CN113533269A - Portable urine glucose meter and detection method thereof - Google Patents

Portable urine glucose meter and detection method thereof Download PDF

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CN113533269A
CN113533269A CN202110635124.7A CN202110635124A CN113533269A CN 113533269 A CN113533269 A CN 113533269A CN 202110635124 A CN202110635124 A CN 202110635124A CN 113533269 A CN113533269 A CN 113533269A
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quantum dot
glucose
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倪中华
胡涛
徐康恺
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Southeast University
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    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
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    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
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    • G01—MEASURING; TESTING
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    • G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
    • G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
    • G01N21/64—Fluorescence; Phosphorescence
    • G01N21/6486—Measuring fluorescence of biological material, e.g. DNA, RNA, cells
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/01—Arrangements or apparatus for facilitating the optical investigation
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    • G01N2021/0112—Apparatus in one mechanical, optical or electronic block

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Abstract

The invention discloses a portable urine glucose meter and a detection method thereof, which can realize portable urine glucose monitoring. The portable urine glucose meter comprises a shell, a paper-based sensor, a sample feeding pool, an ultraviolet light source, a power supply, an industrial camera and a processing system, wherein the sample feeding pool is of a drawing structure and is arranged at the bottom of the shell; the paper-based sensor is positioned on the sample injection pool; the ultraviolet light source is connected in the inner cavity of the shell and is positioned at two sides of the sample injection pool; the power supply supplies power to the ultraviolet light source; the industrial camera is positioned above the ultraviolet light source and used for shooting the fluorescence change of the paper-based sensor; the processing system is used for processing the pictures shot by the industrial camera to obtain the fluorescence R value of the paper-based sensor and the glucose concentration of the object to be detected.

Description

Portable urine glucose meter and detection method thereof
Technical Field
The invention relates to the field of micro-nano medical instruments, in particular to a portable urine glucose meter and a detection method thereof.
Background
The number of people died due to diabetes is more than 100 million people per year, and simultaneously, the diabetes is also easy to cause various complications such as cardiovascular diseases, renal failure, vision deterioration and the like. It is the third most serious chronic non-infectious disease threatening human health, following tumors, cardiovascular pathologies, characterized by high mortality, high disability rate and high medical costs.
When a person's blood glucose level exceeds the renal glucose threshold, sugar (urine sugar) is present in the urine and urine sugar positivity is an important clue for the diagnosis of diabetes. Compared with blood sugar detection, urine sugar detection avoids sampling processes such as acupuncture and the like, belongs to noninvasive detection, and can greatly reduce the pain of a user. But no portable instrument for urine glucose detection is available on the market at present. Urine glucose detection is carried out in hospitals, a medical worker operates a special urine analyzer to carry out conventional diagnosis of urine, and the medical urine analyzer is large in size, high in cost and complex in operation, so that great inconvenience is brought to daily urine glucose monitoring and health self-management of diabetics.
Disclosure of Invention
The invention aims to solve the problem of long-term technical pain in the screening and management of the diabetes at present, provides a portable urine glucose meter and a detection method thereof, and can realize portable urine glucose monitoring.
In order to solve the technical problems, the technical scheme provided by the invention is as follows:
on one hand, the portable urine glucose meter comprises a shell, a paper-based sensor, a sample injection pool, an ultraviolet light source, a power supply, an industrial camera and a processing system, wherein the sample injection pool is of a drawing structure and is arranged at the bottom of the shell; the paper-based sensor is positioned on the sample injection pool; the ultraviolet light source is connected in the inner cavity of the shell and is positioned at two sides of the sample injection pool; the power supply supplies power to the ultraviolet light source; the industrial camera is positioned above the ultraviolet light source and used for shooting the fluorescence change of the paper-based sensor; the processing system is used for processing the pictures shot by the industrial camera to obtain the fluorescence R value of the paper-based sensor and the glucose concentration of the object to be detected.
Preferably, the ultraviolet light source excites the ultraviolet light with the wavelength of 365 nm; the ultraviolet light source is a strip-shaped LED ultraviolet lamp.
Preferably, an ultraviolet filter is arranged in the industrial camera and used for filtering light with a wave band below 400 nm.
Preferably, the paper-based sensor comprises a substrate layer, an adhesive layer and a paper substrate layer, wherein the substrate layer is used for bearing and holding, and the paper substrate layer is used for feeding and detecting; the bonding layer is connected between the substrate layer and the paper base layer; the paper-based fiber structure of the paper base layer is provided with a quantum dot aerogel structure for detecting glucose.
Preferably, the quantum dot aerogel in the paper-based fiber structure is prepared by adopting cadmium telluride quantum dots emitting red fluorescence and glucose oxidase through a freeze drying method.
Preferably, the preparation method of the quantum dot aerogel comprises the following steps:
step 10) synthesizing cadmium telluride quantum dot aqueous solution from 2.5 hydrated cadmium chloride, sodium borohydride, glutathione and sodium tellurite by using a water phase synthesis method, and purifying the cadmium telluride quantum dot aqueous solution to obtain cadmium telluride quantum dot stock solution;
step 20) diluting the cadmium telluride quantum dot stock solution prepared in the step 10) by 1-3 times, mixing and adding glucose oxidase, and introducing into a detection cavity of a paper substrate after uniformly mixing;
and step 30) freeze-drying the paper base layer obtained in the step 20) to obtain the quantum dot aerogel in the paper base layer.
Preferably, in the step 10), the preparation method of the cadmium telluride quantum dot stock solution comprises the following steps:
step 101) weighing 0.1-0.5 g of 2.5 hydrated cadmium chloride and 0.1-0.5 g of glutathione, dissolving in 40-70 mL of ultrapure water, stirring by using magnetons, and adjusting the pH value of the solution to 9.5-11.5;
step 102), 0.02-0.04 g of sodium tellurite and 0.001-0.006 g of sodium borohydride are weighed, dissolved in the solution obtained in the step 101), stirred, and the mixed solution is heated at 100-120 ℃ for 5-10 hours to obtain a cadmium telluride quantum dot solution;
step 103) mixing the cadmium telluride quantum dot solution obtained in the step 102) with isopropanol according to the volume ratio of 2-5: 1,
and centrifuging at the rotating speed of 4000-8000 rpm to obtain a precipitate, and dissolving the precipitate in ultrapure water to be used as a cadmium telluride quantum dot stock solution.
Preferably, in the step 20), the diluted cadmium telluride quantum dot solution and glucose oxidase are uniformly mixed by adding 25-50U of glucose oxidase per 100ul of cadmium telluride quantum dot solution.
Preferably, in the step 30), the freeze drying is to freeze the paper substrate at-20 ℃ for 2-48 hours, take out the paper substrate after freezing, and freeze-dry the paper substrate in a freeze dryer at-100 ℃ for 1-8 hours.
On the other hand, the embodiment of the invention also provides a detection method of the portable glucose meter, which comprises the following steps: mixing glucose and PBS buffer solution to prepare glucose solutions with different concentrations, injecting the glucose solutions with various concentrations into a detection cavity of a paper base layer through a sample injector, irradiating a paper-based sensor by using a 350-380nm ultraviolet light source, shooting to obtain a fluorescent image, reading the R value of the fluorescent image through a processing system, calculating the average R value of the fluorescent image, and obtaining the glucose concentration of a substance to be detected according to the average R value.
Compared with the prior art, the invention has the advantages that: the whole detection process is carried out in a closed instrument, so that the influence of external light interference is avoided. The urine glucose detection paper base is modified with a nano material, and has higher accuracy and sensitivity than the test paper on the market. The instrument has small volume, convenient carrying, low cost and strong use popularity, and is beneficial to large-scale screening and management of diabetes.
Drawings
FIG. 1(a) is a schematic structural diagram of an embodiment of the present invention;
FIG. 1(b) is an exploded view of the structure of an embodiment of the present invention;
FIG. 2 is a schematic diagram of the structure of a paper-based sensor in an embodiment of the present invention;
FIG. 3 is a photograph and a topographical map of an ultraviolet lamp according to example 1 of the present invention;
FIG. 4 is a graph comparing the results of the present invention with those of an Uritest-500B automatic urine chemistry Analyzer;
FIG. 5 is a graph comparing the performance of the test strips of the present invention with commercial urine glucose test strips.
Detailed Description
The present application will be described in detail with reference to specific examples.
As shown in fig. 1(a) and 1(b), the portable urine glucose meter according to the embodiment of the present invention includes a housing 2, a paper-based sensor 1, a sample cell 3, an ultraviolet light source 4, a power supply 5, an industrial camera 6, and a processing system. The sample feeding pool 3 is of a drawing structure and is arranged at the bottom of the shell 2. The paper-based sensor 1 is positioned on the sample feeding pool 3. The ultraviolet light source 4 is connected in the inner cavity of the shell 2 and is positioned at two sides of the sample injection pool 3. The power supply 5 supplies power to the ultraviolet light source 4. An industrial camera 6 is positioned above the ultraviolet light source 4 to photograph the fluorescence change of the paper based sensor 1. The processing system is used for processing the pictures shot by the industrial camera 6 to obtain the fluorescence R value of the paper-based sensor 1 and the glucose concentration of the object to be detected. Above-mentioned structural arrangement makes the urine glucose meter small in size, conveniently carries, and provides well airtight space, has got rid of the influence of other interference light, helps improving the test result degree of accuracy.
Preferably, the ultraviolet light source excites the ultraviolet light with the wavelength of 365 nm; the ultraviolet light source is a strip-shaped LED ultraviolet lamp.
Preferably, an ultraviolet filter is arranged in the industrial camera and used for filtering light with a wave band below 400 nm.
Preferably, the paper-based sensor 1 comprises a substrate layer 102, an adhesive layer 101 and a paper substrate layer 100, wherein the substrate layer 102 is used for bearing and holding, and the paper substrate layer 100 is used for sample feeding and detection; the adhesive layer 101 is connected between the base layer 102 and the paper base layer 100; the paper-based fibrous structure of the paper base layer 100 has a quantum dot aerogel structure therein for detecting glucose.
Preferably, the quantum dot aerogel in the paper-based fiber structure is prepared by adopting cadmium telluride quantum dots emitting red fluorescence and glucose oxidase through a freeze drying method. The preparation method of the quantum dot aerogel comprises the following steps:
step 10) utilizing a water phase synthesis method to synthesize 2.5 hydrated cadmium chloride (the molecular formula of the 2.5 hydrated cadmium chloride is CdCl)2·2.5H2O), sodium borohydride (the molecular formula of sodium borohydride is NaBH)4) Synthesizing aqueous solution of cadmium telluride quantum dots (molecular formula of cadmium telluride is CdTe) by glutathione (molecular formula of glutathione is L-GSH) and sodium tellurite, and purifying to obtain stock solution of cadmium telluride quantum dots;
and 20) diluting the cadmium telluride quantum dot stock solution prepared in the step 10) by 1-3 times, mixing and adding glucose oxidase, and introducing into a detection cavity of the paper substrate after uniformly mixing. The paper fibers of the paper base layer have good protection and packaging effects on the quantum dots and the glucose oxidase, and are beneficial to the fixation and storage of the quantum dots and the glucose oxidase.
And step 30) freeze-drying the paper base layer obtained in the step 20) to obtain the quantum dot aerogel in the paper base layer. In the vacuum freeze drying process, due to the reduction of air pressure, moisture is directly sublimated and changed into gas to escape, so that a plurality of holes are formed in the frozen aerogel, a three-dimensional porous structure is formed, the specific surface area of the probe is improved, and the improvement of the reaction sensitivity and the reaction rate is facilitated.
In the step 10), the preparation method of the cadmium telluride quantum dot stock solution comprises the following steps:
step 101) weighing 0.1-0.5 g of 2.5 hydrated cadmium chloride and 0.1-0.5 g of glutathione, dissolving in 40-70 mL of ultrapure water, stirring by using magnetons, and adjusting the pH value of the solution to 9.5-11.5.
Step 102), 0.02-0.04 g of sodium tellurite and 0.001-0.006 g of sodium borohydride are weighed, dissolved in the solution obtained in the step 101), stirred, and the mixed solution is heated at 100-120 ℃ for 5-10 hours to obtain a cadmium telluride quantum dot solution. In the heating process, the particle size of the quantum dots is continuously increased along with the increase of the heating time, and the quantum dots with the desired target waveband can be obtained by controlling the heating time.
Step 103) mixing the cadmium telluride quantum dot solution obtained in the step 102) with isopropanol according to the volume ratio of 2-5: 1,
and centrifuging at the rotating speed of 4000-8000 rpm to obtain a precipitate, and dissolving the precipitate in ultrapure water to be used as a cadmium telluride quantum dot stock solution. In the centrifugal process, impurities in the solution can move upwards to the isopropanol solution to be taken away, so that the purity of the quantum dots can be greatly improved.
Preferably, in the step 20), the diluted cadmium telluride quantum dot solution and glucose oxidase are uniformly mixed by adding 25-50U of glucose oxidase per 100ul of cadmium telluride quantum dot solution.
Preferably, in the step 30), the freeze drying is to freeze the paper substrate at-20 ℃ for 2-48 hours, take out the paper substrate after freezing, and freeze-dry the paper substrate in a freeze dryer at-100 ℃ for 1-8 hours.
The quantum dot aerogel of the embodiment has a porous three-dimensional structure, so that the specific surface area of the quantum dot aerogel is enlarged, and the reaction sensitivity and the reaction rate can be remarkably improved in the application of glucose detection. And because of the polypeptide encapsulation, the polypeptide has good biocompatibility, provides rich enzyme attachment sites, and remarkably improves the detection performance.
The sensor of this embodiment includes the bed course that has bearing and handheld effect, the adhesive linkage of pasting the effect and advance kind and detect the effect paper substrate. A quantum dot aerogel structure that can be used for detecting glucose is synthesized in the fiber structure of the paper substrate. The aerogel structure can reflect different fluorescence colors aiming at glucose solutions with different contents, and can enable people to obtain the glucose content of the detected solution through naked eyes and instrument analysis. The detection device is convenient to carry, and can realize qualitative rapid visual analysis and high-sensitivity quantitative analysis.
The detection method of the portable glucose meter of the embodiment comprises the following steps: mixing glucose and PBS buffer solution to prepare glucose solutions with different concentrations, injecting the glucose solutions with various concentrations into a detection cavity of a paper base layer through a sample injector, irradiating a paper-based sensor by using a 350-380nm ultraviolet light source, shooting to obtain a fluorescent image, reading the R value of the fluorescent image through a processing system, calculating the average R value of the fluorescent image, and obtaining the glucose concentration of a substance to be detected according to the average R value. The method for reading the R value is the prior art, and the picture reading is opened through Photoshop.
In this example, in order to construct a paper-based sensor for glucose, a three-dimensional porous CdTe-GOx aerogel was prepared within a paper-based layer. The CdTe quantum dots can emit red fluorescence under the irradiation of ultraviolet light of 350-380nm, so that the whole paper chip can emit red fluorescence under the excitation of the ultraviolet light of 350-380 nm. When glucose is added, the glucose will act as GOxBy oxidative decomposition under hydrogen2O2，H2O2The red fluorescence of the CdTe quantum dots is quenched. Thus, as the concentration of glucose increases, H is produced2O2The quantity of red fluorescence emitted by CdTe quantum dots in the paper chip gradually decreases, and visual qualitative detection is further realized. Meanwhile, as the intensity of the red fluorescence of the paper chip is reduced, the R value of the fluorescence color of the paper chip is changed. In particular, the decrease in the R value can be detected to indirectly detect the concentration of glucose by detecting the R value.
In this example, a quantum dot aerogel structure that can be used for detecting glucose was synthesized in the paper-based fiber structure. The aerogel structure can reflect different fluorescence colors aiming at glucose solutions with different contents, and can enable people to obtain the glucose content of the detected solution through naked eyes and instrument analysis. The detection device is convenient to carry, and can realize qualitative rapid visual analysis and high-sensitivity quantitative analysis.
In order to construct a paper-based sensor for glucose, a three-dimensional porous CdTe-GOx quantum dot aerogel was prepared within a paper-based layer. The CdTe quantum dots can emit red fluorescence under the irradiation of 350-380nm ultraviolet light, so that the whole paper base layer can emit red fluorescence under the excitation of 350-380nm ultraviolet light. When glucose is added, the glucose can be oxidized and decomposed under the action of GOx to generate H2O2，H2O2The red fluorescence of the CdTe quantum dots is quenched. Thus, as the concentration of glucose increases, H is produced2O2The quantity of the red fluorescence emitted by the CdTe quantum dots in the paper base layer gradually decreases, and visual qualitative detection is further realized. Meanwhile, as the intensity of the red fluorescence of the paper base layer is reduced, the R value of the fluorescence color of the paper base layer is changed, particularly the R value is reduced, and the concentration of the glucose can be indirectly detected by detecting the R value.
The Whatman #1 filter paper is punched into small round pieces with a diameter of 8mm by a punching machine, and then the small round pieces are orderly and uniformly stuck on a biochemical glass slide by double-sided adhesive, and the structure is shown in figure 2. The substrate layer 102 is a slide substrate. The adhesive layer 101 is a double-sided tape. The paper substrate 100 is a circular lattice filter paper. The inside of the circular lattice filter paper is modified with a glucose recognition unit quantum dot aerogel which is used as a detection probe and integrates sample adding and detection. The double-sided adhesive tape is used as an adhesive layer for fixing the circular dot matrix on the glass slide. The glass slide is used as a substrate, provides a handheld area and rigidity, and is convenient to take and detect.
Several methods of making quantum dot aerogel paper-based sensors are exemplified below.
Embodiment 1 a method of making a quantum dot aerogel paper-based sensor:
step 10) hydration of cadmium chloride CdCl 2.5 by aqueous phase synthesis2·2.5H2O, sodium borohydride NaBH4Glutathione L-GSH, sodium tellurite Na2TeO3Synthesizing a cadmium telluride CdTe quantum dot aqueous solution, and purifying the cadmium telluride CdTe quantum dot aqueous solution to obtain a cadmium telluride CdTe quantum dot stock solution; the preparation method of the cadmium telluride CdTe quantum dot stock solution comprises the following steps:
step 101) weighing 0.1 g of 2.5 hydrated cadmium chloride CdCl2·2.5H2Dissolving O and 0.1 g of glutathione L-GSH in 40 mL of ultrapure water, stirring by utilizing magnetons, and adjusting the pH value of the solution to 9.5;
step 102) weighing 0.02 g of sodium tellurite Na2TeO3With 0.001 g of sodium borohydride NaBH4Dissolving the cadmium telluride CdTe quantum dot in the solution obtained in the step 101), stirring, and heating the mixed solution at 100 ℃ for 5 hours to obtain a cadmium telluride CdTe quantum dot solution;
and 103) mixing the CdTe-QDs solution of the cadmium telluride quantum dots obtained in the step 102) with isopropanol according to the volume ratio of 2: 1, centrifuging at the rotating speed of 4000 rpm to obtain precipitate, and dissolving the precipitate in ultrapure water to obtain the stock solution of the cadmium telluride CdTe quantum dots.
Step 20) diluting the cadmium telluride CdTe quantum dot stock solution prepared in the step 10) by 1 time, mixing and adding glucose oxidase GOx, and introducing into a detection cavity of the paper substrate after uniform mixing. And adding 25U of glucose oxidase into every 100ul of the cadmium telluride quantum dot solution and uniformly mixing the diluted cadmium telluride quantum dot solution and the glucose oxidase.
And step 30) putting the paper base layer obtained in the step 20) into a freezer at-20 ℃ for 2 h, taking out after freezing, and putting the paper base layer into a freezer dryer for freeze drying at-100 ℃ for 1 h. The adhesive layer 101 connects the base layer 102 and the paper base layer 100.
The CdTe-GOx aerogel paper-based sensor prepared in the embodiment 1 is placed under a 365nm ultraviolet lamp to emit red fluorescence, which indicates that quantum dots are successfully synthesized. The results are shown in fig. 3, where fig. 3 (a) is a photograph of the sensor in daylight, fig. 3 (b) is a photograph of the sensor under an ultraviolet lamp, showing a bright red color, and fig. 3 (c) is a photomicrograph of the sensor, showing a clear view of the flocculent aerogel structure within the paper fibers. The three-dimensional porous structure has larger specific surface area, provides abundant enzyme attachment sites and accelerates the reaction rate and sensitivity.
Embodiment 2 a method of making a quantum dot aerogel paper based sensor:
step 10) hydration of cadmium chloride CdCl 2.5 by aqueous phase synthesis2·2.5H2O, sodium borohydride NaBH4Glutathione L-GSH, sodium tellurite Na2TeO3Synthesizing a cadmium telluride CdTe quantum dot aqueous solution, and purifying the cadmium telluride CdTe quantum dot aqueous solution to obtain a cadmium telluride CdTe quantum dot stock solution; the preparation method of the cadmium telluride CdTe quantum dot stock solution comprises the following steps:
step 101) weighing 0.5g of 2.5 hydrated cadmium chloride CdCl2·2.5H2Dissolving O and 0.5g of glutathione L-GSH in 70mL of ultrapure water, stirring by utilizing a magneton, and adjusting the pH value of the solution to 11.5;
step 102) weighing 0.04g of sodium tellurite Na2TeO3With 0.006g of sodium borohydride NaBH4Dissolving the cadmium telluride CdTe quantum dot in the solution obtained in the step 101), stirring, and heating the mixed solution at 120 ℃ for 10 hours to obtain a cadmium telluride CdTe quantum dot solution;
and 103) mixing the CdTe-QDs solution of the cadmium telluride quantum dots obtained in the step 102) with isopropanol according to the volume ratio of 5: 1, centrifuging at the rotating speed of 8000rpm to obtain precipitate, and dissolving the precipitate in ultrapure water to obtain the stock solution of the cadmium telluride CdTe quantum dots.
And step 20) diluting the cadmium telluride CdTe quantum dot stock solution prepared in the step 10) by 3 times, mixing and adding glucose oxidase GOx, and introducing into a detection cavity of the paper substrate after uniform mixing. And adding 50U of glucose oxidase into every 100ul of the cadmium telluride quantum dot solution and uniformly mixing the diluted cadmium telluride quantum dot solution and the glucose oxidase.
And step 30) putting the paper substrate obtained in the step 20) into a freezer at-20 ℃ for 48h, taking out after freezing, and putting the paper substrate into a freezer dryer for freeze drying at-100 ℃ for 8 h. The adhesive layer 101 connects the base layer 102 and the paper base layer 100.
Embodiment 3 a method of making a quantum dot aerogel paper based sensor:
step 10) hydration of cadmium chloride CdCl 2.5 by aqueous phase synthesis2·2.5H2O, sodium borohydride NaBH4Glutathione L-GSH, sodium tellurite Na2TeO3Synthesizing a cadmium telluride CdTe quantum dot aqueous solution, and purifying the cadmium telluride CdTe quantum dot aqueous solution to obtain a cadmium telluride CdTe quantum dot stock solution; the preparation method of the cadmium telluride CdTe quantum dot stock solution comprises the following steps:
step 101) weighing 0.3 g of 2.5 hydrated cadmium chloride CdCl2·2.5H2Dissolving O and 0.3 g of glutathione L-GSH in 55 mL of ultrapure water, stirring by utilizing a magneton, and adjusting the pH value of the solution to 10.5;
step 102) weighing 0.03 g of sodium tellurite Na2TeO3With 0.004 g of sodium borohydride NaBH4Dissolving the cadmium telluride CdTe quantum dot in the solution obtained in the step 101), stirring, and heating the mixed solution at 110 ℃ for 8 hours to obtain a cadmium telluride CdTe quantum dot solution;
and 103) mixing the CdTe-QDs solution of the cadmium telluride quantum dots obtained in the step 102) with isopropanol according to the volume ratio of 3: 1, centrifuging at the rotating speed of 6000 rpm to obtain precipitate, and dissolving the precipitate in ultrapure water to obtain the stock solution of the cadmium telluride CdTe quantum dots.
Step 20) diluting the cadmium telluride CdTe quantum dot stock solution prepared in the step 10) by 2 times, mixing and adding glucose oxidase GOx, and introducing into a detection cavity of the paper substrate after uniform mixing. And uniformly mixing the diluted cadmium telluride quantum dot solution and glucose oxidase according to the condition that 40U of glucose oxidase is added into every 100ul of cadmium telluride quantum dot solution.
And step 30) putting the paper substrate obtained in the step 20) into a freezer at-20 ℃ for 24 hours, taking out after freezing, and putting the paper substrate into a freezer dryer for freeze drying at-100 ℃ for 5 hours. The adhesive layer 101 connects the base layer 102 and the paper base layer 100.
By adopting the structure of the embodiment of the invention, the quantum dot aerogel paper-based sensor is prepared by adopting the embodiment. 208 clinical urine samples were tested with a medical Uritest-500B automated urine chemistry Analyzer. The test results were analyzed by alignment, as shown in FIG. 4. As can be seen from FIG. 4, the test results of the urine glucose meter of this embodiment substantially match the test results of the medical meter, and the test results within each urine glucose concentration gradient are substantially the same. In fig. 4, the abscissa is the respective urine glucose concentration gradient, and the ordinate is the number of samples in the respective concentration gradient. Wherein negative means normal urine sugar content, specific concentration interval is 0-5.6 mM, plus sign means positive urine sugar concentration, 1+ concentration interval is 5.6-14 mM, 2+ concentration interval is 14-28 mM, and 3+ concentration interval is 28 mM or more.
The portable glucose-in-urine meter (using the quantum dot aerogel paper-based sensor prepared in example 2) of the present invention was compared with five commercially available colorimetric chemical analysis test strips (ulilite, aiwei, angora, anjian, and golbao) for testing performance. Five common urine glucose test strips and the portable urine glucose analyzer of the invention are respectively used for detecting 208 real clinical urine samples, and the detection comparison result is shown in fig. 5. As can be seen from FIG. 5, compared with various commercially available urine glucose test strips, the detection result of the urine glucose meter of this embodiment is closest to the standard value, and the measurement result in each urine glucose concentration gradient is substantially identical to the standard value. In FIG. 5, "-" indicates negative, the measured urine glucose value was 0 to 5.6 mM, the plus sign indicates positive urine glucose concentration, the 1+ concentration range was 5.6 to 14 mM, the 2+ concentration range was 14 to 28 mM, and the 3+ concentration range was 28 mM or more. The ordinate represents the number of samples in each concentration interval.
The present invention and its embodiments have been described above, without limitation, and the embodiments shown in the drawings are only one of the specific embodiments of the present invention, and the actual hardware and software structures are not limited thereto. In conclusion, it should be understood that those skilled in the art should be able to devise similar arrangements and embodiments without the inventive step, without the teaching of this patent.

Claims (10)

1. A portable urine glucose meter is characterized by comprising a shell, a paper-based sensor, a sample injection pool, an ultraviolet light source, a power supply, an industrial camera and a processing system, wherein the sample injection pool is of a drawing structure and is arranged at the bottom of the shell; the paper-based sensor is positioned on the sample injection pool; the ultraviolet light source is connected in the inner cavity of the shell and is positioned at two sides of the sample injection pool; the power supply supplies power to the ultraviolet light source; the industrial camera is positioned above the ultraviolet light source and used for shooting the fluorescence change of the paper-based sensor; the processing system is used for processing the pictures shot by the industrial camera to obtain the fluorescence R value of the paper-based sensor and the glucose concentration of the object to be detected.
2. The portable glucose meter of claim 1, wherein the ultraviolet light source excites ultraviolet light having a wavelength of 365 nm; the ultraviolet light source is a strip-shaped LED ultraviolet lamp.
3. The portable glucose meter of claim 1, wherein the industrial camera incorporates an ultraviolet filter for filtering light in a wavelength range below 400 nm.
4. The portable urine glucose meter according to claim 1, wherein the paper-based sensor comprises a substrate layer, an adhesive layer and a paper substrate layer, the substrate layer is used for bearing and holding, and the paper substrate layer is used for sample feeding and detection; the bonding layer is connected between the substrate layer and the paper base layer; the paper-based fiber structure of the paper base layer is provided with a quantum dot aerogel structure for detecting glucose.
5. The portable urine glucose meter according to claim 4, wherein the quantum dot aerogel in the paper-based fiber structure is prepared by adopting cadmium telluride quantum dots emitting red fluorescence and glucose oxidase through a freeze drying method.
6. The portable urine glucose meter according to claim 5, wherein the preparation method of the quantum dot aerogel comprises the following steps:
step 10) synthesizing cadmium telluride quantum dot aqueous solution from 2.5 hydrated cadmium chloride, sodium borohydride, glutathione and sodium tellurite by using a water phase synthesis method, and purifying the cadmium telluride quantum dot aqueous solution to obtain cadmium telluride quantum dot stock solution;
step 20) diluting the cadmium telluride quantum dot stock solution prepared in the step 10) by 1-3 times, mixing and adding glucose oxidase, and introducing into a detection cavity of a paper substrate after uniformly mixing;
and step 30) freeze-drying the paper base layer obtained in the step 20) to obtain the quantum dot aerogel in the paper base layer.
7. The quantum dot aerogel paper-based sensor for glucose detection according to claim 6, wherein in the step 10), the preparation method of the cadmium telluride quantum dot stock solution comprises the following steps:
step 101) weighing 0.1-0.5 g of 2.5 hydrated cadmium chloride and 0.1-0.5 g of glutathione, dissolving in 40-70 mL of ultrapure water, stirring by using magnetons, and adjusting the pH value of the solution to 9.5-11.5;
step 102), 0.02-0.04 g of sodium tellurite and 0.001-0.006 g of sodium borohydride are weighed, dissolved in the solution obtained in the step 101), stirred, and the mixed solution is heated at 100-120 ℃ for 5-10 hours to obtain a cadmium telluride quantum dot solution;
and 103) mixing the cadmium telluride quantum dot solution obtained in the step 102) with isopropanol according to the volume ratio of 2-5: 1, centrifuging at the rotating speed of 4000-8000 rpm to obtain a precipitate, and dissolving the precipitate in ultrapure water to obtain the cadmium telluride quantum dot stock solution.
8. The portable urine glucose meter according to claim 6, wherein in the step 20), the diluted cadmium telluride quantum dot solution and the glucose oxidase are uniformly mixed by adding 25-50U of glucose oxidase per 100ul of cadmium telluride quantum dot solution.
9. The portable urine glucose meter according to claim 6, wherein in the step 30), the freeze drying is performed by freezing the paper substrate at-20 ℃ for 2-48 h, taking out the paper substrate after freezing, and freeze drying the paper substrate in a freeze dryer at-100 ℃ for 1-8 h.
10. A method of testing a portable glucose meter, the method comprising: mixing glucose and PBS buffer solution to prepare glucose solutions with different concentrations, injecting the glucose solutions with various concentrations into a detection cavity of a paper base layer through a sample injector, irradiating a paper-based sensor by using a 350-380nm ultraviolet light source, shooting to obtain a fluorescent image, reading the R value of the fluorescent image through a processing system, calculating the average R value of the fluorescent image, and obtaining the glucose concentration of a substance to be detected according to the average R value.
CN202110635124.7A 2021-06-08 2021-06-08 Portable urine glucose meter and detection method thereof Pending CN113533269A (en)

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CN110487759A (en) * 2019-08-22 2019-11-22 东南大学 For the double-colored Ratio-type quantum dot aeroge microsensor of glucose and its application
CN210487600U (en) * 2019-04-09 2020-05-08 江南大学 Fluorescent whitening agent ultraviolet quick detection box and device
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CN106370637A (en) * 2016-10-13 2017-02-01 东南大学 Quantum-dot aerogel micro-sensor for glucose, method for preparing quantum-dot aerogel and application of quantum-dot aerogel micro-sensor
CN106706590A (en) * 2017-02-16 2017-05-24 韶关市食品药品检验所 Portable fluorescence chip data collector
CN106770264A (en) * 2017-03-01 2017-05-31 福建医科大学 A kind of method that nanoscale molybdenum oxide analogue enztme based on paper micro-fluidic chip detects glucose
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