CN115586230A - Flexible wearable sweat electrochemical sensor, sweat monitoring method and application - Google Patents
Flexible wearable sweat electrochemical sensor, sweat monitoring method and application Download PDFInfo
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Abstract
The invention discloses a flexible wearable sweat electrochemical sensor, which comprises an electrochemical sweat sensor electrode device 1, a Bluetooth transmission device 2 and a personal mobile data terminal 3; the electrochemical sweat sensor electrode device 1 comprises a three-electrode system and an ion introduction electrode 8 printed on a flexible stretchable substrate 7, wherein the ion introduction electrode 8 is modified with pilocarpine, and the working electrode 6 is modified with polypeptide composite hydrogel. The conductive hydrogel disclosed by the invention has good biocompatibility, high sensitivity, good flexibility and a self-healing function. The invention develops a novel flexible self-healing material with good biocompatibility and good anti-pollution performance, further constructs a portable wearable electronic sensor based on the novel flexible material, constructs a wireless electrochemical sweat sensor to observe a dynamic biochemical signal output in real time on a mobile phone, and constructs a drug-stimulated sweating device, and can realize direct monitoring of biochemical molecules in sweat under a static state.
Description
Technical Field
The invention belongs to the technical field of electrochemical sensors, and particularly relates to a wireless flexible wearable sweat electrochemical sensor capable of in-situ monitoring, a sweat monitoring method and application.
Background
In recent years, wearable sensors have received much attention due to their great potential in vital sign monitoring. However, wearable sensors on the market, mainly monitoring physical signals such as heart rate, body temperature and humidity, cannot provide information at a deeper molecular level. This gap creates an opportunity for non-invasive monitoring of body fluids. Compared to body fluids such as blood, interstitial fluid, tears and urine, sweat is a promising but relatively unexplored biological fluid, an important and valuable body fluid that can be used for non-invasive monitoring, since it contains important markers related to the physiological state of the human body, including vitamin C, ascorbic acid, uric acid, glucose and lactic acid. Its composition changes dynamically with changes in health, stress and dietary conditions. The literature reports a fundamental correlation between the levels of chemical molecules in blood and sweat, that is sweat analysis can replace blood analysis. Therefore, sweat analysis can provide continuous detection information, and can be used for non-invasively detecting physiological health conditions and disease diagnosis and treatment. If the limit of large-scale equipment in hospitals can be removed, the high-performance wearable sweat electrochemical sensor is researched, the noninvasive, continuous, in-situ and visual monitoring of the markers is realized, and the method has important significance for realizing 'intelligent medical treatment'.
However, many problems are currently faced in the sweat monitoring research, mainly focusing on the following aspects:
one of the key challenges in sweat analysis is the lack of materials that combine high flexibility, high conductivity, high sensitivity, high biocompatibility, and resistance to contamination. At present, most wearable sensing devices are constructed on the basis of hard and brittle rigid substrate 7 materials, which easily causes the problems that data monitoring is not timely and accurate output cannot be realized, and the like, so that more biochemical information of the human metabolic molecule level cannot be accurately provided. Therefore, the development of flexible electrochemical sensors is a prerequisite for the development of high performance wearable sweat electrochemical sensing devices. Most of the flexible sensors use flexible materials such as flexible metal materials, polymer elastomers, polymer films, and the like as a substrate 7, and are combined with conductive materials (such as metal nanowires, metal nanoparticles, graphene, carbon nanotubes, and the like) having active functions, so that the combination of the flexibility and the sensitivity function can be realized. However, because of the disadvantages of the conductive materials with such active functions, such as inherent rigidity, easy pollution, short fatigue life, etc., it is difficult to better adhere to human skin and bear the complicated mechanical shapes of natural skin, such as: twisting, bending, stretching, folding, etc., which presents significant challenges to the real-world application of wearable electronics. Different from the traditional conductive flexible material, the conductive hydrogel has a network structure similar to living tissues, can show physiological characteristics and mechanical properties similar to human skin and organs, such as biocompatibility, high stretchability and low modulus, and becomes one of the ideal flexible matrix materials of human-computer interfaces. Moreover, the polypeptide hydrogel flexible material has a complex three-dimensional network structure, so that the functional material can be dispersed, and the stacking of the material can be avoided, thereby improving the detection sensitivity based on the polypeptide composite material.
In addition, the ideal flexible wearable sensing device for sweat analysis, preferably unprocessed, allows for direct determination of biochemical indicators therein, and is free of contamination and effects in sweat of complex composition and typically low acquisition volumes. A great amount of coexisting chemical species in sweat can be adsorbed to a sensing interface to pollute and passivate an electrode, so that the reliability of a detection result is reduced, in-situ monitoring application is not easy to realize, and the electrode is easy to pollute at present and is one of the problems to be solved urgently.
The second key challenge in sweat analysis is the lack of wireless, miniature, highly integrated, multi-functional, flexible electronics. Compared with non-in-situ detection, the sensor for in-situ detection needs to directly face complex and dynamic micro environments, needs to challenge the complex environment, has various biological elements, and is easy to pollute sensing elements. How to develop flexible new material and antipollution performance that have good biocompatibility concurrently to further construct the portable wearable electronic sensor based on this novel flexible material, and construct wireless sensor and observe the dynamic biochemical signal of real-time output on the cell-phone, realize the direct detection of biochemical molecule in the sweat, become the technological bottleneck that wearable equipment marketization needs to break through urgently.
Therefore, how to develop an anti-pollution polypeptide hydrogel material with high flexibility, high sensitivity and anti-pollution and other comprehensive properties, and configure a micro flexible wearable electrochemical sweat sensor based on the multifunctional material, and an attached sweat-emitting stimulation electrode, and in a human static state, a biochemical sensing signal in sweat can be transmitted to a mobile phone interface through bluetooth by a small bluetooth transmission system, so as to monitor the sweat.
Disclosure of Invention
In view of this, the present invention provides an in-situ monitorable wireless flexible wearable sweat electrochemical sensor, a sweat monitoring method and applications thereof.
In order to achieve the purpose, the invention adopts the following technical scheme:
a flexible wearable sweat electrochemical sensor comprises an electrochemical sweat sensor electrode device 1, a Bluetooth transmission device 2 and a personal mobile data terminal 3, wherein the Bluetooth transmission device 2 is connected with the electrochemical sweat sensor electrode device 1 through a circuit, and the Bluetooth transmission device 2 is in wireless communication connection with the personal mobile data terminal 3;
the electrode device 1 of the electrochemical sweat sensor comprises a counter electrode 4, a reference electrode 5 and a working electrode 6 which are printed on a flexible stretchable substrate 7, wherein the working electrode 6 is modified with polypeptide composite hydrogel, and the polypeptide composite hydrogel comprises polypeptide, au NPs and MoS 2 The amino acid sequence of the polypeptide is (hydrophobic group) -Lys- (hydrophobic group) - (Lys-NH) 2 ) - (Phe-COOH), lys and Phe were all D-form amino acids.
Further, the electrochemical sweat sensor electrode device 1 comprises an ion-introduction electrode 8 printed on the flexible stretchable substrate 7, and the ion-introduction electrode 8 is modified with pilocarpine.
Further, the above flexible stretchable substrate 7 is a TPU flexible stretchable substrate 7.
Further, the material of the above-mentioned flexible stretchable substrate 7 may also be a PC film or a textile fabric.
Further, the TPU flexible stretchable substrate 7 is manufactured by DuPont and has the model number of TL644-TE-11C.
Further, the printing mode is screen printing, ink jet printing or etching microfluidics.
Further, the above-mentioned hydrophobic group is
One or two of them.
The adoption of the further beneficial effects is as follows: the hydrophobic groups facilitate self-assembly into hydrogels.
Furthermore, the paste used for printing the reference electrode 5 is a stretchable silver paste, and the paste used for printing the working electrode 6 and the counter electrode 4 is a stretchable carbon paste.
Further, the manufacturer of the stretchable silver paste is Engineered Materials Systems, inc, with the model number of CI-1036; the above-described stretchable carbon paste is manufactured by Engineered Materials Systems, inc. model CI-2062.
Adopt above-mentioned further beneficial effect to be: stretchable printing pastes have good stability and stretchability properties.
Further, the personal mobile data terminal 3 is a smart phone or a tablet computer.
Further, the preparation method of the polypeptide composite hydrogel comprises the following steps:
(1) Reacting NaBH 4 Adding into water, dissolving in ice bath to obtain ice NaBH 4 Aqueous solution of HAuCl 4 ·H 2 O aqueous solution dropwise into MoS 2 Stirring in the aqueous solution, and then adding the newly prepared ice NaBH under stirring 4 Stirring the aqueous solution at normal temperature, centrifuging, washing and drying to obtain AuNPs/MoS 2 ；
(2) Dissolving a powder of the polypeptide of claim 1 or 2 in dimethylsulfoxide to obtain a raw solution of the polypeptide, and adding AuNPs/MoS 2 The aqueous solution is evenly mixed and stood to obtain AuNPs/MoS 2 A/D-Pep hydrogel.
Further, in the step (1), ice NaBH 4 The concentration of the aqueous solution is 10-20mol/L, HAuCl 4 ·H 2 The concentration of the O aqueous solution is 10-20mmol/L, moS 2 The concentration of the aqueous solution is 10-50mg/mL, and the ice NaBH is added 4 Aqueous solution, HAuCl 4 ·H 2 Aqueous O solution and MoS 2 The volume ratio of the aqueous solution is 1.
Further, in the step (1), the stirring speed is 200-500r/min, and HAuCl is added 4 ·H 2 O aqueous solution dropwise into MoS 2 Stirring in water solution for 10-30min, and stirring at normal temperature for 8-12 hr.
Further, in the step (1), the dropping speed is 10 to 20 drops/min.
Further, in the step (1), the ice-bath time is 5-10min.
Further, in the step (1), the centrifugal rotating speed is 8000-10000r/min, and the centrifugal time is 5-10min.
Further, in the above step (1), washing is performed three times using ethanol and water, respectively.
Further, in the step (1), the drying temperature is 30-50 ℃, and the drying time is 5-8h.
Further, in the step (2), the concentration of the original polypeptide solution is 150mg/mL, and Au NPs/MoS 2 The concentration of the aqueous solution is 2-10mg/mL, the original solution of the polypeptide and Au NPs/MoS 2 The volume ratio of the aqueous solution was 35.
Further, in the step (2), the standing time is 0.2-0.5h.
The invention also provides a method for monitoring sweat by using the flexible wearable sweat electrochemical sensor, which comprises the following steps:
1) Modifying 7-10 microliter of polypeptide composite hydrogel on the surface of the working electrode 6, wherein the polypeptide composite hydrogel modified on the surface of the working electrode 6 is used for absorbing and storing sweat which is used as a natural electrolyte,
2) Cleaning skin by adopting isopropanol through friction, and fixing the flexible wearable sweat electrochemical sensor on the human epidermis by using medical double faced adhesive tape;
3) Scanning AA and UA in sweat by using a differential pulse voltammetry technology under the conditions that the potential range is 0.4-0.8V, the amplitude is 50mV and the pulse width is 0.05 s;
4) Monitoring AA and UA in sweat by time-current technique under the condition that the optimum potential is 0.3V and 0.5V respectively;
5) The sweat monitoring signal is transmitted to the personal mobile data terminal 3 through the Bluetooth transmission device 2.
Further, the method for monitoring sweat by the flexible wearable sweat electrochemical sensor further comprises the following steps:
6) Cutting the agarose gel into the size same as that of the ion introduction electrode 8, and modifying the agarose gel on two sides of the anode and the cathode of the ion introduction electrode 8, wherein the preparation method of the agarose gel comprises the following steps: dissolving 0.4-1.0g of agarose in 10-25mL of 0.1mol/L potassium phosphate buffer solution (pH 7.0), stirring at 170 deg.C until the agarose is completely dissolved, pouring the agarose gel into a mold, and cooling to room temperature;
7) Before stimulating sweat, modifying an electrode interface with agarose hydrogel by a dropping method for configuring an ion introduction electrode, after freeze-drying, dropping 3-5wt% of pilocarpine solution into the anode agarose hydrogel, storing for 1-2h, containing a pilocarpine drug with positive charge in the agarose hydrogel, after electrifying, repelling the pilocarpine close to a skin part due to charge repulsion at the anode part, and then stimulating sweat.
The invention also provides application of the flexible wearable sweat electrochemical sensor or the sweat monitoring method in vital sign monitoring.
The invention has the beneficial effects that:
1) Before the existing electrochemical sensor is detected, a detection sample needs to be pretreated, most of substances which can pollute an electrode are removed, and then the detection is carried out; the invention can directly measure the biochemical index without treating the sweat, and can avoid the pollution and the influence in the sweat with complex components and small collection amount.
2) The conductive material modified with active function at the electrode interface (such as metal nano wire, metal nano particle, graphene, carbon nano tube, etc.) has the disadvantages of large inherent rigidity, easy pollution, short fatigue life, etc., and is difficult to better adhere to the skin of a human body and bear the complicated mechanical shape of the natural skin, such as: twisting, bending, stretching, folding, etc., which presents significant challenges to the real-world application of wearable electronics. The conductive hydrogel disclosed by the invention has good biocompatibility, high sensitivity, good flexibility and a self-healing function.
3) At present, a highly integrated, portable and small electrochemical sweat sensor which can be directly monitored on a mobile phone and is used for monitoring biochemical indexes of a human body is lacked. The invention develops a novel flexible material with good biocompatibility and anti-pollution performance, further constructs a portable wearable electronic sensor based on the novel flexible material, constructs a wireless electrochemical sweat sensor to observe a dynamic biochemical signal output in real time on a mobile phone, and constructs a drug-stimulated sweating device, and can realize direct monitoring of biochemical molecules in sweat under a static state.
Drawings
Fig. 1 is a schematic diagram of the structure of a flexible wearable sweat electrochemical sensor, wherein 1-electrochemical sweat sensor electrode device, 2-bluetooth transmission device, 3-personal mobile data terminal;
FIG. 2 is a schematic of the counter, reference, working electrode of the electrochemical sweat sensor electrode device 1, wherein 4-counter, 5-reference, 6-working, 7-flexible stretchable substrate;
FIG. 3 is a schematic illustration of the principle of iontophoresis electrodes of a collection of electrochemical sweat sensor electrode devices 1 for stimulating sweat, wherein 8-iontophoresis electrodes;
FIG. 4 is a schematic and physical representation of the structure of a polypeptide-complexed hydrogel material;
FIG. 5 is a diagram illustrating the self-healing effect of the polypeptide-compounded hydrogel material;
FIG. 6 is a pictorial representation of an electrochemical sweat sensor electrode device 1;
FIG. 7 is a diagram of a flexible wearable electrochemical sensor stretched longitudinally in physical form;
FIG. 8 is a graph of electrochemical I-T signals after 200,400,600, 800 and 1000 stretches of the electrochemical sweat sensor electrode device 1 at 20% longitudinal stretch, respectively;
FIG. 9 is a diagram of a flexible wearable electrochemical sensor stretched across a physical object;
FIG. 10 is a graph of electrochemical I-T signals after 200,400,600, 800 and 1000 stretches when the electrochemical sweat sensor electrode device 1 is stretched 20% across;
FIG. 11 Flexible wearable sweat electrochemical sensor in 100% sweat for 5.0mM [ Fe (CN) 6 ] 3-/4- A DPV response map of (a);
figure 12 DPV signal response plot for detection of Uric Acid (UA) and vitamin C (AA) in 100% sweat by a flexible wearable sweat electrochemical sensor;
figure 13I-T signal response plots for flexible wearable sweat electrochemical sensors monitoring Uric Acid (UA) in 100% sweat.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The polypeptide of the present invention is prepared by entrusting Hefei peptide Biotechnology Limited company according to the amino acid sequence of the polypeptide of the present invention.
The TPU flexible stretchable substrate 7 in the example was manufactured by DuPont model number TL644-TE-11C.
The stretchable silver paste is manufactured by Engineered Materials Systems, inc, with the model number of CI-1036; the stretchable carbon paste was manufactured by Engineered materials Systems, inc. model CI-2062.
Example 1
As shown in fig. 1, the flexible wearable sweat electrochemical sensor comprises an electrochemical sweat sensor electrode device (1), a bluetooth transmission device (2) and a personal mobile data terminal (3) smart phone, wherein the bluetooth transmission device (2) is connected with the electrochemical sweat sensor electrode device (1) through a circuit, and the bluetooth transmission device (2) is in wireless communication connection with the smart phone;
as shown in fig. 2 and 3, the electrochemical sweat sensor electrode device (1) comprises a counter electrode (4), a reference electrode (5), a working electrode (6) and an ion introduction electrode (8) which are screen-printed on a TPU flexible stretchable substrate (7), wherein the ion introduction electrode (8) is modified with pilocarpine, the working electrode (6) is modified with a polypeptide composite hydrogel, and the polypeptide composite hydrogel comprises polypeptide, auNPs and MoS 2 The amino acid sequence of the polypeptide is (Nap) -Lys- (Nap) - (Lys-NH) 2 ) - (Phe-COOH), lys and Phe are both D-form amino acids.
The electrode device (1) of the electrochemical sweat sensor comprises a counter electrode (4), a reference electrode (5), a working electrode (6) and an ion introduction electrode (8) which are printed on a TPU flexible stretchable substrate (7) by using paste screen printing, wherein the paste used for printing the reference electrode (5) is stretchable silver paste, and the paste used for printing the working electrode (6) and the counter electrode (4) is stretchable carbon paste. The ion introduction electrode (8) is modified with a pilocarpine, the pilocarpine can be released to the surface of the skin under the condition that the electrode is electrified to stimulate sweating, the working electrode (6) is modified with a polypeptide composite hydrogel which has a natural sweat absorbent and is used for storing sweat, and as shown in figure 5, the polypeptide composite hydrogel has self-healing performance, good conductivity and a selective catalysis function on vitamin C and uric acid in the sweat.
As shown in fig. 6, which is a pictorial representation of an electrochemical sweat sensor electrode device (1), the key point of which is the electrochemical sweat sensor electrode portion. Electrode section a three-electrode system and an iontophoretic electrode (8) were screen printed on a flexible stretchable substrate (7), TPU.
As shown in fig. 7 to 10, the TPU flexible stretchable substrate (7) has good flexibility and stretchability, and the stretchable printing paste also has good stability and stretchability. After 20% of the transverse stretching and the longitudinal stretching, respectively, the electron transfer effect of the working electrode (6) is not influenced. In addition, the polypeptide composite hydrogel modified on the working electrode (6) is the core and innovation point of the whole flexible wearable sweat electrochemical sensor, and the composite multifunctional material has self-healing performance and can be smoothThe compound enzyme can better transmit electrons in response to the movements of twisting, bending, stretching, folding and the like of the skin, and exert good conductivity and high-specificity catalytic function on vitamin C and uric acid in sweat. MoS in the polypeptide composite hydrogel 2 The two-dimensional nano material is combined with the hydrophobic part of the polypeptide due to a large amount of pi-pi accumulation, so that the polypeptide composite hydrogel material has a self-healing function.
The amino acid sequence of the polypeptide is (Nap) -Lys- (Nap) - (Lys-NH) 2 ) - (Phe-COOH), (Lys and Phe both being D-amino acids, the hydrophobic radical being
The preparation method of the polypeptide composite hydrogel comprises the following steps:
(1) Reacting NaBH 4 Adding into water, dissolving in ice bath for 5min to obtain ice NaBH with concentration of 10mol/L 4 Aqueous solution, 100. Mu.L of HAuCl with a concentration of 10mmol/L 4 ·H 2 O aqueous solution is dripped into 10mL MoS with concentration of 10mg/mL 2 Stirring in water solution for 10min at a dropping speed of 10 drops/min, and adding 100 μ L of newly-prepared ice NaBH under stirring 4 Continuously stirring the aqueous solution at normal temperature for 8h, centrifuging at 8000r/min for 5min, washing with ethanol and water for three times, drying at 30 deg.C for 6h to obtain AuNPs/MoS 2 ；
(2) 150mg of the polypeptide powder was dissolved in dimethyl sulfoxide to obtain 1mL of a 150 mg/mL-concentration original polypeptide solution, 35. Mu.L of the original polypeptide solution was taken out, and 965. Mu.L of 2 mg/mL-concentration Au NPs/MoS was added thereto 2 Uniformly mixing the aqueous solution of the composite nano material, and standing for 0.5h to obtain AuNPs/MoS 2 D-Pep hydrogel.
A method of flexible wearable sweat electrochemical sensor monitoring sweat comprising the steps of:
1) Cutting the agarose gel into the size same as that of the ion introduction electrode (8) and modifying the agarose gel on the two sides of the anode and the cathode of the ion introduction electrode (8), wherein the preparation method of the agarose gel comprises the following steps: dissolving every 0.4 agarose in 10mL of 0.1mol/L potassium phosphate buffer solution with pH of 7.0, continuously stirring at 170 ℃ until the agarose is completely dissolved, pouring the agarose gel into a mold, and cooling to room temperature;
2) Before stimulating sweat, modifying an electrode interface with agarose hydrogel by a dropping method for configuring an ion introduction electrode, after freeze-drying, dropping a 3wt% of pilocarpine solution into the agarose hydrogel of an anode, storing for 1h, containing a pilocarpine drug with positive charge in the agarose hydrogel, after electrifying, repelling the pilocarpine close to a skin part due to charge repulsion at the anode part, and then stimulating sweat.
3) Modifying 10 mu L of polypeptide composite hydrogel on the surface of the working electrode (6), wherein the polypeptide composite hydrogel modified on the surface of the working electrode (6) is used for absorbing and storing sweat which is used as natural electrolyte,
4) Cleaning skin by adopting isopropanol friction, and fixing a flexible wearable sweat electrochemical sensor on the human epidermis by using medical double faced adhesive tape;
5) Scanning AA and UA in sweat by using a differential pulse voltammetry technology under the conditions that the potential range is 0.4-0.8V, the amplitude is 50mV and the pulse width is 0.05 s;
6) Monitoring AA and UA in sweat by time-current technique under the condition that the optimal potential is 0.3V and 0.5V respectively;
7) The sweat monitoring signal is transmitted to the personal mobile data terminal (3) through the Bluetooth transmission device (2).
1. The electrode construction process comprises the following steps: and modifying 10 mu L of polypeptide composite hydrogel on the interface of a flexible printed electrode by a dripping method to construct a flexible electrochemical sensor based on the composite hydrogel.
Evaluation of antifouling property: the antifouling performance of the surfaces of the electrodes modified by different kinds was evaluated by using pure proteins (respectively with negative charges, positive charges and neutral charges) of proteins BSA, lys and Mb with different charges in a pure protein environment. In addition, the sensor is subjected to pollution prevention performance test in a complex environment (human sweat), and different concentrations of protein and human sweat are recordedDifferential Pulse Voltammetry (DPV) signal change rates before and after 0.5h of immersion of the liquid sample to evaluate short-time antifouling performance. Meanwhile, a long-term antifouling test was performed for 20 days with 100% human sweat. As shown in FIG. 11, the sensor was subjected to an anti-contamination performance test in a complex environment (in human sweat), and 5.0mM [ Fe (CN) ] before and after soaking for 0.5h in human sweat samples of different contents was recorded 6 ] 3-/4- The DPV signal is kept unchanged along with the increase of sweat content, and the result shows that the polypeptide composite hydrogel has good short-term antifouling performance.
And (3) sensing test: the potential range is set to be 0.4-0.8V, the amplitude is 50mV, and the pulse width is 0.05s. The catalytic performance and specificity of the flexible electrochemical sensor on markers such as vitamin C, uric acid and the like in a PBS (0.2M, pH 7.0) buffer solution are investigated through a differential pulse voltammetry technology (DPV), and under the condition that the optimal potential is 0.3V and 0.5V respectively, the vitamin C and uric acid with different concentrations are detected through a time-current technology (I-T technology); finally, the electrochemical sensor monitors vitamin C and uric acid in human sweat by using an I-T technology, and transmits monitoring signals to a mobile phone through Bluetooth equipment to realize family monitoring of human metabolic function.
As shown in fig. 12, DPV signal response plots for detection of Uric Acid (UA) and vitamin C (AA) in 100% sweat with AA response potential of approximately 0.3V and UA response potential of approximately 0.55V for wearable sweat electrochemical sensor based on polypeptide composite hydrogel. As shown in FIG. 13, based on AuNPs/MoS 2 I-T response graph of wearable sweat electrochemical sensor of/D-Pep hydrogel flexible material to UA in 100% sweat at 0.55V respectively shows that the sensor has good and stable response capability to UA in sweat.
Example 2
The amino acid sequence of the polypeptide is (Fomc) -Lys- (Fomc) - (Lys-NH) 2 ) - (Phe-COOH), lys and Phe are all D-amino acids, the hydrophobic group being
The preparation method of the polypeptide composite hydrogel comprises the following steps:
(1) Reacting NaBH 4 Adding into water, dissolving in ice bath for 8min to obtain ice NaBH with concentration of 15mol/L 4 Aqueous solution, 100. Mu.L of HAuCl with a concentration of 15mmol/L 4 ·H 2 O aqueous solution is dropped into 10mL of MoS with the concentration of 30mg/mL 2 Stirring in water solution for 20min at a dropping speed of 15 drops/min, and adding 100 μ L of newly-prepared ice NaBH under stirring 4 Continuously stirring the aqueous solution for 10h at normal temperature, centrifuging at 9000r/min for 8min, washing with ethanol and water for three times, drying at 40 deg.C for 5h to obtain AuNPs/MoS 2 ；
(2) 150mg of the polypeptide powder was dissolved in dimethyl sulfoxide to obtain 1mL of a 150mg/mL polypeptide original solution, 35. Mu.L of the polypeptide original solution was taken out, and 965. Mu.L of 7mg/mL AuNPs/MoS was added thereto 2 Uniformly mixing the nano composite material aqueous solution, and standing for 0.4h to obtain Au NPs/MoS 2 A/D-Pep hydrogel.
A method of flexible wearable sweat electrochemical sensor monitoring sweat comprising the steps of:
1) Cutting the agarose gel into the size same as that of the ion introduction electrode (8) and modifying the agarose gel on the two sides of the anode and the cathode of the ion introduction electrode (8), wherein the preparation method of the agarose gel comprises the following steps: dissolving 0.8g of agarose in 15mL of 0.1mol/L potassium phosphate buffer solution with pH of 7.0, continuously stirring at 170 ℃ until the agarose is completely dissolved, pouring the agarose gel into a mold, and cooling to room temperature;
2) Before stimulating sweat, agarose hydrogel is modified on an electrode interface through a dropping method and used for constructing an ion introduction electrode, after freeze-drying, 4wt% of pilocarpine solution is dropped into the agarose hydrogel of an anode, the agarose hydrogel is stored for 1.5h, a pilocarpine medicament with positive charge is contained in the agarose hydrogel, after electrifying, the pilocarpine medicament repels the pilocarpine to be close to a skin part due to charge repulsion at the anode part, and then, sweat is stimulated.
3) Modifying 9 mu L of polypeptide composite hydrogel on the surface of the working electrode (6), wherein the polypeptide composite hydrogel modified on the surface of the working electrode (6) is used for absorbing and storing sweat which is used as natural electrolyte,
4) Cleaning skin by adopting isopropanol friction, and fixing a flexible wearable sweat electrochemical sensor on the human epidermis by using medical double faced adhesive tape;
5) Scanning AA and UA in sweat by using a differential pulse voltammetry technology under the conditions that the potential range is 0.4-0.8V, the amplitude is 50mV and the pulse width is 0.05 s;
6) Monitoring AA and UA in sweat by time-current technique under the condition that the optimal potential is 0.3V and 0.5V respectively;
7) The sweat monitoring signal is transmitted to the personal mobile data terminal (3) through the Bluetooth transmission device (2).
Example 3
The amino acid sequence of the polypeptide is (Pyrene) -Lys- (Pyrene) - (Lys-NH) 2 ) - (Phe-COOH), lys and Phe are all D-amino acids, the hydrophobic group being
The preparation method of the polypeptide composite hydrogel comprises the following steps:
(1) Reacting NaBH 4 Adding into water, dissolving in ice bath for 10min to obtain ice NaBH with concentration of 20mol/L 4 Aqueous solution, 100. Mu.L of HAuCl with a concentration of 20mmol/L 4 ·H 2 O aqueous solution is dropped into 10mL of MoS with the concentration of 50mg/mL 2 Stirring in water solution for 30min at a dropping speed of 20 drops/min, and adding 100 μ L of newly-prepared ice NaBH under stirring 4 Stirring the aqueous solution for 12h at normal temperature, centrifuging at 10000r/min for 10min, washing with ethanol and water for three times, drying at 50 deg.C for 8h to obtain AuNPs/MoS 2 ；
(2) 150mg of the polypeptide powder was dissolved in dimethyl sulfoxide to obtain 1mL of a 150mg/mL polypeptide stock solution, 35. Mu.L of the polypeptide stock solution was taken out, and 965. Mu.L of the polypeptide stock solution was added thereto10mg/mL AuNPs/MoS 2 Uniformly mixing the nano composite material aqueous solution, and standing for 0.2h to obtain Au NPs/MoS 2 D-Pep hydrogel.
A method of flexible wearable sweat electrochemical sensor monitoring sweat comprising the steps of:
1) Cutting the agarose gel into the size same as that of the ion introduction electrode (8) and modifying the agarose gel on the two sides of the anode and the cathode of the ion introduction electrode (8), wherein the preparation method of the agarose gel comprises the following steps: dissolving 1.0g of agarose in 25mL of 0.1mol/L potassium phosphate buffer (pH 7.0), stirring at 170 deg.C until the agarose is completely dissolved, pouring the agarose gel into a mold, and cooling to room temperature;
2) Before stimulating sweat, modifying an electrode interface with agarose hydrogel by a dropping method for configuring an ion introduction electrode, after freeze-drying, dropping 5wt% of pilocarpine solution into the agarose hydrogel of an anode, storing for 2h, containing a pilocarpine drug with positive charge in the agarose hydrogel, after electrifying, repelling the pilocarpine close to a skin part due to charge repulsion at the anode part, and then stimulating sweat.
3) Modifying 7 mu L of polypeptide composite hydrogel on the surface of the working electrode (6), wherein the polypeptide composite hydrogel modified on the surface of the working electrode (6) is used for absorbing and storing sweat which is used as natural electrolyte,
4) Cleaning skin by adopting isopropanol friction, and fixing a flexible wearable sweat electrochemical sensor on the human epidermis by using medical double faced adhesive tape;
5) Scanning AA and UA in sweat by using a differential pulse voltammetry technology under the conditions that the potential range is 0.4-0.8V, the amplitude is 50mV and the pulse width is 0.05 s;
6) Monitoring AA and UA in sweat by time-current technique under the condition that the optimal potential is 0.3V and 0.5V respectively;
7) The sweat monitoring signal is transmitted to the personal mobile data terminal (3) through the Bluetooth transmission device (2).
The description of the disclosed embodiments is provided to enable any person skilled in the art to make or use the present invention. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to other embodiments without departing from the spirit or scope of the invention. Thus, the present invention is not intended to be limited to the embodiments shown herein but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.
Claims (10)
1. A flexible wearable sweat electrochemical sensor comprises an electrochemical sweat sensor electrode device 1, a Bluetooth transmission device 2 and a personal mobile data terminal 3, wherein the Bluetooth transmission device 2 is connected with the electrochemical sweat sensor electrode device 1 through a circuit, and the Bluetooth transmission device 2 is in wireless communication connection with the personal mobile data terminal 3;
the electrochemical sweat sensor electrode device 1 comprises a counter electrode 4, a reference electrode 5 and a working electrode 6 printed on a flexible stretchable substrate 7, wherein the working electrode 6 is modified with polypeptide composite hydrogel, and the polypeptide composite hydrogel comprises polypeptides, auNPs and MoS 2 The amino acid sequence of the polypeptide is (hydrophobic group) -Lys- (hydrophobic group) - (Lys-NH) 2 ) - (Phe-COOH), lys and Phe are both D-form amino acids.
2. The flexible wearable sweat electrochemical sensor of claim 1 wherein the hydrophobic group is
One or two of them.
3. The flexible wearable sweat electrochemical sensor of claim 1, wherein the method of making the polypeptide composite hydrogel comprises the steps of:
(1) Reacting NaBH 4 Adding into water, dissolving in ice bath to obtain ice NaBH 4 Aqueous solution of HAuCl 4 ·H 2 Dropping O aqueous solution into MoS 2 Stirring in the aqueous solution, and then adding the newly prepared ice NaBH under stirring 4 Stirring the aqueous solution at normal temperature, centrifuging, washing and drying to obtain AuNPs/MoS 2 ；
(2) Dissolving a powder of the polypeptide of claim 1 or 2 in dimethylsulfoxide to give a raw polypeptide solution, and adding AuNPs/MoS 2 The aqueous solution is evenly mixed and stood to obtain AuNPs/MoS 2 A/D-Pep hydrogel.
4. A flexible wearable sweat electrochemical sensor of claim 3 where in step (1) ice NaBH 4 The concentration of the aqueous solution is 10-20mol/L, HAuCl 4 ·H 2 The concentration of the O aqueous solution is 10-20mmol/L, moS 2 The concentration of the aqueous solution is 10-50mg/mL, and the ice NaBH is added 4 Aqueous solution, HAuCl 4 ·H 2 Aqueous O solution and MoS 2 The volume ratio of the aqueous solution is 1.
5. The flexible wearable sweat electrochemical sensor of claim 3 wherein in step (1), the agitation speed is 200-500r/min, and HAuCl is added 4 ·H 2 Dropping O aqueous solution into MoS 2 Stirring the aqueous solution for 10-30min, and continuing stirring for 8-12h at normal temperature.
6. The flexible wearable sweat electrochemical sensor of claim 3 wherein in step (2), the concentration of the original solution of polypeptide is 150mg/mL, auNPs/MoS 2 The concentration of the aqueous solution is 2-10mg/mL, the original solution of the polypeptide and AuNPs/MoS 2 The volume ratio of the aqueous solution was 35.
7. A flexible wearable sweat electrochemical sensor according to claim 1 where the reference electrode 5 printed with a stretchable silver paste and the working electrode 6 and counter electrode 4 printed with a stretchable carbon paste.
8. A flexible wearable sweat electrochemical sensor according to claim 1 where the personal mobile data terminal 3 is a smartphone or tablet.
9. A method of monitoring a flexible wearable sweat electrochemical sensor as claimed in any one of claims 1 to 8 including the steps of:
1) Modifying 7-10 mu L of polypeptide composite hydrogel on the surface of the working electrode 6, wherein the polypeptide composite hydrogel modified on the surface of the working electrode 6 is used for absorbing and storing sweat as natural electrolyte;
2) Cleaning the skin by adopting isopropanol through friction, and fixing the flexible wearable sweat electrochemical sensor on the epidermis of a human body by using medical double faced adhesive tape;
3) Scanning AA and UA in sweat by using a differential pulse voltammetry technology under the conditions that the potential range is 0.4-0.8V, the amplitude is 50mV and the pulse width is 0.05 s;
4) Monitoring AA and UA in sweat by time-current technique under the condition that the optimal potential is 0.3V and 0.5V respectively;
5) The sweat monitoring signal is transmitted to the personal mobile data terminal 3 through the Bluetooth transmission device 2.
10. Use of a flexible wearable sweat electrochemical sensor of any one of claims 1-8 or a method of monitoring sweat of claim 9 for vital signs monitoring.
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