CN108565048B - Conformal biodegradable implantable flexible energy supply device and preparation method thereof - Google Patents
Conformal biodegradable implantable flexible energy supply device and preparation method thereof Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01B5/00—Non-insulated conductors or conductive bodies characterised by their form
- H01B5/14—Non-insulated conductors or conductive bodies characterised by their form comprising conductive layers or films on insulating-supports
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
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Abstract
一种共形的生物可降解植入式柔性供能器件及其制备方法，用于给埋设在体内的微/纳米植入式医疗器械提供电能，包括有柔性基底层，分别设置在所述柔性基底层上的柔性供能器件负极和柔性供能器件正极，所述的柔性供能器件负极和柔性供能器件正极通过与人体生物组织液中的葡萄糖和氧气的氧化还原反应获得电能，所述的柔性供能器件负极和柔性供能器件正极上分别引出用于连接埋设在体内的微/纳米植入式医疗器械进行供电的负极引线和正极引线。本发明具有一定的抗弯曲和抗拉伸的功能，能够与其他植入式器件共形，可以用于给任意形状的微/纳米植入式医疗器械供能，能长时间稳定供能，能量传输效率高。
A conformal biodegradable implantable flexible energy supply device and a preparation method thereof, which are used for providing electrical energy to micro/nano implantable medical devices embedded in the body, comprising a flexible base layer, respectively arranged on the flexible The negative electrode of the flexible energy supply device and the positive electrode of the flexible energy supply device on the substrate layer, the negative electrode of the flexible energy supply device and the positive electrode of the flexible energy supply device obtain electrical energy through redox reactions with glucose and oxygen in human biological tissue fluid, and the said The negative electrode of the flexible energy supply device and the positive electrode of the flexible energy supply device respectively lead out a negative electrode lead and a positive electrode lead for connecting the micro/nano implantable medical device embedded in the body for power supply. The invention has certain anti-bending and anti-stretching functions, can conform to other implantable devices, can be used to supply energy to micro/nano implantable medical devices of any shape, and can supply energy stably for a long time. High transmission efficiency.
Description
Technical Field
The invention relates to an implantable energy supply device. In particular to a conformal biodegradable implanted flexible energy supply device and a preparation method thereof.
Background
In recent years, with the rapid development of new technologies, new processes, new materials and the like, implantable medical devices break through the technical bottleneck continuously, and more micro/nano implantable medical devices are applied to human bodies. The micro/nano implantable medical devices can be used for continuously monitoring the physiological health state of a human body so as to provide disease change trend and help the treatment of diseases; can also be used for accurately treating diseases at specific positions and the like. Among these micro/nano-implantable medical devices, there is a class of devices known as biodegradable devices that have received widespread attention from various societies in recent years. The device can be automatically decomposed after working in a human body for a period of time, and is discharged out of the body along with the physiological circulation of the human body, and the device has the advantages of no harm to the human body and no need of secondary operation for extraction.
While these biodegradable micro/nano-implantable medical devices are mostly operated with electrical energy, limited by the state of the art, it remains a challenge to power implantable devices in vivo. Researchers use degradable wireless radio frequency energy transmission modules for energy supply, but the method firstly needs an external energy supply source and secondly has the problems of limitation of energy transmission direction and low energy transmission efficiency. There are also ways that researchers can collect mechanical energy from human body movement by an energy collector and then convert it into electrical energy, however this method requires implanting the device in a specific long-term moving part, such as the heart, etc., which limits the range of use of the device. More importantly, due to the limitations of the development of materials science, none of the implantable energizing devices utilized in these current methods are completely degradable, yet require a secondary operation for removal. In contrast, the conformal biodegradable implantable flexible energy supply device has high energy transmission efficiency, can be conformally combined with implantable devices in various shapes, is not limited by an implantation position, can be completely biodegraded, and can be used for solving the energy supply problem of biodegradable micro/nano implantable medical devices.
Disclosure of Invention
The invention aims to solve the technical problem of providing a conformal biodegradable implantable flexible energy supply device which can be used for supplying energy to a micro/nano implantable medical device in any shape and a preparation method thereof.
The technical scheme adopted by the invention is as follows: the utility model provides a flexible energy supply device of conformal biodegradable implantation for bury underground in vivo little/nanometer implantation type medical instrument provide the electric energy, including flexible stratum basale, set up respectively flexible energy supply device negative pole and flexible energy supply device positive pole on the flexible stratum basale, flexible energy supply device negative pole and flexible energy supply device positive pole obtain the electric energy through the redox reaction with glucose and oxygen in the human biological tissue liquid, flexible energy supply device negative pole and flexible energy supply device positive pole on draw respectively and be used for connecting the negative pole lead wire and the positive lead wire that bury underground in vivo little/nanometer implantation type medical instrument and supply power.
The flexible energy supply device negative pole set up in proper order from bottom to top can biodegradable negative electrode layer, can biodegradable ferroferric oxide and glucose oxidase molecular layer and can biodegradable negative pole chitosan film layer on the flexible substrate layer, negative pole lead integrative formation is in a side of negative electrode layer.
The positive electrode of the flexible energy supply device comprises a biodegradable positive electrode layer, a biodegradable ferroferric oxide and laccase molecular layer and a biodegradable positive chitosan film layer which are sequentially arranged on a flexible substrate layer from bottom to top, and a positive lead is integrally formed on one side edge of the positive electrode layer.
The flexible substrate layer is made of polylactic acid or polyvinyl alcohol or polycaprolactone or polybutylene succinate which can be completely biodegraded.
The negative electrode layer, the positive electrode layer, the negative lead and the positive lead are made of conductive materials which can be completely biodegraded by doping aluminum with zinc oxide or magnesium with zinc oxide or zinc or magnesium.
A preparation method of a conformal biodegradable implantable flexible energy supply device comprises the following process steps:
1) processing the flexible substrate layer: melting the flexible substrate material particles into dichloromethane to form a uniform solution, extracting a set amount of the solution, placing the solution on a flat plate, uniformly coating the solution on the flat plate by using a coating rod, and obtaining a flexible substrate layer after dichloromethane in the solution is completely evaporated;
2) respectively printing conductive ink on the prepared PLA flexible substrate layer according to the patterns of the cathode electrode layer and the anode electrode layer by using an ink-jet printing system, wherein the printing comprises correspondingly printing a cathode lead and an anode lead, and then heating to finish the annealing of the electrodes, namely finishing the processing of the cathode electrode layer and the anode electrode layer as well as the cathode lead and the anode lead;
3) printing ferroferric oxide nanoparticle ink and glucose oxidase ink on a negative electrode layer to form a ferroferric oxide and glucose oxidase molecular layer, then dripping chitosan solution to form a negative chitosan film layer, and air-drying to finish the preparation of the negative electrode of the flexible energy supply device;
4) and printing ferroferric oxide nanoparticle ink and laccase ink on an anode electrode layer to form a ferroferric oxide and laccase molecular layer, dripping chitosan solution to form an anode chitosan thin layer, and air-drying to finish the preparation of the anode of the flexible energy supply device, thereby finishing the preparation of the conformal biodegradable implantable flexible energy supply device.
The flat plate in the step 1) is a polypropylene plate or a glass plate or a stainless steel plate or an aluminum plate which does not react with dichloromethane.
The flexible substrate material is polylactic acid or polyvinyl alcohol or polycaprolactone or poly butylene succinate material which can be completely biodegraded.
The negative electrode layer, the positive electrode layer, the negative lead and the positive lead are made of conductive materials which can be completely biodegraded by doping aluminum with zinc oxide or magnesium with zinc oxide or zinc or magnesium.
The conformal biodegradable implantable flexible energy supply device and the preparation method thereof have the following advantages:
1. the energy supply device is manufactured on a polylactic acid (PLA) film substrate, and the chitosan film and the PLA which form the energy source device are both flexible materials, have certain bending resistance and stretching resistance, can be conformal with other implanted devices, and can be used for supplying energy to micro/nano implanted medical equipment in any shape.
2. The energy source of the energy supply device is derived from the redox reaction of glucose and oxygen in the tissue fluid in vivo, and the glucose concentration in the tissue fluid in vivo is relatively stable and the glucose source is continuous, so the energy supply device can stably supply energy for a long time and is not limited by the implantation position.
3. The energy source of the energy supply device comes from the redox reaction of glucose and oxygen in tissue fluid in vivo, and compared with other energy devices, the energy source based on glucose has high energy transmission efficiency and does not need external energy excitation.
4. All the components of the energy supply device, including PLA, aluminum-doped zinc oxide, trimaran tetroxide nanoparticles, glucose oxidase, laccase and chitosan, are biodegradable materials, so that the formed energy supply device can be completely biodegraded, and the problem of taking out the energy supply device in a secondary operation is avoided.
Drawings
Fig. 1 is a schematic diagram of a use state of the conformal biodegradable implantable flexible energy supply device of the invention;
fig. 2 is a schematic structural diagram of a conformal biodegradable implantable flexible energy supply device according to the present invention;
FIG. 3 is a schematic structural diagram of a negative electrode of the flexible energy supply device of the present invention;
fig. 4 is a schematic structural diagram of the anode of the flexible energy supply device in the invention.
In the drawings
1: human biological tissue 2: micro/nano implantation type medical apparatus
3: conformal biodegradable implantable flexible energy supply device
4: negative pole 5 of flexible energy supply device: flexible energy supply device anode
6 a: negative chitosan film layer 6 b: positive chitosan film layer
7: molecular layer of ferroferric oxide and glucose oxidase 8: molecular layer of ferroferric oxide and laccase
9 a: negative electrode layer 9 b: positive electrode layer
10: flexible substrate layer 11: negative electrode lead
12: positive electrode lead
Detailed Description
The following provides a detailed description of the conformal biodegradable implantable flexible energy supply device and the preparation method thereof according to the present invention with reference to the following embodiments and the accompanying drawings.
The conformal biodegradable implantable flexible energy supply device mainly comprises a flexible substrate layer, a substrate electrode layer, nano particles, an enzyme molecular layer and a chitosan film layer from bottom to top; ferroferric oxide nano particles and a laccase molecular layer are solidified between the substrate electrode layer and the chitosan film layer, and a primary battery anode is formed after solidification; ferroferric oxide nano particles and a glucose oxidase molecular layer are solidified between the substrate electrode layer and the chitosan film layer, and the primary battery cathode is formed after solidification. The flexible substrate layer is a polylactic acid film layer. The substrate electrode layer is an aluminum-doped zinc oxide electrode.
The conformal biodegradable implantable flexible energy supply device of the invention, as shown in fig. 1, is used for supplying electric energy to a micro/nano implantable medical device 2 embedded in a body. The conformal biodegradable implantable flexible energy supply device 3 supplies energy to the micro/nano implantable medical device 2 implanted into the human biological tissue 1, and the conformal biodegradable implantable flexible energy supply device 3 can be conformal to the micro/nano implantable medical device 2 in any shape, so that stable electric energy is supplied to the micro/nano implantable medical device. The conformal biodegradable implantable flexible energy supply device has the advantages of flexibility and conformality, high energy transmission efficiency, complete biodegradation and no limitation of an implantation position, and can be used for supplying energy to a micro/nano implantable medical device.
The specific structure is as shown in fig. 2, including flexible substrate layer 10, set up respectively flexible energy supply device negative pole 4 and flexible energy supply device positive pole 5 on the flexible substrate layer 10, flexible energy supply device negative pole 4 and flexible energy supply device positive pole 5 obtain the electric energy through the redox reaction with glucose and oxygen in human biological tissue 1 liquid, flexible energy supply device negative pole 4 and flexible energy supply device positive pole 5 on draw out respectively and be used for connecting the interior little/nanometer implanted medical instrument 2 of burying underground and carry out the negative pole lead 11 and the positive pole lead 12 of supplying power.
The flexible substrate layer 10 is made of polylactic acid (PLA), polyvinyl alcohol (PHA), Polycaprolactone (PCL), polybutylene succinate (PBS) and other materials which can be completely biodegraded.
As shown in fig. 3, the flexible energy supply device negative electrode 4 includes a biodegradable negative electrode layer 9a, a biodegradable ferroferric oxide and glucose oxidase molecular layer 7 and a biodegradable negative chitosan thin film layer 6a, which are sequentially disposed on the flexible substrate layer 10 from bottom to top, and the negative electrode lead 11 is integrally formed at one side of the negative electrode layer 9 a.
As shown in fig. 4, the flexible energy supply device positive electrode 5 includes a biodegradable positive electrode layer 9b, a biodegradable ferroferric oxide and laccase molecular layer 8 and a biodegradable positive chitosan thin film layer 6b, which are sequentially disposed on the flexible substrate layer 10 from bottom to top, and the positive lead 12 is integrally formed on one side of the positive electrode layer 9 b.
The negative electrode layer 9a, the positive electrode layer 9b, the negative lead 11 and the positive lead 12 are made of conductive materials which can be completely biodegraded by aluminum-doped zinc oxide or magnesium-doped zinc oxide or zinc or magnesium.
The conformal biodegradable implantable flexible energy supply device disclosed by the invention has the working process that the energy supply device is conformally attached to the surface of an implantable micro/nano implantable medical device, and a small amount of aluminum-doped zinc oxide ink is used for bonding an electrode and a power supply input end of the device together and implanting the electrode and the power supply input end of the device into human tissues for working together. The energy is generated by oxidation-reduction reaction between two electrodes, and glucose molecules in the biological tissue fluid are oxidized by glucose oxidase to generate carbon dioxide and water at the negative electrode of the primary battery; in the process, glucose molecules are decomposed into hydrogen peroxide, the ferroferric oxide nanoparticles are used for catalyzing and decomposing the hydrogen peroxide, the hydrogen peroxide is prevented from influencing the activity of the glucose oxidase, and meanwhile, the nanoparticles are also used for enhancing the electron transfer efficiency. At the anode of the primary battery, oxygen in biological tissue fluid is reduced into water by laccase, and the ferroferric oxide nanoparticles are used for enhancing the electron transfer efficiency. Electrons are transferred from the negative electrode to the positive electrode of the cell. Thus, an electromotive force is generated at both ends of the power input of the external micro/nano implantable medical device.
After working for a period of time, the conformal biodegradable implantable flexible energy supply device can be degraded by an organism together with the degradable implantable micro/nano medical apparatus, so that the problem of taking out in a secondary operation is avoided.
The preparation method of the conformal biodegradable implantable flexible energy supply device comprises the following process steps:
1) processing a PLA flexible substrate layer: melting flexible substrate material particles into dichloromethane to form a uniform solution, extracting a set amount of solution, placing the solution on a flat plate, uniformly coating the solution on the flat plate by using a coating rod, and obtaining a PLA flexible substrate layer after dichloromethane in the solution is completely evaporated; the flat plate is a polypropylene plate or a glass plate or a stainless steel plate or an aluminum plate which does not react with dichloromethane. The flexible substrate material is polylactic acid or polyvinyl alcohol or polycaprolactone or poly butylene succinate material which can be completely biodegraded.
2) Respectively printing the aluminum-doped zinc oxide ink on a prepared PLA flexible substrate layer according to the patterns of a negative electrode layer and a positive electrode layer by using an ink-jet printing system (or other printing processes), respectively printing a negative lead and a positive lead, and then heating at 100 ℃ for one hour to finish annealing, namely finishing the processing of the negative electrode layer and the positive electrode layer as well as the negative lead and the positive lead;
3) printing ferroferric oxide nanoparticle ink and glucose oxidase ink on a negative electrode layer to form a ferroferric oxide and glucose oxidase molecular layer, then dripping chitosan solution to form a negative chitosan film layer, and air-drying to finish the preparation of the negative electrode of the flexible energy supply device;
4) and printing ferroferric oxide nanoparticle ink and laccase ink on an anode electrode layer to form a ferroferric oxide and laccase molecular layer, dripping chitosan solution to form an anode chitosan thin layer, and air-drying to finish the preparation of the anode of the flexible energy supply device, thereby finishing the preparation of the conformal biodegradable implantable flexible energy supply device.
The negative electrode layer, the positive electrode layer, the negative lead and the positive lead are made of conductive materials which can be completely biodegraded by doping aluminum with zinc oxide or magnesium with zinc oxide or zinc or magnesium.
All combinations of the invention disclosed and disclosed herein can be made by reference to the present disclosure, and although the combinations of the invention have been described in terms of detailed implementation, it will be apparent to those skilled in the art that the apparatus described herein can be combined or modified or certain parts can be added or removed without departing from the spirit, scope and range of the invention, and more particularly, all such similar substitutes and modifications will be apparent to those skilled in the art and are intended to be included within the spirit, scope and range of the invention.
Claims (3)
1. The utility model provides a flexible energy supply device of conformal biodegradable implantation for bury underground in vivo little/nanometer implantation medical instrument (2) provide the electric energy, its characterized in that, be attached to the implanted little/nanometer medical instrument surface of arbitrary shape with the energy supply device is conformal, implant in human tissue, the energy supply device is including flexible stratum basale (10), set up respectively flexible energy supply device negative pole (4) and flexible energy supply device positive pole (5) on flexible stratum basale (10), flexible energy supply device negative pole (4) and flexible energy supply device positive pole (5) obtain the electric energy through the redox reaction with glucose and oxygen in human biological tissue (1) liquid, flexible energy supply device negative pole (4) and flexible energy supply device positive pole (5) on draw out negative pole lead (11) and the positive lead that are used for connecting the implanted power supply of the little/nanometer medical instrument (2) of burying underground in vivo respectively and carry out the negative pole lead (11) and the positive pole of lead that supply power (12) (ii) a
The flexible energy supply device cathode (4) comprises a biodegradable cathode electrode layer (9 a), a biodegradable ferroferric oxide and glucose oxidase molecular layer (7) and a biodegradable cathode chitosan film layer (6 a) which are sequentially arranged on the flexible substrate layer (10) from bottom to top, and the cathode lead (11) is integrally formed on one side of the cathode electrode layer (9 a);
the flexible energy supply device anode (5) comprises a biodegradable anode electrode layer (9 b), a biodegradable ferroferric oxide and laccase molecular layer (8) and a biodegradable anode chitosan film layer (6 b) which are sequentially arranged on the flexible substrate layer (10) from bottom to top, and an anode lead (12) is integrally formed on one side of the anode electrode layer (9 b); the flexible substrate layer (10) is made of polylactic acid or polyvinyl alcohol or polycaprolactone or polybutylene succinate which can be completely biodegraded;
the negative electrode layer (9 a), the positive electrode layer (9 b), the negative lead (11) and the positive lead (12) are made of conductive materials which are formed by doping aluminum with zinc oxide or magnesium with zinc oxide or zinc or magnesium and can be completely biodegraded.
2. A method for preparing a conformal biodegradable implantable flexible energy supply device according to claim 1, which comprises the following steps:
1) processing the flexible substrate layer: melting flexible substrate material particles into dichloromethane to form a uniform solution, extracting a set amount of solution, placing the solution on a flat plate, uniformly coating the solution on the flat plate by using a coating rod, and obtaining a flexible substrate layer after the dichloromethane in the solution is completely evaporated, wherein the flexible substrate material is a polylactic acid or polyvinyl alcohol or polycaprolactone or polybutylene succinate material which can be completely biodegraded;
2) respectively printing conductive ink on the prepared PLA flexible substrate layer according to the patterns of the cathode electrode layer and the anode electrode layer by using an ink-jet printing system, wherein the steps of respectively and correspondingly printing a cathode lead and an anode lead are included, then heating is carried out to finish the annealing of the electrodes, namely, the processing of the cathode electrode layer, the anode electrode layer, the cathode electrode layer, the anode lead and the anode lead is finished, and the cathode electrode layer, the anode lead and the anode lead are made of conductive materials which are doped with aluminum zinc oxide or magnesium and can be completely biodegraded;
3) printing ferroferric oxide nanoparticle ink and glucose oxidase ink on a negative electrode layer to form a ferroferric oxide and glucose oxidase molecular layer, then dripping chitosan solution to form a negative chitosan film layer, and air-drying to finish the preparation of the negative electrode of the flexible energy supply device;
4) and printing ferroferric oxide nanoparticle ink and laccase ink on an anode electrode layer to form a ferroferric oxide and laccase molecular layer, dripping chitosan solution to form an anode chitosan thin layer, and air-drying to finish the preparation of the anode of the flexible energy supply device, thereby finishing the preparation of the conformal biodegradable implantable flexible energy supply device.
3. The method for preparing a conformal flexible energy supply device with biodegradable implant according to claim 2, wherein the flat plate in step 1) is a polypropylene plate or a glass plate or a stainless steel plate or an aluminum plate which does not react with dichloromethane.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201810350519.0A CN108565048B (en) | 2018-04-18 | 2018-04-18 | Conformal biodegradable implantable flexible energy supply device and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201810350519.0A CN108565048B (en) | 2018-04-18 | 2018-04-18 | Conformal biodegradable implantable flexible energy supply device and preparation method thereof |
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