Research Outputs

Now showing 1 - 10 of 73
  • Publication
    Enhanced Photocatalytic Efficacy and Stability in Antibiotic Pollution Mitigation Using BiVO4 Nanoballs Encased in Ultrathin Polymeric g-C3N4 Nanocomposites under Visible Light Exposure
    (ACS Publications, 2024) ;
    Govinda raj, Muniyandi
    ;
    Sundaram-Ganeshraja, Ayyakannu
    ;
    Kaviyarasan, Kulandaivelu
    ;
    Pugazhenthiran, Nalandhiran
    ;
    Katayama, Kenji
    ;
    Theja-Vaskuri, Chandra
    ;
    Bosco, Aruljothy
    ;
    Neppolian, Bernaurdshaw
    Antibiotic overuse and indiscriminate disposal ultimately lead to overexploitation of the ecosystems expanding requirements, producing significant environmental and biological consequences. Advanced oxidation processes (AOPs) have kindled the interest of many researchers in targeting the destruction of antimicrobial and waterborne pollutants. As a result, an improvement of low-cost, high-efficiency photocatalysts for the successful decomposition of antibiotics is critical for the cleaning of harmful contaminants in rivers and lakes. In the current work, a simple hydrothermal approach was used to create the bismuth vanadate nanoballs (BiVO4) anchored to the exterior of the ultrathin g-C3N4.It was named g-C3N4/BiVO4(X) (X = 5, 10, 15, and 20%) nanocomposites, and the photocatalytic removal of ciprofloxacin (CPX) and amoxicillin (AMX) was investigated using synthesized composites. According to the advanced characterization techniques, the synthesized composites exhibit superior purity and crystalline nature. The electron transfer occurring within the g-C3N4, in conjunction with the extension of BiVO4 nanoballs, enhances the generation of photoexcited electron−hole (e−/h+) pairs. This phenomenon contributes significantly to the improved photocatalytic activity observed in the g-C3N4/BiVO4 system. Furthermore, the photocatalytic efficiency exhibited by g-C3N4/BiVO4(10%) nanocomposites in antibiotic removal surpasses that of both bare materials and other composite counterparts. The elimination of antibiotics was aided by reactive oxygen species (ROS)such as O2•−, h+, and OH. Finally, g-C3N4/BiVO4(10%), the intermediate byproduct of CPX and AMX decomposition, was discovered, and a probable CPX and AMX removal route was postulated. The g-C3N4/BiVO4(10%) composite exhibits long-term stability after five cycles. This study applies a green and ecologically responsive technique to the development of high-performance photocatalysts for wastewater remediation.
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    Publication
    Impact of Copper(II)-Imidazole complex modification on Polycrystalline TiO2: Insights into formation, characterization, and photocatalytic performance
    (MDPI, 2024) ;
    Ayyakannu-Sundaram, Ganeshraja
    ;
    Kanniah, Rajkumar
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    Anbalagan, Krishnamoorthy
    ;
    Kulandaivelu, Kaviyarasan
    Micrometer-sized polycrystalline anatase particles are widely used in materials and life sciences, serving as essential components in photocatalytic materials. The ability to tailor their composition, shape, morphology, and functionality holds significant importance. In this study, we identified and examined the non-destructive route of Copper(II) implantation at the surface of polycrystalline TiO2. The [Cu(en)(Im)2]2+ complex ion demonstrated a remarkable affinity to concentrate and bind with the semiconductor’s surface, such as anatase, forming a surface-bound adduct: ≡TiO2 + [Cu(en)(Im)2]2+ → ≡TiO2//[Cu(en)(Im)2]2+. The misalignment of Fermi levels in TiO2//[Cu(en)(Im)2]2+ triggered electron transfer, leading to the reduction of the metal center, releasing Copper(I) in the process. Although less efficient, the released Copper(I) encountered a highly favorable environment, resulting in the formation of the surface complex TiO2:CuIIsc. The implanted Cu(I) was converted back into Cu(II) due to re-oxidation by dissolved oxygen. The penetration of the metal ion into the surface level of the polycrystalline TiO2 lattice was influenced by surface residual forces, making surface grafting of the Cu(II) ion inevitable due to surface chemistry. FTIR, UV–vis, Raman, XRD, EPR, and surface morphological (SEM, EDAX, and HRTEM) analyses identified the typical surface grafting of the Cu(II) cluster complex on the anatase surface matrix. Moreover, the XRD results also showed the formation of an impure phase. The TiO2 polycrystalline materials, modified by the incorporation of copper complexes, demonstrated an enhanced visible-light photocatalytic capability in the degradation of Rhodamine B dye in aqueous solutions. This modification significantly improved the efficiency of the photocatalytic process, expanding the applicability of TiO2 to visible light wavelengths. These studies open up the possibility of using copper complexes grafted on metal oxide surfaces for visible-light active photocatalytic applications. Moreover, this investigation not only showcases the improved visible-light photocatalytic behavior of copper-modified TiO2 polycrystalline materials, but also underscores the broader implications of this improvement in the advancement of sustainable and efficient water treatment technologies.
  • Publication
    Building a novel noble metal-free Cu3P/ZnS/g-C3N4 ternary nanocomposite with multi interfacial charge transfer pathways for highly enhanced photocatalytic water splitting
    (Elsevier, 2024) ;
    Rameshbabu, R.
    ;
    Siaw Paw, Johnny Koh
    ;
    Kaviyarasan, Kulandaivelu
    ;
    Jadoun, Sapana
    ;
    Amalraj, John
    ;
    Kiong, Tiong Sieh
    For renewable energy, it is crucial to create effective photocatalysts with enhanced photo charge separation and transfer to produce photocatalytic hydrogen (H2) efficiently utilizing light energy. Due to their distinct qualities and features, carbonaceous materials have so far been shown to be high-performance co-catalysts to substitute some conventionally costly metal materials in photocatalytic water splitting. Here, a novel ternary nanocomposite, simple hydrothermal process ball milling assisted and wet impregnation approach, a promising ternary nanocomposite is created as an efficient solar light driven photocatalyst. Utilizing a variety of analytical techniques, 3 % Cu3P/ZnS/g-C3N4 nanocomposites as catalysts were characterized in order to check the hydrogen production and investigate their structural properties. The hydrogen production capability of the catalyst is studied by irradiating Na2SO3 + Na2S solutes using a halogen bulb (250 W). The results demonstrated that in terms of photocatalytic activity towards H2 production, 3 % Cu3P/ZnS/g-C3N4 catalyst performed better than 3 % Cu3P/ZnS, Cu3P, ZnS, and g-C3N4. A composite containing 7.5 wt% g-C3N4 demonstrated exceptional durability during photocatalytic hydrogen production, resulting in a 23,086 mol h− 1 g− 1 rate. Higher stability in electron-hole pairs created a higher absorption level of solar light could be responsible for this remarkable performance.
  • Publication
    Rationalizing Fe-Modified TiO2 through doping, composite formation, and single-phase structuring for enhanced photocatalysis via inter- and intra-charge transfers
    (Elsevier, 2024) ;
    Sivakumar, Bharathkumar
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    Vijayarangan, R.
    ;
    Mohan, Sakar
    ;
    Ilangovan, R.
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    Amin, Mohammed
    ;
    Vyas, Shweta
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    El-Bahy, Zeinhom
    This study sheds light on how the properties of titanium dioxide (TiO2) are influenced when it is modified with iron (Fe), leading to the formation of Fe-doped-TiO2, Fe2O3-TiO2 composite, and single-phase FeTiO3 systems. The structural formation of the materials, oxidation state, and chemical environments of the elements are analyzed using XRD and XPS techniques. Band structures with UV–visible light driven properties and suitable redox potentials with improved recombination resistance along with an active inter- and intra-charge transfers were observed for Fe2O3-TiO2 and FeTiO3 systems. The photocatalytic efficiency was found to be superior for FeTiO3 system, degrading ~97 and 100 % of phenol, malachite green and rhodamine B dyes in 150 min, respectively along with enhanced recyclability. Interestingly, a competitive S- and Z-scheme was predicted for Fe2O3-TiO2 composite, explaining its photocatalytic mechanism. The scavenger and total organic carbon analyses revealed the radicals driving the photocatalytic reactions and the nature of degradation products, respectively.
  • Publication
    Exploring the antimicrobial activity of hydrothermally synthesized copper pyrophosphate nanoflakes
    (Elsevier BV, 2024)
    Aswini, Ravi
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    Manivannan, Nandhagopal
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    Padmanaban, Annamalai
    ;
    ;
    Dhandapani, Kathirvelu
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    SaravanaVadivu, Arunachalam
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    Rameshkumar, Perumal
    ;
    Hajinur Hirad, Abdurahman
    In recent years, infections and the escalating resistance to antimicrobial drugs have emerged as significant health concerns. Due to their remarkable effectiveness and minimal potential for bacteria to develop resistance, copper-based nanomaterials are being considered as prospective alternatives to conventional antibiotics. In this study, copper pyrophosphate nanoflakes were synthesized using a simple hydrothermal technique with an inorganic phosphate source. These nanoflakes, characterized by a high aspect ratio, exert a substantial impact on bacterial cell walls, effectively eliminating microbial pathogens. X-ray diffraction (XRD) analysis confirmed the monoclinic phase of the copper pyrophosphate nanomaterial, while the band gap energy of 2.7 eV was estimated from the Tauc plot. Additionally, the antimicrobial efficacy of Cu2P2O7 was evaluated against various gram-negative, gram-positive, and fungal pathogens at different concentrations. Notably, all tested bacterial strains exhibited moderate antimicrobial effects at concentrations of 5 mg/mL. For instance, S. aureus and E. coli displayed a 13 mm zone of inhibition, demonstrating excellent activity and lower cytotoxicity. These findings underscore the potential of Cu2P2O7 as a promising candidate for the development of novel drugs targeting pathogenic bacteria affecting human health.
  • Publication
    Praseodymium doping-induced band structure tunning in bismuth ferrite (Bi1-Pr FeO3) nanofibers for the enhanced photocatalytic properties
    (Elsevier, 2024) ;
    Bharathkumar, S.
    ;
    Sakar, M.
    ;
    Balakumar, S.
    The study investigates the influence of praseodymium (Pr) doping on bismuth ferrite (BiFeO3/BFO) nanofibers and their structural, morphological, magnetic, optical, and photocatalytic properties. A series of bismuth ferrite nanofibers with varying concentration of Pr (Bi1-xPrxFeO3, x = 0.00, 0.05, 0.10, and 0.15 mol%) were successfully synthesized using an electrospinning technique. XRD patterns revealed that structural transformation occurred from rhombohedral to orthorhombic upon effective doping of Pr3+ into BFO nanofibers. The X-ray photoelectron spectroscopy analysis confirmed that Bi, Fe, and O maintained their native oxidation states of +3 and -2, respectively in the bare and doped systems. Furthermore, the optical band gap value was significantly reduced from 2.35 to 2.22 eV as well as the recombination rates of charge carriers in the doped systems, especially in BP0.15O system. The photocatalytic performance of the prepared samples was studied by measuring the decomposition of rhodamine B (RhB) under sunlight irradiation. Outcomes showed that the doped-BFO nanofibers exhibited enhanced photocatalytic performance compared to pure BFO, with the BP0.15O system showing the 98 % degradation in 60 min. This enhancement could be attributed to the presence of Pr-energy levels, which facilitating enhanced separation, and charge transfer to the surface for the effective redox reactions.
  • Publication
    Morphological impact of Perovskite-Structured Lanthanum CobaltOxide (LaCoO3) nanoflakes toward supercapacitor applications
    (ACS Publications, 2024) ;
    Moorthi, Kanmani
    ;
    Sivakumar, Bharathkumar
    ;
    Chokkiah, Bavatharani
    ;
    Mohan, Sakar
    In this study, perovskite-structured lanthanum cobalt oxide(LaCoO3/LCO) systems with particle and flake morphologies were developed using sol−gel and hydrothermal methods, respectively, in order to investigate their morphological structure-dependent properties for potential supercapacitor applications. The structural analysis confirms that both methods yield LaCoO3with improved crystalline properties. The energy storage performance of the developed materials is studied in a three-electrode configuration using a 1 MKOH electrolyte. The results indicated superior electrochemical performance for the LCO nanoflakes, exhibiting specific capacitances of ∼215 F g−1 at a scan rate of 5 mV s−1 and ∼136 F g−1 at a current density of 1 A g−1. In comparison, the LCO nanoparticles showed ∼119 F g−1 at a scan rate of 5 mV s−1 and ∼99F g−1 at a current density of 1 A g−1. This difference can be largely attributed to their respective morphologies, porous structures, and surface defects. Further, the nanoflakes demonstrated an exceptional capacitance retention of ∼97% even after 5000 charge−discharge cycles. The findings of this study suggest that the properties of perovskite LaCoO3 can be tuned by adjusting its morphology through various synthesis methods, making LaCoO3 a viable and robust system for energy storage applications.
  • Publication
    Carbon Dots: A multifunctional nano-sized giant tool forthe detection probe and physical reformation of NiMoO 4 inSolid-State for enriched energy storage application
    (Wiley, 2024) ;
    Annamalai, Arun
    ;
    Annamalai, Kumaresan
    ;
    Ayyanduarai, Nagarajan
    ;
    Ravichandran, Ramya
    ;
    Annamalai, Padmanaban
    ;
    Elumalai, Sundaravadivel
    Designing low-cost, effective and greener materials via a non-sophisticated strategy is most important for future research. Here, they made a new dual endeavor using carbon dots (CDs) as an environment protection probe for selective detection of environmental toxins, followed by the solid-state structural reformer to prepare NiMoO4 (NM) via mechanochemical-based solid grinding method. The prepared CDs, NM and NM-CDs combination is examined through various techniques. The prepared CDs selectively detect Cr6+, Ru3+, and Doxycycline independently. Also, in this work, a groundbreaking strategy is found to prepare morphology-tailored NM using CDs through a solid-state grinding method without adding any other toxic solvents or reagents. The CDs-induced NM-CDs (15) look like a 2D nano-sheet with enriched surface area compared to its bare NM. The fabricated electrode provides the highest capacitance value of 1947 F g−1, almost three times grander than the bare 1D rod-like electrode. Then, fabricated asymmetric supercapacitor NM-CDs (15)//AC system delivers a high energy density of 43.9 Wh Kg−1 at a power density of 684 W Kg−1. Overall, a single CDs serve multiple roles in the environment and energy applications with a greener structure tailoring agent and a better booster for re energy storage properties.
  • Publication
    Construction novel highly active photocatalytic H2 evolution over noble-metal-free trifunctional Cu3P/CdS nanosphere decorated g-C3N4 nanosheet
    (Elsevier, 2024) ;
    Rameshbabu, R.
    ;
    Paw-Koh, Siaw
    ;
    Kaviyarasan, Kulandaivelu
    ;
    Tak-Yaw, Chong
    ;
    Kiong-Tiong, Sieh
    ;
    Benedict, F.
    ;
    Yusaf, Talal
    ;
    Kadirgama, K.
    ;
    Pasupuleti, Jagadeesh
    Hydrogen energy possesses immense potential in developing a green renewable energy system. However, a significant problem still exists in improving the photocatalytic H2 production activity of metal-free graphitic carbon nitride (g-C3N4) based photocatalysts. Here is a novel Cu3P/CdS/g-C3N4 ternary nanocomposite for increasing photocatalytic H2 evolution activity. In this study, systematic characterizations have been carried out using techniques like X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HR-TEM), Raman spectra, UV–Vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy (XPS), surface area analysis (BET), electrochemical impedance (EIS), and transient photocurrent response measurements. Surprisingly, the improved 3CP/Cd-6.25CN photocatalyst displays a high H2 evolution rate of 125721 μmol h− 1 g− 1. The value obtained exceeds pristine g-C3N4 and Cu3P/CdS by 339.8 and 7.6 times, respectively. This could be the maximum rate of hydrogen generation for a g–C3N4–based ternary nanocomposite ever seen when exposed to whole solar spectrum and visible light (λ > 420 nm). This research provides fresh perspectives on the rational manufacture of metal-free g-C3N4 based photocatalysts that will increase the conversion of solar energy. By reusing the used 3CP/Cd/g-C3N4 photocatalyst in five consecutive runs, the stability of the catalyst was investigated, and their individual activity in the H2 production activity was assessed. To comprehend the reaction mechanisms and emphasise the value of synergy between the three components, several comparison systems are built.
  • Publication
    Tailored engineering of rod-shaped core@shell ZnO@CeO2 nanostructures as an optical stimuli-responsive in sunscreen cream
    (Elsevier, 2024) ;
    Sahlevani, Saeed
    ;
    Pandiyarajan, Thangaraj
    ;
    Arulraj, Arunachalam
    ;
    Sanhueza, Felipe
    ;
    Contreras, David
    ;
    Gracia-Pinilla, M.
    ;
    Mangalaraja, Ramalinga
    The catalytic efficiency of the materials can be boosted with the selective designing (nanostructures) including the core@shell which aids in attaining the separation of photoinduced charge carriers. However, to effectively separate the carriers and reduce the rate of recombination, tuning the thickness of the shell wall is a vital one. The one-dimensional (1D) rod-like shell wall-controlled ZnO@CeO2 core@shell structures were successfully prepared via co-precipitation and hydrothermal methods using the hexamethylenetetramine (HMTA) as a reagent. The CeO2 shell wall thickness was fine-tuned between 15 and 70 nm with a variation in the concentration of HMTA reagent. The results revealed that the concentration of HMTA played a significant role in the formation of ZnO@CeO2 core@shell structures and in tuning their thickness. The FE-SEM images evidenced the core-shell structures formation with the specific thickness and uniformity. The HR-TEM images confirmed the homogeneity and regular form of the shell thickness. The unit cell and crystallite size were identified from the XRD analysis. The constructed core-shell structures were further employed in the formula of the prototypes of sunscreen and their photoprotective performance was analyzed in the view to cut the solar light irradiation in a new sunscreen formulation. The developed core-shell ZnO@CeO2 structures showed the excellent optical absorption in both the UV as well as visible regions.