KR20200097522A - Method for providing printed electrochemical sensor tags using roll-to-roll gravure printing scheme - Google Patents

Abstract

A method for manufacturing an electrochemical sensor tag by using a roll-to-roll (R2R) gravure printing method according to the present invention comprises the steps of: printing first to third conductive wires spaced apart from each other on a flexible PET film substrate by using a hydrophobic Ag nanoparticle ink; printing a first electrode pattern on at least a part of the first conductive wire and the third conductive wire by using a conductive carbon ink; and printing a second electrode pattern on at least a part of the second conductive wire by using an Ag/AgCl ink, wherein the first to the third conductive wires are an auxiliary electrode, a reference electrode, and a working electrode, respectively, and form a three-electrode system. The present invention can function as a low-cost wearable electrochemical multi-sensor in conjunction with an NFC function of a smartphone.

Description

Electrochemical sensor tag manufacturing method using R2R gravure printing method {METHOD FOR PROVIDING PRINTED ELECTROCHEMICAL SENSOR TAGS USING ROLL-TO-ROLL GRAVURE PRINTING SCHEME}

The present invention relates to a method of manufacturing an electrochemical sensor using an R2R (Roll-to-Roll) gravure printing method, and specifically, a method of manufacturing an electrochemical sensor tag applicable to a wearable medical device using an R2R gravure printing method About.

Wearable devices, which are widely distributed, mostly provide only functions to measure movement distance or momentum or measure pulse. A smart watch that works with a smart phone is also not far away from such a function.

Meanwhile, with the rapid development of biometric information diagnostic technology, small wearable devices are starting to replace expensive diagnostic equipment. The US market research firm IDC (International Data Corporation) predicts that the global wearable medical device market will reach 4.6 billion dollars (about 5 trillion won) in 2020.

In particular, a portable medical device that simplifies a blood sugar blood pressure test as a wearable medical device for diagnosing biometric information is being actively developed. Google is working with global pharmaceutical company Novartis to develop a smart contact lens that checks for diabetes by regularly checking the glucose in tears. Apple is also conducting research to equip the "Apple Watch" with a function that checks blood sugar and blood pressure from time to time.

The Ulsan Institute of Science and Technology in Korea developed a smart contact lens that can be worn on the eyes and checked for blood sugar through LEDs. The smart contact lens unveiled by the Ulsan Institute of Science and Technology can easily check the blood sugar level by blinking the LED.

However, in the case of contact lenses for glucose detection, there are various limitations. When the sensor-attached lens is worn on the eye, dryness may occur in the user's eye due to the thickness of the lens. In addition, it is difficult to secure the amount of tear required for measurement at once, and correction must be made between measurement and measurement for accurate data, but since the eyes are always wet with moisture, it is difficult to reliably refresh. In addition, since the smart lens is directly attached to the body and operates, it is not yet free from safety issues.

A wearable prototype that provides the level of accuracy of a medical device even during exercise is being developed at a domestic university. The healthcare smart dressing, which is aimed at commercialization in 2020, is implemented as a system that measures the temperature of the wound (wound) where the skin is peeled off and the pH value of exudate from the wound using a biosensor and transmits it to a mobile phone or a dedicated terminal. do. In the healthcare smart dressing, a wireless communication biosensor is applied that helps the patient himself, his or her guardian, or a medical staff located at a distance to check whether there is bacterial infection in the wound area in real time.

In addition, researchers at Tufts University in the United States have unveiled a prototype of a smart bandage that integrates pH and temperature sensors to monitor the wound. This smart bandage has built-in pH and temperature sensors that track infection and inflammation, so that the collected data can accurately measure the condition of the wound and provide correct medication based on it. The pH measured from the wound is an important factor for monitoring the healing process of chronic wounds, the pH index of a normal wound is 5.5 to 6.5, and the infected wound has a pH index greater than 6.5. A microprocessor mounted in a smart bandage is implemented to inject drugs while collecting data from pH and temperature sensors.

In the case of such a wound area detection band or tag, since it directly contacts the skin, it must be manufactured to be disposable and flexible, but at the current technology level, it is presented only as a prototype due to the price aspect and technical difficulties. In addition, the performance of the electrode included in the detection sensor may be deteriorated due to sweat or skin waste. When measuring the pH index, water is the basic solvent, so water stability must be secured.

Medtronic, a renowned medical device company in the United States, has developed a vest-type wearable medical device that diagnoses cardiac arrhythmia. This vest is equipped with a total of 252 electrode sensors, allowing users to perform atrial and ventricular examinations while wearing clothes as usual. In addition, by combining ECG (electrocardiogram) data and CT scan images of the examined data, the heart structure is reconstructed into a 3D electro-anatomical image to be displayed. However, it is difficult to actually carry the electrocardiogram data, CT scan image, and electrode structure, and it is being developed for patient treatment in some hospitals.

The present invention has been conceived to solve the above-described problems, and an object of the present invention is to provide a method of manufacturing an electrochemical sensor tag that can be applied to a wearable medical device using an R2R gravure printing method. The present invention uses an R2R gravure printing method to print electrochemical sensor electrodes (working electrode, reference electrode, and auxiliary electrode) using hydrophobic Ag nanoparticle ink and conductive carbon ink to implement a three-electrode system. It provides a method of manufacturing a sensor tag.

The present invention is to provide a method of manufacturing an electrochemical sensor tag that can be implemented in a flexible form by printing an insulating layer that prevents each electrode constituting a three-electrode system from being electrically connected to other elements using polyethylene insulating ink.

The present invention is to provide a method for manufacturing an electrochemical sensor tag that can be used as a medical device capable of selectively detecting glucose, pH, K ⁺ , Na ⁺ , Cu ²⁺ , caffeine, etc. through chemical treatment on the surface of a working electrode. .

The present invention is to provide a method of manufacturing an electrochemical sensor tag capable of detecting glucose (or caffeine, K ^+, etc.) in a non-blood sampling method.

An object of the present invention is to provide a manufacturing method for an electrochemical sensor that can be produced at an ultra-low cost in large quantities through a roll-to-roll (R2R) gravure printing device and an application of a wearable medical device using the same.

The method of manufacturing an electrochemical sensor tag using the R2R gravure printing method according to the present invention includes the steps of printing first to third conductive wires spaced apart from each other on a flexible substrate of a PET film using hydrophobic Ag nanoparticle ink, Printing a first electrode pattern using conductive carbon ink on at least a portion of the first conductive wiring and the third conductive wiring, and a second electrode using AgCl ink on at least a portion of the second conductive wiring And printing a pattern, wherein the first electrode pattern is an auxiliary electrode or a reference electrode, and the third electrode pattern is a working electrode to form a three electrode system.

In an embodiment, a third electrode using a material sensitive to at least one of pH, Na ⁺ , K ⁺ , glucose, and caffeine on at least a portion of the third conductive wiring on which the first electrode pattern is printed It may further include forming a pattern.

In one embodiment, the printing of the plurality of conductive wires includes a viscosity of 80 to 150 cp and a tension of 28 to 33 mN/m using polyvinyl butyral (PVB) and terpineol. Eggplant may include the step of preparing the Ag nanoparticle ink.

In an exemplary embodiment, the step of forming the reference electrode by sequentially coating an agarose gel and an SU-8 photoresist on an upper portion on which the second electrode pattern is printed may be further included.

In one embodiment, the method of manufacturing an electrochemical sensor tag according to the present invention includes a viscosity of 250 to 350 cP and a surface tension of 28 to 33 mN/m using polyethylene and ethylene glycol monoethyl ether acetate (ECA). The step of preparing an insulating ink having, and printing an insulating layer on the conductive wiring excluding the first electrode pattern, the second electrode pattern, and or the third electrode pattern using the insulating ink. Can include.

In an embodiment, the printing of the first electrode pattern includes preparing the conductive carbon ink having a viscosity of 250 to 350 cP and a surface tension of 30 to 33 mN/m using the ECA. can do.

In one embodiment, the printing of the third electrode pattern includes preparing a conductive polyaniline ink using polyaniline and camphorsulfonic acid (CSA), and the conductive polyaniline ink of the third conductive wiring. It may include the step of forming a working electrode sensitive to the pH by printing on at least a portion.

In one embodiment, the method of manufacturing an electrochemical sensor tag according to the present invention may further include bonding a chip to the first to third conductive wires.

According to the method of manufacturing an electrochemical sensor according to the present invention, it is possible to mass-produce an electrochemical sensor tag that has high sensitivity to various factors such as pH, Na+, K+, and glucose and is flexible and easy to attach to the human body at a low unit price.

The electrochemical sensor tag manufacturing method according to the present invention includes a printing Ag/AgCl reference electrode manufacturing method having a constant potential, an insulating layer ink manufacturing method for protecting the electrode and minimizing the influence of the external environment, and a polyaniline/carbon-based pH sensitive operation. An electrode manufacturing method may be provided, and as a wearable medical device, an electrochemical sensor tag capable of reading pH (or glucose) from sweat of human skin without blood collection may be provided.

The method of manufacturing an electrochemical sensor tag according to the present invention may provide an electrochemical sensor tag capable of functioning as a low-cost wearable electrochemical multi-sensor in connection with an NFC function of a smartphone.

1 is a flowchart illustrating a method of manufacturing an electrochemical sensor tag according to an embodiment of the present invention, and FIG. 2 is a method of manufacturing an electrochemical sensor tag using an R2R gravure printing method according to an embodiment of the present invention. It is a schematic diagram for explanation.
3 to 7 are plan views illustrating an embodiment of an electrochemical sensor tag according to a method of manufacturing an electrochemical sensor tag.
8 is a view showing an electrochemical sensor tag actually printed using the R2R gravure printing method according to an embodiment of the present invention.
9 is a plan view showing an electrochemical sensor tag connected to a chip according to an embodiment of the present invention.
10 is a graph showing different potentials according to pH of an electrochemical sensor tag manufactured according to an embodiment of the present invention, and a graph showing a voltage change according to a continuous pH change.
11 are graphs showing results according to a case in which different materials are used for the working electrode to be sensitive to glucose and Cu ²⁺ , respectively.
12 is a diagram showing a state in which a printed antenna and a chip are bonded to a completed electrochemical sensor tag to communicate with a smart phone.

Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the accompanying drawings in order to clarify the technical idea of the present invention. In describing the present invention, when it is determined that a detailed description of a related known function or component may unnecessarily obscure the subject matter of the present invention, a detailed description thereof will be omitted. Constituent elements having substantially the same functional configuration among the drawings are assigned the same reference numerals and reference numerals as possible, even though they are displayed on different drawings. If necessary for convenience of explanation, the device and the method will be described together.

1 is a flowchart illustrating a method of manufacturing an electrochemical sensor tag according to an embodiment of the present invention, and FIG. 2 is a method of manufacturing an electrochemical sensor tag using an R2R gravure printing method according to an embodiment of the present invention. It is a schematic diagram for explanation. 3 to 7 are plan views illustrating an embodiment of an electrochemical sensor tag according to a method of manufacturing an electrochemical sensor tag.

The method of manufacturing an electrochemical sensor tag according to the present invention is based on a continuous R2R gravure printing process, and thus, an electrochemical sensor tag can be mass-produced at a low cost.

A PET (polyethylene terephthalate) film substrate is prepared to print the electrochemical sensor (step S110). For application to the R2R process, the PET film substrate may be prepared in a rolled form.

The electrochemical sensor wiring and the conductive wiring serving as an electrode are printed on the PET substrate using a hydrophobic Ag nanoparticle ink (step S120). Existing Ag nanoparticle-based inks for gravure are not suitable for aqueous solution-based measurements due to their hydrophilic properties. In the present invention, the pH measurement is facilitated by using the Ag nanoparticle ink having hydrophobic properties, and further, the conductive wiring using the Ag nanoparticle ink has high conductivity and low resistance.

In addition, in the present invention, an electrochemical sensor circuit using a three-electrode system is implemented, and the conductive wire may include at least three spaced conductive wires.

3 is a plan view showing an embodiment of an electrochemical sensor tag on which a plurality of conductive wires are printed according to the present invention.

Referring to FIG. 3, three spaced apart conductive wires may include a first conductive wire 310, a second conductive wire 320, and a third conductive wire 330, which are not electrically connected respectively. . Thereafter, through an additional process, the first conductive wire 310 may be manufactured to correspond to the auxiliary electrode, the second conductive wire 320 to the reference electrode, and the third conductive wire 330 to correspond to the working electrode.

In the present invention, the conductive wires 310, 320, 330 may be composed of a measurement unit SEN and a connection unit CON, in which a current or voltage value is measured, and specifically, a measurement unit of the first conductive line 310 (SEN) may be an auxiliary electrode, a measurement unit SEN of the second conductive wiring 320 may be a reference electrode, and a measurement unit SEN of the third conductive wiring 330 may be a working electrode.

In the three-electrode system, the working electrode corresponds to an electrode in which an actual oxidation or reduction reaction takes place, and the reference electrode is an electrode that serves as a reference for measuring an accurate voltage at the working electrode. In addition, the auxiliary electrode does not directly participate in the reaction, does not affect the potential value, and is an electrode through which current flows. According to the three-electrode system, a voltage can be obtained through a reference electrode and a current value can be obtained through an auxiliary electrode.

Step S110 is a step of printing wirings that are basic for forming electrodes constituting a three-electrode system using a hydrophobic Ag nanoparticle ink, and in this step, a step of preparing a hydrophobic Ag nanoparticle ink.

Hydrophobic Ag nanoparticle ink is prepared to have a viscosity of 80 to 150 cp, and a surface tension of 28 to 33 mN/m, using PVB (Polyvinyl butyral) and terpineol for R2R gravure printing. I can.

After the plurality of conductive wires are printed in this way, they may be dried for about 1 minute at 150° C. through a drying oven through an R2R process (see step S125 of FIG. 2). Referring to FIG. 2, after each of the following steps such as printing or coating, a process of drying the printed or coated material for the next process may be involved (steps S135, S145, S155, and S165 of FIG. 2 Reference).

A first electrode pattern is printed on a part of the first conductive wire (310 of FIG. 4) and the third conductive wire (330 of FIG. 4) among the plurality of conductive wires (step S130). The first electrode pattern may be printed on conductive wiring printed using hydrophobic Ag nanoparticle ink using conductive carbon ink.

4 is a plan view showing an embodiment of an electrochemical sensor tag on which a first electrode pattern is printed. Referring to FIG. 4, a first electrode pattern 311 is printed on a partial area of the first conductive wire 310, specifically, on the measurement unit SEN of the first conductive wire 310, and the third conductive wire 310 The first electrode pattern 331 may be printed on a partial area of the wiring 330 and on the measurement unit SEN of the third conductive wiring 310.

Depending on the embodiment, the conductive carbon ink may be prepared to have a viscosity of 250 to 350 cP and a surface tension of 30 to 33 mN/m using Ethylene glycol monoethyl ether acetate (ECA).

According to an embodiment, after the first electrode pattern is printed, a drying process may be performed (step S135 in FIG. 2 ).

In the present invention, an insulating layer may be printed in order to exclude an unintended reaction from the printed electrode surface or wiring portion (step S140). The insulating layer cancels unintended chemical reactions and prevents unnecessary exposure of other parts other than the electrodes to the outside. The insulating ink for printing the insulating layer may be prepared by adding an ECA solvent based on polyethylene (PE). In the case of insulating ink, it is possible to apply an insulating layer (effectively used for short) to a printing element (for example, a printing transistor). For example, an insulating ink having a viscosity of 250 to 350 cP and a surface tension of 28 to 33 mN/m may be prepared.

5 is a plan view showing an electrochemical sensor tag on which an insulating layer is printed according to an embodiment of the present invention.

Referring to FIG. 5, as the insulating layer 400 is printed on all areas except for the measurement unit SEN in the conductive wires 310, 320, and 330, the conductive wires are electrically connected to other elements in addition to the measurement. Avoid contact with.

In this specification, it has been described that the insulating layer is printed after the first electrode pattern is printed, but the order in which the insulating layer is printed is not limited thereto.

Depending on the embodiment, the drying step may be further performed after printing the insulating layer (step S145 of FIG. 2).

In the three-electrode system, since the reference electrode must stably provide voltage despite external influences, the second electrode pattern may be printed on a partial area of the second conductive wiring using Ag/AgCl ink (step S150).

6 is a plan view showing an electrochemical sensor tag on which a second electrode pattern is printed according to an embodiment of the present invention.

Referring to FIG. 6, it can be seen that the second electrode pattern 321 is printed on the measurement unit SEN of the second conductive line 320. Depending on the embodiment, the step of printing the second electrode pattern is sequentially coating an agarose film saturated with 3 M KCl and an SU-8 photoresist (specifically, dip coating). It may include the step of. Accordingly, the measurement unit SEN of the second electrode pattern 320 may be manufactured as a reference electrode.

Depending on the embodiment, the printing of the second electrode pattern may use not only R2R gravure printing, but also inkjet or screen printing.

According to an embodiment, referring to FIG. 2, in order to prevent damage from other electrolytes, the Ag/AgCl electrode may be dip coated on SU-8 once more and then dried at 80° C. for 2 hours (step S155). .

Depending on the embodiment, the working electrode of the present invention has different voltage or current values in response to specific components. When the above-described steps are completed, printing by Ag nanoparticle ink and printing by conductive carbon ink are completed in the measurement unit SEN of the third conductive wiring. Cu ²⁺ can be detected using a stripping voltammetry method even if no other additional process is performed afterwards.

Meanwhile, an additional process may be included in order to implement a multi-sensor (sensitization to pH, Na ⁺ , K ⁺ , glucose, caffeine, etc.) (step S160). This process may be understood as forming a third electrode pattern using a material sensitive to at least one of pH, Na ⁺ , K ⁺ , glucose, and caffeine on a partial region of the third conductive wiring.

7 is a plan view showing an electrochemical sensor tag on which a third electrode pattern is formed according to an embodiment of the present invention. Referring to FIG. 7, as the third electrode pattern 332 is formed on the measurement unit SEN of the third conductive line 330, it becomes possible to operate as a multi-sensor sensitive to a specific material.

According to an embodiment, it may further include printing a pH-sensitive third electrode pattern using a conductive polyaniline ink on a carbon/Ag electrode-based working electrode for pH sensitivity. For example, in the conductive polyaniline ink, polyaniline powder and CAS (camphorsulfonic acid) are ground in a mortar at a weight ratio of 1:1, and the mixed powder is mixed in a m-cresol solution in an amount of 1.6 wt%, and then Triethoxy(3-isocyanatopropyl) ) silane is added in an amount of 1 wt%, and after ultra-sonication of this mixture for about 3 hours, it can be prepared by dispersing using a homogenizer for about 1 hour. Depending on the embodiment, the third electrode pattern may be printed using an inkjet or screen printing method.

Depending on the embodiment, it may include coating a glucose oxidizing solution on the measurement portion of the third conductive wiring for glucose sensitivity. Here, the glucose oxidation solution may contain 100 μL of an aqueous PBS solution in 1 mg enzyme.

Depending on the embodiment, for caffeine sensitivity, it may include coating 0.8 μL of 0.01% multiwall carbon nanotubes and 0.01% of Nafion on the measurement portion of the third conductive wiring. . The thus-coated working electrode reacts to caffeine, and consequently, the electrochemical sensor tag can function as a caffeine-sensitive sensor.

Similarly, after forming the third electrode pattern, a drying process may be performed (step S165 in FIG. 2).

8 is a view showing an electrochemical sensor tag actually printed using the R2R gravure printing method according to an embodiment of the present invention.

In order to cope with various types of products, the total electrochemical sensor size can be designed to correspond from 0.5 mm to 3.00 mm. In addition, it is printed on a flexible and thin PET film base so that it can be used as a disposable electrode so that it is easy to deform, and it is designed to be cut and used as needed.

Returning to FIGS. 1 and 2 again, the electrochemical sensor tag printed in this way according to an embodiment may be bonded to a chip for actual operation (step S170). The chip may include a silicon-based chip, and may include a controller and a transducer. The chip can read and store a current or voltage value from each electrode. Further, an antenna may be bonded to allow the electrochemical sensor tag to communicate with an external device (eg, a smart phone), and a value measured from the electrode may be provided to the outside through a chip.

9 is a plan view showing an electrochemical sensor tag connected to a chip according to an embodiment of the present invention. Referring to FIG. 9, a part 350 of a connection part CON of a conductive wire on which the insulating layer 400 is not printed may be connected to the chip 500. Accordingly, values collected from the electrochemical sensor tag may be transmitted to the outside.

10 is a graph showing different potentials according to pH of an electrochemical sensor tag manufactured according to an embodiment of the present invention, and a graph showing a voltage change according to a continuous pH change.

Referring to Figure 10 (a), it is confirmed that the electrochemical sensor tag manufactured according to the present invention outputs a linearly decreasing potential value as the pH (eg, within the range of pH 7 to 11) increases. In addition, referring to FIG. 10B, it can be seen that even when the environment in which the pH is continuously changed continues for several hours, different output voltage values according to the pH are stably output.

11 are graphs showing results according to a case in which different materials are used for the working electrode to be sensitive to glucose and Cu ²⁺ , respectively.

As described above, in the electrochemical sensor tag according to the present invention, in order to be used as a multi-sensor, an additional surface addition process may be performed on the working electrode, and the corresponding material can be identified from the value of a potential or current for each material.

12 is a diagram showing a state in which a printed antenna and a chip are bonded to a completed electrochemical sensor tag to communicate with a smart phone. Figure 12 (a) is a prototype of a smart phone reading the corresponding pH (or glucose, Cu ²⁺ , caffeine, etc.) value in real time using an NFC function from an actual printed electrochemical sensor tag. 12(b) is a conceptual diagram showing a process of attaching an electrochemical sensor tag according to the present invention to a human body to transmit various values including pH to a smart phone. The electrochemical sensor tag proposed in the present invention may be attached to the wrist in a non-blood collection form to check the user's pH or glucose concentration in real time.

So far, the present invention has been looked at in detail centering on the preferred embodiments shown in the drawings. These embodiments are not intended to limit the present invention, but are merely illustrative, and should be considered from an illustrative point of view rather than a restrictive point of view. The true technical protection scope of the present invention should be determined not by the above description but by the technical spirit of the appended claims. Although specific terms have been used in the present specification, they are used only for the purpose of describing the concept of the present invention, and are not used to limit the meaning or the scope of the present invention described in the claims. Each step of the present invention need not necessarily be performed in the order described, and may be performed in parallel, selectively or individually. Those of ordinary skill in the technical field to which the present invention pertains will understand that various modifications and other equivalent embodiments are possible without departing from the essential technical idea of the present invention claimed in the claims. It is to be understood that equivalents include not only currently known equivalents but also equivalents to be developed in the future, that is, all components invented to perform the same function regardless of structure.

Claims (8)

In the method of manufacturing an electrochemical sensor tag using a R2R (Roll-to-Roll) gravure printing method,
Printing first to third conductive wires spaced apart from each other on a flexible substrate of a PET film using a hydrophobic Ag nanoparticle ink;
Printing a first electrode pattern using conductive carbon ink on at least a portion of the first conductive wire and the third conductive wire; And
And printing a second electrode pattern using AgCl ink on at least a portion of the second conductive wiring,
The method of manufacturing an electrochemical sensor tag, wherein the first electrode pattern is an auxiliary electrode or a reference electrode, and the third electrode pattern is a working electrode to form a three electrode system. The method of claim 1
Forming a third electrode pattern using a material sensitive to at least one of pH, Na ⁺ , K ⁺ , glucose, and caffeine on at least a portion of the third conductive wiring on which the first electrode pattern is printed. The method for manufacturing an electrochemical sensor tag, characterized in that it further comprises. The method of claim 1 or 2,
Printing the plurality of conductive wires,
Using PVB (Polyvinyl butyral) and terpineol, an electrochemical sensor comprising the step of preparing the Ag nanoparticle ink having a viscosity of 80 to 150 cp and a tension of 28 to 33 mN/m Tag manufacturing method. The method of claim 1 or 2,
The method of manufacturing an electrochemical sensor tag further comprising the step of forming the reference electrode by sequentially coating an agarose gel and an SU-8 photoresist on the upper portion on which the second electrode pattern is printed. According to claim 4
Preparing an insulating ink having a viscosity of 250 to 350 cP and a surface tension of 28 to 33 mN/m using polyethylene and ethylene glycol monoethyl ether acetate (ECA); And
The method of manufacturing an electrochemical sensor tag, further comprising printing an insulating layer on the conductive wiring excluding the first electrode pattern, the second electrode pattern, and the third electrode pattern using the insulating ink. The method of claim 5
Printing the first electrode pattern,
Comprising the step of preparing the conductive carbon ink having a viscosity of 250 to 350 cP and a surface tension of 30 to 33 mN / m by using the ECA, electrochemical sensor tag manufacturing method. According to claim 2
Printing the third electrode pattern,
Preparing a conductive polyaniline ink using polyaniline and camphorsulfonic acid (CSA); And
And forming a working electrode responsive to the pH by printing the conductive polyaniline ink on at least a portion of the third conductive line. According to claim 7
The method of manufacturing an electrochemical sensor tag, further comprising bonding a chip to the first to third conductive wires.

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