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941.
Suzuka Kinoshita Ryota Yamano Dr. Yu Shibata Yusuke Tanaka Kyoichi Hanada Dr. Takashi Matsumoto Prof. Dr. Kazunori Miyamoto Dr. Atsuya Muranaka Prof. Dr. Masanobu Uchiyama Prof. Dr. Ken Tanaka 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(27):11113-11120
An S-shaped double helicene-like molecule (>99 % ee), possessing stable helical chirality, has been synthesized by the rhodium(I)/difluorphos complex-catalyzed highly diastereo- and enantioselective intramolecular double [2+2+2] cycloaddition of a 2-naphthol- and benzene-linked hexayne. The collision between two terminal naphthalene rings destabilizes the helical chirality of the S-shaped double helicene-like molecule, but the introduction of two additional fused benzene rings significantly increases the configurational stability. Thus, no epimerization and racemization were observed even at 100 °C. The enantiopure S-shaped double helicene-like molecule forms a trimer through the multiple C−H⋅⋅⋅π and C−H⋅⋅⋅O interactions in the solid-state. The trimers stack to form columnar packing structures, in which neighboring stacks have opposite dipole directions. The accumulation of helical structures in the same direction in the S-shaped double helicene-like molecule enhanced the chiroptical properties. 相似文献
942.
Light-Driven Crawling of Molecular Crystals by Phase-Dependent Transient Elastic Lattice Deformation
Yanjun Gong Yongxian Guo Fayuan Ge Wei Xiong Jie Su Yang Sun Chuang Zhang An-Min Cao Yifan Zhang Jincai Zhao Yanke Che 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(26):10423-10428
The light-driven crawling of a molecular crystal that can form three phases, (α, β, and γ) is presented. Laser irradiation of the molecular crystal can generate phase-dependent transient elastic lattice deformation. The resulting elastic lattice deformation that follows scanning irradiation of a laser can actuate the different phases of molecular crystal to move with different velocity and direction. Because the γ phase has a large Young's modulus (ca. 26 GPa), a force of 0.1 μN can be generated under one laser spot. The generated force is sufficient to actuate the γ-formed molecular crystals in a wide dimensional range to move longitudinally at a velocity of about 60 μm min−1, which is two orders of magnitude faster than the α and β phases. 相似文献
943.
Dr. Ding Yi Fei Lu Fengchu Zhang Dr. Shoujie Liu Dr. Bo Zhou Denglei Gao Prof. Xi Wang Prof. Jiannian Yao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):15989-15993
Single-atom catalysts have attracted much attention. Reported herein is that regulating charge transfer of lattice oxygen atoms in serial single-atom-doped titania enables tunable hydrogen evolution reaction (HER) activity. First-principles calculations disclose that the activity of lattice oxygen for the HER can be regularly promoted by substituting its nearest metal atom, and doping-induced charge transfer plays an essential role. Besides, the realm of the charge transfer of the active site can be enlarged to the second nearest atom by creating oxygen vacancies, resulting in further optimization for the HER. Various single-atom-doped titania nanosheets were fabricated to validate the proposed model. Taking advantage of the localized charge transfer to the lattice atom is demonstrated to be feasible for realizing precise regulation of the electronic structures and thus catalytic activity of the nanosheets. 相似文献
944.
Dr. Linzhou Zhuang Dr. Yi Jia Hongli Liu Zhiheng Li Dr. Mengran Li Dr. Longzhou Zhang Dr. Xin Wang Prof. Dongjiang Yang Prof. Zhonghua Zhu Prof. Xiangdong Yao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14772-14778
The oxygen vacancies of defective iron–cobalt oxide (FeCoOx-Vo) nanosheets are modified by the homogeneously distributed sulfur (S) atoms. S atoms can not only effectively stabilize oxygen vacancies (Vo), but also form the Co−S coordination with Co active site in the Vo, which can modulate the electronic structure of the active site, enabling FeCoOx-Vo-S to exhibit much superior OER activity. FeCoOx-Vo-S exhibits a mass activity of 2440.0 A g−1 at 1.5 V vs. RHE in 1.0 m KOH, 25.4 times higher than that of RuO2. The Tafel slope is as low as 21.0 mV dec−1, indicative of its excellent charge transfer rate. When FeCoOx-Vo-S (anode catalyst) is paired with the defective CoP3/Ni2P (cathode catalyst) for overall water splitting, current densities of as high as 249.0 mA cm−2 and 406.0 mA cm−2 at a cell voltage of 2.0 V and 2.3 V, respectively, can be achieved. 相似文献
945.
Guoyu Zhang Song Zhou Dr. Liang Fu Dr. Pinhong Chen Prof. Yibiao Li Prof. Dr. Jianping Zou Prof. Dr. Guosheng Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20619-20624
The first copper-catalyzed asymmetric cyanation and etherification reactions of enamides have been established, where a carbon-centered radical adjacent to a nitrogen atom (CRAN) is enantioselectively trapped by a chiral copper(II) species. Moreover, the asymmetric cyanation of vinyl esters was disclosed as well. These reactions feature very mild reaction conditions and high functional group tolerance, and give a series of chiral α-cyano amides, α-cyano esters and α-hemiaminals in good yields with excellent enantioselectivity. The chiral α-cyano amides can be easily converted into enantioenriched 1,2-diamines and amino acids. 相似文献
946.
Dr. Pengfei Cheng Lu Feng Prof. Dr. Yuefeng Liu Dr. Daoyuan Zheng Youbao Sang Wenyuan Zhao Dr. Yang Yang Dr. Songqiu Yang Prof. Dr. Donghui Wei Prof. Dr. Guoxiong Wang Prof. Dr. Keli Han 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21598-21602
All-inorganic zero-dimensional (0D) metal halides have recently received increasing attention due to their excellent photoluminescence (PL) performance and high stability. Herein, we present the successful doping of copper(I) into 0D Cs2ZnBr4. The incorporating of Cu+ cations enables the originally weakly luminescent Cs2ZnBr4 to exhibit an efficient blue emission centered at around 465 nm, with a high photoluminescence quantum yield (PLQY) of 65.3 %. Detailed spectral characterizations, including ultrafast transient absorption (TA) techniques, were carried out to investigate the effect of Cu+ dopants and the origin of blue emission in Cs2ZnBr4:Cu. To further study the role of the A-site cation and halogen, A2ZnCl4:Cu (A=Cs, Rb) were also synthesized and found to generate intense sky-blue emission (PLQY≈73.1 %). This work represents an effective strategy for the development of environmentally friendly, low-cost and high-efficiency blue-emitting 0D all-inorganic metal halides. 相似文献
947.
Yun Liu Guangze Yang Song Jin Run Zhang Peng Chen Tengjisi Lianzhou Wang Dong Chen David A. Weitz Chun-Xia Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20240-20249
Understanding drug-release kinetics is critical for the development of drug-loaded nanoparticles. We developed a J-aggregate-based Förster-resonance energy-transfer (FRET) method to investigate the release of novel high-drug-loading (50 wt %) nanoparticles in comparison with low-drug-loading (0.5 wt %) nanoparticles. Single-dye-loaded nanoparticles form J-aggregates because of the high dye-loading (50 wt %), resulting in a large red-shift (≈110 nm) in the fluorescence spectrum. Dual-dye-loaded nanoparticles with high dye-loading using FRET pairs exhibited not only FRET but also a J-aggregate red-shift (116 nm). Using this J-aggregate-based FRET method, dye-core–polymer-shell nanoparticles showed two release processes intracellularly: the dissolution of the dye aggregates into dye molecules and the release of the dye molecules from the polymer shell. Also, the high-dye-loading nanoparticles (50 wt %) exhibited a slow release kinetics in serum and relatively quick release in cells, demonstrating their great potential in drug delivery. 相似文献
948.
Yi-Fan Wang Yiyu Liang Yan-Fang Wu Jian Yang Xu Zhang Dr. Dandan Cai Dr. Xu Peng Dr. Mohamedally Kurmoo Prof. Dr. Ming-Hua Zeng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13334-13339
The in situ tracking of the pyrolysis of a binary molecular cluster [Zn7(μ3-CH3O)6(L)6][ZnLCl2]2 is presented with one brucite disk and two mononuclear fragments (L=mmimp: 2-methoxy-6-((methylimino)-methyl)phenolate) to porous carbon using TG-MS from 30 to 900 °C. Following up the spilled gas product during the decomposed reaction of zinc cluster along the temperature rising, and in conjunction with XRD, SEM, BET and other materials characterization, where three key steps were observed: 1) cleavage of the bulky external ligand; 2) reduction of ZnO and 3) volatilization of Zn. The real-time-dependent phase-sequential evolution of the remaining products and the processing of pore forming template transformation are proposed simultaneously. The porous carbon structure featuring a uniform nano-sized pore distribution synthesized at 900 °C with the highest surface area of 1644 m2 g−1 and pore volume of 0.926 cm3 g−1 exhibits the best known capacitance of 662 F g−1 at 0.5 A g−1. 相似文献
949.
Dr. Xueting Pan Dr. Weiwei Wang Dr. Zhijun Huang Shuang Liu Juan Guo Fengrong Zhang Hongjun Yuan Xin Li Prof. Fengyong Liu Prof. Huiyu Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13659-13663
The high reactive oxygen species (ROS) generation ability and simple construction of sonosensitizer systems remain challenging in sonodynamic therapy against the hypoxic tumor. In this work, we rationally prepared MOF-derived double-layer hollow manganese silicate nanoparticle (DHMS) with highly effective ROS yield under ultrasound irradiation for multimodal imaging-guided sonodynamic therapy (SDT). The presence of Mn in DHMS increased ROS generation efficiency because it could be oxidized by holes to improve the electron–hole separation. Moreover, DHMS could produce oxygen in the tumor microenvironment, which helps overcome the hypoxia of the solid tumor and thus enhance the treatment efficiency. In vivo experiments demonstrated efficient tumor inhibition in DHMS-mediated SDT guided by ultrasound and magnetic resonance imaging. This work presents a MOF-derived nanoparticle with sonosensitive and oxygen generating ability, which provides a promising strategy for tumor hypoxia in SDT. 相似文献
950.
Bastien Delayre Dr. Cyril Piemontesi Dr. Qian Wang Prof. Dr. Jieping Zhu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):14094-14101
2,3,3-Trisubstituted indolenine constitutes an integral part of many biologically important monoterpene indole alkaloids. We report herein an unprecedented access to this skeleton by a TiCl3-mediated reductive cyclization of tetrasubstituted alkenes bearing a 2-nitrophenyl substituent. The proof of concept is demonstrated firstly by accomplishing a concise total synthesis of (+)-1,2-dehydroaspidospermidine featuring a late-stage application of this key transformation. A sequence of reduction of nitroarene to nitrosoarene followed by 6π-electron-5-atom electrocyclization and a 1,2-alkyl shift of the resulting nitrone intermediate was proposed to account for the reaction outcome. A subsequent total synthesis of (+)-condyfoline not only illustrates the generality of the reaction, but also provides a mechanistic insight into the nature of the 1,2-alkyl shift. The exclusive formation of (+)-condyfoline indicates that the 1,2-alkyl migration follows a concerted Wagner–Meerwein pathway, rather than a stepwise retro-Mannich/Mannich reaction sequence. Conditions for almost quantitative conversion of (+)-condyfoline to (−)-tubifoline by way of a retro-Mannich/1,3-prototropy/transannular cyclization cascade are also documented. 相似文献