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Item Kinetic and thermodynamic studies on the adsorption of heavy metals from aqueous solution by melanin nanopigment obtained from marine source: Pseudomonas stutzeri(Academic Press, 2018) Manirethan, V.; Raval, K.; Rajan, R.; Thaira, H.; Mohan Balakrishnan, R.M.The difficulty in removal of heavy metals at concentrations below 10 mg/L has led to the exploration of efficient adsorbents for removal of heavy metals. The adsorption capacity of biosynthesized melanin for Mercury (Hg(II)), Chromium (Cr(VI)), Lead (Pb(II)) and Copper (Cu(II)) was investigated at different operating conditions like pH, time, initial concentration and temperature. The heavy metals adsorption process was well illustrated by the Lagergren's pseudo-second-order kinetic model and the equilibrium data fitted excellently to Langmuir isotherm. Maximum adsorption capacity obtained from Langmuir isotherm for Hg(II) was 82.4 mg/g, Cr(VI) was 126.9 mg/g, Pb(II) was 147.5 mg/g and Cu(II) was 167.8 mg/g. The thermodynamic parameters revealed that the adsorption of heavy metals on melanin is favorable, spontaneous and endothermic in nature. Binding of heavy metals on melanin surface was proved by Fourier Transform Infrared Spectroscopy (FT-IR) and X-ray Photoelectron Spectroscopy (XPS). Contemplating the results, biosynthesized melanin can be a potential adsorbent for efficient removal of Hg(II), Cr(VI), Pb(II) and Cu(II) ions from aqueous solution. © 2018 Elsevier LtdItem Melanin nano-pigments for heavy metal remediation from water(Taylor and Francis Inc. 325 Chestnut St, Suite 800 Philadelphia PA 19106, 2019) Thaira, H.; Raval, K.; Manirethan, V.; Mohan Balakrishnan, R.M.Melanins are water insoluble polyphenol compounds. The metal ion chelating property of natural melanin is exploited for removal of heavy metals from contaminated water. We optimized biosynthesis of melanin from marine bacterium using different growth media, media components, and operating conditions. Optimized medium yielded 513 mg/L melanin at 36 h of incubation, which was 3.15 times higher than the yield before optimization. Particle size analysis of the biosynthesized melanin indicated a size of 32 ± 0.98 nm. Preliminary investigation indicated that melanin nanoparticles could adsorb different heavy metals such as chromium, selenium, and lead from very low initial concentrations. © 2018, © 2018 Taylor & Francis.Item Adsorption of ibuprofen using cysteine-modified silane-coated magnetic nanomaterial(Springer, 2019) Kollarahithlu, S.C.; Mohan Balakrishnan, R.M.Industrialization and growth of the pharmaceutical companies have been a boon to the mankind in our day to day life in myriad ways. However, due to the uninhibited release of these active pharmaceutical compounds into the water systems has caused detrimental effects to the genetic pool. In this study, l-cysteine-modified 3-glycidyloxypropyltrimethoxysilane-coated magnetic nanomaterial showed a maximum removal of the efficiency of 82.90% for the nanomaterial dosage of 30 mg at an initial concentration of 50 mg L?1 at pH 6.0. Further, the nanomaterial showed reusability efficiency up to 80% for three cycles. The adsorption kinetics follow the pseudo-second-order reaction and the adsorption isotherm model best fits the Langmuir isotherm proving the adsorption process to be a monolayer sorption on a monolayer surface. This magnetic nanomaterial could serve as a promising tool for the removal of pharmaceutical compounds from aqueous solutions. [Figure not available: see fulltext.]. © 2018, Springer-Verlag GmbH Germany, part of Springer Nature.Item Adsorptive removal of trivalent and pentavalent arsenic from aqueous solutions using iron and copper impregnated melanin extracted from the marine bacterium Pseudomonas stutzeri(Elsevier Ltd, 2020) Manirethan, V.; Raval, K.; Mohan Balakrishnan, R.M.The metalloid arsenic is one of the most conspicuous groundwater contaminants in the Indian subcontinent and its removal from aqueous medium is the main focus of this study. The study aims at functionalising melanin using iron and copper for the efficient removal of arsenic and rendering water fit for consumption. Melanin obtained from the marine bacteria Pseudomonas stutzeri was functionalised by iron impregnation (Fe-melanin) and copper impregnation (Cu-melanin). Morphological studies using FESEM portrayed the impregnated iron and copper granules on the surface of melanin, while XRD analysis confirmed the presence of Fe2O3 and CuO on melanin. Adsorption studies on As (V) and As (III) were conducted using Fe-melanin and Cu-melanin for different operating variables like pH, temperature and contact time. More than 99% per cent of As (III) and As (V) from water was removed at a pH range between 4 and 6 within 50 min in the case of Fe-melanin and 80 min for Cu-melanin. Adsorption equilibrium studies showed better fit with Langmuir adsorption isotherm and had good agreement with Redlich-Peterson's three-parameter model. The maximum adsorption capacities of Fe-melanin and Cu-melanin obtained from Langmuir adsorption model are 50.12 and 20.39 mg/g, respectively, for As (V) and similarly 39.98 and 19.52 mg/g, respectively, for As (III). Arsenic-binding to the functionalised melanin was confirmed using FT-IR and the XPS analysis. Reuse of the adsorbent was effectively done by desorbing the iron and copper together with the bound As (III) and As (V) and further re-impregnation of iron and copper in melanin. Re-functionalised melanin showed 99% adsorption efficiency up to four cycles of adsorption/desorption. A novel iron and copper impregnated melanin was synthesized to remove As (III) and As (V) from groundwater and the adsorption process was optimized. © 2019 Elsevier LtdItem Batch and continuous studies on the removal of heavy metals from aqueous solution using biosynthesised melanin-coated PVDF membranes(Springer, 2020) Manirethan, V.; Gupta, N.; Mohan Balakrishnan, R.M.; Raval, K.Heavy metals like mercury, chromium, lead and copper present in groundwater at lower concentrations cause severe health issues and can even be fatal when consumed. The biopigment/biopolymer melanin can be reaped from different sources like bacterium, fungus, and human hair. It has excellent heavy metal ion scavenging property and can be exploited for non-biological applications, substantially including water purification. In this work, melanin nanoparticles were derived from the marine bacterium Pseudomonas stutzeri and were coated onto hydrophobic polyvinylidene fluoride (PVDF) membrane as a support, for batch and continuous removal of heavy metal studies. Batch studies on the effect of pH, temperature and adsorbate dose and continuous adsorption studies on the effect of flow rate, adsorbate and adsorbent mass loadings were carried out by using biosynthesised melanin-coated PVDF membranes for the removal of Hg(II), Cr(VI), Pb(II) and Cu(II). Scanning electron microscope (SEM) images revealed the surface morphology, Fourier-transform infrared spectroscopy (FTIR) and energy-dispersive X-ray spectroscopy (EDS) deciphered the chemical characteristics of melanin-coated PVDF membranes before and after adsorption. Contact angle measurement confirmed the improvement in hydrophilicity of PVDF membrane upon coating with melanin. The maximum removal percentages of heavy metals achieved by melanin-coated PVDF membranes under batch mode operation were 87.6%, 88.45%, 91.8% and 95.8% for mercury, chromium, lead and copper, respectively optimised at 318 K and pH of 3 for chromium and 5 for other metals. However, the continuous mode of operation with a flow rate of 0.5 mL/min having 1 mg/L of heavy metal solution concentration exposed to 50 mg of melanin loading with a working volume of 200 mL showed better removal efficiencies compared with batch mode. The dynamic studies using Thomas and Yoon–Nelson models described the transient stage of the breakthrough curve and the model constants were calculated for column design and scale-up. © 2019, Springer-Verlag GmbH Germany, part of Springer Nature.Item Adsorption of pharmaceuticals pollutants, Ibuprofen, Acetaminophen, and Streptomycin from the aqueous phase using amine functionalized superparamagnetic silica nanocomposite(Elsevier Ltd, 2021) Chandrashekar Kollarahithlu, S.; Mohan Balakrishnan, R.M.Pharmaceuticals are one of the emerging pollutants that pose a severe threat to the aquatic habitats, which in turn affects other species in the biosphere. The superparamagnetic based silica nanocomposites modified with aminosilane were characterized for their physicochemical properties and also the purity of the nanocomposite obtained was determined. The adsorptive properties of the nanocomposites were investigated for the removal of pharmaceutical pollutants such as Ibuprofen, Acetaminophen, and Streptomycin from aqueous solutions. The adsorption process of pharmaceuticals was found to reach equilibrium within the first 15 min reporting high removal efficiency of up to 97% for Ibuprofen (IBF) followed by (94%) acetaminophen (ACE) and (70%) streptomycin (STR) for a concentration of 12 mg L?1. The adsorption process was found to follow the pseudo-second-order kinetics and fits well with the Langmuir isotherm model, confirming the adsorption on to the homogenous surface of the nanocomposite. The amine functional groups formed on the nickel ferrite nanocomposites by coating aminopropyltrimethoxysilane (APTS) were observed to aid the adsorption process. The adsorption capacity of the nanocomposites varies for IBF, ACE, and STR as 59, 58, and 49 mg g?1 at pH 7.0, 6.0, and 5.0, respectively. The amine coated magnetic nanocomposite also showed excellent regeneration capacity for up to four cycles and can be a promising adsorbent, especially for removing of pharmaceutical pollutants from aqueous streams. © 2021 Elsevier LtdItem Nano-Clay and Iron Impregnated Clay Nanocomposite for Cu2+ and Pb2+ Ions Removal from Aqueous Solutions(SAGE Publications Ltd, 2022) Tarekegn, M.M.; Mohan Balakrishnan, R.M.; Hiruy, A.M.; Hussen, A.H.; Maanyam, H.S.Several physicochemical techniques have been widely studied for heavy metals removal despite most of them are associated with challenges of higher cost, accessibility, and complex technical feasibility. In this study, nano-sorbent materials were developed from a naturally available clay matrices and its heavy metals (Cu2+ and Pb2+) removal capacity was tested at its pristine and iron impregnated form. Both top to down and borohydride reduction methods were used to produce the nano-sorbents. The nano-sorbents were characterized by XRD, XRF, SEM, FTIR, BET, and TGA/DGA. The sorption was studied in batch experiments. The surface area, pore-volume, and pore diameter of nano-clay were found 43.49 m2/g, 0.104 cm3/g, and 2.81 nm, respectively while iron impregnated nano-clay has shown a surface area (73.11 m2/g), pore-volume (0.153 m3/g), and pore diameter (3.83 nm). Both nanoparticles have shown a mesoporous nature. The highest Cu2+ and Pb2+ removal capacity of nano-clay was 99.2% (~11.9 mg/g) and 99.6% (~11.95 mg/g), respectively. Whereas, the iron impregnated nano-clay has achieved the highest Cu2+ and Pb2+ removal efficiency 99.8% (~11.97 mg/g) and 99.7% (11.96 mg/g), respectively. The highest Cu2+ adsorption efficiency of iron impregnated nanoclay was achieved at pH 5.0, adsorbent dose 0.83 g/L, contact time 150 minutes, and Cu2+ initial concentration 4 ppm while its highest Pb2+ adsorption activity was achieved at pH 5.0, contact time (90 minutes), Pb2+ initial concentration (6 ppm), and the adsorbent dose (0.67 g/L). Whereas, the Cu2+ adsorption using nano-clay was highest at pH 5.0, contact time (180 minutes), adsorbent dose (1.0 g/L), and Cu2+ initial concentration (2 ppm). While, pH 5.0, contact time (90 minutes), adsorbent dose (0.83 g/L), and Pb2+ initial concentration (4 ppm) was found to the conditions of highest Pb2+ removal. In all cases, the pseudo-second-order kinetics indicated the presence of chemisorption. Langmuir adsorption characteristics has been reflected on Pb2+ and Cu2+ removal activities of the nanoclay and iron impregnated nanoclay, respectively. Whereas, Freundlich isotherm model was better fitted for Cu2+ adsorption activity of the nanoclay. The −ΔG (<−20 KJ/mol), +ΔH°, and +ΔS° have shown a spontaneous and endothermic adsorption activity with a high level of adsorbents disorder. In general, the result of iron impregnated nano-clay has shown a promising result for the removal of Cu2+ and Pb2+ aqueous solution. © The Author(s) 2022.Item Adsorption of selective fluoroquinolones by cysteine modified silane magnetic nanocomposite from the aqueous phase(Institute for Ionics, 2023) Senathiraja, T.; Lolla, S.A.; Singh, Y.; Kollarahithlu, S.C.; Mohan Balakrishnan, R.M.Elevated levels of pharmaceutical pollutants in the aquatic environment have caused detrimental effects on water quality and biodiversity. Nanomaterials are among the most promising technologies to detect, adsorb, and remove these pollutants from the aqueous systems. The current work explores the applicability of nickel ferrite nanocomposite functionalized with L-cysteine attached 3-glycidyloxypropyltrimethoxysilane to remove a selective class of antibiotics known as fluoroquinolones (Lomefloxacin, Ciprofloxacin, and Norfloxacin). 20 mg of this nanocomposite achieve maximum removal efficiencies of 61%, 67%, and 75% for 40 mg L−1 of lomefloxacin, norfloxacin, and ciprofloxacin, respectively. The nanocomposites also show good regeneration capacity with negligible reduction in the efficiencies up to three cycles. Furthermore, adsorption isotherms such as Langmuir and Freundlich isotherms were used to characterize the removal of fluoroquinolones from the aqueous phase by the nanocomposites. The results show that the adsorption process was in good agreement with the Langmuir isotherm, thus confirming its monolayer sorption process and also reveals that adsorption kinetics follows a pseudo-second-order model. The maximum adsorption capacity of functionalized nickel ferrite nanocomposites are 122 mg g−1, 135 mg g−1, and 150 mg g−1 for lomefloxacin, norfloxacin, and ciprofloxacin, respectively. Overall, all the results obtained indicate that the nickel ferrite nanocomposite functionalized with L-cysteine attached 3-glycidyloxypropyltrimethoxysilane is an effective adsorbent to remove fluoroquinolones from the aqueous systems and could be potentially incorporated in water treatment processes under well-defined parameters. © 2022, The Author(s) under exclusive licence to Iranian Society of Environmentalists (IRSEN) and Science and Research Branch, Islamic Azad University.Item Amino acid functionalized metal oxide nanocomposite for the removal of fluoroquinolones(Elsevier Ltd, 2023) Ilango, I.; Mohan Balakrishnan, R.M.Antibiotic consumption has increased globally, and its discharge into water bodies at concentrations ranging from a few ng/L to mg/L has a detrimental effect on the ecosystems. Amino acid functionalized nickel ferrite nanoparticles were chosen to improve the stability of bare nanoparticles and prevent oxidation and leaching ions in nanoparticles thereby targeting the antibiotics in the contaminated water bodies. The removal of ciprofloxacin and lomefloxacin hydrochloride in the aqueous phase was investigated using a hydrothermally synthesized L-Leucine functionalized nickel ferrite nanocomposite (NFO@L). Various analytical techniques were used to analyze L-Leucine functionalized nickel ferrite, and the nanocomposite's average particle diameter was determined to be between 11 and 15 nm. The maximal measured zeta potential was −21.5 mV. Fourier transform infrared spectroscopy (FTIR), ninhydrin assay and X-ray diffraction (XRD) analysis confirmed the attachment of L-Leucine onto nickel ferrite. The nanocomposite's surface-to-volume ratio was calculated to be 92.916 m2/g. The S-shaped curve from the vibrating sample magnetometer analysis reflected the superparamagnetic behaviour of the nanocomposite with a saturation magnetization of 0.665 emu/g. Various parametric experiments were conducted, in which 93.549% ciprofloxacin was removed in 120 min at 303 K, pH 8 and NFO@L dosage of 100 mg in 100 mL whereas 75.192% lomefloxacin hydrochloride was removed in 140 min at 333 K, pH 9 and NFO@L dosage of 70 mg in 100 mL. The plot of experimental datum in kinetic and isotherm studies fitted well with the Pseudo second order kinetic model and Langmuir isotherm. There was no evidence of iron ions leaching from the final analyte. The recycle and regeneration studies showed good stability with a small reduction after four cycle runs. Based on these findings, the Leucine functionalized nickel ferrite nanocomposite could be a potent adsorbent for the removal of low-concentrated ciprofloxacin and lomefloxacin hydrochloride in the wastewater. © 2023Item Functionalization of β-cyclodextrin onto NiFe2O4 nanoparticles for the removal of ketoprofen and diclofenac from the aqueous solutions(Institute for Ionics, 2024) Ilango, I.; Mohan Balakrishnan, R.M.; Visvanathan, C.; Bui, X.-T.; Velusamy, P.A new β-CD functionalized nickel ferrite nanocomposite was synthesized and used to remove pharmaceutical drugs, such as ketoprofen (KF) and diclofenac (DCF). The co-precipitation approach was utilised to synthesize nickel ferrite (NFO) nanoparticles, which were then functionalized with TEOS to form NFO@SiO2; β-cyclodextrin was then functionalized using GPTMS as an interface to form NFO@SiO2@β-CD. FTIR, ZD, FE-SEM, EDX, TGA/DTG, VSM, BET, zeta potential and particle size analysis were then used to characterise the nanocomposites. The NFO@SiO2@β-CD has an average diameter of 109.1 nm, superparamagnetic behaviour, a mesoporous surface and a specific surface of 20.78 m2/g. The functionalized NFO@SiO2@ β-CD nanocomposite removed 94% of diclofenac in 5 min and 80% of ketoprofen in 360 min with the adsorption capacities of 8.46 and 0.54 mg/g, respectively. The obtained experimental datum for both the pollutants was fitted in kinetic and isotherm models, with the pseudo-second-order kinetic model and Freundlich adsorption isotherm showing the best fit with the highest regression of R 2 = 0.99. The nanocomposite was regenerated using 0.1 M NaOH and recycled for about four consecutive cycles in which the reduction in the removal efficiency of ketoprofen and diclofenac was observed to be 51.36% and 64%, respectively. These results suggested that the NFO@SiO2@β-CD nanocomposite could be used specifically to target the low-concentrated pharmaceutical pollutants. Graphical Abstract: Schematic representation of Functionalization of β-Cyclodextrin onto NiFe2O4 nanoparticles for the removal of ketoprofen and diclofenac from the aqueous solutions. [Figure not available: see fulltext.] © 2023, The Author(s) under exclusive licence to Iranian Society of Environmentalists (IRSEN) and Science and Research Branch, Islamic Azad University.