, and a through hole is formed in the first electrode layer or the second electrode layer, and exposes a part of a main surface of the polymer power generation film.
6. The power generation device of claim 5, wherein the materials of the first electrode layer and the second electrode layer each independently comprise at least one of gold, silver, and graphite.
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