Catalytic template assisted chemical vapor deposition method for the synthesis of graphitic carbon nanostructures

( Raji Atchudan ),이용록 한국공업화학회 2015 한국공업화학회 연구논문 초록집 Vol.2015 No.0

The graphitic carbon nanostructures (GCNs) were synthesized over the catalytic templates using acetylene as carbon precursor by simple chemical vapor deposition (CVD) method. The catalytic templates such as iron oxide nanoparticles (IONPs) and Mn impregnated MgO (Mn-MgO) were characterized and were used for the production GCNs. The reaction parameters such as temperature and flow of carbon precursor were optimized in order to achieve GCNs with excellent quality and quantity. The interlayer distance of resulted GCNs is match well with the bulk graphite. All the analytical results strongly support that the prepared GCNs to be highly ordered and well graphitic in nature. Further, the results demonstrate that the GMC/g-CNTs synthesized over Mn-MgO/IONPs might be a promising contender for the large-scale process. Moreover, the produced GCNs might be an ideal candidate for nanoelectronic applications.

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>

Eco-friendly Chebulic Myrobalan-Derived Porous Carbon Employed as an Electrocatalyst for the Production of Hydrogen

Atchudan Raji,Perumal Suguna,Sundramoorthy Ashok K.,Manoj Devaraj,Kumar Raju Suresh,Almansour Abdulrahman I.,Sangaraju Sambasivam,Lee Wonmok,Lee Yong Rok 한국화학공학회 2024 Korean Journal of Chemical Engineering Vol.41 No.6

The growing energy demand and environmental issues have encouraged the development of novel and sustainable energy. Hydrogen is one of the cleanest and most sustainable energy sources that provides an environmentally friendly alternative future fuel. The recent development in hydrogen production through electrocatalytic water-splitting is somewhat highperformance. The potential electrocatalysts play an essential role in hydrogen evolution reactions (HER) for electrochemical water splitting, where expensive and low-abundance platinum-based materials are the standard catalysts for HER. Herein, metal-free, low-cost, and naturally abundant chebulic myrobalan was employed as a source for the preparation of porous carbon by direct pyrolysis route, and the resulting porous carbon was utilized as an electrocatalyst for the production of hydrogen gas. The various analytical techniques confi rmed the existence of sulfur, nitrogen, and oxygen in the prepared chebulic myrobalan-derived porous carbon (CM-PC). The presence of eff ective heteroatoms in the CM-PC may lead to interactive eff ects between the heteroatoms and porous carbon structures; this suggests the enhancement of the electrochemical performance of HER. The surface area of CM-PC was obtained as 675 m 2 g −1 by BET measurement. The CM-PC exhibited a moderate degree of graphitization with hydrophilic functionalities. Based on these excellent properties, the CM-PC was used as an electroactive material to fabricate the working electrode and as a metal-free electrocatalyst for HER in a 0.5 M H 2 SO 4 aqueous solution. The resulting CM-PC delivered a superior catalytic activity toward HER with a Tafel slope of ~ 79 mV decade –1 (Overpotential − 166 mV RHE at a current density of − 10 mA cm –2 ) and excellent long-term stability in an acidic medium. Importantly, these fi ndings prove that the chebulic myrobalan (biomass) was turned into an eff ective electrocatalyst for hydrogen generation in the economical route, thereby challenging the uniqueness of platinum catalysts in the hydrogen economy. The result indicates that as-prepared catalysts (CM-PC) have excellent application value in energy and environment.

Green synthesis of nitrogen-doped carbon nanograss for supercapacitors

Atchudan, Raji,Edison, Thomas Nesakumar Jebakumar Immanuel,Perumal, Suguna,Thirukumaran, Periyasamy,Vinodh, Rajangam,Lee, Yong Rok Elsevier 2019 Journal of the Taiwan Institute of Chemical Engine Vol.102 No.-

<P><B>Abstract</B></P> <P>In the present study, a novel N-doped carbon nanograss (NCNG) were synthesized from the used baby-diaper absorbent via carbonization under the argon atmosphere and has been applied as an electroactive material for flexible supercapacitor. The synthesized NCNG display a grass-like morphology with an acceptable degree of graphitization. The surface areas and average pore size of NCNG were 183 m<SUP>2</SUP> g<SUP>−1</SUP> and 3.3 nm, respectively. On the basis of good structural ordering with reasonable surface area, the NCNG was coated on a carbon cloth and studied their electrochemical performance toward the supercapacitors. The obtained quasi-rectangular shaped cyclic voltammetry curves indicate good capacitive behavior of the NCNG. The galvanostatic charge-discharge experimental results showed that the specific capacitance of NCNG was 81 F g<SUP>−1</SUP> at a current density of 0.5 A g<SUP>−1</SUP> with capacitance retention of 95% after 10,000 cycles of charge-discharge. The slow decrements of specific capacitance with the increment of current density indicate superior rate capability of synthesized NCNG. These excellent electrochemical performances of the synthesized NCNG from used (waste) baby-diaper extend their potential applications in various nanoelectronics field. To the best of authors knowledge, first time the NCNG synthesized from the garbage-waste and can extend their synthesis in large-scale.</P> <P><B>Highlights</B></P> <P> <UL> <LI> The first time, N-doped carbon nanograss was synthesized using used baby-diaper. </LI> <LI> The synthesized NCNG is good structural ordering with a reasonable surface area. </LI> <LI> NCNG delivered a high specific capacitance with good capacitance retention. </LI> <LI> In addition, NCNG from used baby-diaper extend their synthesis in large-scale. </LI> <LI> Importantly, the waste diaper derived energy storage is alternative clean energy. </LI> </UL> </P>

Electrocatalytic and energy storage performance of bio-derived sulphur-nitrogen-doped carbon

Atchudan, Raji,Edison, Thomas Nesakumar Jebakumar Immanuel,Perumal, Suguna,Parveen, Asrafali Shakila,Lee, Yong Rok Elsevier 2019 Journal of Electroanalytical Chemistry Vol.833 No.-

<P><B>Abstract</B></P> <P>Sulphur and nitrogen-rich carbon layers (S/N-CLs) have been derived successfully <I>via</I> a simple calcination for high energy applications including supercapacitor and electrocatalytic hydrogen evolution reaction (HER). The flexible working electrode was fabricated using thoroughly analyzed S/N-CLs composite as an active electrode energy material for supercapacitor and HER. The S/N-CLs composite shows a higher specific capacitance of 266Fg<SUP>−1</SUP> at a current density of 0.5Ag<SUP>−1</SUP> and a satisfied cycling stability with 84% capacitance retention even after 5000cycles of galvanostatic charge-discharge. On the other hand, the synthesized S/N-CLs composite was used as an electrocatalyst for HER and it exhibits an excellent HER performance with an onset overpotential of −75mV, and a Tafel slope of 73mVdec<SUP>−1</SUP> in 0.5M H<SUB>2</SUB>SO<SUB>4</SUB> aqueous electrolyte. Also, the S/N-CLs composite displayed good stability and strong durability. The high electrocatalytic activity and stability of S/N-CLs composite toward HER due to the active site of a compound which may originate from the heteroatom-functional groups including N and S in the carbon structure. Overall, the high-performance supercapacitors and enhancing HER based on heteroatom-doped carbon structures could be promising in replacing traditional supercapacitors for many electronic devices and electrocatalyst for HER.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Conversion of <I>Magnolia liliiflora</I> into S/N-CLs composite by a simple carbonization </LI> <LI> S/N-CLs delivered a higher C<SUB>s</SUB> of 266Fg<SUP>−1</SUP> at 0.5Ag<SUP>−1</SUP> with a satisfied stability. </LI> <LI> S/N-CLs exhibits an excellent HER performance with a Tafel slope of 73mVdec<SUP>−1</SUP>. </LI> <LI> This is the first attempt in synthesis of S/N-CLs using <I>Magnolia liliiflora</I> flower. </LI> <LI> S/N-CLs will be an alternative for traditional energy storage material and electrocatalyst. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

An efficient synthesis of graphenated carbon nanotubes over the tailored mesoporous molecular sieves by chemical vapour deposition method

( Raji Atchudan ),주진,( Arumugam Pandurangan ),( Kyungpook National University ),( Anna University ) 한국공업화학회 2014 한국공업화학회 연구논문 초록집 Vol.2014 No.0

Facile green synthesis of nitrogen-doped carbon dots using <i>Chionanthus retusus</i> fruit extract and investigation of their suitability for metal ion sensing and biological applications

Atchudan, Raji,Edison, Thomas Nesakumar Jebakumar Immanuel,Chakradhar, Dasagrandhi,Perumal, Suguna,Shim, Jae-Jin,Lee, Yong Rok Elsevier 2017 Sensors and actuators. B, Chemical Vol.246 No.-

<P><B>Abstract</B></P> <P>Nitrogen-doped carbon dots (N-CDs) were synthesized from <I>Chionanthus retusus (C. retusus)</I> fruit extract using a simple hydrothermal-carbonization method. Their ability to sense metal ions, and their biological activity in terms of cell viability and bioimaging applications were evaluated. The resulting N-CDs were characterized by various physicochemical techniques such as high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and Raman spectroscopy. The optical properties were characterized by ultraviolet visible (UV-vis) fluorescence spectroscopy techniques. The average size of the N-CDs was approximately 5±2nm with an interlayer distance of 0.21nm, as calculated from the HRTEM images. The presence of phytoconstituent functionalities and the percentages of components in the N–CDs were confirmed by XPS studies, and a nitrogen content of 5.3% was detected. The N–CDs demonstrated highly durable fluorescence properties and low cytotoxicity with a quantum yield of 9%. The synthesized N–CDs were then used as probes for the detection of metal ions. The N–CDs exhibited high sensitivity and selectivity towards Fe<SUP>3+</SUP>, with a linear relationship between 0 and 2μM and a detection limit of 70μM. The synthesized N–CDs are anticipated to have diverse biomedical applications, particularly for bioimaging, given their high fluorescence, excellent water solubility, good cell permeability, and negligible cytotoxicity. Finally, the potential of N–CDs as biological probes was investigated using fungal (<I>Candida albicans</I> and <I>Cryptococcus neoformans</I>) strains via fluorescent microscopy. We found that N–CDs were suitable candidates for differential staining applications in yeast cells with good cell permeability, localization with negligible cytotoxicity. Hence, N–CDs may find dual utility as probes for the detection of cellular pools of metal ions (Fe<SUP>3+</SUP>) and also for early detection of opportunistic yeast infections in biological samples.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Durable fluorescent N-CDs prepared using <I>C. Retusus</I> via hydrothermal-carbonization. </LI> <LI> This method of synthesis and N-CDs is an ideal for sensing of Fe<SUP>3+</SUP> and bio-imaging. </LI> <LI> N-CDs was used as a promising fluorescent probe for the direct detection of Fe<SUP>3+</SUP>. </LI> <LI> N-CDs were used as selective probes for yeast <I>C. albicans</I> and <I>C. neoformans</I>. </LI> <LI> N-CDs exhibits selective uptake, good biocompatibility and negligible cytotoxicity. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Synthesis of high-quality carbon nanotubes by using monodisperse spherical mesoporous silica encapsulating iron oxide nanoparticles

Raji Atchudan,차봉근,나스리나론,김재윤,주진 한국화학공학회 2019 Korean Journal of Chemical Engineering Vol.36 No.1

Well-graphitized carbon nanotubes (CNTs) were grown by using monodisperse spherical mesoporous silica encapsulating single iron oxide (Fe3O4) nanoparticles (MSEINPs) as catalytic templates by chemical vapor deposition (CVD) and using acetylene as carbon source. The catalytic templates were synthesized by a sol-gel method. The MSEINPs exhibited better activity and selectivity in CNT synthesis than bare Fe3O4 catalysts. The synthesized multiwall carbon nanotubes (MWCNTs) were analyzed by powder X-ray diffraction (PXRD), thermogravimetric analysis (TGA), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Raman spectroscopy. The carbon deposits are rich in MWCNTs, as confirmed by FESEM and TGA. The wall thickness of the MWCNTs is controlled primarily by the size of the spherical mesoporous silica layer encapsulating the Fe3O4 NPs, while the inner diameter of the CNTs is determined by the size of the Fe3O4 NPs at the center of the MSEINPs. The average diameter of the MWCNTs increased significantly with increases in the growth temperature and acetylene flow rate. The analytical results show that the CNTs prepared on MSEINPs are well graphitized with a narrow size distribution in thickness, and straight and longer tubes are obtained without major defects as compared to the CNTs grown on bare Fe3O4 NPs.

Facile Synthesis of Monodispersed Cubic and Spherical Calcite Nanoparticles in the Presence of Cetyltrimethylammonium Bromide.

Atchudan, Raji,Na, Hyon Bin,Cheong, In Woo,Jool, Jin American Scientific Publishers 2015 Journal of Nanoscience and Nanotechnology Vol.15 No.4

<P>We report the synthesis of monodisperse calcium carbonate (CaCO3) (nano)particles having either a cubic or spherical structure by reacting calcium nitrate with either sodium carbonate or citric acid, respectively, in the presence of cetyltrimethylammonium bromide (CTAB) via the sonication method. For comparison, CaCO3 (nano)particles were synthesized by the same method in the absence of CTAB and also via the standard hydrothermal method using CTAB. The synthesized CaCO3 (nano)particles were analyzed by various physico-chemical characterization techniques such as X-ray diffraction (XRD), Fourier transform infra-red spectroscopy, thermogravimetric analysis, and scanning electron microscopy with energy-dispersive spectrometer. It was found that the CaCO3 (nano)particles were highly pure with high crystallinity and exhibited the calcite polymorph phase as revealed by the XRD analysis. In addition, the analytical results showed that the (nano)particles prepared in the presence of CTAB by the sonication method had high structural ordering and no agglomeration as compared to the (nano)particles prepared by the hydrothermal method. Therefore, our sonication method is a new way to prepare shape-controlled CaCO3 (nano)particles under mild reaction conditions.</P>

Hydrothermal conversion of <i>Magnolia liliiflora</i> into nitrogen-doped carbon dots as an effective turn-off fluorescence sensing, multi-colour cell imaging and fluorescent ink

Atchudan, Raji,Edison, Thomas Nesakumar Jebakumar Immanuel,Aseer, Kanikkai Raja,Perumal, Suguna,Lee, Yong Rok Elsevier 2018 Colloids and Surfaces B Vol.169 No.-

<P><B>Abstract</B></P> <P>The present work illustrates the potential uses of nitrogen-doped multi-fluorescent carbon dots (N-CDs) for Fe<SUP>3+</SUP> sensing, cellular multi-colour imaging, and fluorescent ink. N-CDs were synthesized using <I>Magnolia liliiflora</I> flower by the simple hydrothermal method. The resulted N-CDs was found to be nearly spherical in shape with the size of about 4 ± 1 nm and showed competitive quantum yield around 11%. The synthesized N-CDs with uniform size distribution and high content of nitrogen and oxygen-bearing functional groups exhibit excellent dispersibility in aqueous media. The N-CDs were able to detect a high concentration of Fe<SUP>3+</SUP> ions (1–1000 μM) with a limit of detection is about 1.2 μM by forming N-CDs-Fe<SUP>3+</SUP> complex due to the functional groups such as nitrogen, carbonyl and carboxyl on the surface of N-CDs. Thus they could be used to remove pollutants from industrial wastewater. The electronic charge on the surface of the N-CDs and N-CDs-Fe<SUP>3+</SUP> complex (zeta potential) is around −36 and 18 mV, respectively. In addition, these N-CDs show excitation-dependent fluorescence that was utilized for multi-colour in vitro cellular imaging in rat liver cells (<I>Clone 9 hepatocytes</I>). The N-CDs are rapidly uptake in the cell cytoplasm and showed high cytocompatibility on cellular morphology. Moreover, as the N-CDs possess strong fluorescence and anti-coagulation they could be utilized in fluorescent ink pens.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Hydrothermal conversion of <I>M. liliiflora</I> into N-CDs by one-pot hydrothermal method. </LI> <LI> N-CDs was applied as a fluorescent probe for the effective detection of Fe<SUP>3+</SUP> ions. </LI> <LI> N-CDs could offer a multi-colour cell imaging without any chemical modification. </LI> <LI> N-CDs was used as a fluorescent ink without any pretreatment of the sample. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>N-CDs were synthesized using <I>M. liliiflora</I> flower and were potentially utilized for the detection of Fe<SUP>3+</SUP> ions, multi-colour cellular imaging and fluorescent ink.</P> <P>[DISPLAY OMISSION]</P>