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81.
Self‐assembly of a resorcin[4]arene‐based ligand (TMR4A) with metal salts and H3PMo12O40·xH2O offers two isostructural complexes, namely, [Ni2Cl(TMR4A)2(CH3CN)2]·[PMo12O40]·4CH3CN ( 1 ) and [Co2Cl(TMR4A)2(CH3CN)2]·[PMo12O40]·4CH3CN ( 2 ). In both 1 and 2 , one Cl? anion bridges two metal cations, and each metal cation is further chelated by four 2‐mercaptopyridine N‐oxide groups of one TMR4A, producing a [M2Cl(TMR4A)2]3+ dimer (M = Ni or Co). The negative [PMo12O40]3? as a counter‐anion balances the positive charge. Markedly, 1 and 2 exhibit high stability in aqueous solutions with different pH values and in organic solvents. Remarkably, the efficient heterogeneous catalytic capability for oxidative desulfurization was studied by suing 1 and 2 as recycled catalysts. Moreover, the electrochemical behaviors of the two compounds were discussed as well. 相似文献
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84.
Yong Xia Armido Studer 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(29):9941-9945
The diversity‐oriented desulfonylative functionalization of alkyl allyl sulfones with various sulfone‐type reagents by radical chemistry has been developed. The readily installed allylsulfonyl moiety acts as a C‐radical precursor, which is substituted by various functionalities using sulfur‐based radical trapping reagents. The generality of this approach is documented by the successful desulfonylative alkynylation, azidation, trifluoromethylthiolation, sulfenylation, trifluoromethylselenylation, halogenation, and deuteration. The method is compatible with a wide range of functional groups. Considering the deuteration, products are obtained in good yields with a high level of deuterium incorporation. 相似文献
85.
Fang Chen Hongwei Huang Lin Guo Yihe Zhang Tianyi Ma 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(30):10164-10176
Semiconductor photocatalysis as a desirable technology shows great potential in environmental remediation and renewable energy generation, but its efficiency is severely restricted by the rapid recombination of charge carriers in the bulk phase and on the surface of photocatalysts. Polarization has emerged as one of the most effective strategies for addressing the above‐mentioned issues, thus effectively promoting photocatalysis. This review summarizes the recent advances on improvements of photocatalytic activity by polarization‐promoted bulk and surface charge separation. Highlighted is the recent progress in charge separation advanced by different types of polarization, such as macroscopic polarization, piezoelectric polarization, ferroelectric polarization, and surface polarization, and the related mechanisms. Finally, the strategies and challenges for polarization enhancement to further enhance charge separation and photocatalysis are discussed. 相似文献
86.
Xuan B. Nguyen Yuji Nakano Nisharnthi M. Duggan Lydia Scott Martin Breugst David W. Lupton 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(33):11607-11614
Direct polarity inversion of conjugate acceptors provides a valuable entry to homoenolates. N‐heterocyclic carbene (NHC) catalyzed reactions, in which β‐unsubstituted conjugate acceptors undergo homoenolate formation and C?C bond formation twice, have been developed. Specifically, the all‐carbon (5+1) annulations give a range of mono‐ and bicyclic cyclohexanones (31 examples). In the first family of annulations, β‐unsubstituted acrylates tethered to a divinyl ketone undergo cycloisomerization, providing hexahydroindenes and tetralins. In the second, partially untethered substrates undergo an intermolecular (5+1) annulation involving dimerization followed by cycloisomerization. While enantioselectivity was not possible with the former, the latter proved viable, allowing cyclohexanones to be produced with high levels of enantiopurity (most >95:5 e.r.) and exclusive diastereoselectivity (>20:1 d.r.). Derivatizations and mechanistic studies are also reported. 相似文献
87.
88.
Let K and S be locally compact Hausdorff spaces and let X be a strictly convex Banach space of finite dimension at least 2. In this paper, we prove that if there exists an isomorphism T from onto satisfying then K and S are homeomorphic. Here denotes the Schäffer constant of X. Even for the classical cases , and , this result is the X‐valued Banach–Stone theorem via isomorphism with the largest distortion that is known so far, namely . On the other hand, it is well known that this result is not true for , even though K and S are compact Hausdorff spaces. 相似文献
89.
Waleed A. El‐Said Mona A. Abdel‐Rahman Eman M. Sayed Aboel‐Magd A. Abdel‐Wahab 《Electroanalysis》2019,31(5):829-837
Here, we reported on a one‐step fabrication of magnetite Fe3O4 nanoparticles/indium tin oxide (ITO) electrode based on the direct growing of Fe3O4 nanoparticles on the ITO surface by using a solvothermal process. The modified electrode was used as electrochemical methotrexate (MTX) biosensor with high sensitivity based on cyclic voltammetry and square wave voltammetry techniques. The results demonstrated a linear relationship between the MTX concentration and its oxidation current peak over a wide range from 10?5 to 10?14 mole/L with a limit of detection of 0.4×10?15 M based on the square wave voltammetry (SWV) technique. In addition, Fe3O4/ITO electrode showed a good capability for measuring very low concentrations of MTX drug dissolved in human serum solution. Also, Fe3O4/ITO electrode was used for detecting MTX in blood serum samples collected from patients after their treatment with MTX. The prepared electrode showed the higher sensitivity that higher than the Viva‐E instrument, which opens the door for developing a cheap, simple and higher sensitive MTX sensor. 相似文献
90.
Upon activation with diethylaluminium chloride (Et2AlCl), a series of phenyl‐substituted α‐diimine nickel precatalysts conducted 4‐methyl‐1‐pentene (4MP) and ethylene (E) (co)polymerizations via controlled chain‐walking to generate branched amorphous polymers with high molecular weight and narrow molecular weight distribution (Mw/Mn < 1.6). The obtained poly(4MP)s were amorphous elastomers with glass transition temperature (Tg) of ?10 ~ ?24 °C, which are higher than that of E‐4MP copolymer ( ? 63.0 °C). At room temperature (25 °C), 4MP polymerization proceeds in a living manner. The microstructures of the produced poly(4MP)s indicated the 2,1‐ and 1,2‐insertion followed by chain‐walking, the latter being predominant. The NMR analyses of the polymers showed that the obtained poly(4MP) possessed methyl, isobutyl, 2,4‐dimethylpentyl and 2‐methylhexyl groups, while the isobutyl and 2,4‐dimethylalkyl branches derived from 4MP were observed in the E‐4MP copolymer. The branch structures and the insertion‐type of monomer were depended on the polymerization temperature, and the content of methyl branch increased with an increase in the polymerization temperature. 相似文献