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Enhancing Visible Light Absorption of Yellow-Colored Peroxo-Titanate Nanotubes Prepared Using Peroxo Titanium Complex Ions.

ABSTRACT: Visible light-activated yellow titanate nanotubes (TNTs) modified by peroxo groups were directly synthesized via a facile chemical reaction route using peroxo titanium complex ions as a precursor. Obtained peroxo-modified TNTs (PTNTs) possessed a cylindrical-shaped tubular morphology with an outer diameter of approximately 10 nm. The peroxo titanium functional group (Ti-O-O) was formed between the interlayers of the lepidocrocite-type titanate crystal that was the base structure of TNTs, with the interlayer distance estimated at approximately 10.02 Å. The formation of the peroxo functional groups reduced the electron density adjacent to the titanium atom, raising the valence band to 1.35 eV and forming a band gap of 2.50 eV, which is lower than that of TNTs (3.19 eV). In addition, the peroxo titanium functional group had a negative potential, which increased the chemical adsorption performances with positively charged rhodamine B molecules in water. Meanwhile, the photocatalytic investigation indicated that the PTNTs have enhanced the photocatalytic performance for RhB decolorization under visible light irradiating in comparison with TNTs. These findings show not only the improvement in the photocatalytic performance but also the potential of processing design by selecting the precursor with arbitrary characteristics.

SUBMITTER: Park H

PROVIDER: S-EPMC7469391 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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Enhancing Visible Light Absorption of Yellow-Colored Peroxo-Titanate Nanotubes Prepared Using Peroxo Titanium Complex Ions.

Park Hyunsu H Goto Tomoyo T Cho Sunghun S Nishida Hisataka H Sekino Tohru T

ACS omega 20200820 34

Visible light-activated yellow titanate nanotubes (TNTs) modified by peroxo groups were directly synthesized via a facile chemical reaction route using peroxo titanium complex ions as a precursor. Obtained peroxo-modified TNTs (PTNTs) possessed a cylindrical-shaped tubular morphology with an outer diameter of approximately 10 nm. The peroxo titanium functional group (Ti-O-O) was formed between the interlayers of the lepidocrocite-type titanate crystal that was the base structure of TNTs, with th ...[more]

PMID: 32905404

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Project description:Inspired by the remarkable electronic and optical properties of single walled carbon nanotubes (SWNTs), various molecular sensing devices with sensitivity down to the single molecule level have been developed. However, most sensing approaches such as field effect transistors or near infrared (NIR) fluorescence require the rigorous debundling and separation of metallic tubes and semiconducting tubes in order to reach the desired high sensitivity. Interestingly, all carbon nanomaterials including carbon nanotubes, graphite, graphene, and even amorphous carbon exhibit extremely strong π-plasmon absorption in the ultraviolet region. This strong absorption has been studied as an undesired optical background for applications based on visible and NIR absorptions. For the first time, we found that the strong π-plasmon absorption of SWNTs in the ultraviolet region is extremely sensitive to ion binding. It is even much more sensitive than the absorption in the visible and NIR regions. Herein, we present our first exploration into using the extremely strong plasmon absorption of SWNTs to develop a new sensing platform for the detection of metallic ions. The detection selectivity is realized by modifying the surface of SWNTs with molecular ligands that have a high specificity for metal ions. As a demonstration, the new method is applied to selectively detect iron ions (Fe3+) by modifying the surface of the SWNTs with deferoxamine (DFO), a natural bacterial siderophore, which has a high specificity and affinity for Fe3+. The selective detection of Fe3+ in both aqueous solution and complex rain water is achieved with a pM level of sensitivity and detection limit. In situ resonant Raman spectroscopy demonstrated that the sensitive detection possibly involves electron transfer between the formed Fe-DFO complexes and the SWNTs. We envisage that it can be used to detect other metal ions when a specific binding chelator is attached to the carbon nanotube surface.

Project description:Redox-inactive metal ions that function as Lewis acids play pivotal roles in modulating reactivities of oxygen-containing metal complexes in a variety of biological and biomimetic reactions, including dioxygen activation/formation and functionalization of organic substrates. Mononuclear nonheme iron(III)-peroxo species are invoked as active oxygen intermediates in the catalytic cycles of dioxygen activation by nonheme iron enzymes and their biomimetic compounds. Here, we report mononuclear nonheme iron(III)-peroxo complexes binding redox-inactive metal ions, [(TMC)FeIII(O2)]+-M3+ (M3+ = Sc3+ and Y3+; TMC = 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane), which are characterized spectroscopically as a 'side-on' iron(III)-peroxo complex binding a redox-inactive metal ion, (TMC)FeIII-(?,?2:?2-O2)-M3+ (2-M). While an iron(III)-peroxo complex, [(TMC)FeIII(O2)]+, does not react with electron donors (e.g., ferrocene), one-electron reduction of the iron(III)-peroxo complexes binding redox-inactive metal ions occurs readily upon addition of electron donors, resulting in the generation of an iron(IV)-oxo complex, [(TMC)FeIV(O)]2+ (4), via heterolytic O-O bond cleavage of the peroxide ligand. The rates of the conversion of 2-M to 4 are found to depend on the Lewis acidity of the redox-inactive metal ions and the oxidation potential of the electron donors. We have also determined the fundamental electron-transfer properties of 2-M, such as the reduction potential and the reorganization energy in electron-transfer reaction. Based on the results presented herein, we have proposed a mechanism for the reactions of 2-M and electron donors; the reduction of 2-M to the reduced species, (TMC)FeII-(O2)-M3+ (2'-M), is the rate-determining step, followed by heterolytic O-O bond cleavage of the reduced species to form 4. The present results provide a biomimetic example demonstrating that redox-inactive metal ions bound to an iron(III)-peroxo intermediate play a significant role in activating the peroxide O-O bond to form a high-valent iron(IV)-oxo species.

Dataset Information

Enhancing Visible Light Absorption of Yellow-Colored Peroxo-Titanate Nanotubes Prepared Using Peroxo Titanium Complex Ions.

Publications

Enhancing Visible Light Absorption of Yellow-Colored Peroxo-Titanate Nanotubes Prepared Using Peroxo Titanium Complex Ions.

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