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Induced-fit expansion and contraction of a self-assembled nanocube finely responding to neutral and anionic guests.

ABSTRACT: Induced-fit or conformational selection is of profound significance in biological regulation. Biological receptors alter their conformation to respond to the shape and electrostatic surfaces of guest molecules. Here we report a water-soluble artificial molecular host that can sensitively respond to the size, shape, and charged state of guest molecules. The molecular host, i.e. nanocube, is an assembled structure consisting of six gear-shaped amphiphiles (GSAs). This nanocube can expand or contract its size upon the encapsulation of neutral and anionic guest molecules with a volume ranging from 74 to 535 Å³ by induced-fit. The responding property of this nanocube, reminiscent of a feature of biological molecules, arises from the fact that the GSAs in the nanocubes are connected to each other only through the hydrophobic effect and very weak intermolecular interactions such as van der Waals and cation-? interactions.

SUBMITTER: Zhan YY

PROVIDER: S-EPMC6208372 | biostudies-literature | 2018 Oct

REPOSITORIES: biostudies-literature

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Induced-fit expansion and contraction of a self-assembled nanocube finely responding to neutral and anionic guests.

Zhan Yi-Yang YY Kojima Tatsuo T Nakamura Takashi T Takahashi Toshihiro T Takahashi Satoshi S Haketa Yohei Y Shoji Yoshiaki Y Maeda Hiromitsu H Fukushima Takanori T Hiraoka Shuichi S

Nature communications 20181031 1

Induced-fit or conformational selection is of profound significance in biological regulation. Biological receptors alter their conformation to respond to the shape and electrostatic surfaces of guest molecules. Here we report a water-soluble artificial molecular host that can sensitively respond to the size, shape, and charged state of guest molecules. The molecular host, i.e. nanocube, is an assembled structure consisting of six gear-shaped amphiphiles (GSAs). This nanocube can expand or contra ...[more]

PMID: 30382098

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Project description:Layered perovskites have been extensively investigated in many research fields, such as electronics, catalysis, optics, energy, and magnetics, because of the fascinating chemical properties that are generated by the specific structural features of perovskite frameworks. Furthermore, the interlayers of these structures can be chemically modified through ion exchange to form nanosheets. To further expand the modification of layered perovskites, we have demonstrated an advance in the new structural concept of layered perovskite "charge-neutral perovskite layers" by manipulating the perovskite layer itself. A charge-neutral perovskite layer in [CeIVTa2O7] was synthesized through a soft chemical oxidative reaction based on anionic [CeIIITa2O7]- layers. The Ce oxidation state for the charge-neutral [CeIVTa2O7] layers was found to be tetravalent by X-ray absorption fine structure (XAFS) analysis. The atomic arrangements were determined through scattering transmission electron microscopy and extended XAFS (EXAFS) analysis. The framework structure was simulated through density functional theory (DFT) calculations, the results of which were in good agreement with those of the EXAFS spectra quantitative analysis. The anionic [CeIIITa2O7]- layers exhibited optical absorption in the near infrared (NIR) region at approximately 1000 nm, whereas the level of NIR absorption decreased in the [CeIVTa2O7] charge-neutral layer due to the disappearance of the Ce 4f electrons. In addition, the chemical reactivity of the charge-neutral [CeIVTa2O7] layers was investigated by chemical reduction with ascorbic acid, resulting in the reduction of the [CeIVTa2O7] layers to form anionic [CeIIITa2O7]- layers. Furthermore, the anionic [CeIIITa2O7]- layers exhibited redox activity which the Ce in the perovskite unit can be electrochemically oxidized and reduced. The synthesis of the "charge-neutral" perovskite layer indicated that diverse features were generated by systematically tuning the electronic structure through the redox control of Ce; such diverse features have not been found in conventional layered perovskites. This study could demonstrate the potential for developing innovative, unique functional materials with perovskite structures.

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Induced-fit expansion and contraction of a self-assembled nanocube finely responding to neutral and anionic guests.

Publications

Induced-fit expansion and contraction of a self-assembled nanocube finely responding to neutral and anionic guests.

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