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WIREs Nanomed Nanobiotechnol
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Graphene nanocomposites for transdermal biosensing

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Abstract Transdermal biosensors for the real‐time and continuous detection and monitoring of target molecules represent an intriguing pathway for enhancing health outcomes in a cost‐effective and non‐invasive fashion. Many transdermal biosensor devices contain microneedles and other miniaturized components. There remains an unmet clinical need for microneedle transdermal biosensors to obtain a more accurate, rapid, and reliable insight into the real‐time monitoring of disease. The ability to monitor biomarkers at an intradermal molecular level in a non‐invasive manner remains the next technological gap to solve real‐world clinical problems. The emergence of the two‐dimensional material graphene with unique material properties and the ability to quantify analytes and physiological status can enable the detection of critical biomarkers indicative of human disease. The development of a user‐friendly, affordable, and non‐invasive transdermal biosensing device for continuous and personalized monitoring of target molecules could be beneficial for many patients. This focus article considers the use of graphene‐based transdermal biosensors for health monitoring, evaluation of these sensors for glucose and hydrogen peroxide detection via in vitro, in vivo, and ex vivo studies, recent technological innovations, and potential challenges. This article is categorized under: Diagnostic Tools > Biosensing
A schematic illustration of structures of various forms of graphene. (a) Graphene—a sp2 hybridized model of carbon atoms in a repeated fashion, (b) graphene oxide—chemical synthesis of graphene facilitates the formation of functional groups onto the surface and basal plane of graphene, (c) reduced graphene oxide—chemical reduction of graphene oxide shows defects and vacancies introduced into graphene as a result of reduction, (d) porous graphene—pores of varying size into the sheets of graphene, (e) graphene quantum dots—zero dimensional graphene which has bandgap and reveals excellent photoluminescent features, and (f) three‐dimensional graphene foam—three‐dimensional interconnected architecture of graphene and found in the form of foam, aerogels and sponge. Reproduced with permission of Elsevier, Copyright 2018 (Tabish, Zhang, & Winyard, 2018)
(a) Optical microscopic image of three‐electrode platform comprising of counter, working and reference electrodes. (b) Scanning electron microscopy (SEM) image of Ag/AgCl coated microneedle patch. (c) Image of microneedle patch used on the pig skin. (d) Amperometric responses of microneedles. (e) Statistical analysis of the steady‐state currents in (d). (f) Photographic image of microneedle patch used on mice to monitor H2O2. (g) Amperometric responses of microneedle patches on mice. The mice were s.c. injected with 1 × 10−3 and 10 × 10−3 M H2O2 solutions at the time points t = 70 s and t = 230 s (indicated with arrows). (h) Amperometric responses of MN sensors upon the sensing on mice. The mice were i.p. injected with 10 × 10−3 M H2O2 solutions at the time points t = 70 s and t = 130 s (indicated with arrows). (i) Optical microscopic images of skin irritation assay. Microneedle‐treated skin tissue was stained with hematoxylin and eosin (H&E). Reproduced with permission from Wiley (Jin et al., 2019)
(a) Electrodes 1–3 used in extraction–detection (4, unused). (b) Left: linear response of a pixel sensor to 0.006–0.7 mM glucose. Right: response to glucose, PBS, acetaminophen and ascorbic acid. (c) 10 mM subdermal glucose was extracted across porcine skin ex vivo for 5 min. Left: sensitivity calibration curves for the four pixel devices, demonstrating very similar current–concentration dependencies. Middle: detected current versus time after glucose extraction. Right: detected current versus time after extractions using the same pixel device for 10 and 100 mM subdermal glucose concentrations. Extracted, in‐gel glucose concentrations agree with calculations based on the follicular extraction flux and the number of follicles probed. (d) Left: visual correlation between number of follicles probed by each array pixel. Right: current detected after extraction of 10 mM subdermal glucose. Reproduced with permission from Nature Publishing Group (Lipani et al., 2018)

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