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RSC Advances RSC Advances View Article Online REVIEW View Journal | View Issue A review on graphene-based nanocomposites for electrochemical and fluorescent biosensors Cite this: RSC Adv.,2019,9,8778 Siva Kumar Krishnan, a Eric Singh, b Pragya Singh, c Meyya Meyyappan*d and Hari Singh Nalwa *e 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 Creative Commons Attribution-NonCommercial 3.0 Unported Licence. 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 This article is licensed under a 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 Open Access Article. Published on 18 March 2019. Downloaded 10/11/2021 10:48:39 AM. 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, Received 21st November 2018 toxic heavy metal ions, mycotoxins, and pesticides. The sensitivity and selectivity of graphene-based Accepted 15th February 2019 electrochemical and fluorescent biosensors are also examined with respect to interfering analytes DOI: 10.1039/c8ra09577a present in biological systems. Finally, the future outlook for the development of graphene based rsc.li/rsc-advances biosensing technology is outlined. aCONACYT-Instituto de F´ısica, Benem´erita Universidad Autonoma´ de Puebla, Apdo. 1. Introduction Postal J-48, Puebla 72570, Mexico bDepartment of Computer Science, Stanford University, Stanford, California 94305, Biosensors with high sensitivity, able to detect femto- or pico- USA molar concentrations of analyte molecules, are of paramount cDepartment of Electrical Engineering and Computer Science, National Chiao Tung importance not only in biomedical applications such as glucose University, Hsinchu 30010, Taiwan monitoring and clinical diagnostics1 but also in the agriculture2 dCenter for Nanotechnology, NASA Ames Research Center, Moffett Field, Mountain and food industries3 and environmental monitoring.4,5 The View, California 94035, USA. E-mail: [email protected] development of highly sensitive devices and new approaches eAdvanced Technology Research, 26650 The Old Road, Valencia, California 91381, that can provide efficient point-of-care testing with high USA. E-mail: [email protected] 8778 | RSC Adv.,2019,9, 8778–8881 This journal is © The Royal Society of Chemistry 2019 View Article Online Review RSC Advances À À accuracy and low cost is an urgent need in the healthcare (200 000 cm2 V 1 s 1),45 high optical transparency toward industry.6–8 In addition, in vivo biosensors have received atten- visible light (2.3% absorption)46 and a large specic surface À tion since they enable the long-term monitoring of target ana- area (2630 m2 g 1).47 As a result, graphene-based materials lytes within live cells with high sensitivity, selectivity and (GBMs) have been explored for a wide range of applications, biocompatibility.9,10 Notably, biosensor research is considered including bulk-heterojunction48 and dye-sensitized solar cells,49 to be an important eld since it covers a wide range of sensing energy storage devices,50 electronic skin and touchscreen-panel capabilities, including pulse, heart rate, blood pressure, body devices,51 eld effect transistors,52 light-emitting diodes motions, blood oxygen level, glucose, cholesterol, antibodies, (LEDs),53 gas and chemical sensors,54 nanomedicine,37 drug nucleic acids, proteins, cancer cells, toxins in food products, delivery,55 and many other applications.56 Graphene and its and heavy metals in drinking water.11–13 Numerous approaches oxidized derivatives, such as graphene oxide (GO), which have been explored, including colorimetric biosensors,14 contain various oxygen functional groups (hydroxyl, carboxyl potentiometric biosensors,15 electrochemical biosensors,16 and epoxy functional groups), have emerged for potential use in uorescent biosensors,17 and Raman spectroscopy-based plat- biosensors.57 The presence of these functional groups makes forms.18 Compared with other detection methods, an electro- GO sheets strongly hydrophilic and allows the integration of chemistry-19,20 and uorescence-based21 approach offers a much various types of inorganic nanoparticles, including noble less expensive, more facile and highly sensitive detection metals, metal oxides, semiconducting nanoparticles, quantum method, which enables the monitoring of different analytes, dots (QDs), and nanoclusters (NCs), to enhance the perfor- fast response–recovery times and very low detection limits.22 mance of sensors based on them.58,59 Moreover, the reduction of A er the discovery of buckminsterfullerene (C60) molecules GO into reduced GO (rGO) results in a high density of defects in 1985, the eld of nanotechnology focused intently on devel- that leads to high electrochemical activity compared with that oping new materials and devices within the 1–100 nm scale of CVD-grown graphene, which is particularly useful for devel- because nanoscale materials show unique chemical and phys- oping electrochemical biosensors. Graphene-based nano- 23 Creative Commons Attribution-NonCommercial 3.0 Unported Licence. ical properties compared to their counterpart bulk materials. composites also inherit unique morphological structures and A wide variety of nanoscale materials have been developed, properties useful for sensing.60 The 3D interconnected hier- including zero-dimensional (0D) nanoparticles (such as archical structures of graphene nanocomposites facilitate the metallic and semiconducting nanoparticles),24,25 one- diffusion of different types of biomolecules and preserve their dimensional (1D) nanostructures (nanowires, nanorods, nano- biocatalytic functions to optimize biosensing function- tubes),26 and two-dimensional (2D) nanostructures including ality.61–63 Graphene-based hybrids with polymers64,65 and graphene nanosheets (GNs), transition metal dichalcogenides surface-decorated metal nanoparticles58 have been explored (TMDs), etc.,27 with substantial progress on their synthesis, for biosensing due to their excellent biocompatibility, high processing, characterization and potential applications. Over surface area, and site-selective conjugation with biomolecules. This article is licensed under a the past two decades, these nanoscale materials have been used Various nanostructures have been explored for biosensors, in many applications, including light-emitting diodes, memory including the detection of glucose and hydrogen peroxide,66 devices, communication devices, magnetic disks, solar cells, cancer biomarkers,67–69 nucleic acids,11 antibodies,70 heavy batteries, fuel cells, supercapacitors, and catalysts.28,29 Inter- metals,71,72 pathogenic bacteria,73 and many other targets19,74–77 Open Access Article. Published on 18 March 2019. Downloaded 10/11/2021 10:48:39 AM. facing with various probe biomolecules has been studied in However, no comprehensive review focused on a wide range of order to develop highly sensitive biosensors with signicantly electrochemical and uorescent biosensors utilizing graphene- enhanced sensitivity.30 Due to the size and unprecedented based nanocomposites is yet available in the literature. There physical properties of these nanomaterials, the development of are no reviews on graphene-based uorescent biosensors. biosensors with extremely small dimensions and substantially Therefore, this review is intended to summarize
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