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The stability enhancement factor beyond eight-electron shell closure in thiacalix[4]arene-protected silver clusters.

ABSTRACT: We report the synthesis and structures of two 34-atom metal nanoclusters, namely [Ag34(BTCA)3(C[triple bond, length as m-dash]CBu t )9(tfa)4(CH3OH)3]SbF6 and [AuAg33(BTCA)3(C[triple bond, length as m-dash]CBu t )9(tfa)4(CH3OH)3]SbF6, where H4BTCA is p-tert-butylthiacalix[4]arene and tfa is trifluoroacetate. Their compositions and structures have been determined by single-crystal X-ray structural analysis and ESI-MS. The cationic cluster consists of a centered icosahedron M@Ag12 (M = Ag or Au) core that is surrounded by 21 peripheral silver atoms. Surrounding protection is provided by four kinds of ligands, including three BTCA, nine t BuC[triple bond, length as m-dash]C, four tfa, and three methanol solvent ligands. It was found that the Ag5@BTCA ?5-coordination motif of thiacalixarene is critical for high stability of the title clusters, and extra stability enhancement can be achieved by doping a gold atom at the center of the silver cluster. This work suggests that coordination saturation should be taken into account in addition to electronic and geometric factors for analyzing metal nanocluster stabilities.

SUBMITTER: Guan ZJ

PROVIDER: S-EPMC6430012 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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The stability enhancement factor beyond eight-electron shell closure in thiacalix[4]arene-protected silver clusters.

Guan Zong-Jie ZJ Hu Feng F Yuan Shang-Fu SF Nan Zi-Ang ZA Lin Yu-Mei YM Wang Quan-Ming QM

Chemical science 20190204 11

We report the synthesis and structures of two 34-atom metal nanoclusters, namely [Ag34(BTCA)3(C[triple bond, length as m-dash]CBu t )9(tfa)4(CH3OH)3]SbF6 and [AuAg33(BTCA)3(C[triple bond, length as m-dash]CBu t )9(tfa)4(CH3OH)3]SbF6, where H4BTCA is p-tert-butylthiacalix[4]arene and tfa is t ...[more]

PMID: 30996924

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Project description:An effective method for synthesizing acridinedione derivatives using a xanthan gum (XG), Thiacalix[4]arene (TC4A), and iron oxide nanoparticles (IONP) have been employed to construct a stable composition, which is named Thiacalix[4]arene-Xanthan Gum@ Iron Oxide Nanoparticles (TC4A-XG@IONP). The process used to fabricate this nanocatalyst includes the in-situ magnetization of XG, its amine modification by APTES to get NH2-XG@IONP hydrogel, the synthesis of TC4A, its functionalization with epichlorohydrine, and eventually its covalent attachment onto the NH2-XG@IONP hydrogel. The structure of the TC4A-XG@IONP was characterized by different analytical methods including Fourier-transform infrared spectroscopy, X-Ray diffraction analysis (XRD), Energy Dispersive X-Ray, Thermal Gravimetry analysis, Brunauer-Emmett-Teller, Field Emission Scanning Electron Microscope and Vibration Sample Magnetomete. With magnetic saturation of 9.10 emu g-1 and ~ 73% char yields, the TC4As-XG@IONP catalytic system demonstrated superparamagnetic property and high thermal stability. The magnetic properties of the TC4A-XG@IONP nanocatalyst system imparted by IONP enable it to be conveniently isolated from the reaction mixture by using an external magnet. In the XRD pattern of the TC4As-XG@IONP nanocatalyst, characteristic peaks were observed. This nanocatalyst is used as an eco-friendly, heterogeneous, and green magnetic catalyst in the synthesis of acridinedione derivatives through the one-pot pseudo-four component reaction of dimedone, various aromatic aldehydes, and ammonium acetate or aniline/substituted aniline. A combination of 10 mg of catalyst (TC4A-XG@IONP), 2 mmol of dimedone, and 1 mmol of aldehyde at 80 °C in a ethanol at 25 mL round bottom flask, the greatest output of acridinedione was 92% in 20 min.This can be attributed to using TC4A-XG@IONP catalyst with several merits as follows: high porosity (pore volume 0.038 cm3 g-1 and Pore size 9.309 nm), large surface area (17.306 m2 g-1), three dimensional structures, and many catalytic sites to active the reactants. Additionally, the presented catalyst could be reused at least four times (92-71%) with little activity loss, suggesting its excellent stability in this multicomponent reaction. Nanocatalysts based on natural biopolymers in combination with magnetic nanoparticles and macrocycles may open up new horizons for researchers in the field.

Dataset Information

The stability enhancement factor beyond eight-electron shell closure in thiacalix[4]arene-protected silver clusters.

Publications

The stability enhancement factor beyond eight-electron shell closure in thiacalix[4]arene-protected silver clusters.

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