Glucose biosensors - state of the art and prospects

An optical glucose sensor is comprised of light source(s), a detector, and an optical transducer that converts the detected light into a measurable electrical signal. There are two modes of operation for an optical sensor, reflection and transmission. For reflection mode, both the light source and the photodetector are located on the same side. In transmission mode, the photodetector is located on one side of the sample and the light source is on the opposite side [11]. An example of optical biosensor is real-time colorimetric biosensor using affordable devices such as LDR, TCS230, and webcam, real-time color detectors have been successfully created [7].

These detectors were able to accurately detect changes in color depending on the concentration of hydrogen peroxide and titanium oxysulfate in test solutions. The TCS230-based detector proved to be the most sensitive, measuring test solutions of 0.1-1.0 mM this color sensor was used to construct a real-time colorimetric glucose biosensor with good linearity and high selectivity to detect glucose in blood samples, The glucose biosensor's performance was comparable to that of commercial glucose biosensors in a study conducted by Maryamsadat shokrekhodaei et al. [13].

A highly sensitive electrochemical biosensor was developed using a Prussian blue-enzyme cascade catalytic system for glucose detection. Coral-like gold micro/nanostructures were formed on carbon cloth electrodes, followed by Prussian blue deposition to enhance electrochemical activity. The biosensor showed a sensitivity of 454.97 pA mM^-1 cm^-2 for hydrogen peroxide (H2O2) detection, with a linear range of 0.002 mM to 13.97 mM and a detection limit of 0.5 pM. Glucose biosensor was constructed by immobilizing glucose oxidase on the modified electrode, exhibiting a linear response to glucose from 0.05 mM to 3.15 mM. The sensitivity was 70.76 pA mM^-1 cm^-2 and the detection limit was 10 pM. The biosensor demonstrated strong resistance to interference from other electroactive materials and showed good reproducibility and long-term stability. It also successfully detected glucose in human serum samples. This biosensor holds promise for various biosensor applications [14].

Electrochemical biosensors

Electrochemical sensors use electrochemical cells to detect analytes through binding or electrochemical reactions at the surface under an applied potential. This potential can be applied using various methods, including amperometry, potentiometry, impedometry, and cyclic voltammetry. Transistor configurations, such as organic electrochemical transistors (OECTs), can amplify signals and improve biosensor sensitivity. Organic electrochemical biosensors can operate in two modes of detection mechanism: chemically modified organic semiconductors and functionalized semiconductors with complex moieties. Chemical synthesis is crucial for accessing novel material properties and functionalities tailored to detecting specific biomolecules. Recent research has focused on synthesizing organic polymers with semiconducting backbones for electrochemical biosensors, particularly conjugated polymers and polymers of semiconducting organic dyes.

In a study conducted by Wang et al. [5] the immobilization of GOx onto a glassy carbon electrode modified with natural sulfide minerals using glutaraldehyde is shown. The resulting biosensor displayed effective HQ-mediated bioelectrocatalytic activities in an air atmosphere. The biosensors exhibited a broad linear range for all four modified electrodes and showed exceptional repeatability, reproducibility, and applicability. This GOx/GA/SFMs/GCE system has immense potential for understanding the bio-interfaces between GOx and SFMs and expanding the application platform for sulfide minerals [15].

Electrochemical paper-based glucose biosensors have gained popularity due to their advantages such as low cost, simplicity of operation, portability, and disposability. While colorimetric mPADs offer qualitative and semi-quantitative analyte determination using simple imaging tools, they have limitations such as low sensitivity and unsuitability for colored samples. In contrast, electrochemical paper-based analytical devices (ePADs) provide quantitative detection with improved sensitivity, selectivity, and the ability to analyze complex matrices. The pioneering work in colorimetric mPADs was done by the Whiteside group from Harvard University, while the Henry group from Colorado State University [11] developed the first ePAD for quantifying glucose, lactate, and uric acid in human serum samples. The ePAD consisted of microfluidic channels created on filter paper using photolithography and an electrochemical cell printed with screenprinting technology. Glucose oxidase, lactate oxidase, and uricase enzymes were selectively entrapped in different zones on the paper to detect their respective analytes. The detection was achieved by measuring the enzymatic by-product H2O2 at the working electrode modified with the electrochemical mediator Prussian Blue. The ePAD showed good performance in terms of reproducibility and accuracy compared to control levels and spectrophotochemical methods.

Other ePAD configurations have been developed for point-of-care glucose detection. Some ePADs allow for the direct detection of glucose in untreated whole blood samples without the need for plasma separation protocols. For example, the Henry group designed an ePAD [11] with a commercially available electrochemical sensor and blood separation zones on paper to achieve glucose detection.

The accuracy of this ePAD was evaluated and compared to spectrophotochemical methods, showing negligible variance. Kong et al. [6] simplified the configuration by using commercially available sensors printed on alumina and Whatman chromatography paper. The blood sample solution was loaded onto the paper and allowed to air dry before conducting electrochemical measurements. To improve sustainability, wax printing techniques have been employed to create hydrophobic and hydrophilic zones on ePADs without the use of organic solvents. Cinti et al. [6] utilized a Xerox ColorQube 8570 printer to create a green hydrophobic zone on the paper-based strip for glucose detection. The paper-based strip offered filtering properties, porosity for reagent loading, and the ability for in situ synthesis of Prussian Blue nanoparticles. Glucose detection in blood samples using this ePAD showed good linearity and correlation with commercial glucose strips.

Amperometric biosensors

Amperometry is a method used by biosensors to measure the current flow between electrodes during a redox reaction. One of the most extensively studied amperometric biosensor systems is the glucose biosensor. Glucose oxidase (GOx) catalyzes the reaction of glucose with oxygen to form gluconolactone and hydrogen peroxide in this system. The signal is typically represented as current (ampere) versus glucose concentration, induced by a redox reaction of a mediator or hydrogen peroxide at the working electrode. It is worth noting that most conjugated polymer (CP)-based amperometric biosensors belong to the third generation of biosensors, where the enzyme and mediator are directly immobilized on the transducer. Therefore, signal detection does not rely on the diffusion of reaction products or mediators. Singh et al. and Habermuller et al. [8] have published excellent reviews on PPY-based biosensors and general electron transfer principles, respectively.

A study conducted by Izadyar in 2021 [8]: the research involved analyzing a Nafion/PPMP- GOx-BSA/Au biosensor that uses an amperometric enzyme-based approach. This biosensor is not only cost-effective and simple to use, but it is also highly sensitive, selective, and stable. It can detect a wide range of glucose concentrations, as demonstrated by successful LSV and amperometric measurements. The biosensor responded well to glucose concentrations ranging from 3.1 p,M to 13.2 mM [8]. To test the selectivity of the biosensor, they used an experimental solution containing ascorbic acid and citric acid, which are common interferents in physiological samples. Our results showed that the biosensor exhibited excellent selectivity towards glucose monitoring, detecting concentrations ranging from 3.3 цМ to 13.0 mM. The studies have also shown that the recombinant enzyme from the corn kernel production system used in this biosensor is a low-cost, reproducible, sensitive, and selective alternative to conventional enzymes like HRP for glucose detection. In the future, we plan to improve the LOD of the PPMP-based biosensor by incorporating nanomaterials and conductive polymers. This will make the biosensor even more effective in measuring various biofluids in real sample use [8].

Wearable biosensors

Wearable sensors have emerged as a significant advancement in sensor technology for diabetic patients. These sensors are designed to monitor glucose levels and provide clinically relevant data for diabetes management [11]. Wearable sensors involve the integration of devices into wearable objects or directly with the body. Initially, rigid electronic devices were developed in the semiconductor electronics industry, but there has been a shift towards the design of stretchable and flexible electronics. These flexible sensors address the need for cost-effective, non-invasive, and self-testing analysis, eliminating the discomfort associated with finger pricks and skin irritation caused by devices like GlucoWatch.

While sweat sensors face challenges related to sweat collection and extraction of glucose through intact skin using electro-osmotic flow, microneedle sensors offer a solution by enabling analysis in the transdermal compartment with minimal pain. These sensors can be mass-produced at a lower cost and are designed for short-term use before replacement. Commercially available subcutaneous microneedle-based sensors for continuous glucose monitoring include Enlite, G5, and the FreeStyle Libre. Next-generation microneedle sensors provide advantages such as easy insertion and replacement, reduced biofouling effects, larger electrode surface area for improved sensitivity, and the ability to perform multiplexing analyses [17].

In addition to sensors integrated into the skin, another appliable sensor option is contact lenses for continuous glucose monitoring in tear fluid. Contact lens biosensors have utilized fluorescent indicators absorbed into the lens material or embedded photonic crystals in a hydrogel patch for glucose monitoring. Electrochemical sensors on flexible plastic supports have also been developed for attachment onto the eye or insertion into the tear canal. However, accuracy and interference from electroactive species in tear fluid remain challenges. A miniaturized integrated amperometric glucose biosensor integrated into a contact lens was developed to address these issues. This contact lens biosensor demonstrated fast response, high sensitivity, good linearity, and low detection limit for glucose in the tear film [11].

Although the development of contact lens sensors dates back several years, there is still significant interest from major industrial entities, including Novartis in collaboration with Google, who aim to build revolutionary devices that measure glucose levels and assist individuals with diabetes and eye problems.

Conclusion

Acknowledgments: The article was formed in activity of Russian science foundation project number 21-19-00192.

References

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2. Bagyalakshmi, S., Sivakami, A., & Balamurugan, K. S. (2020). A ZnO nanorods based enzymatic glucose biosensor by immobilization of glucose oxidase on a chitosan film. Obesity Medicine, 18, 100229. https://doi.org/10.1016/j.obmed.2020.100229

3. Deng, H., Teo, A. K. L., & Gao, Z. (2014). An interference-free glucose biosensor based on a novel low potential redox polymer mediator. Sensors and Actuators B: Chemical, 191, 522-528. https://doi.org/10.1016/j.snb.2013.10.059

4. Fatoni, A., Aziz, A. N., & Anggraeni, M. D. (2020). Low-cost and real-time color detector developments for glucose biosensor. Sensing and Bio-Sensing Research, 28, 100325.https://doi.Org/10.1016/j.sbsr.2020.100325

5. German, N., Ramanaviciene, A., & Ramanavicius, A. (2021). Dispersed conducting polymer nanocomposites with glucose oxidase and gold nanoparticles for the design of enzymatic glucose biosensors. Polymers, 13(13), 2173. https://doi.org/10.3390/polym13132173

6. Hassan, M. H., Vyas, C., Grieve, B., & Bartolo, P (2021). Recent advances in enzymatic and non-enzymatic electrochemical glucose sensing. Sensors, 21(14), 4672.https://doi.org/10.3390/s2n44672

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8. Izadyar, A., Van, M. N., Rodriguez, K. A., Seok, I., & Hood, E. E. (2021). A bienzymatic amperometric glucose biosensor based on using a novel recombinant Mn peroxidase from corn and glucose oxidase with a Nafion membrane. Journal of Electroanalytical Chemistry, 895, 115387. https://doi.org/10.1016/jjelechem.2021.n5387

9. Karyakin, A. A. (2021). Glucose biosensors for clinical and personal use. Electrochemistry Communications, 125, 106973. https://doi.org/10.1016/j.elecom.2021.106973

10. Mehrotra, P. (2016). Biosensors and their applications-A review. Journal of oral biology and craniofacial research, 6(2), 153-159. https://doi.org/10.1016/jjobcr.2015.12.002

11. Scognamiglio, V., & Arduini, F. (2019). The technology tree in the design of glucose biosensors. TrAC Trends in Analytical Chemistry, 120, 115642.https://doi.org/10.1016/j.trac.2019.115642

12. Arduini, F., Cinti, S., Scognamiglio, V., Moscone, D., & Palleschi, G. (2017). How cutting-edge technologies impact the design of electrochemical (bio) sensors for environmental analysis. A review. Analytica Chimica Acta, 959, 15-42. https://doi.org/10.1016/j.aca.2016.12.035

13. Shokrekhodaei, M., & Quinones, S. (2020). Review of non-invasive glucose sensing techniques: optical, electrical and breath acetone. Sensors, 20(5), 1251.https://doi.org/10.3390/s20051251

14. Van Tuan, D., Ngan, D. T. T., Thuy, N. T., Lan, H., Nguyet, N. T., Van Thu, V., ... &Tam, P. D. (2020). Effect of nanostructured MoS2 morphology on the glucose sensing of electrochemical biosensors. Current Applied Physics, 20(9), 1090-1096.https://doi.org/10.1016/j.cap.2020.06.027

15. Wang, Y., Zhao, J., Yang, T., Zhang, Y., Tao, D., Hasebe, Y., & Zhang, Z. (2021). Electrochemical evaluation of sulfide mineral modified glassy carbon electrode as novel mediated glucose biosensor. Journal of Electroanalytical Chemistry, 894, 115357.

16. Yan, L., Miao, K., Ma, P., Ma, X., Bi, R., & Chen, F. (2021). A feasible electrochemical biosensor for determination of glucose based on Prussian blue - Enzyme aggregates cascade catalytic system. Bioelectrochemistry, 141, 107838. https://doi.org/10.1016/j.bioelechem.2021.107838

17. Zou, L., Wang, S. S., & Qiu, J. (2020). Preparation and properties of a glucose biosensor based on an ionic liquid-functionalized graphene/carbon nanotube composite. New Carbon Materials, 35(1), 12-19. https://doi.org/10.1016/S1872-5805(20)60472-3

Список литературы

1. Apetrei R. M., Camurlu P. The effect of montmorillonite functionalization on the performance of glucose biosensors based on composite montmorillonite/PAN nanofibers // Electrochimica Acta. 2020. V. 353. P. 136484. https://doi.org/10.1016/j.electacta.2020.136484

2. Bagyalakshmi S., Sivakami A., Balamurugan K. S. A ZnO nanorods based enzymatic glucose biosensor by immobilization of glucose oxidase on a chitosan film // Obesity Medicine. 2020. V. 18. P. 100229. https://doi.org/10.1016/j.obmed.2020.100229

3. Deng H., Teo A. K. L., Gao Z. An interference-free glucose biosensor based on a novel low potential redox polymer mediator // Sensors and Actuators B: Chemical. 2014. V. 191. P. 522-528. https://doi.org/10.1016/j.snb.2013.10.059

4. Fatoni A., Aziz A. N., Anggraeni M. D. Low-cost and real-time color detector developments for glucose biosensor // Sensing and Bio-Sensing Research. 2020. V. 28. P. 100325. https://doi.org/10.1016/j.sbsr.2020.100325

5. German N., Ramanaviciene A., Ramanavicius A. Dispersed conducting polymer nanocomposites with glucose oxidase and gold nanoparticles for the design of enzymatic glucose biosensors // Polymers. 2021. V. 13. №13. P. 2173. https://doi.org/10.3390/polym13132173

6. Hassan M. H., Vyas C., Grieve B., Bartolo P. Recent advances in enzymatic and non- enzymatic electrochemical glucose sensing // Sensors. 2021. V 21. №14. P. 4672. https://doi.org/10.3390/s21144672

7. Hopkins J., Fidanovski K., Lauto A., Mawad D. All-organic semiconductors for electrochemical biosensors: An overview of recent progress in material design // Frontiers in bioengineering and biotechnology. 2019. V. 7. P. 237. https://doi.org/10.3389/fbioe.2019.00237

8. Izadyar A., Van M. N., Rodriguez K. A., Seok I., Hood E. E. A bienzymatic amperometric glucose biosensor based on using a novel recombinant Mn peroxidase from corn and glucose oxidase with a Nafion membrane // Journal of Electroanalytical Chemistry. 2021. V 895. P. 115387. https://doi.org/10.1016/jjelechem.2021.115387

9. Karyakin A. A. Glucose biosensors for clinical and personal use // Electrochemistry Communications. 2021. V. 125. P. 106973. https://doi.org/10.1016/j.elecom.2021.106973

10. Mehrotra P. Biosensors and their applications-A review // Journal of oral biology and craniofacial research. 2016. V. 6. №2. P. 153-159. https://doi.org/10.1016/jjobcr.2015.12.002

11. Scognamiglio V., Arduini F. The technology tree in the design of glucose biosensors //TrAC Trends in Analytical Chemistry. 2019. V. 120. P. 115642.

https://doi.org/10.1016/j.trac.2019.115642

12. Arduini F., Cinti S., Scognamiglio V., Moscone D., Palleschi G. How cutting-edge technologies impact the design of electrochemical (bio) sensors for environmental analysis. A review // Analytica Chimica Acta. 2017. V. 959. P. 15-42. https://doi.org/10.1016/j.aca.2016.12.035

13. Shokrekhodaei M., Quinones S. Review of non-invasive glucose sensing techniques: optical, electrical and breath acetone // Sensors. 2020. V 20. №5. P. 1251.https://doi.org/10.3390/s20051251

14. Van Tuan D., Ngan D. T. T., Thuy N. T., Lan H., Nguyet N. T., Van Thu V, Tam P. D. Effect of nanostructured MoS2 morphology on the glucose sensing of electrochemical biosensors // Current Applied Physics. 2020. V. 20. №9. P. 1090-1096. https://doi.org/10.1016/j.cap.2020.06.027

15. Wang Y., Zhao J., Yang T., Zhang Y., Tao D., Hasebe Y, Zhang Z. Electrochemical evaluation of sulfide mineral modified glassy carbon electrode as novel mediated glucose biosensor // Journal of Electroanalytical Chemistry. 2021. V. 894. P. 115357.

16. Yan L., Miao K., Ma P., Ma X., Bi R., Chen F. A feasible electrochemical biosensor for determination of glucose based on Prussian blue - Enzyme aggregates cascade catalytic system // Bioelectrochemistry. 2021. V. 141. P. 107838. https://doi.org/10.1016/j.bioelechem.2021.107838

Zou L., Wang S., Qiu J. Preparation and properties of a glucose biosensor based on an ionic liquid-functionalized graphene/carbon nanotube composite // New Carbon Materials. 2020. V. 35. №1. P. 12-19. https://doi.org/10.1016/S1872-5805(20)60472-3

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