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Disposable Paper-Based Biosensors: Optimizing the Electrochemical Properties of Laser-Induced Graphene.

ABSTRACT: Laser-induced graphene (LIG) on paper substrates is a desirable material for single-use point-of-care sensing with its high-quality electrical properties, low fabrication cost, and ease of disposal. While a prior study has shown how the repeated lasing of substrates enables the synthesis of high-quality porous graphitic films, however, the process-property correlation of lasing process on the surface microstructure and electrochemical behavior, including charge-transfer kinetics, is missing. The current study presents a systematic in-depth study on LIG synthesis to elucidate the complex relationship between the surface microstructure and the resulting electroanalytical properties. The observed improvements were then applied to develop high-quality LIG-based electrochemical biosensors for uric acid detection. We show that the optimal paper LIG produced via a dual pass (defocused followed by focused lasing) produces high-quality graphene in terms of crystallinity, sp² content, and electrochemical surface area. The highest quality LIG electrodes achieved a high rate constant k₀ of 1.5 × 10^-2 cm s^-1 and a significant reduction in charge-transfer resistance (818 Ω compared with 1320 Ω for a commercial glassy carbon electrode). By employing square wave anodic stripping voltammetry and chronoamperometry on a disposable two-electrode paper LIG-based device, the improved charge-transfer kinetics led to enhanced performance for sensing of uric acid with a sensitivity of 24.35 ± 1.55 μA μM^-1 and a limit of detection of 41 nM. This study shows how high-quality, sensitive LIG electrodes can be integrated into electrochemical paper analytical devices.

SUBMITTER: Bhattacharya G

PROVIDER: S-EPMC9284512 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Biosensors with high sensitivity, selectivity and a low limit of detection, reaching nano/picomolar concentrations of biomolecules, are important to the medical sciences and healthcare industry for evaluating physiological and metabolic parameters. Over the last decade, different nanomaterials have been exploited to design highly efficient biosensors for the detection of analyte biomolecules. The discovery of graphene has spectacularly accelerated research on fabricating low-cost electrode materials because of its unique physical properties, including high specific surface area, high carrier mobility, high electrical conductivity, flexibility, and optical transparency. Graphene and its oxygenated derivatives, including graphene oxide (GO) and reduced graphene oxide (rGO), are becoming an important class of nanomaterials in the field of biosensors. The presence of oxygenated functional groups makes GO nanosheets strongly hydrophilic, facilitating chemical functionalization. Graphene, GO and rGO nanosheets can be easily combined with various types of inorganic nanoparticles, including metals, metal oxides, semiconducting nanoparticles, quantum dots, organic polymers and biomolecules, to create a diverse range of graphene-based nanocomposites with enhanced sensitivity for biosensor applications. This review summarizes the advances in two-dimensional (2D) and three-dimensional (3D) graphene-based nanocomposites as emerging electrochemical and fluorescent biosensing platforms for the detection of a wide range of biomolecules with enhanced sensitivity, selectivity and a low limit of detection. The biofunctionalization and nanocomposite formation processes of graphene-based materials and their unique properties, surface functionalization, enzyme immobilization strategies, covalent immobilization, physical adsorption, biointeractions and direct electron transfer (DET) processes are discussed in connection with the design and fabrication of biosensors. The enzymatic and nonenzymatic reactions on graphene-based nanocomposite surfaces for glucose- and cholesterol-related electrochemical biosensors are analyzed. This review covers a very broad range of graphene-based electrochemical and fluorescent biosensors for the detection of glucose, cholesterol, hydrogen peroxide (H2O2), nucleic acids (DNA/RNA), genes, enzymes, cofactors nicotinamide adenine dinucleotide (NADH) and adenosine triphosphate (ATP), dopamine (DA), ascorbic acid (AA), uric acid (UA), cancer biomarkers, pathogenic microorganisms, food toxins, toxic heavy metal ions, mycotoxins, and pesticides. The sensitivity and selectivity of graphene-based electrochemical and fluorescent biosensors are also examined with respect to interfering analytes present in biological systems. Finally, the future outlook for the development of graphene based biosensing technology is outlined.

Project description:Laser-induced graphene (LIG) has gained preponderance in recent years, as a very attractive material for the fabrication and patterning of graphitic structures and electrodes, for multiple applications in electronics. Typically, polymeric substrates, such as polyimide, have been used as precursor materials, but other organic, more sustainable, and accessible precursor materials have emerged as viable alternatives, including cellulose substrates. However, these substrates have lacked the conductive and chemical properties achieved by conventional LIG precursor substrates and have not been translated into fully flexible, wearable scenarios. In this work, we expand the conductive properties of paper-based LIG, by boosting the graphitization potential of paper, through the introduction of external aromatic moieties and meticulous control of laser fluence. Colored wax printing over the paper substrates introduces aromatic chemical structures, allowing for the synthesis of LIG chemical structures with sheet resistances as low as 5 Ω·sq-1, translating to an apparent conductivity as high as 28.2 S·cm-1. Regarding chemical properties, ID/IG ratios of 0.28 showcase low defect densities of LIG chemical structures and improve on previous reports on paper-based LIG, where sheet resistance has been limited to values around 30 Ω·sq-1, with more defect dense and less crystalline chemical structures. With these improved properties, a simple transfer methodology was developed, based on a water-induced peel-off process that efficiently separates patterned LIG structures from the native paper substrates to conformable, flexible substrates, harnessing the multifunctional capabilities of LIG toward multiple applications in wearable electronics. Proof-of concept electrodes for electrochemical sensors, strain sensors, and in-plane microsupercapacitors were patterned, transferred, and characterized, using paper as a high-value LIG precursor for multiples scenarios in wearable technologies, for improved sustainability and accessibility of such applications.

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Disposable Paper-Based Biosensors: Optimizing the Electrochemical Properties of Laser-Induced Graphene.

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