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1.
[structure: see text] Platinum(II) terpyridyl acetylide complex (1) was incorporated into Nafion membranes as a photosensitizer, and the Nafion was immersed in an aqueous or organic solution of 7-dehydrocholesterol, alpha-pinene, or cyclopentadiene. This photosensitizer system can generate singlet oxygen ((1)O(2)) in high quantum yield to oxidize the alkenes in the solution outside the Nafion and can be easily removed from the reaction vessel at the end of the photooxidation. 相似文献
2.
Photosensitized oxidation of trialkylalkenes 2-methyl-2-pentene (1), 1-methylcyclohexene (2), trans-3-methyl-2-pentene (3), cis-3-methyl-2-pentene (4), and 2-methyl-2-butene (5) included in the internal framework of Na-ZSM-5 zeolites was investigated. The zeolite samples having adsorbed the alkenes were suspended in isooctane, and the sensitizer, tetraphenylporphyrin (TPP), was dissolved in the solution. Singlet oxygen produced in the solution diffused into the internal framework of the zeolites and reacted with alkenes. For all the substrates studied, the ene-type allylic hydroperoxides were obtained in a highly regioselective manner. The regiochemistry for 1-4 in favor of the allylic hydrogen abstraction from the largest substituents is in contrast to their photooxidation within the dye-supported zeolite Na-Y, where the secondary hydroperoxides are preferentially produced. The tight confinement of the alkenes within the narrow channels of the ZSM-5 zeolites is likely to be responsible for this selectivity. 相似文献
3.
Rakesh Kumar Gupta Li Li Zhi Wang Bao-Liang Han Lei Feng Zhi-Yong Gao Chen-Ho Tung Di Sun 《Chemical science》2023,14(5):1138
Precise control over the shape and size of metal nanoclusters through anion template-driven self-assembly is one of the key scientific goals in the nanocluster community, however, it is still not understood comprehensively. In this work, we report the controllable synthesis and atomically precise structures of silver nanowheels Ag37 and Ag46, using homo (Cl− ions) and heteroanion (Cl− and CrO42− ions) template strategies, along with macrocyclic p-phenyl-thiacalix[4]arene and small iPrS− ligands. Structural analyses revealed that in Ag37, Cl− ions serve as both local and global templates, whereas CrO42− ions function as local and Cl− ions as global templates in Ag46, resulting in a pentagonal nanowheel (Ag37) and a hexagonal (Ag46) nanowheel. The larger ionic size and more negative charges of CrO42− ions than Cl− ions offer more coordination sites for the silver atoms and are believed to be the key factors that drive the nanowheel core to expand significantly. Also, by taking advantage of the deep cavity of thiacalix[4]arene with an extended phenyl group, Ag46 has been used as a host material for dye adsorption depending on the charge and size of organic dyes. The successful use of heteroanions to control the expansion of well-defined silver nanowheels fills the knowledge gap in understanding the directing role of heteroanions in dictating the shape and size of nanoclusters at the atomic level.A heteroanion self-assembly strategy for regulating the shape and expanding the size of the silver cluster from Ag37 to Ag46 with a macrocyclic (p-phenyl-thiacalix[4]arene) ligand has been presented. 相似文献
4.
Xiang-Zhu Wei Tian-Yu Ding Dr. Yang Wang Dr. Bing Yang Dr. Qing-Qing Yang Prof. Dr. Shengfa Ye Prof. Dr. Chen-Ho Tung Prof. Dr. Li-Zhu Wu 《Angewandte Chemie (International ed. in English)》2023,62(36):e202308192
High-valent iron-oxo species are appealing for conducting O−O bond formation for water oxidation reactions. However, their high reactivity poses a great challenge to the dissection of their chemical transformations. Herein, we introduce an electron-rich and oxidation-resistant ligand, 2-[(2,2′-bipyridin)-6-yl]propan-2-ol to stabilize such fleeting intermediates. Advanced spectroscopies and electrochemical studies demonstrate a high-valent FeV(O) species formation in water. Combining kinetic and oxygen isotope labelling experiments and organic reactions indicates that the FeV(O) species is responsible for O−O bond formation via water nucleophilic attack under the real catalytic water oxidation conditions. 相似文献
5.
Ya-Hang Wu Prof. Dr. Hongyan Xiao Prof. Dr. Bin Chen Prof. Dr. Richard G. Weiss Prof. Dr. Yu-Zhe Chen Prof. Dr. Chen-Ho Tung Prof. Dr. Li-Zhu Wu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(25):10259-10264
Three rigid and structurally simple heterocyclic stilbene derivatives, (E)-3H,3′H-[1,1′-biisobenzofuranylidene]-3,3′-dione, (E)-3-(3-oxobenzo[c] thiophen-1(3H)-ylidene)isobenzofuran-1(3H)-one, and (E)-3H,3′H-[1,1′-bibenzo[c] thiophenylidene]-3,3′-dione, are found to fluoresce in their neat solid phases, from upper (S2) and lowest (S1) singlet excited states, even at room temperature in air. Photophysical studies, single-crystal structures, and theoretical calculations indicate that large energy gaps between S2 and S1 states (T2 and T1 states) as well as an abundance of intra and intermolecular hydrogen bonds suppress internal conversions of the upper excited states in the solids and make possible the fluorescence from S2 excited states (phosphorescence from T2 excited states). These results, including unprecedented fluorescence quantum yields (2.3–9.6 %) from the S2 states in the neat solids, establish a unique molecular skeleton for achieving multi-colored emissions from upper excited states by “suppressing” Kasha's rule. 相似文献
6.
Xiao-Qin Liu Ke Zhang Prof. Jian-Feng Gao Prof. Yu-Zhe Chen Prof. Chen-Ho Tung Prof. Li-Zhu Wu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):23662-23666
Hypoxia is a parameter related to many diseases. Ratiometric hypoxia probes often rely on a combination of an O2-insensitive fluorophore and an O2-sensitive phosphor in a polymer matrix, which require high cost and multi-step synthesis of transition metal complexes. The two-chromophore hypoxia probes encounter unfavorable energy transfer processes and different stabilities of the chromophores. Reported herein is a pure organic ratiometric hypoxia nanoprobe, assembled by a monochromophore, naphthalimide ureidopyrimidinone (BrNpA-UPy), bridged by a bis-UPy-functionalized benzyl skeleton. The joint factors of quadruple hydrogen bonding, the rigid backbone of UPy, and bromine substitution of the naphthalimide derivative facilitate bright phosphorescence (ΦP=7.7 %, τP=3.2 ms) and fluorescence of the resultant nanoparticles (SNPs) at room temperature, which enable accurate, ratiometric, sensitive oxygen detection (Ksv=189.6 kPa−1) in aqueous solution as well as in living HeLa cells. 相似文献
7.
Rui Guo Xin Zhang Tong Li Qianli Li David A. Ruiz Liu Leo Liu Chen-Ho Tung Lingbing Kong 《Chemical science》2022,13(8):2303
A cationic terminal iminoborane [Mes*N B ← IPr2Me2][AlBr4] (3+[AlBr4]−) (Mes* = 2,4,6-tri-tert-butylphenyl and IPr2Me2 = 1,3-diisopropyl-4,5-dimethylimidazol-2-ylidene) has been synthesized and characterized. The employment of an aryl group and N-heterocyclic carbene (NHC) ligand enables 3+[AlBr4]− to exhibit both B-centered Lewis acidity and BN multiple bond reactivities, thus allowing for the construction of tri-coordinate boron cations 5+–12+. More importantly, initial reactions involving coordination, addition, and [2 + 3] cycloadditions have been observed for the cationic iminoborane, demonstrating the potential to build numerous organoboron species via several synthetic routes.An NHC-stabilized aryliminoboryl cation exhibits both boron-centered Lewis acidity and multiple bond reactivity and could be utilized as an effective synthon for unusual cationic boron species. 相似文献
8.
Dr. Tao Lei Chao Zhou Xiang-Zhu Wei Dr. Bing Yang Prof. Dr. Bin Chen Prof. Dr. Chen-Ho Tung Prof. Dr. Li-Zhu Wu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(3):879-884
[2+2] Photocycloaddition of two olefins is a general method to assemble the core scaffold, cyclobutane, found in numerous bioactive molecules. A new approach to synthesize cyclobutanes through multicomponent cascade reactions by merging aldol reaction and Witting reaction with visible-light-induced [2+2] cycloaddition is reported. An array of cyclobutanes with high selectivity has been achieved from commercially available aldehydes, ketones (or phosphorus ylide), and olefins with visible-light irradiation of a catalytic amount of (fac-tris(2-phenylpyridinato-C2,N)iridium) ([Ir(ppy)3]) at room temperature. Control experiments and spectroscopic studies revealed that the triplet–triplet energy transfer from the excited [Ir(ppy)3]* to enones, generated in situ from aldehyde and ketone or aldehyde and phosphorus ylide, is responsible for these simple and efficient muticomponent transformations. 相似文献
9.
Photoluminescence with high quantum yield and long lifetime from a triplet metal-to-ligand charge transfer (MLCT) excited state in fluid solution at room temperature has been observed for a series of platinum(II) 4'-p-tolyl-terpyridyl acetylide complexes. 相似文献
10.
[reaction: see text] Water- and methanol-swollen Nafion membranes were used as microreactors to successfully control the photochemical reaction pathway of stilbazole derivatives. Of particular interest is the production of azaphenanthrene (the product not obtainable in homogeneous solution) in high yield under high bulk concentration. 相似文献