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Sharma e , Carmen A. E-mail: drbeerpal gmail. E-mail: singhal ccsu. The present study represents the advancements achieved over the past ten years towards the development of electrochemical sensors based on nanomaterials. The versatility, sensitivity, selectivity, and capability of analyzing samples with minimal to no pre-treatment means that electrochemical sensors are an attractive and powerful tool for detecting some analgesic and antipyretic drugs such as acetaminophen AP , ibuprofen IB , aspirin ASP , and diclofenac DCF. These analgesic and antipyretic drugs are very popular as minor pain and fever medications. Controlled doses of these drugs do not harm the human body, but higher concentrations can be hazardous for humans. These drugs are also considered to be emerging chemical pollutants in the environment. Reliable and powerful analytical techniques are thus necessary for the detection of these drugs, for the quality control of pharmaceuticals as well as for environmental control. This review emphasizes the synthesis of nanostructured materials and their use in the electrochemical sensing of analgesic and antipyretic drugs. Manika Chaudhary. Presently, she is pursuing PhD from C. She has published six research papers and one book chapter in reputed joumals. Her research interests comprise of nanostructured materials and metal oxide semiconducting materials for energy storage devices and sensors. Beer Pal Singh. University, Meerut UP , India. He is holding faculty position in Physics at C. University, Meerut since He has also visited Germany, France, China, and Boston and presented his research work. His research interests comprise of thin films, 2D materials, nanostructured materials, metal oxides, semiconducting materials, thin film transistors, sensors and energy storage devices. Bansi D. Kushagr Singhal. He is actively engaged in the research related to synthesis and characterizations of transition metal oxide nanomaterials for electrochemical energy storage devices. Rakesh K. He has nine patents and transferred five technologies in bio-fuel, energy storage, environmental technologies, and automotive applications. His research interest includes catalysis for biofuels and fine chemicals, natural clay catalyst, plasma catalysis for environmental remediation, and advanced materials for energy generation and storage. Rahul Singhal. He received his MSc degree in physics from G. He published over 60 articles in peer-reviewed jornals and 4 book chapters. With noticeable accomplishments in nanoscience and nanotechnology, nanomaterial-based electrochemical signal amplification has acquired an incredible capability for improving both the selectivity and sensitivity of electrochemical sensors. It is broadly known that the electrode materials play a crucial role in the development of superior electrochemical sensing platforms that can distinguish target molecules through different analytical principles. Furthermore, useful nanomaterials not only produce a synergic impact on the conductivity, biocompatibility, and catalytic activity, which speeds up signal transduction, but also enhance biorecognition events using explicitly designed signal labels, leading to highly sensitive biosensing. The prepared nanocomposite based sensor showed excellent reproducibility and stability, with wider linear concentration ranges 0. This report also discusses some common methods for the synthesis of nanomaterials and their use in electrochemical sensors for the detection of different drugs. First pinecones were carbonized into the BC material, and then the Co-based zeolitic imidazolate framework ZIF was grown in situ on a porous BC matrix; the product was used as the precursor material. It was reported that the ZIF crystals show rhombic dodecahedral shapes Fig. The FeCo 2 O 4 powder showed a nanorod like morphology with a diameter in the range of — nm Fig. The electrochemical sensor developed using this prepared composite exhibited superior electro-conductivity and a vast active surface area because of the synergy effects of the BC, MOF-derived Co 3 O 4 and FeCo 2 O 4. They developed a sensor with the prepared nanocomposite and used it for the simultaneous detection of morphine and diclofenac. Sivakumar et al. It was observed that each ZnO nanoflake microsphere was formed via interconnected ultrathin nanosheets Fig. In this study, it was reported that AC provided a large surface area and a better electrochemical performance for sensor applications. They constructed an electrochemical sensor based on these ZnO nanoflowers for the detection of dopamine and diclofenac sodium. In the mids, coated-wire electrodes CWEs were first introduced by Freiser. In classical CWEs, a conductor is coated with a suitable ion-selective polymer membrane to make an electrode framework that is sensitive to the electrolyte concentration. The response of CWEs is nearly the same as for classical ISEs, with respect to the detectability and concentration range. Shamsipur et al. The working electrode materials strongly affect the performance of amperometric sensors. Therefore, great efforts have been dedicated to the fabrication and maintenance of working electrodes. In recent years, solid electrodes, fabricated using noble metals and different forms of carbon, have been found to be of great interest for the development of sensors. Effective advancements in electroanalytical chemistry have led to the development of various electrochemical sensors. For several years, mercury was a very attractive material for electrodes due to its renewable surface, extended cathodic potential range window, and high reproducibility. However, its applications were limited because of its toxicity and limited anodic potential. Alternatively, solid electrodes such as nickel, platinum, gold, carbon, and dimensionally stable anions have become very well-known as electrode materials because they are low cost and demonstrate a multifaceted potential window, chemical inertness, a low background current, and the capability for use in different sensing and detection applications. Currently, various nanomaterials are being developed for application in electrochemical sensors. The sensitivity for dopamine and catechol was found to be 0. Ghosh and co-workers developed a low-cost conductometric glucose sensor, which can detect glucose concentrations as low as 10 nM. It was reported that the optimum sensitivity of the sensor was The BP nanosheet electrodes decorated with titanium dioxide nanoparticles were found to be suitable to detect NH 3 in the linear range of 0. The various voltammetric techniques that are used are differentiated from each other by the material that is used as the working electrode and the potential function that is applied to the working electrode. Some voltammetric techniques are explained briefly in the following sections. This technique is generally used in polarography under well-defined conditions; the limiting current derived from a redox process in a solution during LSV may be used to quantitatively determine the concentration of electroactive species in the solution. This prepared sensor showed two well-defined voltammetric potential peaks at 0. Ozcan et al. The response of the sensor to detect AP was found to be in the linear range of 0. The characterization results displayed that the Au nanoparticles were well anchored onto the ZnO nanospheres. Wang et al. It was reported that pore architectures of the hollow carbon polyhedra were found to be favorable for interface features. CV, DPV, and amperometry were employed to investigate the electrochemical behavior of the NiO modified glassy carbon electrodes 3 mm diameter. The size of the NiO nanoparticles obtained was between 15 and 20 nm. It was found from the electrochemical studies that the sensor exhibited a linear detection range from 7. The repeatability and dynamic stability of the constructed sensor is shown in Fig. These prepared oxides were further used to modify graphene electrodes for the detection of dopamine, acetaminophen, and tryptophan. The modified electrode displayed linear response ranges of 0. These modified electrodes were utilized for the simultaneous detection of melatonin, dopamine, and acetaminophen. Cao and co-workers synthesized CeBiO x nanofibers via a simple two-step procedure, which includes electrospinning and calcination with Ce : Bi ratios of 0. SEM studies showed uniform, long, and continuous Ce 0. They prepared CeBiO x nanofiber modified screen printed carbon electrodes for the detection of acetaminophen. From DPV studies, it was reported that the Ce 0. The developed sensor showed a very low detection limit of 2. The constructed sensor showed a detection limit of 0. This designed sensor also demonstrated high sensitivity, good selectivity, and long term stability. Various studies have confirmed the use of carbon-based materials for the detection of acetaminophen. They used eggshell bio-waste-based hydroxyapatite materials for the sensing applications. Morphology characterization techniques revealed the cauliflower-like structure of the Pt particles. The prepared electrochemical sensor was able to detect acetaminophen in a linear concentration range from 0. They also mentioned that this improvement was because of the electron transfer capability and high conductivity of the MWCNTs, which also had a high surface-to-volume ratio, and that the higher surface area of the sensor was due to the porous structure of the CD. The sensor showed a linear range of Liang and co-workers developed a sensor based on glassy carbon electrodes modified with nitrogen-rich porous carbon for acetaminophen detection. They synthesized nitrogen rich porous carbon nanotubes via assisted carbonization of the zeolitic imidazolate framework ZIF-8 using polyvinylpyrrolidone. The pore size of P-NC was found to be distributed in the 4—4. According to them, the highly porous structure of the prepared electrodes provided an interweaving network that facilitated more active sites and helped the better transportation of reactants and products, which contributed to the better electrochemical performance. Amiri et al. The paste design consisted of a hydrophobic binder, hydrophobic graphite as the conducting component, and a nanoparticulate thin film with a hydrophilic surface to provide sensitivity and selectivity. Tsierkezos studied the effect of the incorporation of nitrogen on the electrocatalytic activity of MWCNTs. They synthesized vertically aligned MWCNTs on an oxidized porous silicon wafer using a catalytic CVD technique with acetonitrile as the carbon source material and ferrocene as the catalyst. The modified carbon nanotubes were utilized to develop the electrochemical sensor for acetaminophen sensing. It was noted that the sensor detection ability was enhanced by the nitrogen doping in the CNTs. It was reported that the modified electrode with six layers exhibited a good sensitivity of 2. Using the DPV technique, the prepared electrode showed linear calibration curves in the concentration range of 0. The developed sensor showed a limit of detection of 18 nM for diclofenac and nM for indomethacin. In this study, it was observed that a layer of Au nanoparticles can improve the electrochemical performance as well as the electron transfer due to the layer's large surface area. The designed sensor demonstrated good reproducibility and long-term stability. The detection limit was found to be 0. The constructed sensor showed good repeatability and recorded a detection limit LOD of 0. It was reported that this type of sensor can be successfully used for both drugs AP and IB in commercial tablets. These obtained data were found to be in agreement with the data of many manufacturing companies. The limit of detection for acetaminophen and tramadol was confirmed to be 0. It was found that the sensitivity of the sensor was enhanced by the combination of graphene and NiFe 2 O 4 in the nanocomposite. The fabricated sensor possessed high sensitivity and good stability for clinical assays of tramadol and acetaminophen. It was reported that the sensor showed a high electrocatalytic performance for the oxidation of acetaminophen with a low detection limit of 0. The sensor was also used for the detection of acetaminophen in urine and drug samples with acceptable recovery values. It was also reported that the synergy between the nitrogen-doped graphene and the platinum nanoparticles enhanced the interfacial electron transfer process and showed a higher catalytic performance towards the electrochemical oxidation of acetaminophen. The sensor was found to be suitable for the detection of acetaminophen in a linear range of 0. Shaikshavali et al. A good linear response of 0. The superior electrochemical performance resulted because of the robust composite structure and the synergistic effects between the layered MoS 2 and graphene. Using the DPV technique, a linear range of 0. At pH 7. It was observed that the modified electrode demonstrated an excellent catalytic activity compared with the bare electrode. In this investigation, they used the SWV technique to determine diclofenac in biological and pharmaceutical samples. The developed sensor showed good results which may be attributed to the large surface area of the prepared nanocomposite and the fast electron transfer rate of the AuNPs. Charithra et al. The prepared electrode showed a very low detection limit of 4. It was observed that the formed nanocomposite provided an effective electroactive surface area. The CV and ASV techniques were used to determine the electrochemical behavior of all the mentioned drugs. The oxidation peaks of the designed electrochemical sensor were observed at 0. They formed a nanocomposite with nitrogen doped GQDs and gold nanoparticles which have a unique matrix for covalently attaching the aptamer molecules. The modified GCE with prepared nanocomposite provided higher surface area and electrical conductivity. In this study, riboflavin was first used for the electrochemical detection of ibuprofen. The detection limit was found to be The obtained results revealed that this type of strategy can be implicated in the design of biosensors and electrochemical sensors for the detection of different targets. DOI: Received 10th September , Accepted 21st November Abstract The present study represents the advancements achieved over the past ten years towards the development of electrochemical sensors based on nanomaterials. Table 1 Comparison data for nanomaterial based electrochemical sensors for the detection of drugs.

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