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Mechanism of Macroscopic Motion of Oleate Helical Assemblies: Cooperative Deprotonation of Carboxyl Groups Triggered by Photoisomerization of Azobenzene Derivatives 下载免费PDF全文
Dr. Yoshiyuki Kageyama Tomonori Ikegami Yuta Kurokome Prof. Dr. Sadamu Takeda 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(25):8669-8675
Macroscopic and spatially ordered motions of self‐assemblies composed of oleic acid and a small amount of an azobenzene derivative, induced by azobenzene photoisomerization, was previously reported. However, the mechanism of the generation of submillimeter‐scale motions by the nanosized structural transition of azobenzene was not clarified. Herein, an underlying mechanism of the motions is proposed in which deprotonation of carboxyl groups in cooperation with azobenzene photoisomerization causes a morphological transition of the self‐assembly, which in turn results in macroscopic forceful dynamics. The photoinduced deprotonation was investigated by potentiometric pH titration and FTIR spectroscopy. The concept of hierarchical molecular interaction generating macroscale function is expected to promote the next stage of supramolecular chemistry. 相似文献
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Sonomi Arata Dr. Yuna Kim Prof. Norihisa Hoshino Dr. Keishiro Tahara Dr. Kiyonori Takahashi Dr. Tomofumi Kadoya Tomonori Inoue Prof. Takayoshi Nakamura Prof. Tomoyuki Akutagawa Prof. Jun-ichi Yamada Prof. Kazuya Kubo 《欧洲无机化学杂志》2023,26(12):e202300017
Unsymmetrical gold(III)-dithiolene complexes are potential candidates for molecular materials that exhibit thermal structural phase transitions. In this study, unsymmetrical ppy-gold(III) (ppy−=C-deprotonated-2-phenylpyridine(−)) complexes [AuC5] and [AuC6] coordinated by dithiolene ligands containing tetrathiafulvalene (TTF) skeletons with pentylthio (2-{bis(pentylthio)-1,3-dithiol-2-ylidene}-1,3-dithiol-4,5-dithiolate(2−)) and hexylthio groups (2-{bis(hexylthio)-1,3-dithiol-2-ylidene}-1,3-dithiol-4,5-dithiolate(2−)) were synthesized. Both complexes exhibited a large absorption band at approximately 508 nm, owing to intramolecular ligand-to-ligand charge transfer. One-dimensional columnar structures with head-to-tail molecular arrangements around the metal ions were constructed in the crystals. The flexible alkylthio groups were intercalated into crystalline spaces between dithiolene ligands in the columns. [AuC5] exhibits a simple phase transition at 198 °C between crystalline and isotropic phases irreversibly. The crystalline phase of [AuC6] observed at 25 °C melted at 148 °C. Another crystalline phase grew above 148 °C with a very slow crystallization rate from the liquid phase and was completely transformed into an isotropic phase at 200 °C. 相似文献
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Hirohito Ikeda Yukiko Sano Tomonori Matsubara Mitsunobu Kawahara Miho Yukawa Masao Fujisawa Eiji Yukawa Hatsumi Aki 《Journal of Thermal Analysis and Calorimetry》2013,113(3):1135-1138
Propericiazine (PCZ) is an antipsychotic agent used for the treatment and the prevention of relapse of schizophrenia. We found that when an oral solution containing PCZ was mixed with a green tea drink, the residual content of PCZ was reduced by forming an insoluble complex between PCZ and tea polyphenol. In this study, the mechanism underlying the incompatibility of PCZ with green tea polyphenol (GTP) in the solution was clarified by isothermal titration microcalorimetry (ITC). Both solutions of 27.4 mM PCZ and 2.2 mM (?)-epigallocatechin gallate (EGCg), which is a main ingredient of GTP, were mixed and then PCZ in the filtrate was reduced to approximately 60 %. According to measurement at 298 K by ITC, PCZ formed an insoluble complex with EGCg at an associate constant (K) of 4.75 × 102 M?1 exothermically, ΔH = ?40.0 kJ mol?1. When (?)-epicatechin gallate (ECg) was used as the GTP, PCZ interacted with ECg with K and ΔH values of 3.74 × 102 M?1 and ?22.1 kJ mol?1, respectively. On the other hand, little heat of the reaction between PCZ and (?)-epigallocatechin or (?)-epicatechin was observed. The results indicated that the main reason for this incompatibility was the formation of an insoluble complex by PCZ and a gallate-type GTP such as EGCg and ECg in the aqueous solution. 相似文献
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Natural products often possess various spin systems consisting of a methine group directly bonded to a methyl group (e.g. –CHa–CHb(CH3)–CHc–). The methine proton Hb splits into a broadened multiplet by coupling with several vicinal protons, rendering analysis difficult of nJC–H with respect to Hb in the J‐resolved HMBC‐1. In purpose of the reliable and easy measurements of nJC–H and nJH–H in the aforesaid spin system, we have developed a new technique, named BASHD‐J‐resolved‐HMBC. This method incorporates band selective homo decoupled pulse and J‐scaling pulse into HMBC. In this method, high resolution cross peaks can be observed along the F1 axis by J‐scaling pulse, and band selective homo decoupled pulse simplified multiplet signals. Determinations of nJC–H and nJH–H of multiplet signals can easily be performed using the proposed pulse sequence. Copyright © 2013 John Wiley & Sons, Ltd. 相似文献
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Kazuhisa Sato Shunya Tashiro Shuhei Matsunaga Yohei Yamaguchi Takanori Kiguchi Toyohiko J. Konno 《哲学杂志》2018,98(21):1945-1960
We have studied three-dimensional (3D) structures and growth processes of 14H-type long-period stacking order (LPSO) formed in Mg97Zn1Gd2 cast alloys by single tilt-axis electron tomography (ET) using high-angle annular dark-field scanning transmission electron microscopy. Evolution of the solute-enriched stacking faults (SFs) and the 14H LPSO by ageing were visualised in 3D with a high spatial resolution in multi-scale fields of views from a few nanometres to ~10 μm. Lateral growth of the solute-enriched SFs and the LPSO in the (0?0?0?1)Mg plane is notable compared to the out-of-plane growth in the [0?0?0?1]Mg direction. The 14H LPSO grows at the cost of decomposition of the (Mg, Zn)3Gd-type precipitates, and accompany a change of in-plane edge angles from 30 to 60°. We have updated the Time–Temperature–Transformation diagram for precipitation in Mg97Zn1Gd2 alloys: starting temperatures of both solute-enriched SFs and LPSO formation shifted to a shorter time side than those in the previous diagram. 相似文献
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Tomonori Yuasa Ryosuke Honma Hideki Funamizu Izumi Nishidate Yoshihisa Aizu 《Optical Review》2014,21(3):369-372
We are developing a daily health monitoring system that uses mobile phones with cameras and analyzes physiological conditions from R, G, and B intensity levels. However, since it is affected by various imaging conditions of the image input, color correction is required for accurate health monitoring. Therefore, we developed and validated a colorcorrection algorithm to derive reliable color information by correcting the spectral reflectance using the Wiener estimation and a color chart. 相似文献