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Prof. Dr. Munenori Numata Daiki Kinoshita Naoya Hirose Dr. Tomohiro Kozawa Prof. Hitoshi Tamiaki Yoshihiro Kikkawa Dr. Masatoshi Kanesato 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(5):1592-1598
Developing new strategies for controlling polymer conformations through precise molecular recognition can potentially generate a machine‐like motion that is dependent on molecular information—an important process for the preparation of new intelligent nanomaterials (e.g., polymer‐based nanomachines) in the field bordering between polymer chemistry and conventional supramolecular sciences. Herein, we propose a strategy to endow a helical polymer chain with dynamic spring‐like (contraction/expansion) motion through the one‐dimensional self‐assembly (aggregation/disaggregation) of peripheral amphiphilic molecules. In this developing system, we employed a semi‐artificial helical polysaccharide presenting peripheral amphiphilic chlorophyll units as a power device that undergoes contractive motion in aqueous media, driven by strong π–π interactions of its chlorophyll units or by cooperative molecular recognition of bipyridyl‐type ligands through pairs of chlorophyll units, thereby converting molecular information into the regulated motion of a spring. In addition, this system also undergoes expansive motion through coordination of pyridine. We anticipate that this strategy will be applicable (when combined with the established wrapping chemistry of the helical polysaccharide) to the development of, for example, drug carriers (e.g., nano‐syringes), actuators (stimuli‐responsive films), and directional transporters (nano‐railways), thereby extending the frontiers of supramolecular science. 相似文献
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D Umeyama S Horike M Inukai T Itakura S Kitagawa 《Journal of the American Chemical Society》2012,134(30):12780-12785
We synthesized a coordination polymer consisting of Zn(2+), 1,2,4-triazole, and orthophosphates, and demonstrated for the first time intrinsic proton conduction by a coordination network. The compound has a two-dimensional layered structure with extended hydrogen bonds between the layers. It shows intrinsic proton conductivity along the direction parallel to the layers, as elucidated by impedance studies of powder and single crystals. From the low activation energy for proton hopping, the conduction mechanism was found to be of the Grotthuss fashion. The hopping is promoted by rotation of phosphate ligands, which are aligned on the layers at appropriate intervals. 相似文献
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Appointment systems are widely used to facilitate customers’ access to services in many industries such as healthcare. A number of studies have taken a queueing approach to analyse service systems and facilitate managerial decisions on staffing requirements by assuming independent and stationary customer arrivals. This paper is motivated by the observation that the queueing-based method shows relatively poor performance when customers arrive according to their appointment times. Because customer arrivals are dependent on their appointment times, this study, unlike queueing-based methods, conducts a detailed analysis of appointment-based customer arrivals instead of making steady-state assumptions. We develop a new model that captures the characteristics of appointment-based customer arrivals and computes the probability of transient system states. Through the use of this model, which relaxes stationary and independent assumptions, we propose a heuristic algorithm that determines staffing requirements with aims to minimizing staff-hours while satisfying a target service level. The simulation results show that the proposed method outperforms the queueing-based method. 相似文献
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Electrospray droplet impact (EDI)/secondary ion mass spectrometry (SIMS) is a new desorption/ionization technique for mass spectrometry in which highly charged water clusters produced from the atmospheric‐pressure electrospray are accelerated in vacuum by several kV and impact the sample deposited on the metal substrate. In this study, several industrial synthetic polymers, e.g. polystyrene (PS) and polyethylene glycol (PEG) were analyzed by EDI/SIMS mass spectrometry. For higher molecular weight analytes, e.g. PS4000 and PEG4600, EDI/SIMS mass spectra could be obtained when cationization salts are added. For the polymers of lower molecular weights, e.g. PEG300 and PEG600, they could be readily detected as protonated ions without the addition of cationization agents. Anionized PS was also observed in the negative ion mode of operation when acetic acid was added to the charged droplet. Compared to matrix‐assisted laser desorption/ionization (MALDI), ion signal distribution with lower background signals could be obtained particularly for the low‐molecular weight polymers. Copyright © 2009 John Wiley & Sons, Ltd. 相似文献
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It has been established that a cationic rhodium(I)/dppp complex catalyzes the aldehyde C-H bond activation/[4 + 2] annulation/aromatization cascade to produce phenol, naphthol, phenanthrenol, and triphenylenol derivatives from readily available conjugated alkynyl aldehydes and alkynes. 相似文献
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Ogoshi T Yamafuji D Aoki T Yamagishi TA 《Chemical communications (Cambridge, England)》2012,48(54):6842-6844
A [2]rotaxane constructed from a per-ethylated pillar[6]arene as a wheel and a pyridinium derivative as an axle was prepared. The wheel segment of the per-ethylated pillar[6]arene moved from one station to another along the axle as a result of thermal stimuli. 相似文献
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Reaction of o-alkynylbenzothioamide with molecular iodine was investigated. Unique benzo[c]thiophen-1-aminium iodide was obtained when the tertiary thioamide was used as a reactant. The reaction proceeded efficiently in less polar solvent, whereas the corresponding product was also obtained in a polar solvent. Single crystal X-ray analysis revealed that the benzo[c]thiophen-1-aminium structure possesses a resonance structure in N–C–S bond. Its stabilization shows a clear difference in the result from the reaction of amide analogue with iodine to give no stable compound. 相似文献
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Nucleophilic Aromatic Substitution Reactions of meso‐Bromosubporphyrin: Synthesis of a Thiopyrane‐Fused Subporphyrin
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Daiki Shimizu Hirotaka Mori Masaaki Kitano Won‐Young Cha Juwon Oh Dr. Takayuki Tanaka Prof. Dr. Dongho Kim Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(49):16194-16202
meso‐Bromosubporphyrin undergoes nucleophilic aromatic substitution (SNAr) reactions with arylamines, diarylamines, phenols, ethanol, thiophenols, and n‐butanethiol in the presence of suitable bases to provide the corresponding substitution products. The SNAr reactions also proceed well with pyrrole, indole, and carbazole to provide substitution products in moderate to good yields. Finally, the SNAr reaction with 2‐bromothiophenol and subsequent intramolecular peripheral arylation reaction affords a thiopyrane‐fused subporphyrin. 相似文献