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91.
Silver‐Catalyzed Decarboxylative Trifluoromethylthiolation of Aliphatic Carboxylic Acids in Aqueous Emulsion 下载免费PDF全文
Dr. Feng Hu Xinxin Shao Dianhu Zhu Prof. Dr. Long Lu Prof. Dr. Qilong Shen 《Angewandte Chemie (International ed. in English)》2014,53(24):6105-6109
A silver‐catalyzed decarboxylative trifluoromethylthiolation of secondary and tertiary carboxylic acids under mild conditions tolerates a wide range of functional groups. The reaction was dramatically accelerated by its performance in an aqueous emulsion, which was formed by the addition of sodium dodecyl sulfate to water. It was proposed that the radical, which was generated from the silver‐catalyzed decarboxylation in the “oil‐in‐water” droplets, could easily react with the trifluoromethylthiolating reagent to form the product. 相似文献
92.
Peng-Bo Jin Yuan-Qi Zhai Ke-Xin Yu Prof. Dr. Richard E. P. Winpenny Prof. Dr. Yan-Zhen Zheng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(24):9436-9440
The dicarbollide ion, nido-C2B9H112− is isoelectronic with cyclopentadienyl. Herein, we make dysprosiacarboranes, namely [(C2B9H11)2Ln(THF)2][Na(THF)5] (Ln=Dy, 1Dy ) and [(THF)3(μ-H)3Li]2[{η5-C6H4(CH2)2C2B9H9}Dy{η2:η5-C6H4(CH2)2C2B9H9}2Li] 3Dy and show that dicarbollide ligands impose strong magnetic axiality on the central DyIII ion. The effective energy barrier (Ueff) for the loss of magnetization can be varied by the substitution pattern on the dicarbollide. This finding is demonstrated by comparing complexes of nido-C2B9H112− and nido-[o-xylylene-C2B9H9]2−, which show a Ueff of 430(5) K and 804(7) K, respectively. The blocking temperature defined by the open hysteresis temperature of 3Dy reaches 6.8 K. Moreover, the linear complex [Dy(C2B9H11)2]− is predicted to have comparable properties with the linear [Dy(CpMe3)2]+ complex. As such, carboranyl ligands and their derivatives may provide a new type of organometallic ligand for high-performance single-molecule magnets. 相似文献
93.
Dr. Fei Xu Yixuan Zhai En Zhang Qianhui Liu Guangshen Jiang Xiaosa Xu Yuqian Qiu Prof. Xiaoming Liu Prof. Hongqiang Wang Prof. Stefan Kaskel 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(44):19628-19635
The development of ultrastable carbon materials for potassium storage poses key limitations caused by the huge volume variation and sluggish kinetics. Nitrogen-enriched porous carbons have recently emerged as promising candidates for this application; however, rational control over nitrogen doping is needed to further suppress the long-term capacity fading. Here we propose a strategy based on pyrolysis–etching of a pyridine-coordinated polymer for deliberate manipulation of edge-nitrogen doping and specific spatial distribution in amorphous high-surface-area carbons; the obtained material shows an edge-nitrogen content of up to 9.34 at %, richer N distribution inside the material, and high surface area of 616 m2 g−1 under a cost-effective low-temperature carbonization. The optimized carbon delivers unprecedented K-storage stability over 6000 cycles with negligible capacity decay (252 mA h g−1 after 4 months at 1 A g−1), rarely reported for potassium storage. 相似文献
94.
Guifa Zhai Wenyan Wang Dr. Wei Xu Guo Sun Chaoqun Hu Xiangming Wu Zisong Cong Liang Deng Yanrong Shi Prof. Dr. Peter F. Leadlay Prof. Dr. Heng Song Prof. Dr. Kui Hong Prof. Dr. Zixin Deng Prof. Dr. Yuhui Sun 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22926-22930
The colinearity of canonical modular polyketide synthases, which creates a direct link between multienzyme structure and the chemical structure of the biosynthetic end-product, has become a cornerstone of knowledge-based genome mining. Herein, we report genetic and enzymatic evidence for the remarkable role of an enoylreductase in the polyketide synthase for azalomycin F biosynthesis. This internal enoylreductase domain, previously identified as acting only in the second of two chain extension cycles on an initial iterative module, is shown to also catalyze enoylreduction in trans within the next module. The mechanism for this rare deviation from colinearity appears to involve direct cross-modular interaction of the reductase with the longer acyl chain, rather than back transfer of the substrate into the iterative module, suggesting an additional and surprising plasticity in natural PKS assembly-line catalysis. 相似文献
95.
Adil Anwar Hiba Anwar Takeshi Yamauchi Ryan Tseng Rajesh Agarwal Lawrence D Horwitz Zili Zhai Mayumi Fujita 《Photochemistry and photobiology》2020,96(4):870-876
Ultraviolet B (UVB) radiation is known as a culprit in skin carcinogenesis. We have previously reported that bucillamine (N-[2-mercapto-2-methylpropionyl]-L-cysteine), a cysteine derivative with antioxidant and anti-inflammatory capacity, protects against UVB-induced p53 activation and inflammatory responses in mouse skin. Since MAPK signaling pathways regulate p53 expression and activation, here we determined bucillamine effect on UVB-mediated MAPK activation in vitro using human skin keratinocyte cell line HaCaT and in vivo using SKH-1 hairless mouse skin. A single low dose of UVB (30 mJ cm−2) resulted in increased JNK/MAPK phosphorylation and caspase-3 cleavage in HaCaT cells. However, JNK activation and casaspe-3 cleavage were inhibited by pretreatment of HaCaT cells with physiological doses of bucillamine (25 and 100 µm ). Consistent with these results, bucillamine pretreatment in mice (20 mg kg−1) inhibited JNK/MAPK and ERK/MAPK activation in skin epidermal cells at 6–12 and 24 h, respectively, after UVB exposure. Moreover, bucillamine attenuated UVB-induced Ki-67-positive cells and cleaved caspase-3-positive cells in mouse skin. These findings demonstrate that bucillamine inhibits UVB-induced MAPK signaling, cell proliferation and apoptosis. Together with our previous report, we provide evidence that bucillamine has a photoprotective effect against UV exposure. 相似文献
96.
Qingju Wang Tian Ke Lifeng Yang Zhaoqiang Zhang Xili Cui Zongbi Bao Qilong Ren Qiwei Yang Huabin Xing 《Angewandte Chemie (International ed. in English)》2020,59(9):3423-3428
The separation of xenon/krypton (Xe/Kr) mixture is of great importance to industry, but the available porous materials allow the adsorption of both, Xe and Kr only with limited selectivity. Herein we report an anion‐pillared ultramicroporous material NbOFFIVE‐2‐Cu‐i (ZU‐62) with finely tuned pore aperture size and structure flexibility, which for the first time enables an inverse size‐sieving effect in separation along with record Xe/Kr selectivity and ultrahigh Xe capacity. Evidenced by single‐crystal X‐ray diffraction, the rotation of anions and pyridine rings upon contact of larger‐size Xe atoms adapts cavities to the shape/size of Xe and allows strong host‐Xe interaction, while the smaller‐size Kr is excluded. Breakthrough experiments confirmed that ZU‐62 has a real practical potential for producing high‐purity Kr and Xe from air‐separation byproducts, showing record Kr productivity (206 mL g?1) and Xe productivity (42 mL g?1, in desorption) as well as good recyclability. 相似文献
97.
Ruixiang Qu Xiangyu Li Yanan Liu Huajun Zhai Shuaiheng Zhao Lin Feng Yen Wei 《Angewandte Chemie (International ed. in English)》2020,59(32):13437-13443
Superwetting membranes with responsive properties have attracted heightened attention because of their fine‐tunable surface wettability. However, their functional diversity is severely limited by the “black‐or‐white” wettability transition. Herein, we describe a coating strategy to fabricate multifunctional responsive superwetting membranes with SiO2/octadecylamine patterns. The adjustable patterns in the responsive region are the key factor for functional diversity. Specifically, the coated part of the membrane displayed a superhydrophobicity/superhydrophilicity transition at different pH values, whereas the uncoated part exhibited invariant superhydrophilicity. On the basis of this anisotropy/isotropy transition, the membranes can serve as either responsive permeable membranes or signal‐expression membranes, thus enabling the responsive separation and permeation of liquids with satisfactory separation efficiency (>99.90 %) and flux (ca. 60 L m?2 h), as well as real‐time liquid signal expression with alterable signals. 相似文献
98.
99.
Xiaoxiao Zheng Rongli Zhai Zihao Zhang Baoqing Zhang Jiangwei Liu Aamir Razaq Muhammad Ashfaq Ahmad Rizwan Raza Muhammad Saleem Syed Rizwan Syed Hassan Mujtaba Jafri Hu Li Raffaello Papadakis 《Molecules (Basel, Switzerland)》2022,27(6)
Composite materials and their applications constitute a hot field of research nowadays due to the fact that they comprise a combination of the unique properties of each component of which they consist. Very often, they exhibit better performance and properties compared to their combined building blocks. Graphene oxide (GO), as the most widely used derivative of graphene, has attracted widespread attention because of its excellent properties. Abundant oxygen-containing functional groups on GO can provide various reactive sites for chemical modification or functionalization of GO, which in turn can be used to develop novel GO-based composites. This review outlines the most recent advances in the field of novel dyes and pigments encompassing GO as a key ingredient or as an important cofactor. The interactions of graphene with other materials/compounds are highlighted. The special structure and unique properties of GO have a great effect on the performance of fabricated hybrid dyes and pigments by enhancing the color performance of dyes, the anticorrosion properties of pigments, the viscosity and rheology of inks, etc., which further expands the applications of dyes and pigments in dyeing, optical elements, solar-thermal energy storage, sensing, coatings, and microelectronics devices. Finally, challenges in the current development as well as the future prospects of GO-based dyes and pigments are also discussed. This review provides a reference for the further exploration of novel dyes and pigments. 相似文献
100.
超分子构筑调控合成结构规整的梯形聚合物及其应用研究 总被引:1,自引:1,他引:0
综述了"超分子构筑调控的逐步偶联/聚合法",该方法将高分子化学与超分子化学相结合,利用多种类型的超分子弱键协同作用首先构筑预期的梯形超分子结构,再经聚合得到共价键梯形高分子.利用该方法合成了一系列结构规整的氧桥基和有机桥基梯形聚硅氧烷以及碳基梯形聚酯,并利用侧基间π-π叠加作用实现了对聚合物立体构型控制.扼要介绍了梯形聚合物在先进材料方面的应用,例如梯形聚硅氧烷液晶光致取向膜;由梯形聚硅氧烷合成的管状聚硅氧烷在高室温储存期微电子环氧塑封料方面的应用;以及基于梯形聚硅氧烷的拟筛板聚合物在二阶非线性光学材料方面的应用等. 相似文献