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        A spick-and-span approach to the immobilization of horseradish peroxidase on Au nanospheres incorporated with a methionine/graphene biomatrix for the determination of endocrine disruptor bisphenol A

        Vilian, A.T. Ezhil,Giribabu, Krishnan,Choe, Sang Rak,Muruganantham, Rethinasabapathy,Lee, Hoomin,Roh, Changhyun,Huh, Yun Suk,Han, Young-Kyu Elsevier Sequoia 2017 Sensors and actuators. B Chemical Vol.251 No.-

        <P><B>Abstract</B></P> <P>In the present study, we employ a straightforward, benign strategy to prepare thiol-functionalized reduced graphene oxide (S-RGO) using methionine as the sulphur source and reducing agent. The immobilization of horseradish peroxidase (HRP) over the AuNPs/S-RGO was developed by incorporating AuNPs on the S-RGO surface. The fabricated HRP/AuNPs/S-RGO electrode exhibits a remarkable decrease in the overpotential and a significantly increased oxidation peak current of bisphenol A (BPA) compared with the bare glassy carbon electrode (GCE) and AuNPs/S-RGO electrode. The biosensor shows an excellent amperometric analytical performance with a low detection limit of 2.6×10<SUP>−12</SUP> M and a linear range from 2.0×10<SUP>−11</SUP> to 1.18×10<SUP>−9</SUP> M, with the response time <2s for BPA. From the results, the apparent Michaelis-Menten constant was calculated as 8.14nM. The HRP/AuNPs/S-RGO biosensor exhibited faster response, adequate storage stability, inexpensive, simple fabrication with disposability, satisfactory reproducibility and repeatability, and outstanding selectivity. Finally, the constructed biosensor was utilized successfully for detecting BPA in tomato juice and milk samples with acceptable results.</P> <P><B>Highlights</B></P> <P> <UL> <LI> HRP/AuNPs/S-RGO biocomposite has been prepared to determine bisphenol A. </LI> <LI> The AuNPs/S-RGO is a promising platform for HRP immobilization. </LI> <LI> The biosensor exhibits excellent stability, reproducibility and high selectivity. </LI> <LI> It exhibits LOD of 2.6×10<SUP>−12</SUP> in a wide linear range from 2.0×10<SUP>−11</SUP> to 1.18×10<SUP>−9</SUP> M. </LI> <LI> It detects bisphenol A in real samples such as tomato juice and milk. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • An enzyme-free electrochemical sensor based on reduced graphene oxide/Co<sub>3</sub>O<sub>4</sub> nanospindle composite for sensitive detection of nitrite

        Haldorai, Yuvaraj,Kim, Jun Yeong,Vilian, A.T. Ezhil,Heo, Nam Su,Huh, Yun Suk,Han, Young-Kyu Elsevier 2016 Sensors and actuators. B, Chemical Vol.227 No.-

        <P><B>Abstract</B></P> <P>Cobalt oxide (Co<SUB>3</SUB>O<SUB>4</SUB>) nanospindles-decorated reduced graphene oxide (RGO) composite is prepared via thermal decomposition of a three-dimensional coordination complex precursor, cobalt benzoate dihydrazinate, at 200°C. Transmission electron microscopy reveals that Co<SUB>3</SUB>O<SUB>4</SUB> nanospindles with an average particle size of <25nm are decorated on the RGO surface. The low decomposition temperature and lack of residual impurities are significant aspects of this simple and facile method. The electrochemical performance of the proposed sensor is investigated using cyclic voltammetry and chronoamperometry. Under optimum conditions, anodic peak currents are linearly proportional to their concentrations, in the range of 1–380μM for nitrite with a regression equation of <I>I</I> (μA)=2.0660C+6.7869 (<I>R</I> <SUP>2</SUP> =0.9992). The sensor exhibits a high sensitivity of 29.5μAμM<SUP>−1</SUP> cm<SUP>−2</SUP>, a rapid response time of 5s, and a low detection of limit of 0.14μM. The proposed electrode shows good reproducibility and long-term stability. The sensor is used to determine the nitrite level in tap water with acceptable recovery, implying its feasibility for practical application.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Facile synthesis of Co<SUB>3</SUB>O<SUB>4</SUB> nanospindles/RGO composite. </LI> <LI> The low detection limit for nitrite sensing was identified as 0.14μM. </LI> <LI> Detection of wide range (1–380μM) of nitrite concentrations. </LI> <LI> High stability and reproducibility of the composite electrode. </LI> <LI> Excellent anti-interference capacity towards various common ions. </LI> </UL> </P>

      • Hexagonal Co<sub>3</sub>O<sub>4</sub> anchored reduced graphene oxide sheets for high-performance supercapacitors and non-enzymatic glucose sensing

        Vilian, A. T. Ezhil,Dinesh, Bose,Rethinasabapathy, Muruganantham,Hwang, Seung-Kyu,Jin, Chang-Soo,Huh, Yun Suk,Han, Young-Kyu The Royal Society of Chemistry 2018 Journal of Materials Chemistry A Vol.6 No.29

        <P>Reduced graphene oxide (RGO) incorporated onto metal-organic framework (MOF)-derived Co3O4 hexagons is prepared <I>via</I> a hydrothermal route for supercapacitor and glucose sensor applications. Various analysis techniques demonstrate that the Co3O4 hexagons were uniformly spread over the thin graphene sheets to assist the electron accessibility of the electrode materials. Under optimized conditions, using 0.1 M KOH electrolyte at a current density of 4 A g<SUP>−1</SUP>, a specific capacitance value of 1300 F g<SUP>−1</SUP> is obtained. The fabricated asymmetric supercapacitor cycled reversibly and exhibits high energy and power density values of 65.8 W h kg<SUP>−1</SUP> and 2048 W kg<SUP>−1</SUP>, respectively, over the voltage range of −0.1 V to 0.4 V. The asymmetric supercapacitor shows 80.5% capacitance retention even after 5000 cycles at a current density of 4 A g<SUP>−1</SUP>, which indicates its high cycling stability in view of the fact that it is binder-free. Furthermore, the RGO-Co3O4 hexagon-modified electrode was optimized to realize the reliable amperometric determination of glucose concentration with a very low detection limit and excellent sensitivity value of 0.4 μM and 1.315 mA mM<SUP>−1</SUP> cm<SUP>−2</SUP>, respectively. All of these remarkable performance indicators suggest that RGO-Co3O4 is a promising electrode material for next-generation energy storage devices and electrochemical sensors.</P>

      • Facile synthesis of MnO2/carbon nanotubes decorated with a nanocomposite of Pt nanoparticles as a new platform for the electrochemical detection of catechin in red wine and green tea samples

        Ezhil Vilian, A. T.,Madhu, Rajesh,Chen, Shen-Ming,Veeramani, Vediyappan,Sivakumar, Mani,Huh, Yun Suk,Han, Young-Kyu The Royal Society of Chemistry 2015 Journal of materials chemistry. B, Materials for b Vol.3 No.30

        <P>Herein, we report a simple and facile synthesis strategy of MnO2/carbon nanotubes decorated with a nanocomposite of Pt nanoparticles using a simple electrodeposition method. The Pt/MnO2/f-MWCNT modified electrode were characterized by several analytical and spectroscopy techniques and were adopted as a composite for a novel catechin sensor. The as-prepared Pt/MnO2/f-MWCNT modified glassy carbon electrode (GCE) exhibited a smaller peak potential separation (Δ<I>E</I>p), and electron transfer kinetics during the oxidation reaction of catechin. This can be attributed to the larger effective surface area, greater porosity, and more reactive sites on the Pt/MnO2/f-MWCNT-modified GCE. Notably, we achieved a very low detection limit (under optimized conditions) of catechin <I>ca.</I> 0.02 μM (S/N = 3); the linear range is 2-950 μM with excellent sensitivity. The real time application of catechin in red wine, black tea, and green tea samples with excellent performance. The proposed sensor was successfully developed and the advantages of low cost, ease of preparation, long-term stability, and good reproducibility were demonstrated which are superior to recently reported modified electrodes, thereby enabling practical industrial applications.</P>

      • SCISCIESCOPUS

        Efficient electron-mediated electrochemical biosensor of gold wire for the rapid detection of C-reactive protein: A predictive strategy for heart failure

        Vilian, A.T. Ezhil,Kim, Wonyoung,Park, Bumjun,Oh, Seo Yeong,Kim, TaeYoung,Huh, Yun Suk,Hwangbo, Chang Kwon,Han, Young-Kyu Elsevier 2019 Biosensors & bioelectronics Vol.142 No.-

        <P><B>Abstract</B></P> <P>C-reactive protein (CRP) is considered a promising biomarker for the rapid and high-throughput real-time monitoring of cardiovascular disease and inflammation in unprocessed clinical samples. Implementation of this monitoring would enable various transformative biomedical applications. We have fabricated a highly specific sensor chip to detect CRP with a detection limit of 2.25 fg/mL. The protein was immobilized on top of a gold (Au) wire/polycarbonate (PC) substrate using 1-ethyl-3-(3-dimethylamino-propyl) carbodiimide hydrochloride/N-hydroxy succinimide-activated 3-mercaptoproponic acid (MPA) as a self-assembled monolayer agent and bovine serum albumin (BSA) as a blocking agent. In contrast to the bare PC substrate, the CRP/BSA/anti-CRP/MPA/Au substrate exhibited a considerably high electrochemical signal toward CRP. The influence of the experimental parameters on CRP detection was assessed via various analysis methods, and these parameters were then optimized. The linear dynamic range of the CRP was 5–220 fg/mL for voltammetric and impedance analysis. Morever, the strategy exhibited high selectivity against various potential interfering species and was capable of directly probing trace amounts of the target CRP in human serum with excellent selectivity. The analytical assay based on the CRP/BSA/anti-CRP/MPA/Au substrate could be exploited as a potentially useful tool for detecting CRP in clinical samples.</P> <P><B>Highlights</B></P> <P> <UL> <LI> The sensor utilizes Au wires to attaching antibodies for specific binding of CRP for heart failure diagnostics. </LI> <LI> A low detection limit of 2.25 fg/mL with linear concentrations of 5–220 fg/mL for CRP was measured. </LI> <LI> The advanced sensor has excellent stability, reproducibility and selective sensing for CRP. </LI> <LI> The offered sensor is used to detect CRP in human serum and saliva with a good recovery. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • Salt-templated three-dimensional porous carbon for electrochemical determination of gallic acid

        Vilian, A.T.Ezhil,Song, Ji Yoon,Lee, Yun Sung,Hwang, Seung-Kyu,Kim, Hae Jin,Jun, Young-Si,Huh, Yun Suk,Han, Young-Kyu Elsevier 2018 Biosensors & bioelectronics Vol.117 No.-

        <P><B>Abstract</B></P> <P>We report an electrochemical sensor based on three-dimensional porous amorphous carbon (3DPAC) for the sensitive and selective determination of gallic acid (GA). The tailor-made carbon was prepared via salt-templating in which the organic molecular precursor, i.e., glucose, was simply ground and carbonized with a eutectic mixture of LiBr and KBr at 800 °C in an inert atmosphere. Salt removal from the carbon-salt mixture with water yielded 3DPAC with a hierarchical porous structure and oxygen-containing functional groups. When employed as an electrochemical sensor, 3DPAC exhibited remarkable sensitivity (0.1045 µA pM<SUP>−1</SUP> cm<SUP>−2</SUP>) with a lower detection limit of 0.434 pM at a signal-to-noise ratio of 3 and a linear response up to 1–150 pM for determination of GA. Under optimized test conditions, 3DPAC showed a superior peak current response for GA as compared to the glassy carbon electrode. In addition, ascorbic, uric, and caffeic acids did not interfere with the voltammetric detection of GA in terms of selectivity, stability, and repeatability. We envision that 3DPAC can provide a promising platform for the development of electrochemical sensors.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Fabrication of 3DPAC using glucose as a carbon source and a eutectic mixture of LiBr and KBr as salt-template. </LI> <LI> A wide linear range of 1–150 pM, LOD of 0.434 pM, and sensitivity of 0.1045 µA pM<SUP>−1</SUP> cm<SUP>−2</SUP> towards GA oxidation. </LI> <LI> Rapid response time, excellent stability, repeatability and reproducibility in GA detection. </LI> <LI> Quantitative analysis of GA in human serum and urine samples with satisfactory results. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • Fabrication of Palladium Nanoparticles on Porous Aromatic Frameworks as a Sensing Platform to Detect Vanillin

        Vilian, A. T. Ezhil,Puthiaraj, Pillaiyar,Kwak, Cheol Hwan,Hwang, Seung-Kyu,Huh, Yun Suk,Ahn, Wha-Seung,Han, Young-Kyu American Chemical Society 2016 ACS APPLIED MATERIALS & INTERFACES Vol.8 No.20

        <P>Here, we report the fabrication of palladium nanoparticles on porous aromatic frameworks (Pd/PAF-6) using a facile chemical approach, which was characterized by various spectro- and electrochemical techniques. The differential pulse voltammetry (DPV) response of Pd/PAF-6 toward the vanillin (VA) sensor shows a linear relationship over concentrations (10-820 pM) and a low detection limit (2 pM). Pd/PAF-6 also exhibited good anti -interference performance toward 2 -fold excess of ascorbic acid, nitrophenol, glutathione, glucose, uric acid, dopamine, ascorbic acid, 4-nitrophenol, glutathione, glucose, uric acid, dopamine, and 100 -fold excess of Na4, Mg2+, and r during the detection of VA. The developed electrochemical sensor based on Pd/PAF-6 had good reproducibility, as well as high selectivity and stability. The established sensor revealed that Pd/PAF-6 could be used to detect VA in biscuit and ice cream samples with satisfactory results.</P>

      • A biocompatible implant electrode capable of operating in body fluids for energy storage devices

        Chae, Ji Su,Heo, Nam-Su,Kwak, Cheol Hwan,Cho, Wan-Seob,Seol, Geun Hee,Yoon, Won-Sub,Kim, Hyun-Kyung,Fray, Derek John,Vilian, A.T. Ezhil,Han, Young-Kyu,Huh, Yun Suk,Roh, Kwang Chul Elsevier 2017 Nano energy Vol.34 No.-

        <P><B>Abstract</B></P> <P>Implantable electronic medical devices (IEMDs) can potentially be used to solve various clinical problems including the monitoring of chronic diseases and electro-organ transplantation. Several recently introduced techniques based on implantable devices that exploit novel metal- or carbon-based hybrid materials are biocompatible owing to their encapsulation in nontoxic polymers. However, such techniques limit the correct functioning of implantable devices, resulting in frequent replacement, difficult miniaturization, and inflammatory side effects in the body. Here, we describe a new technique for application to IEMDs that is capable of providing energy storage using the natural ions of body fluids as electrolytes in a supercapacitor (or ultracapacitor). The system is constructed with a solar cell for energy harvesting and a supercapacitor for energy storage. We assembled IEMDs with two biocompatible electrodes, specifically, MnO<SUB>2</SUB> nanoparticles affixed to multi-walled carbon nanotubes as the positive electrodes and phosphidated activated carbon as the negative electrodes. From the obtained result, this work can be further extended to the use of rats. This technique avoids the problems of performance degradation and toxicity that normally limits the reaction that is permissible in extracellular fluid. We present this concept schematically. The two biocompatible electrodes were successfully implanted into the subcutaneous layer of a rat's skin with both electrodes showing stable performance in use as parts of a supercapacitor. These findings establish a platform for potential biocompatible materials for implantable energy storage devices.</P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • Palladium Supported on an Amphiphilic Triazine-Urea-Functionalized Porous Organic Polymer as a Highly Efficient Electrocatalyst for Electrochemical Sensing of Rutin in Human Plasma

        Vilian, A. T. Ezhil,Sivakumar, Rajamanickam,Huh, Yun Suk,Youk, Ji Ho,Han, Young-Kyu American Chemical Society 2018 ACS APPLIED MATERIALS & INTERFACES Vol.10 No.23

        <P>Metal nanoparticle-containing porous organic polymers have gained great interest in chemical and pharmaceutical applications owing to their high reactivity and good recyclability. In the present work, a palladium nanoparticle-decorated triazine-urea-based porous organic polymer (Pd@TU-POP) was designed and synthesized using 1,3-bis(4-aminophenyl)urea with cyanuric chloride and palladium acetate. The porous structure and physicochemical properties of the electrode material Pd@TU-POP were observed using a range of standard techniques. The Pd@TU-POP material on the electrode surface showed superior sensing ability for rutin (RT) because the Pd dispersion facilitated the electrocatalytic performance of TU-POP by reducing the overpotential of RT oxidation dramatically and improving the stability significantly. Furthermore, TU-POP provides excellent structural features for loading Pd nanoparticles, and the resulting Pd@TU-POP exhibited enhanced electron transfer and outstanding sensing capability in a linear range between 2 and 200 pM having a low detection value of 5.92 × 10<SUP>-12</SUP> M (S/N = 3). The abundant porous structure of Pd@TU-POP not only provides electron transport channels for RT diffusion but also offers a facile route for quantification sensing of RT with satisfactory recoveries in aqueous electrolyte containing human plasma and red wine. These data reveal that the synthetic Pd@TU-POP is an excellent potential platform for the detection of RT in biological samples.</P> [FIG OMISSION]</BR>

      • SCISCIESCOPUS

        Pt-Au bimetallic nanoparticles decorated on reduced graphene oxide as an excellent electrocatalysts for methanol oxidation

        Vilian, A.T. Ezhil,Hwang, Seung-Kyu,Kwak, Cheol Hwan,Oh, Seo Yeong,Kim, Chang-Yeon,Lee, Go-woon,Lee, Jin Bae,Huh, Yun Suk,Han, Young-Kyu Elsevier Sequoia 2016 Synthetic metals Vol.219 No.-

        <P><B>Abstract</B></P> <P>In this study, we report a general and simple strategy for the synthesis of platinum nanoparticles (PtNPs), highly dispersed on reduced graphene oxide (RGO) substrate with Au nanoparticles. The electrochemically active surface area (ECSA) of the Pt-Au-RGO electrocatalyst is found to be higher than the Pt-RGO electrocatalyst, which is more comparable to a commercial Pt/C catalyst. The obtained ratio of the voltammetric forward peak current to the reverse peak current for the Pt-Au-RGO electrocatalyst (<I>I</I> <SUB>f</SUB>/<I>I</I> <SUB>b</SUB> =2.33) is much higher than that of the Pt-RGO electrocatalyst (<I>I</I> <SUB>f</SUB>/<I>I</I> <SUB>b</SUB> =1.16). This phenomenon is attributed to the synergistic effects of the Au and the RGO substrate, which help to enhance the electrochemical activity of Pt nanoparticles for methanol oxidation and carbonaceous poisoning resistance. The reported methanol oxidation is found to exhibit excellent electrocatalytic performance, reliability, and stability, surpassing that of several reported modified electrodes that can also be used for platinum-based catalysts in fuel cell applications.</P> <P><B>Highlights</B></P> <P> <UL> <LI> We prepared an efficient Pt-Au-RGO architecture using an effective strategy to enhancing loading of Au nanoparticles into RGO. </LI> <LI> The electrochemically active surface area (ECSA) of the Pt-Au-RGO heterogeneous electrocatalyst is found to be higher than the Pt-RGO and Pt/C electrocatalysts. </LI> <LI> The Pt-Au-RGO electrocatalyst demonstrated better electrocatalytic activity and stability than the Pt-RGO or Pt/C black for methanol oxidation. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

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