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Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane

In the molecular world, molecular ratchets can realize the unidirectional movement in molecular machines. However, construction of artificial molecular ratchets has been still a great challenge. In this study, we investigate the formation of pseudo-rotaxane of a newly designed two-station axis molec...

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Autores principales: Hashidzume, Akihito, Kuse, Akihiro, Oshikiri, Tomoya, Adachi, Seiji, Okumura, Mitsutaka, Yamaguchi, Hiroyasu, Harada, Akira
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5997654/
https://www.ncbi.nlm.nih.gov/pubmed/29895967
http://dx.doi.org/10.1038/s41598-018-27226-2
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author Hashidzume, Akihito
Kuse, Akihiro
Oshikiri, Tomoya
Adachi, Seiji
Okumura, Mitsutaka
Yamaguchi, Hiroyasu
Harada, Akira
author_facet Hashidzume, Akihito
Kuse, Akihiro
Oshikiri, Tomoya
Adachi, Seiji
Okumura, Mitsutaka
Yamaguchi, Hiroyasu
Harada, Akira
author_sort Hashidzume, Akihito
collection PubMed
description In the molecular world, molecular ratchets can realize the unidirectional movement in molecular machines. However, construction of artificial molecular ratchets has been still a great challenge. In this study, we investigate the formation of pseudo-rotaxane of a newly designed two-station axis molecule with α-cyclodextrin (α-CD) and the deuteration of acidic protons in the axis in D(2)O by (1)H NMR at varying temperatures. Using the NMR data, we roughly estimate apparent rate constants for association, dissociation, and translation of α-CD during the pseudo-rotaxane formation based on a simplified kinetic model. These rate constants are indicative of face-selective and ratchet-like translation of α-CD on the axis because of the 2-methylpyridinium residues in the axis. We also evaluate apparent first-order rate constants for the deuteration. Comparison of these rate constants indicates that the face-selective translation of α-CD somehow couples with the deuteration. On the basis of this study, it is concluded that a translational molecular ratchet can be constructed using a large energy gradient with appropriate energy barriers and an enthalpically-driven coupled reaction.
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spelling pubmed-59976542018-06-21 Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane Hashidzume, Akihito Kuse, Akihiro Oshikiri, Tomoya Adachi, Seiji Okumura, Mitsutaka Yamaguchi, Hiroyasu Harada, Akira Sci Rep Article In the molecular world, molecular ratchets can realize the unidirectional movement in molecular machines. However, construction of artificial molecular ratchets has been still a great challenge. In this study, we investigate the formation of pseudo-rotaxane of a newly designed two-station axis molecule with α-cyclodextrin (α-CD) and the deuteration of acidic protons in the axis in D(2)O by (1)H NMR at varying temperatures. Using the NMR data, we roughly estimate apparent rate constants for association, dissociation, and translation of α-CD during the pseudo-rotaxane formation based on a simplified kinetic model. These rate constants are indicative of face-selective and ratchet-like translation of α-CD on the axis because of the 2-methylpyridinium residues in the axis. We also evaluate apparent first-order rate constants for the deuteration. Comparison of these rate constants indicates that the face-selective translation of α-CD somehow couples with the deuteration. On the basis of this study, it is concluded that a translational molecular ratchet can be constructed using a large energy gradient with appropriate energy barriers and an enthalpically-driven coupled reaction. Nature Publishing Group UK 2018-06-12 /pmc/articles/PMC5997654/ /pubmed/29895967 http://dx.doi.org/10.1038/s41598-018-27226-2 Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Hashidzume, Akihito
Kuse, Akihiro
Oshikiri, Tomoya
Adachi, Seiji
Okumura, Mitsutaka
Yamaguchi, Hiroyasu
Harada, Akira
Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title_full Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title_fullStr Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title_full_unstemmed Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title_short Toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
title_sort toward a translational molecular ratchet: face-selective translation coincident with deuteration in a pseudo-rotaxane
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5997654/
https://www.ncbi.nlm.nih.gov/pubmed/29895967
http://dx.doi.org/10.1038/s41598-018-27226-2
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