Development of a novel photoelectrochemical-electrochemical dual mode sensing platform using a bifunctional nanomaterial

Nallal Muthuchamy,Kwang-Pil Lee,Anantha Iyengar Gopalan 한국분석과학회 2017 학술대회논문집 Vol.2017 No.5

New Titanium Dioxide-Based Heterojunction Nanohybrid for Highly Selective Photoelectrochemical–Electrochemical Dual-Mode Sensors

Nallal, Muthuchamy,Anantha Iyengar, Gopalan,Pill-Lee, Kwang American Chemical Society 2017 ACS APPLIED MATERIALS & INTERFACES Vol.9 No.42

<P>A new titanium dioxide (TiO2)-based heterojunction nanohybrid (HJNH) composed of TiO2, graphene (G), poly[3-aminophenylboronic acid] (PAPBA), and gold nanoparticles (Au NPs) was synthesized and designated as TiO2(G) NW@PAPBA-Au HJNH. The TiO2(G) NW@ PAPBA-Au HJNH possesses dual-mode signal photoelectrochemical (PEC) and electrochemical transduction capabilities to sense glucose and glycated hemoglobin (HbAlc) independently. The synthesis of the HJNH material involved 1GAu 11) NIMP two sequential stages: (i) simple electrospinning synthesis of 1%-3111 APH 4. G-embedded TiO2 nanowires [TiO2(G) NWs] and (ii) onestep synthesis of Au NP-dispersed PAPBA nanocomposite (NC) in the presence of TiO2(G) NWs. The as-synthesized TiO2(G) NW@PAPBA-Au HJNH was characterized by field emission scanning electron microscopy, field emission transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared, thermogravimetric analysis, and UV-visible diffuse reflectance spectroscopy. A PEC platform was developed with TiO2(G) NW@PAPBA-Au HJNH for the selective detection of glucose without any enzyme auxiliary. The PEC glucose sensor presents an acceptable linear range (from 0.5 to 28 mM), good sensitivity (549.58 mu A mM(-1) cm(-2)), and low detection limit (0.11 mM), which are suited for diabetes glucose monitoring. Besides, the boronic acid groups in PAPBA were utilized as a host to capture HbAlc. We fabricated the electrochemical HbAlc sensor based on monitoring the electrocatalytic reduction current of hydrogen peroxide produced by HbAlc tethered to the sensor probe. The amperometric electrochemical sensor for HbAlc exhibited linear responses to HbAlc levels from 2.0 to 10% (with a detection limit of 0.17%). Notably, the performances of the fabricated glucose and HbAlc sensors are superior in the dual-signal transduction modes as compared to the literature, suggesting the significance of the newly designed bifunctional TiO2(G) NW@PAPBA-Au HJNH.</P>

High-performance glucose biosensor based on green synthesized zinc oxide nanoparticle embedded nitrogen-doped carbon sheet

Muthuchamy, Nallal,Atchudan, Raji,Edison, Thomas Nesakumar Jebakumar Immanuel,Perumal, Suguna,Lee, Yong Rok Elsevier S.A 2018 Journal of Electroanalytical Chemistry Vol.816 No.-

<P><B>Abstract</B></P> <P>A new, highly selective, sensitive and stable enzymatic glucose sensor was fabricated on glassy carbon electrode (GCE) using zinc oxide (ZnO) nanoparticles embedded nitrogen-doped carbon sheets (ZnO@NDCS), glucose oxidase (GOx) (assigned as GCE/ZnO@NDCS/GOx). First, ZnO@NDCS were synthesized by a simple hydrothermal method. Zn powder, aqueous ammonia, and peach extract were served as the precursor for ZnO NPs, nitrogen and carbon, respectively. The fabricated GCE/ZnO@NDCS/GOx biosensor exhibited a high and reproducible sensitivity of 231.7 μA mM<SUP>−1</SUP> cm<SUP>−2</SUP>. Also, showed a wide linear range from 0.2 to 12 mM with a correlation coefficient R<SUP>2</SUP> = 0.998 and lowest detection limit (based on S/N ratio = 3) of 6.3 μM. The GCE/ZnO@NDCS/GOx biosensor is acceptably stable, selective, and it was successfully applied to the quantitative monitoring of glucose in human blood serum. The synthesized ZnO@NDCS nanocomposite may be found useful in other applications in the fields of solar cells and optoelectronic devices. These encouraging results suggest a simple and effective method obtain electrode material for the enzymatic glucose sensor.</P> <P><B>Highlights</B></P> <P> <UL> <LI> ZnO@NDCS composite was synthesized from peach fruit by a simple hydrothermal method. </LI> <LI> Fabricated GCE/ZnO@NDCS/GOx sensor delivered a high sensitivity 118.3 μA mM<SUP>−1</SUP> cm<SUP>−2</SUP>. </LI> <LI> This biosensor showed a LOD of 4 μM and fast amperometric current response of (3 s). </LI> <LI> It exhibits a good selectivity, reproducibility, and long term storage stability. </LI> <LI> Moreover, the GCE/ZnO@NDCS/GOx is well suited for the diabetic glucose monitoring. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Palladium-loaded core-shell nanospindle as potential alternative electrocatalyst for oxygen reduction reaction

Yusuf, Mohammad,Nallal, Muthuchamy,Nam, Ki Min,Song, Sehwan,Park, Sungkyun,Park, Kang Hyun Elsevier 2019 ELECTROCHIMICA ACTA Vol.325 No.-

<P><B>Abstract</B></P> <P>A well-dispersed palladium nanoparticle (Pd NP)-loaded α-Fe<SUB>2</SUB>O<SUB>3</SUB>@SiO<SUB>2</SUB> core-shell nanospindle (PdFS-CSNS) composite is employed as a potential electrocatalyst for the oxygen reduction reaction (ORR). PdFS-CSNS comprised a uniform core-shell (α-Fe<SUB>2</SUB>O<SUB>3</SUB>@SiO<SUB>2</SUB>) nanospindle structure with a core diameter of 80 nm and shell thickness of 15 nm; the nano-sized Pd NPs (2 nm) were loaded by the <I>in situ</I> reduction method. The structural properties and elemental composition of the as-prepared PdFS-CSNS catalyst is characterized by scanning electron microscopy, transmission electron microscopy, X-ray powder diffraction, Fourier-transform infrared spectroscopy, N<SUB>2</SUB> sorption isotherms, and X-ray photoelectron spectroscopy. Compared to commercial Pt<SUB>20%</SUB>@C, the PdFS-CSNS electrocatalyst demonstrated effective ORR electrocatalytic activity <I>via</I> the 4-electron pathway, high stability, and durability, as well as great methanol tolerance. Such intriguing electrocatalytic performance is ascribed to the highly active Pd NP component and effective production of the silica layer in the novel PdFS-CSNS electrocatalyst. The remarkable electrocatalytic activity of PdFS-CSNS will promote further interest in the development of core-shell nanomaterials for other energy and environmental applications.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Well-dispersed Pd Nps on α-Fe<SUB>2</SUB>O<SUB>3</SUB>@SiO<SUB>2</SUB> nanospindle (PdFS-CSNS) was fabricated. </LI> <LI> PdFS-CSNS showed high electrocatalytic activity for oxygen reduction reaction. </LI> <LI> PdFS-CSNS was obtained high stability, durability, and great methanol tolerance. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Mechanochemical assisted synthesis of heteroatoms inherited highly porous carbon from biomass for electrochemical capacitor and oxygen reduction reaction electrocatalysis

Rajendiran, Rajmohan,Nallal, Muthuchamy,Park, Kang Hyun,Li, Oi Lun,Kim, Hee-Je,Prabakar, Kandasamy Pergamon Press 2019 Electrochimica Acta Vol. No.

<P><B>Abstract</B></P> <P>It is highly essential to produce cost-effective and efficient multifunctional porous carbon materials for sustainable energy technologies. Here, we report a facile approach to synthesis biomass derived porous carbon having inherited heteroatoms by mechanochemical method and post pyrolyzing treatment. The optimized porous carbon exhibits superior oxygen reduction reaction performances in an alkaline electrolyte with a half-wave potential of 0.76 V (vs. reversible hydrogen electrode) with a small kinetic current density of 35.5 mV dec<SUP>−1</SUP> and outsanding stability with great tolerance against methanol poisoning. It also shows the multifunctional capability of electrochemical energy storage as supercapacitor electrode material (coin cell), showing high gravimetric capacitance of 273 F g<SUP>−1</SUP> in the aqueous electrolyte with superior cycling stability.</P>

Incorporation of silver nanoparticles on the surface of orthodontic microimplants to achieve antimicrobial properties

Adith Venugopal,Nallal Muthuchamy,Harsh Tejani,Anantha-Iyengar-Gopalan,Kwang-Pill Lee,Heon-Jin Lee,Hee Moon Kyung 대한치과교정학회 2017 대한치과교정학회지 Vol.47 No.1

Objective: Microbial aggregation around dental implants can lead to loss/loosening of the implants. This study was aimed at surface treating titanium microimplants with silver nanoparticles (AgNPs) to achieve antibacterial properties. Methods: AgNP-modified titanium microimplants (Ti-nAg) were prepared using two methods. The first method involved coating the microimplants with regular AgNPs (Ti-AgNP) and the second involved coating them with a AgNP-coated biopolymer (Ti-BP-AgNP). The topologies, microstructures, and chemical compositions of the surfaces of the Ti-nAg were characterized by scanning electron microscopy (SEM) equipped with energy-dispersive spectrometer (EDS) and X-ray photoelectron spectroscopy (XPS). Disk diffusion tests using Streptococcus mutans, Streptococcus sanguinis, and Aggregatibacter actinomycetemcomitans were performed to test the antibacterial activity of the Ti-nAg microimplants. Results: SEM revealed that only a meager amount of AgNPs was sparsely deposited on the Ti-AgNP surface with the first method, while a layer of AgNP-coated biopolymer extended along the Ti-BP-AgNP surface in the second method. The diameters of the coated nanoparticles were in the range of 10 to 30 nm. EDS revealed 1.05 atomic % of Ag on the surface of the Ti-AgNP and an astounding 21.2 atomic % on the surface of the Ti-BP-AgNP. XPS confirmed the metallic state of silver on the Ti-BP-AgNP surface. After 24 hours of incubation, clear zones of inhibition were seen around the Ti-BP-AgNP microimplants in all three test bacterial culture plates, whereas no antibacterial effect was observed with the Ti-AgNP microimplants. Conclusions: Titanium microimplants modified with Ti-BP-AgNP exhibit excellent antibacterial properties, making them a promising implantable biomaterial.

Fabrication of PdAg nanoparticle infused metal-organic framework for electrochemical and solution-chemical reduction and detection of toxic 4-nitrophenol

Hira, Shamim Ahmed,Nallal, Muthuchamy,Park, Kang Hyun Elsevier 2019 Sensors and actuators. B, Chemical Vol.298 No.-

<P><B>Abstract</B></P> <P>In this study, we utilized functionalized metal organic frameworks (MOFs) as a host matrix to embed silver and palladium (AgPd) bimetallic nanoparticles. The physicochemical properties of the as-synthesized materials were characterized Via UV, FT-IR, XRD, SEM, TEM, XPS, BET and TGA analysis. The as-synthesized materials presented excellent activities toward the electrochemical detection of 4-nitrophenol and its reduction by NaBH<SUB>4</SUB> under ambient conditions. The constructed sensor displayed selective and sensitive determination of 4-NP in the linear concentration range 100–370 μM with a limit of detection of Σ32 nM. Moreover, because of its high specific surface area, high conductivity, and fast charge transfer ability, the sensor displayed good electrocatalytic activity. Moreover, it exhibited excellent selectivity toward 4-NP in the presence of common interfering species. The synthesized catalyst exhibited good catalytic activity for the reduction of 4-NP. It was reusable for five consecutive cycles without a significant loss in its catalytic activity. The applicability of the constructed sensor was explored via the detection of 4-NP in tap water samples at a recovery of ∼100.97%.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Fabrication of PdAg NPs infused metal organic framework (AgPd@UiO-66-NH<SUB>2</SUB>). </LI> <LI> The material exhibits low detection limit and high sensitivity in 4-NP detection. </LI> <LI> It provides good catalytic activity in 4-NP reduction with good recyclability. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

An ultrasensitive photoelectrochemical biosensor for glucose based on bio-derived nitrogen-doped carbon sheets wrapped titanium dioxide nanoparticles

Atchudan, Raji,Muthuchamy, Nallal,Edison, Thomas Nesakumar Jebakumar Immanuel,Perumal, Suguna,Vinodh, Rajangam,Park, Kang Hyun,Lee, Yong Rok Elsevier 2019 Biosensors & bioelectronics Vol.126 No.-

<P><B>Abstract</B></P> <P>In this work, an ultra-sensing photoelectrochemical (PEC) glucose biosensor has been constructed from the bio-derived nitrogen-doped carbon sheets (NDC) wrapped titanium dioxide nanoparticles (NDC-TiO<SUB>2</SUB> NPs) followed by the covalent immobilization of glucose oxidase (GODx) on them (designated as a GODx/NDC-TiO<SUB>2</SUB>NPs/ITO biosensor). Initially, the TiO<SUB>2</SUB> NPs was synthesized by sol-gel method and then NDC-TiO<SUB>2</SUB> NPs was synthesized utilizing a green source of <I>Prunus persica</I> (peach fruit) through a simple hydrothermal process. The synthesized NDC-TiO<SUB>2</SUB> NPs composite was characterized by FESEM, HRTEM, Raman spectroscopy, XRD, ATR-FTIR spectroscopy and XPS to determine composition and phase purity. These fabricated GODx/NDC-TiO<SUB>2</SUB>NPs/ITO biosensor exhibited a good charge separation, highly enhanced and stable photocurrent responses with switching PEC behavior under the light (λ > 400 nm). As a result, GODx/NDC-TiO<SUB>2</SUB>NPs/ITO PEC glucose sensor exhibits a good photocurrent response to detection of glucose concentrations (0.05–10 μM) with an ultra-low detection limit of 13 nM under optimized PEC experimental conditions. Also, the PEC glucose sensor revealed a high selectivity, good stability, long time durability, and capability to analyze the glucose levels in real human serum. Also, the further development of this work may provide new insights into preparing other bio-derived carbon nanostructure-based photocatalysts for PEC applications.</P> <P><B>Highlights</B></P> <P> <UL> <LI> NDC-TiO<SUB>2</SUB> NPs was synthesized hydrothermally utilizing a green source of peach fruit. </LI> <LI> GODx/NDC-TiO<SUB>2</SUB>NPs/ITO biosensor successfully fabricated for PEC electrode material. </LI> <LI> The biosensor delivers a LOD of 13 nM with a wide linear range of 0.05–10 μM. </LI> <LI> Also, the PEC glucose detection in real human blood serum with good recoveries. </LI> <LI> Green source derived PEC biosensor is an ideal platform for other PEC biosensors. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Photocatalytic activity of a new titanium dioxide/Bismuth oxychloride@ nitrogendoped graphene nanocomposite towards a cationic dye

Seok-Yong Yun(윤석용),Nallal Muthuchamy,Anantha Iyengar Gopalan,Kwang-Pil Lee 한국분석과학회 2017 학술대회논문집 Vol.2017 No.5