CN115683403B - Self-driven hydrogel ionic pressure sensor and manufacturing method thereof - Google Patents
Self-driven hydrogel ionic pressure sensor and manufacturing method thereof Download PDFInfo
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Abstract
The invention provides a self-driven hydrogel ionic pressure sensor and a manufacturing method thereof. The pressure sensor of the present invention comprises: the sensing module converts ion movement induced by pressure into usable output electric signals, and is connected with the detection module to form a working circuit to complete detection work, wherein: the sensing module comprises an upper sealing layer, an upper electrode layer, polycation hydrogel, a porous hydrogel film layer, polyanion hydrogel, a lower electrode layer, a lower sealing layer, wherein the upper sealing layer, the polycation hydrogel, the porous hydrogel film layer, the polyanion hydrogel, the lower electrode layer and the lower electrode layer are sequentially arranged from top to bottom, and the upper electrode layer and the lower electrode layer are connected with the detection module through wires; the detection module comprises a scanning circuit, a signal acquisition circuit, a signal transmission circuit and a signal processor which are sequentially connected. The self-driven hydrogel ionic pressure sensor can effectively complete detection work, has strong mechanical performance, is sensitive and accurate, and can be successfully applied to the aspects of sensing, soft robots, intelligent wearing equipment and the like.
Description
Technical Field
The invention relates to the technical field of sensors, in particular to a self-driven hydrogel ionic pressure sensor and a manufacturing method thereof.
Background
Currently, in the scientific research field, commonly used flexible pressure sensors are classified into resistive, capacitive and piezoelectric sensors. The deformation of the internal structure of the sensor is converted into an external electric signal, and the magnitude and distribution of the applied force are measured according to the change of the electric signal. The resistance type pressure sensor is characterized in that when the resistance type pressure sensor bears a tensile force perpendicular to or parallel to a sample, the resistance value of a sensing material is changed; the capacitive pressure sensor changes the capacitance of a sensing material when being stressed; the piezoelectric pressure sensor changes the voltage in the circuit when receiving a stress. Unlike external circuits, such sensor signal transmission carriers typically need to operate under external circuitry, which in turn limits the miniaturization and practicality of the sensor.
The future flexible sensor not only needs to be suitable for different complex occasions, but also needs to have the basic performances of high sensitivity, flexibility, stretchability, flexibility, low power consumption, good biocompatibility and the like, so as to meet different demands of people in production and life. However, how to design a pressure sensor that combines good stretchability, high sensitivity, and accurate measurement remains a current challenge.
Disclosure of Invention
According to the technical problems, a self-driven hydrogel ionic pressure sensor and a manufacturing method thereof are provided. The self-driven hydrogel ionic pressure sensor device is simple, converts ion movement caused by pressure into usable output electric signals, is connected with a detection module to form a working circuit, can effectively complete detection work, has strong mechanical performance, is sensitive and accurate, and can be successfully applied to sensing, soft robots, intelligent wearing equipment and the like.
The invention adopts the following technical means:
a self-driven hydrogel ionic pressure sensor comprising: the sensing module converts ion movement induced by pressure into usable output electric signals, and is connected with the detection module to form a working circuit to complete detection work, wherein:
the sensing module comprises an upper sealing layer, an upper electrode layer, polycation hydrogel, a porous hydrogel film layer, polyanion hydrogel, a lower electrode layer and a lower sealing layer which are sequentially arranged from top to bottom, wherein the upper electrode layer and the lower electrode layer are connected with the detection module through wires;
the detection module comprises a scanning circuit, a signal acquisition circuit, a signal transmission circuit and a signal processor which are sequentially connected.
Further, the upper sealing layer and the lower sealing layer are made of PDMS.
Further, the electrode strips of the upper electrode layer and the lower electrode layer are processed by using a nano-imprinting technology, the electrode strips of the upper electrode layer are attached below the upper sealing layer, and the electrode strips of the lower electrode layer are attached above the lower sealing layer.
Further, the upper electrode layer comprises a plurality of transverse electrode strips which are distributed in an equidistant array, the lower electrode layer comprises a plurality of longitudinal electrode strips which are distributed in an equidistant array, the transverse electrode strips and the longitudinal electrode strips form vertical crossing points, and the detection module is used for detecting voltage change values at each vertical crossing point and processing current signals.
Further, by increasing the number of electrode bars of the upper electrode layer and the lower electrode layer, the vertical crossing point of the upper electrode layer and the lower electrode layer is further increased, so that the measured pressure distribution information is accurate and used for adjusting the measuring range of the sensor.
Further, the polycationic hydrogel and the polyanionic hydrogel are both double-network hydrogels, the polycationic hydrogel includes free mobile cations inside, and the polyanionic hydrogel includes free mobile anions inside.
Further, the porous hydrogel film layer is arranged between the polycation hydrogel and the polyanion hydrogel, and the polycation hydrogel and the polyanion hydrogel are connected together through the porous hydrogel film layer, and the porous hydrogel film layer is of a porous structure and has rectifying ion transmission characteristics.
The invention also provides a manufacturing method of the self-driven hydrogel ionic pressure sensor based on the above, which comprises the following steps:
step 1, agar, AM, MBA and sodium polystyrene sulfonate are dissolved in deionized water according to a certain concentration;
step 2, putting the dissolved solution into a magnetic stirrer, setting the temperature at 90 ℃, and mixing and stirring for 2 hours;
step 3, vacuum degassing the obtained clear solution, injecting the clear solution into two organic glass plates separated by a silicone sheet, and cooling the clear solution at 4 ℃ for 30 minutes;
step 4, transferring the organic glass mould to the mould with the intensity of 22.4mW/cm 2 Photopolymerization is carried out for 13 minutes under an ultraviolet lamp, and AM polymerization is initiated to obtain polycation hydrogel;
step 5, preparing polydiallyl dimethyl ammonium chloride by adopting the same method as the step 4 to obtain polyanion hydrogel;
step 6, taking the hydrogel out of the organic glass die, covering the hydrogel with a paraffin film, and testing;
step 7, molding two hydrogels into a film with the length of 10cm, the width of 6cm and the thickness of 3mm to be used as a sensor component;
step 8, preparing a nano-imprinted silicon template by utilizing a laser interference lithography technology, wherein the nano-imprinted silicon template is two moulds with the length of 10cm and the width of 6cm and the thickness of 3mm, and the upper part of the nano-imprinted silicon template is provided with an equidistant electrode strip structure;
step 9, taking PDMS as a substrate, adding PEDOT PSS as a matrix at the upper part of the substrate, contacting a template with the matrix, carrying out accurate imprinting shaping, heating at 150 ℃ for 20 minutes, integrally annealing at 120 ℃ for half an hour, demolding, and separating the template;
and 10, separating the two materials through a porous hydrogel film, and respectively attaching sealing layers to the polycation hydrogel layer and the polyanion hydrogel layer to prepare the self-driven hydrogel ionic pressure sensor.
Compared with the prior art, the invention has the following advantages:
1. the self-driven hydrogel ionic pressure sensor provided by the invention has high stretchability, high transparency and good durability, and can realize high-precision monitoring of pressure, and the remarkable characteristics promote the application of the self-driven hydrogel ionic pressure sensor in flexible wearable electronic products such as sensors.
2. The self-driven hydrogel ionic pressure sensor provided by the invention has the advantages of excellent mechanical property, biocompatibility, self-healing property and the like.
3. The self-driven hydrogel ionic pressure sensor provided by the invention has different mechanical properties from the traditional hydrogel, and the breaking strength and the breaking strain of the self-driven hydrogel ionic pressure sensor are improved by several times due to the unique double-network structure, because the effective coordination of the two internal networks greatly dissipates the applied external energy. Therefore, the invention has high strength mechanical property and obviously improved service life.
4. The self-driven hydrogel ionic pressure sensor provided by the invention adopts the unique transverse and longitudinal crossed array type layout electrodes, and can rapidly realize accurate measurement of the pressed position in the sensor so as to complete real-time state monitoring of the wearing part of the sensor when the sensor is worn.
5. The self-driven hydrogel ionic pressure sensor provided by the invention can provide novel flexible pressure sensing equipment based on hydrogel ionic current for sensing, soft robots and human-computer interfaces.
For the reasons, the invention can be widely popularized in the fields of sensors and the like.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described, and it is obvious that the drawings in the following description are some embodiments of the present invention, and other drawings may be obtained according to the drawings without inventive effort to a person skilled in the art.
FIG. 1 is a schematic diagram of the self-driven hydrogel ionic pressure sensor of the present invention.
Fig. 2 is a schematic block diagram of a pressure sensing device based on a self-driven hydrogel ionic pressure sensor.
In the figure: 1. an upper sealing layer; 2. an upper electrode layer; 3. a polycationic hydrogel; 4. a porous hydrogel film layer; 5. a polyanionic hydrogel; 6. a lower electrode layer; 7. and a lower sealing layer.
Detailed Description
It should be noted that, without conflict, the embodiments of the present invention and features of the embodiments may be combined with each other. The invention will be described in detail below with reference to the drawings in connection with embodiments.
For the purpose of making the objects, technical solutions and advantages of the embodiments of the present invention more apparent, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, not all embodiments. The following description of at least one exemplary embodiment is merely exemplary in nature and is in no way intended to limit the invention, its application, or uses. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the present invention. As used herein, the singular is also intended to include the plural unless the context clearly indicates otherwise, and furthermore, it is to be understood that the terms "comprises" and/or "comprising" when used in this specification are taken to specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof.
The relative arrangement of the components and steps, numerical expressions and numerical values set forth in these embodiments do not limit the scope of the present invention unless it is specifically stated otherwise. Meanwhile, it should be clear that the dimensions of the respective parts shown in the drawings are not drawn in actual scale for convenience of description. Techniques, methods, and apparatus known to those of ordinary skill in the relevant art may not be discussed in detail, but are intended to be part of the specification where appropriate. In all examples shown and discussed herein, any specific values should be construed as merely illustrative, and not a limitation. Thus, other examples of the exemplary embodiments may have different values. It should be noted that: like reference numerals and letters denote like items in the following figures, and thus once an item is defined in one figure, no further discussion thereof is necessary in subsequent figures.
In the description of the present invention, it should be understood that the azimuth or positional relationships indicated by the azimuth terms such as "front, rear, upper, lower, left, right", "lateral, vertical, horizontal", and "top, bottom", etc., are generally based on the azimuth or positional relationships shown in the drawings, merely to facilitate description of the present invention and simplify the description, and these azimuth terms do not indicate and imply that the apparatus or elements referred to must have a specific azimuth or be constructed and operated in a specific azimuth, and thus should not be construed as limiting the scope of protection of the present invention: the orientation word "inner and outer" refers to inner and outer relative to the contour of the respective component itself.
Spatially relative terms, such as "above … …," "above … …," "upper surface at … …," "above," and the like, may be used herein for ease of description to describe one device or feature's spatial location relative to another device or feature as illustrated in the figures. It will be understood that the spatially relative terms are intended to encompass different orientations in use or operation in addition to the orientation depicted in the figures. For example, if the device in the figures is turned over, elements described as "above" or "over" other devices or structures would then be oriented "below" or "beneath" the other devices or structures. Thus, the exemplary term "above … …" may include both orientations of "above … …" and "below … …". The device may also be positioned in other different ways (rotated 90 degrees or at other orientations) and the spatially relative descriptors used herein interpreted accordingly.
In addition, the terms "first", "second", etc. are used to define the components, and are only for convenience of distinguishing the corresponding components, and the terms have no special meaning unless otherwise stated, and therefore should not be construed as limiting the scope of the present invention.
As shown in fig. 1-2, the present invention provides a self-driven hydrogel ionic pressure sensor comprising: the sensing module converts ion movement induced by pressure into usable output electric signals, and is connected with the detection module to form a working circuit to complete detection work, wherein:
the sensing module comprises an upper sealing layer 1, an upper electrode layer 2, polycation hydrogel 3, a porous hydrogel film layer 4, polyanion hydrogel 5, a lower electrode layer 6 and a lower sealing layer 7 which are sequentially arranged from top to bottom, wherein the upper electrode layer 2 and the lower electrode layer 6 are connected with the detection module through wires;
the detection module comprises a scanning circuit, a signal acquisition circuit, a signal transmission circuit and a signal processor which are sequentially connected.
In particular, as a preferred embodiment of the present invention, PDMS is used for both the upper seal layer 1 and the lower seal layer 7, and the thickness is 1mm. PDMS was prepared from Sylgard 184silicone kit (dakaning).
In specific implementation, as a preferred embodiment of the present invention, the electrode strips of the upper electrode layer 2 and the lower electrode layer 6 are processed by using a nanoimprint technique, the electrode strip of the upper electrode layer 2 is attached below the upper sealing layer 1, and the electrode strip of the lower electrode layer 6 is attached above the lower sealing layer 7.
In a specific implementation, as a preferred embodiment of the present invention, the upper electrode layer 2 includes a plurality of transverse electrode strips arranged in an equidistant array, the lower electrode layer 6 includes a plurality of longitudinal electrode strips arranged in an equidistant array, the transverse electrode strips and the longitudinal electrode strips form vertical crossing points, and the detection module is used for detecting a voltage variation value at each vertical crossing point and processing a current signal. In this example, each electrode strip was 1cm long, 50nm thick, 0.5cm wide, and 0.25cm apart.
In practice, as a preferred embodiment of the present invention, the number of electrode bars of the upper electrode layer 2 and the lower electrode layer 6 is increased, and thus the vertical crossing points of the upper electrode layer 2 and the lower electrode layer 6 are increased, so that the measured pressure distribution information is accurate, and the pressure distribution information is used for adjusting the sensor range.
In particular, as a preferred embodiment of the present invention, the polycationic hydrogel 3 and the polyanionic hydrogel 5 are dual-network hydrogels, wherein the polycationic hydrogel 3 includes free mobile cations therein, and the polyanionic hydrogel 5 includes free mobile anions therein. In this example, the length of the polycationic hydrogel 3 and the length of the polyanionic hydrogel 5 are 6cm, the width thereof is 4cm, and the thickness thereof is about 1mm.
In particular, as a preferred embodiment of the present invention, the porous hydrogel film layer 4 is disposed between the polycationic hydrogel 3 and the polyanionic hydrogel 5, and the polycationic hydrogel 3 and the polyanionic hydrogel 5 are connected together through the porous hydrogel film layer 4, and the porous hydrogel film layer 4 has a porous structure and has a rectifying ion transport property. In this example, the porous hydrogel film layer 4 has an average pore size of 1 μm and a thickness of 5 μm to 30 μm which is adjustable. The porous hydrogel film is tightly attached to the polycation hydrogel and the polyanion hydrogel, so that ion diffusion movement between the two hydrogels is completed, and electric potential is established. The porous hydrogel film was prepared based on a solution phase inversion method, with an average pore size of 1 μm and a thickness of 20 μm.
The working principle of the self-driven hydrogel ionic pressure sensor is as follows:
the polycationic hydrogels and polyanionic hydrogels in the sensing module of the present invention are separated via porous hydrogel films, similar to p-n semiconductor junctions. The polyanion and polycation hydrogel are connected together through the porous hydrogel film, so that the movable anions and cations in the hydrogel layer diffuse to the corresponding areas through the film, and an initial induced electromotive force is generated when the concentration of the anions and the polycation hydrogel reaches dynamic balance. When the hydrogel layer is subjected to externally applied pressure, the volume of the space of the hydrogel layer is changed, and part of cations or anions which are movable in the hydrogel layer are transferred out, so that the concentration of the anions is larger or smaller than that of the cations, the anions are balanced, and the electrodes induce charges, so that an external circuit generates current. Sensing the pressure by measuring the magnitude of external induced current, thereby realizing accurate measurement of the pressure; when the external pressure is eliminated, the anions and cations return to the initial equilibrium state again, the corresponding induced current starts to decrease, and the induced potential also returns to the initial value, namely, a series of works are completed in a self-driven manner.
In the invention, the upper layer of hydrogel and the lower layer of hydrogel are provided with the cross array type electrodes, and the electrodes are connected with the digital signal processor through leads, so that when the electrodes are under the action of pressure, the sensor generates current. The electrode strips of the upper electrode layer and the lower electrode layer are arranged at equal intervals and are mutually perpendicular, so that voltage change information at each intersection is measured, a scanning circuit is used for scanning and judging whether the voltage at each intersection of the corresponding m-th row and the n-th row of the ion sensor changes, a Digital Signal Processing (DSP) unit is used for collecting and enhancing signals of abnormal scanning in a digital mode, data of each group are recorded, the analog signals obtained through processing are transmitted into a processor, intelligent decision is completed, judgment and feedback of the pressed position are realized, and external pressure distribution information on the sensor is obtained. The DSP has small size, accuracy and high speed, and can accurately monitor the pressure and the position on the sensor in real time by matching with the sensor.
The invention also provides a manufacturing method of the self-driven hydrogel ionic pressure sensor, which comprises the following steps:
step 1, agar (1.26 g), AM (14.52 g), MBA (0.012 g) and sodium polystyrene sulfonate are dissolved in deionized water at a certain concentration;
step 2, putting the dissolved solution into a magnetic stirrer, setting the temperature at 90 ℃, and mixing and stirring for 2 hours;
step 3, vacuum degassing the obtained clear solution, injecting the clear solution into two organic glass plates separated by a silicone sheet, and cooling the clear solution at 4 ℃ for 30 minutes;
step 4, transferring the organic glass mould to the mould with the intensity of 22.4mW/cm 2 Photopolymerization is carried out for 13 minutes under an ultraviolet lamp, and AM polymerization is initiated to obtain polycation hydrogel;
step 5, preparing polydiallyl dimethyl ammonium chloride by adopting the same method as the step 4 to obtain polyanion hydrogel; in this example, the polycationic hydrogels and the polyanionic hydrogels were prepared by a one-pot method, and were prepared by adding agar, AM, MBA, sodium polystyrene sulfonate, etc., and were excellent in mechanical properties.
Step 6, taking the hydrogel out of the organic glass die, covering the hydrogel with a paraffin film, and testing;
step 7, molding two hydrogels into a film with the length of 10cm, the width of 6cm and the thickness of 3mm to be used as a sensor component;
step 8, preparing a nano-imprinted silicon template by utilizing a laser interference lithography technology, wherein the nano-imprinted silicon template is two moulds with the length of 10cm and the width of 6cm and the thickness of 3mm, and the upper part of the nano-imprinted silicon template is provided with an equidistant electrode strip structure;
step 9, taking PDMS as a substrate, adding PEDOT PSS as a matrix at the upper part of the substrate, contacting a template with the matrix, carrying out accurate imprinting shaping, heating at 150 ℃ for 20 minutes, integrally annealing at 120 ℃ for half an hour, demolding, and separating the template; in this example, PEDOT PSS is a polymer blend of PEDOT and PSS formed by ionic interactions, with high stability and processability in aqueous solutions and high conductivity.
And 10, separating the two materials through a porous hydrogel film, and respectively attaching sealing layers to the polycation hydrogel layer and the polyanion hydrogel layer to prepare the self-driven hydrogel ionic pressure sensor.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and not for limiting the same; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some or all of the technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit of the invention.
Claims (8)
1. A self-driven hydrogel ionic pressure sensor, comprising: the sensing module converts ion movement induced by pressure into usable output electric signals, and is connected with the detection module to form a working circuit to complete detection work, wherein:
the sensing module comprises an upper sealing layer, an upper electrode layer, polycation hydrogel, a porous hydrogel film layer, polyanion hydrogel, a lower electrode layer and a lower sealing layer which are sequentially arranged from top to bottom, wherein the upper electrode layer and the lower electrode layer are connected with the detection module through wires;
the detection module comprises a scanning circuit, a signal acquisition circuit, a signal transmission circuit and a signal processor which are sequentially connected.
2. The self-driven hydrogel ionic pressure sensor of claim 1, wherein both the upper sealing layer and the lower sealing layer are PDMS.
3. The self-driven hydrogel ionic pressure sensor of claim 1, wherein the electrode strips of the upper and lower electrode layers are fabricated using nanoimprint techniques, the electrode strips of the upper electrode layer being attached below the upper sealing layer, the electrode strips of the lower electrode layer being attached above the lower sealing layer.
4. A self-driven hydrogel ionic pressure sensor as claimed in claim 3, wherein the upper electrode layer comprises a plurality of transverse electrode strips arranged in an equidistant array, the lower electrode layer comprises a plurality of longitudinal electrode strips arranged in an equidistant array, the transverse electrode strips and the longitudinal electrode strips form vertical crossing points, and the detection module is used for detecting voltage variation values at each vertical crossing point and processing current signals.
5. A self-driven hydrogel ionic pressure transducer as claimed in claim 3, wherein the vertical crossing of the upper and lower electrode layers is increased by increasing the number of electrode strips of the upper and lower electrode layers, thereby allowing accurate measured pressure profile information for adjustment of the transducer range.
6. The self-driven hydrogel ionic pressure transducer of claim 1, wherein the polycationic hydrogel and the polyanionic hydrogel are both double network hydrogels, the polycationic hydrogel comprising free mobile cations within the interior and free mobile anions within the interior of the polyanionic hydrogel.
7. The self-driven hydrogel ionic pressure transducer of claim 1, wherein the porous hydrogel film layer is disposed between the polycationic hydrogel and the polyanionic hydrogel, and the polycationic hydrogel and the polyanionic hydrogel are connected together by the porous hydrogel film layer, the porous hydrogel film layer being of porous structure having rectifying ion transport properties.
8. A method of making a self-driven hydrogel ionic pressure sensor according to any one of claims 1 to 7, comprising:
step 1, agar, AM, MBA and sodium polystyrene sulfonate are dissolved in deionized water according to a certain concentration;
step 2, putting the dissolved solution into a magnetic stirrer, setting the temperature at 90 ℃, and mixing and stirring for 2 hours;
step 3, vacuum degassing the obtained clear solution, injecting the clear solution into two organic glass plates separated by a silicone sheet, and cooling the clear solution at 4 ℃ for 30 minutes;
step 4, transferring the organic glass mould to the mould with the intensity of 22.4mW/cm 2 Photopolymerization is carried out for 13 minutes under an ultraviolet lamp, and AM polymerization is initiated to obtain polycation hydrogel;
step 5, preparing polydiallyl dimethyl ammonium chloride by adopting the same method as the step 4 to obtain polyanion hydrogel;
step 6, taking the hydrogel out of the organic glass die, covering the hydrogel with a paraffin film, and testing;
step 7, molding two hydrogels into a film with the length of 10cm, the width of 6cm and the thickness of 3mm to be used as a sensor component;
step 8, preparing a nano-imprinted silicon template by utilizing a laser interference lithography technology, wherein the nano-imprinted silicon template is two moulds with the length of 10cm and the width of 6cm and the thickness of 3mm, and the upper part of the nano-imprinted silicon template is provided with an equidistant electrode strip structure;
step 9, taking PDMS as a substrate, adding PEDOT PSS as a matrix at the upper part of the substrate, contacting a template with the matrix, carrying out accurate imprinting shaping, heating at 150 ℃ for 20 minutes, integrally annealing at 120 ℃ for half an hour, demolding, and separating the template;
and 10, separating the two materials through a porous hydrogel film, and respectively attaching sealing layers to the polycation hydrogel layer and the polyanion hydrogel layer to prepare the self-driven hydrogel ionic pressure sensor.
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