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121.
Dr. Christina Rest Dr. Divya Susan Philips Torsten Dünnebacke Dr. Papri Sutar Dr. Angel Sampedro Jörn Droste Dr. Vladimir Stepanenko Prof. Dr. Michael Ryan Hansen Dr. Rodrigo Q. Albuquerque Prof. Dr. Gustavo Fernández 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(44):10005-10013
Besides their widespread use in coordination chemistry, 2,2’-bipyridines are known for their ability to undergo cis–trans conformational changes in response to metal ions and acids, which has been primarily investigated at the molecular level. However, the exploitation of such conformational switching in self-assembly has remained unexplored. In this work, the use of 2,2’-bipyridines as acid-responsive conformational switches to tune supramolecular polymerization processes has been demonstrated. To achieve this goal, we have designed a bipyridine-based linear bolaamphiphile, 1 , that forms ordered supramolecular polymers in aqueous media through cooperative aromatic and hydrophobic interactions. Interestingly, addition of acid (TFA) induces the monoprotonation of the 2,2’-bipyridine moiety, leading to a switch in the molecular conformation from a linear (trans) to a V-shaped (cis) state. This increase in molecular distortion along with electrostatic repulsions of the positively charged bipyridine-H+ units attenuate the aggregation tendency and induce a transformation from long fibers to shorter thinner fibers. Our findings may contribute to opening up new directions in molecular switches and stimuli-responsive supramolecular materials. 相似文献
122.
Wenhan Xu Michelle M. S. Lee Jing‐Jun Nie Zhihan Zhang Ryan T. K. Kwok Jacky W. Y. Lam Fu‐Jian Xu Dong Wang Ben Zhong Tang 《Angewandte Chemie (International ed. in English)》2020,59(24):9610-9616
Photodynamic therapy (PDT) has long been shown to be a powerful therapeutic modality for cancer. However, PDT is undiversified and has become stereotyped in recent years. Exploration of distinctive PDT methods is thus highly in demand but remains a severe challenge. Herein, an unprecedented 1+1+1>3 synergistic strategy is proposed and validated for the first time. Three homologous luminogens with aggregation‐induced emission (AIE) characteristics were rationally designed based on a simple backbone. Through slight structural tuning, these far‐red/near‐infrared AIE luminogens are capable of specifically anchoring to mitochondria, cell membrane, and lysosome, and effectively generating reactive oxygen species (ROS). Notably, biological studies demonstrated combined usage of three AIE photosensitizers gives multiple ROS sources simultaneously derived from several organelles, which gives superior therapeutic effect than that from a single organelle at the same photosensitizers concentration. This strategy is conceptually and operationally simple, providing an innovative approach and renewed awareness of improving therapeutic effect through three‐pronged PDT. 相似文献
123.
Zheng Deng Chang‐Jong Kang Mark Croft Wenmin Li Xi Shen Jianfa Zhao Richeng Yu Changqing Jin Gabriel Kotliar Sizhan Liu Trevor A. Tyson Ryan Tappero Martha Greenblatt 《Angewandte Chemie (International ed. in English)》2020,59(21):8240-8246
Given the consensus that pressure improves cation ordering in most of known materials, a discovery of pressure‐induced disordering could require recognition of an order–disorder transition in solid‐state physics/chemistry and geophysics. Double perovskites Y2CoIrO6 and Y2CoRuO6 polymorphs synthesized at 0, 6, and 15 GPa show B‐site ordering, partial ordering, and disordering, respectively, accompanied by lattice compression and crystal structure alteration from monoclinic to orthorhombic symmetry. Correspondingly, the long‐range ferrimagnetic ordering in the B‐site ordered samples are gradually overwhelmed by B‐site disorder. Theoretical calculations suggest that unusual unit‐cell compressions under external pressures unexpectedly stabilize the disordered phases of Y2CoIrO6 and Y2CoRuO6. 相似文献
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Ryan P. Jansonius Phil A. Schauer David J. Dvorak Benjamin P. MacLeod David K. Fork Curtis P. Berlinguette 《Angewandte Chemie (International ed. in English)》2020,59(29):12192-12198
Strain engineering can increase the activity and selectivity of an electrocatalyst. Tensile strain is known to improve the electrocatalytic activity of palladium electrodes for reduction of carbon dioxide or dioxygen, but determining how strain affects the hydrogen evolution reaction (HER) is complicated by the fact that palladium absorbs hydrogen concurrently with HER. We report here a custom electrochemical cell, which applies tensile strain to a flexible working electrode, that enabled us to resolve how tensile strain affects hydrogen absorption and HER activity for a thin film palladium electrocatalyst. When the electrodes were subjected to mechanically‐applied tensile strain, the amount of hydrogen that absorbed into the palladium decreased, and HER electrocatalytic activity increased. This study showcases how strain can be used to modulate the hydrogen absorption capacity and HER activity of palladium. 相似文献
126.
Dayong Lee Ryan Vandrey Garry Milman Mateus Bergamaschi Damodara R. Mendu Jeannie A. Murray Allan J. Barnes Marilyn A. Huestis 《Analytical and bioanalytical chemistry》2013,405(23):7269-7279
Oral fluid (OF) is a valuable biological alternative for clinical and forensic drug testing. Evaluating OF to plasma (OF/P) cannabinoid ratios provides important pharmacokinetic data on the disposition of drug and factors influencing partition between matrices. Eleven chronic cannabis smokers resided on a closed research unit for 51 days. There were four 5-day sessions of 0, 30, 60, and 120 mg oral ?9-tetrahydrocannabinol (THC)/day followed by a five-puff smoked cannabis challenge on Day 5. Each session was separated by 9 days ad libitum cannabis smoking. OF and plasma specimens were analyzed for THC and metabolites. During ad libitum smoking, OF/P THC ratios were high (median, 6.1; range, 0.2–348.5) within 1 h after last smoking, decreasing to 0.1–20.7 (median, 2.1) by 13.0–17.1 h. OF/P THC ratios also decreased during 5-days oral THC dosing, and after the smoked cannabis challenge, median OF/P THC ratios decreased from 1.4 to 5.5 (0.04–245.6) at 0.25 h to 0.12 to 0.17 (0.04–5.1) at 10.5 h post-smoking. In other studies, longer exposure to more potent cannabis smoke and oromucosal cannabis spray was associated with increased OF/P THC peak ratios. Median OF/P 11-nor-9-carboxy-THC (THCCOOH) ratios were 0.3–2.5 (range, 0.1–14.7) ng/μg, much more consistent in various dosing conditions over time. OF/P THC, but not THCCOOH, ratios were significantly influenced by oral cavity contamination after smoking or oromucosal spray of cannabinoid products, followed by time-dependent decreases. Establishing relationships between OF and plasma cannabinoid concentrations is essential for making inferences of impairment or other clinical outcomes from OF concentrations. 相似文献
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Formation and evolution of a carbide superlattice (SL) during C deposition on Mo have been studied using molecular beam epitaxy techniques. The ordering of the SL is energetically driven, such that the interplay between strain and surface energies determines the length scale of the SL. Surface precipitation of C occurs within a narrow range of SL spacing that appears to control the size and spacing of the precipitates leading to a possible mechanism for nucleation of single-walled carbon nanotubes. 相似文献
130.
Bennink RS Wong V Marino AM Aronstein DL Boyd RW Stroud CR Lukishova S Gauthier DJ 《Physical review letters》2002,88(11):113901
We have observed transverse pattern formation leading to highly regular structures in both the near and far fields when a near-resonant laser beam propagates without feedback through an atomic sodium vapor. One example is a regular far-field honeycomb pattern, which results from the transformation of the laser beam within the vapor into a stable three-lobed structure with a uniform phase distribution and highly correlated power fluctuations. The predictions of a theoretical model of the filamentation process are in good agreement with these observations. 相似文献