2022 Fiscal Year Research-status Report
Creation of self-assembled mesoscale chainmail and application
| Project/Area Number |
22K20526
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| Research Institution | Chiba University |
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Principal Investigator |
DATTA SOUGATA 千葉大学, 大学院工学研究院, 特任研究員 (60965036)
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| Project Period (FY) |
2022-08-31 – 2024-03-31
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| Keywords | nanostructures / topological structures / mechanical bonding / self-assembly / supramolecular chemistry |
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| Outline of Annual Research Achievements |
In the last fiscal year, we made our effort toward controlling of catenation of nanotoroids, which is crucial for the creation of mesoscale chainmail. The catenation relies on the size of the void of the nanotoroids and the secondary nucleation on their surface. We faced difficulty to control these factors using the proposed polar molecule. So, we worked on the barbituric acid-based nonpolar molecular design used in the preparation of polycatenanes in our laboratory. Since the corresponding nanotoroids are covered with alkyl chains of the barbiturate monomer, we increased the alkyl chain length of the molecule to prepare nanotoroids with a larger void space and with a higher frequency of secondary nucleation on their surface. Strikingly, atomic force microscopy and small-angle X-ray scattering experiments revealed a decrease in the inner void space of nanotoroids. Spectroscopic studies revealed increased efficiency of secondary nucleation on the surface of these nanotoroids. Interestingly, a combination of these two effects resulted in a higher yield of nano-[2]catenane and suppressed the formation of oligocatenanes. These preliminary results have been published in a paper recently.
Stimulated by the aforementioned surprising observation, we plan to investigate the detailed mechanism of the size modulation of the nanotoroids and its effect on the catenation in the near future.
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| Current Status of Research Progress |
Current Status of Research Progress
2: Research has progressed on the whole more than it was originally planned.
Reason
The suppression of oligocatenation due to a decrease in the size of void space of the nanotoroids that were obtained by elongation of alkyl chain length is an unexpected discovery. Since our original target was the creation of mesoscale chainmail, we are synthesizing barbituric acid-based molecules with shorter alkyl chains to prepare nanotoroids with larger void space to allow catenation of multiple fibers, necessary in the formation of chainmail.
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| Strategy for Future Research Activity |
After finishing the synthesis of barbituric acid-based molecules with shorter alkyl chain lengths, we will investigate the mechanism of variation of the size of the nanotoroids upon variation of alkyl chain length using spectroscopic experiments and theoretical calculation. The suitability for accommodating four fibers in the inner void space of the nanotoroids will be probed by atomic force microscopy and small-angle X-ray scattering experiments. Once a suitable match is found, it will be employed in two-dimensional catenation to create mesoscale chainmail. Importantly, although a decrease in the alkyl chain length produces nanotoroids with larger void space, the efficiency of secondary nucleation on the surface of the nanotoroids is expected to decrease. However, it can be compensated by using a suitable solvent that induces more solvophobic interactions. We also aim to utilize the chainmail structure in the transportation of mesoscale guests.
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| Causes of Carryover |
合成が予定通りに進行せず、次年度も継続して取り組むため。
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Research Products
(5 results)
