Research Papers - School of Natural Sciences
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Publication Open Access Fabrication of dual Z-scheme g-C3N4/Fe2TiO5/Fe2O3 ternary nanocomposite using natural ilmenite for efficient photocatalysis and photosterilization under visible light(Elsevier, 2022-11-11) Thambiliyagodage, C; Liyanaarachchi, H; Kumar, A; Jayanetti, M; Usgodaarachchi, L; Lansakara, BThe advanced oxidation process is a prominent method available to remove dyes released to normal water reservoirs to alleviate water scarcity. We report the fabrication of novel g-C3N4/Fe2TiO5/Fe2O3 using natural ilmenite sand as the precursor of the metallic semi-conductors exploration of a heterostructure for photodegradation of methylene blue under sunlight. Ternary composites were synthesized by varying g-C3N4 with respect to Fe2TiO5/Fe2O3 and varying Fe2TiO5/Fe2O3 with respect to g-C3N4 where the varying component was varied as 8, 24 and 40%, respect to the constant material. The hybridization of the three semi-conductors has been confirmed by the microscopic, chemical, and structural analyses. X-ray diffraction patterns show the presence of all three g-C3N4, Fe2TiO5 and α-Fe2O3 while the transmission electronic microscopic and scanning electronic microscopic images show the heterogeneous distribution of the metal oxide nanoparticles on g-C3N4 matrix forming the composite. HRTEM images further reveal the junction of Fe2TiO5 and α-Fe2O3. X-ray photoelectron spectra show the existence of s-triazine and heptazine rings in the composites with Fe3+ and Ti4+ as the only oxidation states of Fe and Ti. Fe2TiO5/Fe2O3/40% g-C3N4 with bandgap of 2.63 eV calculated by diffuse reflectance UV-Visible spectroscopy showed the highest photocatalytic activity (0.009 min−1) being 1.3 times greater than the Fe2TiO5/Fe2O3 nanoparticles. Enhanced photocatalytic activity over the fabricated composites was observed due to the increased visible light absorption, efficient charge separation and improved charge transportation. g-C3N4 coupled with 40% Fe2TiO5/Fe2O3 showed the highest antibacterial activity against gram-negative E.Coli. The synthesis of dual Z-scheme g-C3N4/Fe2TiO5/Fe2O3 ternary composite provides new sights in developing novel photocatalysts using natural ilmenite sand for environmental applications.Publication Open Access Fabrication of TiO2 Spheres and a Visible Light Active α‑Fe2O3/ TiO2‑Rutile/TiO2‑Anatase Heterogeneous Photocatalyst from Natural Ilmenite(researchgate.net, 2022-07-26) Usgodaarachchi, L; Thambiliyagodage, C; Wijesekera, R; Vigneswaran, S; Kandanapitiye, MHigh-purity (98.8%, TiO2) rutile nanoparticles were successfully synthesized using ilmenite sand as the initial titanium source. This novel synthesis method was cost-effective and straightforward due to the absence of the traditional gravity, magnetic, electrostatic separation, ball milling, and smelting processes. Synthesized TiO2 nanoparticles were 99% pure. Also, highly corrosive environmentally hazardous acid leachate generated during the leaching process of ilmenite sand was effectively converted into a highly efficient visible light active photocatalyst. The prepared photocatalyst system consists of anatase-TiO2/rutile-TiO2/Fe2O3 (TF-800), rutile-TiO2/Fe2TiO5 (TFTO-800), and anatase-TiO2/Fe3O4 (TF-450) nanocomposites, respectively. The pseudo-second-order adsorption rate of the TF-800 ternary nanocomposite was 0.126 g mg–1 min–1 in dark conditions, and a 0.044 min–1 visible light initial photodegradation rate was exhibited. The TFTO-800 binary nanocomposite adsorbed methylene blue (MB) following pseudo-second-order adsorption (0.224 g mg–1 min–1) in the dark, and the rate constant for photodegradation of MB in visible light was 0.006 min–1. The prepared TF-450 nanocomposite did not display excellent adsorptive and photocatalytic performances throughout the experiment period. The synthesized TF-800 and TFTO-800 were able to degrade 93.1 and 49.8% of a 100 mL, 10 ppm MB dye solution within 180 min, respectively.Publication Open Access Efficient Visible-Light Photocatalysis and Antibacterial Activity of TiO2-Fe3C-Fe-Fe3O4/Graphitic Carbon Composites Fabricated by Catalytic Graphitization of Sucrose Using Natural Ilmenite(American Chemical Society, 2022-07-26) Thambiliyagodage, C; Usgodaarachchi, L; Jayanetti, M; Liyanaarachchi, C; Kandanapitiye, M; Vigneswaran, SDyes in wastewater are a serious problem that needs to be resolved. Adsorption coupled photocatalysis is an innovative technique used to remove dyes from contaminated water. Novel composites of TiO2-Fe3C-Fe-Fe3O4dispersed on graphitic carbon were fabricated using natural ilmenite sand as the source of iron and titanium, and sucrose as the carbon source, which were available at no cost. Synthesized composites were characterized by X-ray diffractometry (XRD), Raman spectroscopy, transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray fluorescence spectroscopy (XRF), and diffuse reflectance UV-visible spectroscopy (DRS). Arrangement of nanoribbons of graphitic carbon with respect to the nanomaterials was observed in TEM images, revealing the occurrence of catalytic graphitization. Variations in the intensity ratio (ID/IG), Laand LD, calculated from data obtained from Raman spectroscopy suggested that the level of graphitization increased with an increased loading of the catalysts. SEM images show the immobilization of nanoplate microballs and nanoparticles on the graphitic carbon matrix. The catalyst surface consists of Fe3+and Ti4+as the metal species, with V, Mn, and Zr being the main impurities. According to DRS spectra, the synthesized composites absorb light in the visible region efficiently. Fabricated composites effectively adsorb methylene blue via π-πinteractions, with the absorption capacities ranging from 21.18 to 45.87 mg/g. They were effective in photodegrading methylene blue under sunlight, where the rate constants varied in the 0.003-0.007 min-1range. Photogenerated electrons produced by photocatalysts captured by graphitic carbon produce O2•-radicals, while holes generate OH•radicals, which effectively degrade methylene blue molecules. TiO2-Fe3C-Fe-Fe3O4/graphitic carbon composites inhibited the growth of Escherichia coli (69%) and Staphylococcus aureus (92%) under visible light. Synthesized novel composites using natural materials comprise an ecofriendly, cost-effective solution to remove dyes, and they were effective in inhibiting the growth of Gram-negative and Gram-positive bacteria.Publication Open Access Photocatalytic activity of Go/Fe3O4 fabricated by Sri Lankan graphite under visible light irradiation(Faculty of Science, University of Kelaniya, Sri Lanka, 2021-10) Usgodaarachchi, L; Thambiliyagodage, C. JGraphene oxide (GO) was synthesized using Sri Lankan naturally available graphite by modified Hummer’s method. Fe3O4 nanoparticles were synthesized successfully by co-precipitation of Fe3+ and Fe2+ in a 2:1 molar ratio via the addition of NH4OH. Magnetically separable GO/Fe3O4 nanocomposite was fabricated by synthesizing Fe3O4 nanoparticles in the presence of GO. The synthesized nanocomposites were characterized by X-ray diffractometry (XRD), Scanning electron microscopy (SEM), and FT-IR spectroscopy. The formation of GO was confirmed by the C(002) peak at 9.39° in the XRD pattern. XRD pattern of the nanoparticles confirms the formation of crystalline Fe3O4 nanoparticles, and the diffraction peak corresponds to graphene oxide disappear in the GO/ Fe3O4 due to the absence of the folded structure of graphene oxide. SEM image of GO shows the crumpled and wrinkled lamellae structure of graphene oxide, and the images of GO/ Fe3O4 show the distribution of Fe3O4 nanoparticles with an average size of 107 nm on GO where the folded structure of GO was not present while restacking of the nanosheets, was observed. FT-IR spectrum of GO shows the presence of polar oxygenated functional groups such as carboxylic acid (-COOH), hydroxyl (-OH), and epoxy (-COC-). The photocatalytic performance of the photocatalysts was evaluated on photodegradation of methylene blue under visible light irradiation. The GO/ Fe3O4 shows better adsorption behaviour and excellent photocatalytic activity where it could be successfully used for three cycles without significant activity loss. The rate constant for the degradation of MB (0.0187 min-1 ) at the first cycle decreased to 0.0101 min-1 at the third cycle. The conversion of MB decreased from 98.31% at the first cycle to 92.15% at the third cycle. The drop in the conversion is only 6.16% going from cycle 1 to 3, which could be due to the accumulation of the MB molecules at the pore structure. The obtained high photocatalytic activity could be due to the enhanced charge separation resulted due to the presence of GO sheets and better interactions between GO and Fe 3O4.Publication Embargo Efficient removal of methylene blue by turbostratic carbon/Fe3C/Fe composite synthesized by catalytic graphitization of sucrose(Elsevier, 2021-12-07) Thambiliyagodage, C. J; Usgodaarachchi, LTurbostratic carbon/Fe3C/Fe composite was prepared by catalytic graphitization of sucrose by α-Fe2O3. The synthesized composites were characterized by X-ray diffractometry (XRD), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). XRD patterns revealed the formation of turbostratic carbon with a d spacing of 0.3412 nm and the presence of Fe3C and Fe nanoparticles. Raman spectrum exhibited the D, G and G' peaks. XPS analysis shows the presence of graphitic carbon and +3 oxidation state of iron. Synthesized composite can remove methylene blue with an adsorption capacity of 17.8 mg/g at pH 7. Adsorption follows pseudo second order kinetics and the Langmuir isotherm model. As the synthesized composite is magnetic it could be easily separated from the mixture and could be reused effectively without significant activity loss for five cycles.Publication Embargo Photocatalytic activity of N, Fe and Cu co-doped TiO2 nanoparticles under sunlight(Elsevier, 2021-01-01) Thambiliyagodage, C. J; Usgodaarachchi, LPhotocatalytic activity of N doped with one transition metal is well known. This article reports the synthesis of TiO2 nanoparticles doped with only N, N co-doped with Fe, N co-doped with Cu and N co-doped with both Fe and Cu by sol-gel method. Their photocatalytic activity was evaluated for the degradation of methylene blue under sunlight. Nanoparticles were characterized by X-ray diffractometry (XRD), Raman spectroscopy, transmission electron microscopy (TEM), scanning electron microscopy (SEM), and diffuse reflectance UV–visible spectroscopy (DRS). XRD analysis revealed the presence of anatase phase TiO2 nanoparticles which was confirmed by Raman spectroscopic and TEM analysis. The crystal structure has not been disturbed by doping with N, Fe and Cu as shown by both XRD and Raman analysis. TEM and SEM images exhibit the nanoparticles which are interconnected due to sintering. XPS analysis revealed the presence of the only Ti4+ in undoped TiO2 but both Ti4+ and Ti3+ are present in doped TiO2 nanoparticles. According to the DRS analysis, the band gap of all doped TiO2 is lower than that of the undoped TiO2, where N, Fe and Cu co-doped TiO2 showed the lowest band gap (2.51 eV) proving that the visible light sensitivity of TiO2 increase with metal and non-metal doping. The rate of photodegradation of methylene blue in the presence of undoped TiO2 (0.016 min−1) is higher than all the doped TiO2 nanoparticles. N doped TiO2 show the highest activity among the doped TiO2 nanoparticles (0.006 min−1). Doped TiO2 nanoparticles showed a lower photocatalytic activity due to the electron hole pair recombination and the shielding effect of the dopants.Publication Open Access Efficient photodegradation activity of α-Fe2O3/Fe2TiO5/TiO2 and Fe2TiO5/TiO2 nanocomposites synthesized from natural ilmenite(Elsevier, 2021-12-01) Thambiliyagodage, C. J; Usgodaarachchi, L; Shanitha, M; Wijesekera, R; Lansakara, B; Bakker, MPhotocatalysis is an attractive widely used environmental remediation technique. Ternary (α-Fe2O3/Fe2TiO5/TiO2) and binary (Fe2TiO5/TiO2) nanocomposites were successfully synthesized by using natural ilmenite sand as the raw material. The synthesized nanocomposites were characterized by microscopic and spectroscopic analytical techniques. Both nanocomposites were catalytically active for the photodegradation of methylene blue upon irradiation by a light source (LED and sunlight). The visible light absorption of both composites was improved by the presence of Fe2TiO5 and α-Fe2O3 which absorb in the visible. The ternary nanocomposite with type II band alignments was more active than the binary nanocomposite with type I band alignment in the visible light exposure. Under sunlight exposure, binary nanocomposites were more active than the ternary nanocomposites. Band alignment, percentage of TiO2 in the composites and the proper formation of the structure of the composites govern the photocatalytic activity. OH● is suggested as the main species responsible for the photodegradation of methylene blue.Publication Open Access Synthesis of mesoporous silica nanoparticles derived from rice husk and surface-controlled amine functionalization for efficient adsorption of methylene blue from aqueous solution(Elsevier, 2021-01-01) Usgodaarachchi, L; Thambiliyagodage, C. J; Wijesekera, R; Bakker, M. GMesoporous silica nanoparticles (MSN) were synthesized using rice husk (RH) as the raw material via sol-gel pathway using cetyltrimethylammonium bromide (CTAB) as the structure directing agent. Silica nanoparticles were successfully functionalized with 3-aminopropyl triethoxysilane (APTES) via in-situ and post functionalization methods. Synthesized nanoparticles were characterized by X-Ray diffraction spectroscopy (XRD), scanning electron microscopy (SEM), fourier-transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA) and Brunauer-Emmett-Teller (BET) surface area analysis. The amorphous silica nanoparticles were of 50–60 nm in diameter with a surface area of 150 m2/g, pore volume of 0.237 cm3/g and average pore size of 3.62 nm. Morphology and textural parameters were changed upon functionalization. The equilibrium adsorption capacity of MSN-A (4.94 mg/g) to adsorb 10 mg/L methylene blue (MB), was higher than in amine functionalized silica nanoparticles. The influence of experimental factors such as pH, adsorbent dosage, and initial MB concentration on adsorption of MB to MSN-A were studied. The equilibrium data for MB adsorption on mesoporous silica nanoparticles well fitted to Langmuir equation, with a maximum monolayer capacity of 19.26 mg/g. The adsorption of MB could be best described by the pseudo-second order model. The results indicate that MSN-A is a potential mesoporous material fabricated by cheap natural resources to remove MB from aqueous solutions.