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Synthesis and characterization of Mn/Co/Ti LDH and its utilization as a photocatalyst in visible light assisted degradation of aqueous Rhodamine B.

ABSTRACT: Luminescent Mn/Co/Ti LDH, synthesized by a single step hydrothermal route, has been found to be optically responsive for utilization as a highly efficient photocatalyst in destruction of the cationic dye Rhodamine B, in aqueous solution under visible light irradiation. The material has been found to be better than the commercial catalysts like MnO, CoO, TiO2 and Degussa P25. Multiple techniques like XRD, XPS, FT-IR, EIS, TG, UV-visible DRS, PL, TRES, N2-sorption-desorption, dynamic light scattering, TEM-EDS and AFM analyses were used to characterize the LDH. The results indicated Mn/Co/Ti LDH to have a multilayered crystalline structure with hexagonal morphology that carries metal ions in mixed valences, oxygen vacancies, defect states, thermal stability, narrow band gap, high surface area, and electrostatic surface charge variation with pH. The photocatalytic activity of the LDH could be co-related with the structural aspects such as oxidation states, narrow band gap, high surface area and existence of defects. The active species responsible for photocatalysis have been evaluated with EPR, terephthalic acid fluorescence probe and indirect radical-hole trapping experiments. The photodegradation mechanism involves electron and hole hopping across the material and also photosensitization of the dye. Ex situ 1H-NMR and GC-MS analyses of the colorless end products of Rhodamine B destruction provide further insight into the reaction mechanism. The complete mineralization of the decolorized end product of degradation was evaluated with TOC analysis. The results indicate the potential for using multi metal incorporated LDH in destroying dyes and their degradation products in industrial wastewater.

SUBMITTER: Roy Chowdhury P

PROVIDER: S-EPMC6089547 | biostudies-literature | 2016

REPOSITORIES: biostudies-literature

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Synthesis and characterization of Mn/Co/Ti LDH and its utilization as a photocatalyst in visible light assisted degradation of aqueous Rhodamine B.

Roy Chowdhury Priyadarshi P Bhattacharyya Krishna G KG

RSC advances 20161121 113

Luminescent Mn/Co/Ti LDH, synthesized by a single step hydrothermal route, has been found to be optically responsive for utilization as a highly efficient photocatalyst in destruction of the cationic dye Rhodamine B, in aqueous solution under visible light irradiation. The material has been found to be better than the commercial catalysts like MnO, CoO, TiO<sub>2</sub> and Degussa P25. Multiple techniques like XRD, XPS, FT-IR, EIS, TG, UV-visible DRS, PL, TRES, N<sub>2</sub>-sorption-desorption, ...[more]

PMID: 30112172

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Project description:2 : 1 Co/Ti layered double hydroxide (LDH) was synthesized hydrothermally using commercially available Co(NO3)2·6H2O and TiCl4, on a urea template. The high surface area material (~180 m2 g-1) had a narrow band gap (2.67 eV) and shallow and deep trap defect sites. The layered nanomaterial exhibited remarkable semiconductor properties and demonstrated excellent visible light decolourisation efficiency for the anionic dye Congo Red in aqueous medium. The photocatalytic efficiency of the LDH was better than common commercial materials in use such as ZnO, ZnS, NiO, CoO, TiO2 and Degussa P25. The presence of different surface states of defect sites in the LDH was confirmed by PL, EIS and XPS measurements. XRD, DRS, FT-IR, AFM, TEM, SEM/EDX and TG/DTG analyses yielded information about the structural, morphological properties and thermal stability of the LDH. BET N2 adsorption-desorption measurements at 77 K gave surface area and porosity data for the LDH. The surface charge characteristics of the LDH were evaluated with ξ-potential measurements over a wide pH-range in aqueous medium. The photocatalytic behaviour towards decolourisation of the dye was evaluated depending on the reaction variables of pH, LDH amount, initial dye concentration and effects of quenchers, and variation of molar ratios of Co/Ti LDH. The pseudo-first order model satisfactorily described the degradation kinetics of the anionic dye. The photocatalytic mechanistic pathways of the LDH were explained on the basis of an electron-hole (e--h+) hopping conduction model and also photosensitization of the dye. The maximum catalytic efficiency was observed with 15.0 mg of LDH at pH 4 for the anionic Congo Red dye at a concentration 1 × 10-5 M. The LDH was stable even after the fifth catalytic cycle, indicating its remarkable efficiency in potential decolourisation treatments. The dye degradation products were analysed with GC-MS and a reaction mechanism was proposed for the breakdown of the dye to simple and less toxic components.

Project description:Titanium dioxide is an ubiquitous photocatalyst in water-cleaning technologies, being presently the most promising tools to resolve the global issue of sewage treatment. In this framework, titanium dioxide-graphene nanocomposites are discussed as promising visible-light activated photocatalysts but little is hitherto known about the surface and interface chemistry bridging the metal oxide and carbon phases. In an attempt to spotlight this overlooked issue, we herein designed two different hybrid nanocomposites through covalent grafting and growth of titanium dioxide clusters on graphene oxide and on phosphorylated graphene oxide, which affords GO@TiO2 and PGO@TiO2, respectively. While anatase could be selectively harvested on the surface of GO@TiO2, biphasic anatase-rutile nucleates could be obtained on PGO@TiO2. Thermal annealing treatments improve the metal oxide crystallization and further remove oxygenated groups from the surface of graphene. The interfacial stability of these photocatalysts was also investigated under irradiation, with the graphene support being sensitive to the proximal presence of titanium dioxide. The resulting nanocomposites were also assessed for methylene blue removal through adsorption and photocatalysis. Regardless of their composition, superior photoactivity was noticed for the nanocomposites compared to commercially available degussa that display marginal visible-light photoactivity (11% removal). Within our study, PGO@TiO2-500 stands as the most active catalyst, allowing nearly quantitative removal of the pollutant from water. The superior performance of PGO@TiO2-500 can be explained by the highest stability reached through P-O-Ti bonding, its improved crystallinity, and the reduction of the graphene surface during thermal treatment. On a whole, this study provides a blueprint for comparing semiconducting metal oxide grown on tuneable surface-interfacial graphene environments and highlights the utility of surface-engineering graphene sheets to access efficient visible-light oxidation photocatalysts.

Dataset Information

Synthesis and characterization of Mn/Co/Ti LDH and its utilization as a photocatalyst in visible light assisted degradation of aqueous Rhodamine B.

Publications

Synthesis and characterization of Mn/Co/Ti LDH and its utilization as a photocatalyst in visible light assisted degradation of aqueous Rhodamine B.

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