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21.
Hetero‐tri‐spin [2p‐3d‐4f] Chain Compounds Based on Nitronyl Nitroxide Lanthanide Metallo‐Ligands: Synthesis,Structure, and Magnetic Properties 下载免费PDF全文
Mei Zhu Peng Hu Yungai Li Xiufeng Wang Prof. Licun Li Prof. Daizheng Liao V. M. L. Durga Prasad Goli Prof. S. Ramasesha Dr. Jean‐Pascal Sutter 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(41):13356-13365
Employing nitronyl nitroxide lanthanide(III) complexes as metallo‐ligands allowed the efficient and highly selective preparation of three series of unprecedented hetero‐tri‐spin (Cu?Ln‐radical) one‐dimensional compounds. These 2p–3d–4f spin systems, namely [Ln3Cu(hfac)11(NitPhOAll)4] (LnIII=Gd 1Gd , Tb 1Tb , Dy 1Dy ; NitPhOAll=2‐(4′‐allyloxyphenyl)‐4,4,5,5‐tetramethylimidazoline‐1‐oxyl‐3‐oxide), [Ln3Cu(hfac)11(NitPhOPr)4] (LnIII=Gd 2Gd , Tb 2Tb , Dy 2Dy , Ho 2Ho , Yb 2Yb ; NitPhOPr=2‐(4′‐propoxyphenyl)‐4,4,5,5‐tetramethyl‐imidazoline‐1‐oxyl‐3‐oxide) and [Ln3Cu(hfac)11(NitPhOBz)4] (LnIII=Gd 3Gd , Tb 3Tb , Dy 3Dy ; NitPhOBz=2‐(4′‐benzyloxyphenyl)‐4,4,5,5‐tetramethyl‐imidazoline‐1‐oxyl‐3‐oxide) involve O‐bound nitronyl nitroxide radicals as bridging ligands in chain structures with a [Cu‐Nit‐Ln‐Nit‐Ln‐Nit‐Ln‐Nit] repeating unit. The dc magnetic studies show that ferromagnetic metal–radical interactions take place in these hetero‐tri‐spin chain complexes, these and the next‐neighbor interactions have been quantified for the Gd derivatives. Complexes 1Tb and 2Tb exhibit frequency dependence of ac magnetic susceptibilities, indicating single‐chain magnet behavior. 相似文献
22.
Visible‐Light‐Induced CS Bond Activation: Facile Access to 1,4‐Diketones from β‐Ketosulfones 下载免费PDF全文
Jun Xuan Zhu‐Jia Feng Prof. Dr. Jia‐Rong Chen Dr. Liang‐Qiu Lu Prof. Dr. Wen‐Jing Xiao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(11):3045-3049
A novel method for the synthesis of 1,4‐diketones from β‐ketosulfones was developed by means of a visible light‐induced C?S bond activation process. Symmetrical and unsymmetrical 1,4‐diketones can be easily prepared in moderate to good yields. 相似文献
23.
3位含有季碳手性中心的吲哚啉并环化合物是一类非常重要的化合物, 广泛存在于各种天然产物和具有生物活性的分子中. 化学家们发展了多种有效的途径来合成这类化合物. 其中以方便易得的吲哚衍生物为起始原料, 利用不对称去芳构化\环化串联的方法最为简单高效, 但多数工作都是从色胺或色醇衍生物出发, 合成二氢吡咯并吲哚啉或二氢呋喃并吲哚啉化合物. 因此, 发展其他类型的吲哚衍生物的不对称去芳构化\环化反应显得非常有必要. 作者课题组发展了手性磷酸催化的吲哚衍生物与甲基乙烯基酮的不对称Michael加成\环化串联反应. 以5 mol% (R)-SPINOL为骨架的手性磷酸(R)-4c为催化剂, 以中等到良好的收率和优秀的对映选择性构建了一系列手性吲哚[2,3-b]并氢化喹啉化合物, 而且该催化体系对于克级规模反应同样能够获得很好的结果. 相似文献
24.
Highly Active Bidirectional Electron Transfer by a Self‐Assembled Electroactive Reduced‐Graphene‐Oxide‐Hybridized Biofilm 下载免费PDF全文
Prof. Yang‐Chun Yong Yang‐Yang Yu Prof. Xinhai Zhang Prof. Hao Song 《Angewandte Chemie (International ed. in English)》2014,53(17):4480-4483
Low extracellular electron transfer performance is often a bottleneck in developing high‐performance bioelectrochemical systems. Herein, we show that the self‐assembly of graphene oxide and Shewanella oneidensis MR‐1 formed an electroactive, reduced‐graphene‐oxide‐hybridized, three‐dimensional macroporous biofilm, which enabled highly efficient bidirectional electron transfers between Shewanella and electrodes owing to high biomass incorporation and enhanced direct contact‐based extracellular electron transfer. This 3D electroactive biofilm delivered a 25‐fold increase in the outward current (oxidation current, electron flux from bacteria to electrodes) and 74‐fold increase in the inward current (reduction current, electron flux from electrodes to bacteria) over that of the naturally occurring biofilms. 相似文献
25.
Catalytic Ethanolysis of Kraft Lignin into High‐Value Small‐Molecular Chemicals over a Nanostructured α‐Molybdenum Carbide Catalyst 下载免费PDF全文
Rui Ma Wenyue Hao Xiaolei Ma Ye Tian Prof. Yongdan Li 《Angewandte Chemie (International ed. in English)》2014,53(28):7310-7315
We report the complete ethanolysis of Kraft lignin over an α‐MoC1?x/AC catalyst in pure ethanol at 280 °C to give high‐value chemicals of low molecular weight with a maximum overall yield of the 25 most abundant liquid products (LP25) of 1.64 g per gram of lignin. The LP25 products consisted of C6–C10 esters, alcohols, arenes, phenols, and benzyl alcohols with an overall heating value of 36.5 MJ kg?1. C6 alcohols and C8 esters predominated and accounted for 82 wt % of the LP25 products. No oligomers or char were formed in the process. With our catalyst, ethanol is the only effective solvent for the reaction. Supercritical ethanol on its own degrades Kraft lignin into a mixture of small molecules and molecular fragments of intermediate size with molecular weights in the range 700–1400, differing in steps of 58 units, which is the weight of the branched‐chain linkage C3H6O in lignin. Hydrogen was found to have a negative effect on the formation of the low‐molecular‐weight products. 相似文献
26.
Jun‐Jie Shen Prof. Shou‐Fei Zhu Dr. Yan Cai Huan Xu Xiu‐Lan Xie Prof. Qi‐Lin Zhou 《Angewandte Chemie (International ed. in English)》2014,53(48):13188-13191
An iron‐catalyzed asymmetric intramolecular cyclopropanation was realized in high yields and excellent enantioselectivity (up to 97 % ee) by using the iron complexes of chiral spiro‐bisoxazoline ligands as catalysts. The superiority of iron catalysts exhibited in this reaction demonstrated the potential abilities of this sustainable metal in asymmetric carbenoid transformation reactions. 相似文献
27.
Chiral Metal–Organic Frameworks Bearing Free Carboxylic Acids for Organocatalyst Encapsulation 下载免费PDF全文
Prof. Yan Liu Dr. Xiaobing Xi Chengcheng Ye Tengfei Gong Zhiwei Yang Prof. Yong Cui 《Angewandte Chemie (International ed. in English)》2014,53(50):13821-13825
Two chiral carboxylic acid functionalized micro‐ and mesoporous metal–organic frameworks (MOFs) are constructed by the stepwise assembly of triple‐stranded heptametallic helicates with six carboxylic acid groups. The mesoporous MOF with permanent porosity functions as a host for encapsulation of an enantiopure organic amine catalyst by combining carboxylic acids and chiral amines in situ through acid–base interactions. The organocatalyst‐loaded framework is shown to be an efficient and recyclable heterogeneous catalyst for the asymmetric direct aldol reactions with significantly enhanced stereoselectivity in relative to the homogeneous organocatalyst. 相似文献
28.
锂离子电池的有机正极材料由于具有比容量高、环境友好和廉价等优点,近年来成为研究的热点.但是,有机电极材料在液态电解液中的溶解流失易导致其容量迅速衰减,严重限制了它们的实际应用.本工作基于聚(甲基丙烯酸酯)/聚乙二醇的准固态电解质,考察了以柱[5]醌为正极的准固态锂二次电池的电化学性能.结果显示,柱[5]醌正极不仅保持了高容量的特性(首次放电容量410 mA h/g),并且循环寿命得到了有效提高.0.2 C下循环100周后,电极的容量保持率为88.5%,显示了柱[5]醌在高比能量准固态锂离子电池中的应用潜力. 相似文献
29.
o‐Fluorination of Aromatic Azides Yields Improved Azido‐Based Fluorescent Probes for Hydrogen Sulfide: Synthesis,Spectra, and Bioimaging 下载免费PDF全文
Chao Wei Runyu Wang Dr. Lv Wei Longhuai Cheng Zhifei Li Prof. Dr. Zhen Xi Prof. Dr. Long Yi 《化学:亚洲杂志》2014,9(12):3586-3592
Hydrogen sulfide (H2S) is an endogenously produced gaseous signaling molecule with multiple biological functions. To visualize the endogenous in situ production of H2S in real time, new coumarin‐ and boron‐dipyrromethene‐based fluorescent turn‐on probes were developed for fast sensing of H2S in aqueous buffer and in living cells. Introduction of a fluoro group in the ortho position of the aromatic azide can lead to a greater than twofold increase in the rate of reaction with H2S. On the basis of o‐fluorinated aromatic azides, fluorescent probes with high sensitivity and selectivity toward H2S over other biologically relevant species were designed and synthesized. The probes can be used to in situ to visualize exogenous H2S and D ‐cysteine‐dependent endogenously produced H2S in living cells, which makes them promising tools for potential applications in H2S biology. 相似文献
30.