CN118902445A - Electrochemical transistor portable blood glucose meter based on wettability pattern - Google Patents
Electrochemical transistor portable blood glucose meter based on wettability pattern Download PDFInfo
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Abstract
The invention discloses an electrochemical transistor portable blood glucose meter based on a wettability pattern, which comprises a glucose level sensor, a color-changing display, a button cell, an alarm, a transimpedance amplifier, a flexible shell and an elastic buckle, wherein the sensor is arranged on the sensor; the blood glucose meter is powered by a button battery; blood glucose meters use an electromechanical chemotransistor sensor with a high signal-to-noise ratio and high response speed to detect glucose levels in sweat; the glucose meter uses a color-tunable organic electrochromic device to display the glucose level in the human body to the tester; the glucose level sensor has a patterned wettability surface over it that provides sweat collection and prevents impurities from contaminating the monitoring area, thereby enabling real-time, rapid, convenient and painless monitoring of blood glucose levels. In addition, the meter is provided with three modes, which respectively provide fasting, two hours after meal and other periods of blood glucose monitoring, and when the glucose level in sweat reaches hyperglycemia, a continuous alarm sound is sent to prompt the tester that hyperglycemia exists at the moment, and the tester should seek medical advice.
Description
Technical Field
The invention relates to the technical field of blood glucose monitoring, in particular to an electrochemical transistor portable blood glucose meter based on a wettability pattern.
Background
Diabetes is a metabolic disease characterized by chronic hyperglycemia, and is largely classified into type 1 diabetes, type 2 diabetes, and gestational diabetes. The incidence of diabetes continues to rise as the global population ages, the urbanization process accelerates, and lifestyle changes. Long-term hyperglycemia can lead to a serious set of complications, including cardiovascular disease, kidney disease, neuropathy, retinopathy, etc., and therefore blood glucose management in diabetics is critical. To effectively control blood glucose levels, regular monitoring of blood glucose is one of the key elements in diabetes management. Traditional blood glucose monitoring, including the determination of venous plasma glucose and fingertip blood glucose, often requires blood sampling or micro-invasive testing.
Glucose in sweat is mainly derived from glucose in blood, and is permeated into sweat glands through capillaries of skin and then secreted into sweat. Trace glucose levels in sweat are reported to have a correlation with blood glucose levels in blood, with 0.3 mM glucose in sweat corresponding to 300 mg dL -1 glucose in blood. Thus, monitoring glucose levels in sweat can be used for diagnosis of diabetes. However, to achieve convenient home blood glucose level display, the following features are required: 1. accurately measuring trace glucose levels in sweat; 2. automatic sweat transport; 3. rapidly displaying blood glucose levels; 4. repeated charging is not needed (low power consumption); 5. the blood glucose meter has the advantages of small volume and portability, and the prior art has no blood glucose meter with the characteristics.
Therefore, there is a need to develop an electrochemical transistor portable glucose meter based on wettability patterns to solve the above-mentioned problems.
Disclosure of Invention
The invention aims at: in order to reduce inconvenience and pain of conventional invasive blood glucose tests, the present invention provides an electrochemical transistor portable glucose meter based on a wettability pattern, which monitors glucose levels in sweat by using an organic electrochemical transistor (OECT, organic electrochemical transistor) with high sensitivity and high response speed, and a color voltage-regulated organic electronic display (OECA, organic electrochemical display) displays glucose levels in human body, thereby realizing real-time, rapid, convenient and painless blood glucose concentration tests.
The technical scheme adopted by the invention is as follows:
an electrochemical transistor portable glucose meter based on a wettability pattern, comprising:
A glucose level sensor; the glucose level sensor comprises a flexible substrate, a source electrode, a drain electrode, a gate electrode, a glucose sensitive layer, a wettability pattern and a semiconductor layer, wherein the source electrode, the drain electrode and the gate electrode are arranged above the flexible substrate in parallel and at intervals, the glucose sensitive layer is arranged above the gate electrode, the semiconductor layer is arranged in a hydrophilic area between the source electrode and the drain electrode, and the wettability pattern is arranged above the source electrode, the drain electrode and the gate electrode; the wettability pattern is formed by forming a patterned wettability pattern by chemical vapor deposition of a wettability film on the upper side of an electrode and using plasma and mask treatment;
a color changing display;
A button cell;
An alarm;
A transimpedance amplifier; the drain electrode of the glucose level sensor is connected with the first end of the transimpedance amplifier, the gate electrode of the glucose level sensor is connected with the button cell and the first end of the alarm, the second end of the alarm is connected with the input end of the transimpedance amplifier and the first end of the color-changing display, and the second end of the color-changing display is connected with the output end of the transimpedance amplifier;
A flexible housing; the glucose level sensor, the color-changing display, the button cell, the alarm and the transimpedance amplifier are all arranged in the flexible shell, a first window, a second window and a battery groove are formed in the flexible shell, the button cell is arranged in the battery groove, the first window and the battery groove are all formed in the bottom of the flexible shell, the second window is formed in the top of the flexible shell, the glucose level sensor is in direct contact with human skin through the first window, and the color-changing display is displayed through the second window;
an elastic buckle; the elastic buckle is arranged on two opposite sides of the flexible shell.
The beneficial effects of the invention are as follows:
According to the invention, the OECT with high sensitivity and high response speed is used for detecting the trace glucose concentration in sweat in real time, so that the blood glucose level range can be obtained without the traditional blood sampling operation, the pain and infection risk caused by needling are avoided, and the user experience and comfort are greatly improved.
The pattern of the surface hydrophilicity and hydrophobicity in the invention can be controlled by utilizing liquid drops formed by wettability difference, so as to realize the transmission and collection of sweat.
The wettability pattern in the present invention can prevent contamination from adhering to and interfering with the measurement results. In case of complex ingredients and impurities in sweat, long-term stability and accuracy of the sensor are ensured.
The sensor based on the wettability pattern has simple design and low manufacturing material cost, such as flexible plastic, silicon material and the like. The device is light and portable, is convenient to carry about or attach to the skin for long-time use, and has low production cost.
Three modes are provided, and blood glucose monitoring can be freely regulated for fasting, two hours after meal and other periods respectively.
Drawings
For more clearly describing the technical solution of the embodiments of the present invention, the following description will briefly describe the drawings required to be used in the embodiments, and it should be understood that the proportional relationships of the components in the drawings in this specification do not represent the proportional relationships in actual material selection design, but are merely schematic diagrams of structures or positions, where:
FIG. 1 is a schematic diagram of a glucose level sensor according to the present invention;
FIG. 2 is a schematic diagram of the OECD structure of the color-changing display of the present invention;
FIG. 3 is a schematic circuit diagram of the present invention;
the reference numerals in the drawings indicate:
1-flexible substrate, 2-source electrode, 3-drain electrode, 4-gate electrode, 5-glucose sensitive layer, 6-wettability pattern, 7-semiconductor layer, 8-bottom electrode, 9-electrochromic layer, 10-electrolyte layer, 11-top electrode, 12-flexible housing, 13-button cell, 14-buzzer, 15-elastic buckle, 16-transimpedance amplifier.
Detailed Description
The present invention will be described in further detail with reference to the drawings and examples, in order to make the objects, technical solutions and advantages of the present invention more apparent. It should be understood that the particular embodiments described herein are illustrative only and are not intended to limit the invention, i.e., the embodiments described are merely some, but not all, of the embodiments of the invention.
The present invention will be described in detail with reference to fig. 1 to 3.
An electrochemical transistor portable glucose meter based on a wettability pattern, comprising:
a glucose level sensor; the glucose level sensor comprises a flexible substrate 1, a source electrode 2, a drain electrode 3, a gate electrode 4, a glucose sensitive layer 5, a wettability pattern 6 and a semiconductor layer 7, wherein the source electrode 2, the drain electrode 3 and the gate electrode 4 are arranged above the flexible substrate 1 in parallel and at intervals, the glucose sensitive layer 5 is arranged above the gate electrode 4, the semiconductor layer 7 is arranged in a hydrophilic area between the source electrode 2 and the drain electrode 3, and the wettability pattern 6 is arranged above the source electrode 2, the drain electrode 3 and the gate electrode 4; the wettability pattern 6 is a wettability film which is formed on the upper side of the electrode by chemical vapor deposition and is patterned by plasma and mask treatment; different glucose concentrations will change the gate potential and output different amounts of current;
a color changing display; the color-changing display comprises a bottom electrode 8, an electrochromic layer 9, an electrolyte layer 10 and a top electrode 11 which are sequentially arranged from bottom to top;
a button cell 13;
an alarm 14;
A transimpedance amplifier 16; the drain electrode 3 of the glucose level sensor is connected with the first end of the transimpedance amplifier 16, the gate electrode 4 of the glucose level sensor is connected with the button cell 13 and the first end of the alarm 14, the second end of the alarm 14 is connected with the input end of the transimpedance amplifier 16 and the top electrode 11 of the color-changing display, and the bottom electrode 8 of the color-changing display is connected with the output end of the transimpedance amplifier 16;
A flexible housing 12; the glucose level sensor, the color-changing display, the button cell 13, the alarm 14 and the transimpedance amplifier 16 are all arranged in the flexible shell 12, a first window, a second window and a battery groove are formed in the flexible shell 12, the button cell 13 is arranged in the battery groove, the first window and the battery groove are all formed in the bottom of the flexible shell 12, the second window is formed in the top of the flexible shell 12, the glucose level sensor is in direct contact with human skin through the first window, and the color-changing display is displayed through the second window;
an elastic buckle 15; the resilient catch 15 is mounted on opposite sides of the flexible housing 12.
The flexible housing is mainly used for protecting internal structures and providing supporting functions; the button battery is arranged in a battery groove in the flexible shell, and a battery cover of the battery groove can be opened to be taken out for replacement; the glucose level sensor is an OECT device, has low working voltage and high signal-to-noise ratio, and can effectively amplify an input signal; the glucose level sensor is contacted with human skin through an opening at the inner side of the shell, and a patterned wettability surface is introduced at the sensor part to drain and collect sweat; the color-changing display is an OECD device, the color of which is regulated by the magnitude of input voltage, and is fixed in the shell and used for displaying the glucose level; the alarm is one of a piezoelectric buzzer or an electromagnetic buzzer, and continuously sounds when the glucose level in sweat reaches 0.126 mM to prompt a tester that hyperglycemia exists at the moment, so that the tester should seek medical attention; hyperglycemia occurs when the glucose concentration in blood is higher than 126 mg dL −1 on an empty stomach. The blood glucose meter is provided with three modes, and can be respectively used for fasting blood glucose monitoring, two hours after meal blood glucose monitoring and other periods through the adjustment of a slide rheostat of a transimpedance amplifier.
The flexible housing 12 is made of at least one of polyester mesh fabric, nylon mesh fabric or polyester fiber. The flexible housing 12 is used to protect and secure the internal components; elastic buckles are connected to two ends of the flexible shell and used for fixing the blood glucose meter; transparent waterproof treatment is carried out on the outer side of the flexible shell, and the service life of the display is prolonged. The flexible shell is attached with a color card beside the color-changing display, and the glucose level range can be determined by comparing the colors of the color-changing display.
The flexible substrate 1 is made of at least one of Polyurethane (PU), flexible polyvinyl chloride (PVC), low Density Polyethylene (LDPE), styrene-ethylene/butylene-styrene block copolymer (SEBS), polydimethylsiloxane (PDMS) or elastic rubber.
The glucose sensitive layer 5 is a mixture of a catalyst and glucose oxidase; the catalyst is one of Pt nano particles, pt nano flowers/graphene oxide, ptAu/C, pt 2 Pb alloy, three-dimensional Cu@Cu 2 O aerogel, au nano particles/graphene oxide nano belts, pt 3 Ru alloy nano particles, mesoporous Pt or 3D cellular nano porous gold, and has excellent catalytic performance on oxidation of glucose.
The source electrode 2, the drain electrode 3, and the gate electrode 4 are disposed on the same plane.
In the glucose level sensor, except for an OECT device channel and a grid electrode 4 modified with a glucose sensitive layer 5, other parts are modified with a super-hydrophobic layer. Sweat automatically flows to the grid electrode and the channel region of the sensor under the action of surface energy, so that the sweat is automatically transported and collected.
The electrode in the color-changing display is one of ITO or FTO; the electrochromic layer is made of one of small organic molecules (such as viologen derivatives, aniline derivatives, carbazole, pyrrole and thiophene) and conductive polymers (such as polythiophene derivatives, polyaniline and polycarbazole derivatives).
The glucose level sensor has low working voltage, high sensitivity, high response speed and high signal to noise ratio, and can effectively amplify an input signal in situ; the preparation material of the semiconductor layer of the glucose level sensor is one of PEDOT PSS, pg2T-T, P (g 4 T2-TT) or BBL, a patterned channel is formed between a source electrode and a drain electrode, and the thickness range of the film is 50-100 nm; the electrode structure of the glucose level sensor adopts a side gate structure, the electrode of the glucose level sensor is made of PEDOT, one of PSS, ag nanowires, carbon paste, au nanowires or Au, and the thickness range of the film is 60-120 nm; the patterned wettability material on the upper side of the glucose level sensor is one of trichloro (1H, 2H-perfluorooctyl) silane, triethoxy (1H, 2H-perfluorodecyl) silane (FAS-17) or octadecyl silane (OTS); the patterned wetting surface is treated by UVO or plasma to form a pattern with distinct hydrophilicity and hydrophobicity.
Example 1 (control):
As shown in fig. 3, an electrochemical transistor portable glucose meter based on a wettability pattern includes a flexible housing, a button cell, a glucose level sensor, a color changing display, and an alarm; the button battery is arranged in a battery groove in the elastic shell and can be replaced by opening a battery cover; the glucose sensor is an OECT device which is fixed in the shell and is in direct contact with the skin of a human body through an opening at the inner side of the shell; the display is an OECD device and is fixed in the shell, and the blood sugar concentration range is displayed through an opening at the outer side of the shell; the alarm is a piezoelectric buzzer, and continuously sounds when the glucose level in sweat reaches the hyperglycemia range.
As shown in fig. 3, as a preferred embodiment, the material of the flexible housing is polyester mesh fabric; two ends of the flexible shell are connected with adjustable elastic buckles; transparent waterproof treatment is carried out on the outer side of the flexible shell; the flexible shell is attached with a color card beside the display, and the glucose level range is determined by comparing colors.
As shown in fig. 1, as a preferred embodiment, the glucose level sensor is an OECT device; the glucose level sensor comprises from top to bottom in order: glucose sensitive layer and semiconductor layer, electrode layer and substrate layer; the substrate layer of the glucose level sensor is made of PU; the electrode structure of the glucose level sensor adopts a side gate structure, the electrode material of the glucose level sensor is an Au electrode subjected to vacuum evaporation, and the thickness range of the film is 80-150 nm; the semiconductor layer of the glucose level sensor is made of PEDOT PSS (0.1 wt% DBSA,1 wt% GOPS,5 wt% glycol), the spraying patterning is carried out at the position of a channel and the high-temperature treatment is carried out for crosslinking, and the thickness of the film ranges from 200 nm to 300 nm; the glucose sensitive layer of the glucose level sensor is prepared by electrodepositing Pt nano particles, and then dripping glucose oxidase/SWCNT/chitosan mixture on a grid electrode modified by the Pt nano particles; a glucose sensitive layer of the glucose level sensor is disposed over the gate.
As shown in FIG. 2, as a preferred embodiment, the display is an OECD device, the color of which is regulated by the input glucose sensor output; the display comprises from top to bottom in sequence: a flexible substrate, a bottom electrode, an electrochromic layer, an electrolyte, and a top electrode; the bottom electrode is ITO, and the thickness of the film is about 30-40 nm; the electrochromic layer is electrochromic zwitterionic viologen N, N '-bis (3-sulfonamide propyl) -4-4' -bipyridine, and the thickness of the film is 100-200 nm; the electrolyte layer is PVA/LiCl, and the thickness of the film is 300-400 nm; the top electrode is ITO.
Examples:
As shown in fig. 3, an electrochemical transistor portable glucose meter based on a wettability pattern includes a flexible housing, a button cell, a glucose level sensor, a color changing display, and an alarm; the button battery is arranged in a battery groove in the elastic shell and can be replaced by opening a battery cover; the glucose sensor is an OECT device which is fixed in the shell and is in direct contact with the skin of a human body through an opening at the inner side of the shell; the display is an OECD device and is fixed in the shell, and the blood sugar concentration range is displayed through an opening at the outer side of the shell; the alarm is a piezoelectric buzzer, and continuously sounds when the glucose level in sweat reaches the hyperglycemia range.
As shown in fig. 3, as a preferred embodiment, the material of the flexible housing is polyester mesh fabric; two ends of the flexible shell are connected with adjustable elastic buckles; transparent waterproof treatment is carried out on the outer side of the flexible shell; the flexible shell is attached with a color card beside the display, and the glucose level range is determined by comparing colors.
As shown in fig. 1, as a preferred embodiment, the glucose level sensor is an OECT device; the glucose level sensor comprises from top to bottom in order: glucose sensitive layer and semiconductor layer, electrode layer and substrate layer; the substrate layer of the glucose level sensor is made of PU; the electrode structure of the glucose level sensor adopts a side gate structure, the electrode material of the glucose level sensor is an Au electrode subjected to vacuum evaporation, and the thickness range of the film is 80-150 nm; the wettability film is deposited on the upper side of the electrode through chemical vapor deposition, and a patterned wettability pattern is formed by using plasma and mask treatment; the wettability film material is FAS-17; the semiconductor layer of the glucose level sensor is made of PEDOT PSS (0.1 wt% DBSA,1 wt% GOPS,5 wt% glycol), the spraying patterning is carried out at the position of a channel and the high-temperature treatment is carried out for crosslinking, and the thickness of the film ranges from 200 nm to 300 nm; ; the glucose sensitive layer of the glucose level sensor is prepared by electrodepositing Pt nano particles, and then dripping glucose oxidase/SWCNT/chitosan mixture on a grid electrode modified by the Pt nano particles; a glucose sensitive layer of the glucose level sensor is disposed over the gate.
As shown in FIG. 2, as a preferred embodiment, the display is an OECD device, the color of which is regulated by the input glucose sensor output; the display comprises from top to bottom in sequence: a flexible substrate, a bottom electrode, an electrochromic layer, an electrolyte, and a top electrode; the bottom electrode is ITO, and the thickness of the film is about 30-40 nm; the electrochromic layer is electrochromic zwitterionic viologen N, N '-bis (3-sulfonamide propyl) -4-4' -bipyridine, and the thickness of the film is 100-200 nm; the electrolyte layer is PVA/LiCl, and the thickness of the film is 300-400 nm; the top electrode is ITO.
Example 1a specific blood glucose concentration (fasting) versus display color comparison is shown in table 1.
TABLE 1 comparison of blood glucose concentration (fasting) with display color
Example 2a comparison of specific blood glucose concentrations (on an empty stomach) with display color is shown in table 2.
TABLE 2 comparison of blood glucose concentration (fasting) with display color
It can be seen from examples 1-2 that: after the patterned wettability surface is introduced, sweat on the skin surface is transported by the hydrophobic part of the wettability surface and collected by the hydrophilic part due to the difference of hydrophilicity and hydrophobicity, so that the sweat is concentrated on the sensing part of the glucose sensor, and the result display result is more accurate and cannot be influenced by random flow of the sweat. In summary, the electrochemical transistor portable blood glucose meter based on the wettability pattern provided by the invention reduces inconvenience and pain of traditional invasive blood glucose detection, supplies power to the blood glucose meter by using a replaceable button cell, has high sensitivity and high response speed, detects the glucose level in sweat by OECT, and displays the blood glucose concentration in a human body by OECD with adjustable color, thereby realizing real-time, rapid, convenient and painless blood glucose level detection, and sending out continuous alarm sound when the glucose level in sweat reaches hyperglycemia to prompt a tester that hyperglycemia exists at the moment, and taking immediate measures should be noted. In addition, the blood glucose meter is provided with a plurality of modes, including fasting blood glucose measurement, postprandial blood glucose measurement and blood glucose measurement at other random moments, and can dial the regulation and control of the resistance value of the feedback resistor on the transimpedance amplifier.
The foregoing description of the preferred embodiments of the invention is not intended to be limiting, but rather is intended to cover all modifications, equivalents, and alternatives falling within the spirit and principles of the invention.
Claims (8)
1. An electrochemical transistor portable glucose meter based on a wettability pattern, comprising:
A glucose level sensor; the glucose level sensor comprises a flexible substrate (1), a source electrode (2), a drain electrode (3), a gate electrode (4), a glucose sensitive layer (5), a wettability pattern (6) and a semiconductor layer (7), wherein the source electrode (2), the drain electrode (3) and the gate electrode (4) are arranged above the flexible substrate (1) in parallel and at intervals, the glucose sensitive layer (5) is arranged above the gate electrode (4), the semiconductor layer (7) is arranged in a hydrophilic area between the source electrode (2) and the drain electrode (3), and the wettability pattern (6) is arranged above the source electrode (2), the drain electrode (3) and the gate electrode (4); the wettability pattern (6) is formed by forming a patterned wettability pattern by chemical vapor deposition of a wettability film on the upper side of an electrode and using plasma and mask treatment;
a color changing display;
a button cell (13);
an alarm (14);
A transimpedance amplifier (16); the drain electrode (3) of the glucose level sensor is connected with the first end of the transimpedance amplifier (16), the gate electrode (4) of the glucose level sensor is connected with the button cell (13) and the first end of the alarm (14), the second end of the alarm (14) is connected with the input end of the transimpedance amplifier (16) and the first end of the color-changing display, and the second end of the color-changing display is connected with the output end of the transimpedance amplifier (16);
A flexible housing (12); the glucose level sensor, the color-changing display, the button battery (13), the alarm (14) and the transimpedance amplifier (16) are all arranged in the flexible shell (12), a first window, a second window and a battery groove are formed in the flexible shell (12), the button battery (13) is arranged in the battery groove, the first window and the battery groove are all formed in the bottom of the flexible shell (12), the second window is formed in the top of the flexible shell (12), the glucose level sensor is in direct contact with human skin through the first window, and the color-changing display is displayed through the second window;
An elastic buckle (15); the elastic buckle (15) is arranged on two opposite sides of the flexible shell (12).
2. The electrochemical transistor portable glucose meter based on the wettability pattern of claim 1, wherein the color-changing display comprises a bottom electrode (8), an electrochromic layer (9), an electrolyte layer (10) and a top electrode (11) which are arranged in sequence from bottom to top.
3. The electrochemical transistor portable glucose meter based on the wettability pattern of claim 1, wherein the flexible housing (12) is made of at least one of polyester mesh fabric, nylon mesh fabric or polyester fiber.
4. An electrochemical transistor portable glucose meter based on a wettability pattern of claim 1, wherein: the preparation material of the flexible substrate (1) is at least one of polyurethane, flexible polyvinyl chloride, low-density polyethylene, styrene-ethylene/butylene-styrene block copolymer, polydimethylsiloxane or elastic rubber.
5. An electrochemical transistor portable glucose meter based on a wettability pattern of claim 1, wherein: the glucose sensitive layer (5) is a mixture of a catalyst and glucose oxidase; the catalyst is one of Pt nano particles, pt nano flowers/graphene oxide, ptAu/C, pt 2 Pb alloy, three-dimensional Cu@Cu 2 O aerogel, au nano particles/graphene oxide nano belts, pt 3 Ru alloy nano particles, mesoporous Pt or 3D cellular nano porous gold.
6. An electrochemical transistor portable glucose meter based on a wettability pattern of claim 1, wherein: the source electrode (2), the drain electrode (3) and the gate electrode (4) are arranged on the same plane.
7. An electrochemical transistor portable glucose meter based on a wettability pattern of claim 1, wherein: in the glucose level sensor, except for an OECT device channel and a grid electrode (4) modified with a glucose sensitive layer (5), other parts are modified with a super-hydrophobic layer.
8. An electrochemical transistor portable glucose meter based on a wettability pattern of claim 1, wherein: the color changing display is an OECD device.
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