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Functionalised Mn(VI)-nanoparticles: an advanced high-valent magnetic catalyst.

ABSTRACT: We discover Mn(VI)-nanoparticles (NPs) bearing functional groups, high oxidation state, strong electron affinity, unique redox and paramagnetic nature, which opens up a new avenue to catalysis, magnetism and material application. However, its synthesis is challenging and remains unexplored because of associated serious difficulties. A simple benign synthetic strategy is devised to fabricate the high-valent NPs using mild reducing agent bromide, which transformed Mn(VII) to valuable Mn(VI)-species. The EELS-imaging of individual elements, ESI-MS, XPS and other techniques established its composition as Br(Me3SiO)Mn(VI)O2. It revealed significantly improved magnetic moment (SQUID) with isotropic hyperfine splitting of six line spectrum (EPR). The high-oxidation state and incorporated-ligands of the metals present on the active surface of the NPs led to development of a general catalytic process for oxidative heterodifunctionalisation to C-C triple bond towards formation of a new O-C/N-C/S-C and C-C coupling cum cyclisation to biologically important flavones and their aza- and marcapto-analogues, and valuable enaloxy synthons.

SUBMITTER: Khamarui S

PROVIDER: S-EPMC4345317 | biostudies-literature | 2015 Mar

REPOSITORIES: biostudies-literature

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Functionalised Mn(VI)-nanoparticles: an advanced high-valent magnetic catalyst.

Khamarui Saikat S Saima Yasmin Y Laha Radha M RM Ghosh Subhadeep S Maiti Dilip K DK

Scientific reports 20150302

We discover Mn(VI)-nanoparticles (NPs) bearing functional groups, high oxidation state, strong electron affinity, unique redox and paramagnetic nature, which opens up a new avenue to catalysis, magnetism and material application. However, its synthesis is challenging and remains unexplored because of associated serious difficulties. A simple benign synthetic strategy is devised to fabricate the high-valent NPs using mild reducing agent bromide, which transformed Mn(VII) to valuable Mn(VI)-specie ...[more]

PMID: 25727767

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Project description:Diabetes is a chronic metabolic disease which leads to high glucose levels in the blood, with severe consequences for human health. Due to the worldwide appeal for the reduction in calorie intake, this study presents the development of a nanomaterial able to capture sucrose selectively, thus providing a tool to remove naturally occurring sucrose from food, such as fruit juices, producing low-calorie juices for consumption. Magnetite nanoparticles (Fe3O4 NPs) coated with an inert material (SiO2) and functionalised with the enzyme invertase were designed to remove sucrose from solutions. Fe3O4 NPs were synthesised using the co-precipitation method, whereas the coating with a silica shell was done by the Stöber method. Its physicochemical characteristics were determined, with excellent stability over time. On the other hand, the invertase enzyme was extracted from dry Baker's yeast, purified and immobilised on the surface of the silica-coated Fe3O4 NPs. pH-triggered sucrose capture occurred at pH 3.0 once invertase with protonated catalytic residues was able just to bind with sucrose in a highly selective way. After a short, 1 min interaction, approximately 13.5 mmol L-1 of sucrose was captured per gram of nanomaterial and removed with the use of an external permanent magnet. The complex sucrose/nanomaterial was washed, and the released sucrose was put into buffered solution (pH = 4.8), where it underwent hydrolysis to yield inverted sugar. On the other side, sucrose-free nanomaterial was reused with no loss of enzymatic capability to capture sucrose at pH = 3.0 and maintained the invertase activity at pH 4.8 in ten consecutive rounds of re-use. As sucrose was recovered in the form of inverted sugar, not just low sugar beverage could be obtained, but also a high valued market product. Thus, the developed technology allows for the commercialisation of low-calorie food, offering healthier options to consumers and helping to fight diabetes and obesity.

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Functionalised Mn(VI)-nanoparticles: an advanced high-valent magnetic catalyst.

Publications

Functionalised Mn(VI)-nanoparticles: an advanced high-valent magnetic catalyst.

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