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121.
Dr. Benjamin M. Partridge Jorge Solana González Prof. Hon Wai Lam 《Angewandte Chemie (International ed. in English)》2014,53(25):6523-6527
1,4‐Metal migrations enable the remote functionalization of C? H bonds, and have been utilized in a wide variety of valuable synthetic methods. The vast majority of existing examples involve the 1,4‐migration of palladium or rhodium. Herein, the stereoselective synthesis of complex polycycles by the iridium‐catalyzed arylative cyclization of alkynones with arylboronic acids is described. To our knowledge, these reactions involve the first reported examples of 1,4‐iridium migration. 相似文献
122.
Marcel Scheepstra Dr. Lidia Nieto Dr. Anna K. H. Hirsch Dr. Sascha Fuchs Dr. Seppe Leysen Chan Vinh Lam Leslie in het Panhuis Prof. Dr. Constant A. A. van Boeckel Dr. Hans Wienk Prof. Dr. Rolf Boelens Dr. Christian Ottmann Dr. Lech‐Gustav Milroy Prof. Dr. Luc Brunsveld 《Angewandte Chemie (International ed. in English)》2014,53(25):6443-6448
123.
Synthesis of Two‐Dimensional Transition‐Metal Phosphates with Highly Ordered Mesoporous Structures for Lithium‐Ion Battery Applications
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Dan Yang Dr. Ziyang Lu Dr. Xianhong Rui Xiao Huang Dr. Hai Li Dr. Jixin Zhu Wenyu Zhang Prof. Yeng Ming Lam Prof. Huey Hoon Hng Prof. Hua Zhang Prof. Qingyu Yan 《Angewandte Chemie (International ed. in English)》2014,53(35):9352-9355
Materials with ordered mesoporous structures have shown great potential in a wide range of applications. In particular, the combination of mesoporosity, low dimensionality, and well‐defined morphology in nanostructures may exhibit even more attractive features. However, the synthesis of such structures is still challenging in polar solvents. Herein, we report the preparation of ultrathin two‐dimensional (2D) nanoflakes of transition‐metal phosphates, including FePO4, Mn3(PO4)2, and Co3(PO4)2, with highly ordered mesoporous structures in a nonpolar solvent. The as‐obtained nanoflakes with thicknesses of about 3.7 nm are constructed from a single layer of parallel‐packed pore channels. These uniquely ordered mesoporous 2D nanostructures may originate from the 2D assembly of cylindrical micelles formed by the amphiphilic precursors in the nonpolar solvent. The 2D mesoporous FePO4 nanoflakes were used as the cathode for a lithium‐ion battery, which exhibits excellent stability and high rate capabilities. 相似文献
124.
Catalytic 1,4‐Rhodium(III) Migration Enables 1,3‐Enynes to Function as One‐Carbon Oxidative Annulation Partners in CH Functionalizations
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Dr. David J. Burns Prof. Hon Wai Lam 《Angewandte Chemie (International ed. in English)》2014,53(37):9931-9935
1,3‐Enynes containing allylic hydrogens cis to the alkyne are shown to act as one‐carbon partners, rather than two‐carbon partners, in various rhodium‐catalyzed oxidative annulations. The mechanism of these unexpected transformations is proposed to occur through double C? H activation, involving a hitherto rare example of the 1,4‐migration of a RhIII species. This phenomenon is general across a variety of substrates, and provides a diverse range of heterocyclic products. 相似文献
125.
The Isomerization of Allylrhodium Intermediates in the Rhodium‐Catalyzed Nucleophilic Allylation of Cyclic Imines
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Hamish B. Hepburn Prof. Hon Wai Lam 《Angewandte Chemie (International ed. in English)》2014,53(43):11605-11610
Allylrhodium species generated from potassium allyltrifluoroborates can undergo isomerization by 1,4‐rhodium(I) migration to give more complex isomers, which then react with cyclic imines to provide products with up to three new stereochemical elements. High enantioselectivities are obtained using chiral diene–rhodium complexes. 相似文献
126.
Dr. Weihui Ou Dr. Binbin Zhou Junda Shen Dr. Tsz Wing Lo Prof. Dangyuan Lei Dr. Shengliang Li Jing Zhong Prof. Yang Yang Li Prof. Jian Lu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(17):6856-6859
Hot carriers (HCs) and thermal effects, stemming from plasmon decays, are crucial for most plasmonic applications. However, quantifying these two effects remains extremely challenging due to the experimental difficulty in accurately measuring the temperature at reaction sites. Herein, we provide a novel strategy to disentangle HCs from photothermal effects based on the different traits of heat dissipation (long range) and HCs transport (short range), and quantitatively uncover the dominant and potential-dependent role of photothermal effect by investigating the rapid- and slow-response currents in plasmon-mediated electrochemistry at nanostructured Ag electrode. Furthermore, the plasmoelectric surface potential is found to contribute to the rapid-response currents, which is absent in the previous studies. 相似文献
127.
Dr. Yuanyuan Li Dr. Shunjie Liu Huwei Ni Haoke Zhang Dr. Hequn Zhang Clarence Chuah Chao Ma Prof. Kam Sing Wong Prof. Jacky W. Y. Lam Prof. Ryan T. K. Kwok Prof. Jun Qian Prof. Xuefeng Lu Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(31):12922-12926
The traditional design strategies for highly bright solid-state luminescent materials rely on weakening the intermolecular π–π interactions, which may limit diversity when developing new materials. Herein, we propose a strategy of tuning the molecular packing mode by regioisomerization to regulate the solid-state fluorescence. TBP-e-TPA with a molecular rotor in the end position of a planar core adopts a long-range cofacial packing mode, which in the solid state is almost non-emissive. By shifting molecular rotors to the bay position, the resultant TBP-b-TPA possesses a discrete cross packing mode, giving a quantum yield of 15.6±0.2 %. These results demonstrate the relationship between the solid-state fluorescence efficiency and the molecule's packing mode. Thanks to the good photophysical properties, TBP-b-TPA nanoparticles were used for two-photon deep brain imaging. This molecular design philosophy provides a new way of designing highly bright solid-state fluorophores. 相似文献
128.
Steffen M. Brülls Dr. Valentina Cantatore Zhenping Wang Dr. Pui Lam Tam Dr. Per Malmberg Jessica Stubbe Prof. Dr. Biprajit Sarkar Prof. Dr. Itai Panas Prof. Dr. Jerker Mårtensson Prof. Dr. Siegfried Eigler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6694-6702
Hybridizing graphene and molecules possess a high potential for developing materials for new applications. However, new methods to characterize such hybrids must be developed. Herein, the wet-chemical non-covalent functionalization of graphene with cationic π-systems is presented and the interaction between graphene and the molecules is characterized in detail. A series of tricationic benzimidazolium salts with various steric demand and counterions was synthesized, characterized and used for the fabrication of graphene hybrids. Subsequently, the doping effects were studied. The molecules are adsorbed onto graphene and studied by Raman spectroscopy, XPS as well as ToF-SIMS. The charged π-systems show a p-doping effect on the underlying graphene. Consequently, the tricationic molecules are reduced through a partial electron transfer process from graphene, a process which is accompanied by the loss of counterions. DFT calculations support this hypothesis and the strong p-doping could be confirmed in fabricated monolayer graphene/hybrid FET devices. The results are the basis to develop sensor applications, which are based on analyte/molecule interactions and effects on doping. 相似文献
129.
Wenhan Xu Michelle M. S. Lee Jing‐Jun Nie Zhihan Zhang Ryan T. K. Kwok Jacky W. Y. Lam Fu‐Jian Xu Dong Wang Ben Zhong Tang 《Angewandte Chemie (International ed. in English)》2020,59(24):9610-9616
Photodynamic therapy (PDT) has long been shown to be a powerful therapeutic modality for cancer. However, PDT is undiversified and has become stereotyped in recent years. Exploration of distinctive PDT methods is thus highly in demand but remains a severe challenge. Herein, an unprecedented 1+1+1>3 synergistic strategy is proposed and validated for the first time. Three homologous luminogens with aggregation‐induced emission (AIE) characteristics were rationally designed based on a simple backbone. Through slight structural tuning, these far‐red/near‐infrared AIE luminogens are capable of specifically anchoring to mitochondria, cell membrane, and lysosome, and effectively generating reactive oxygen species (ROS). Notably, biological studies demonstrated combined usage of three AIE photosensitizers gives multiple ROS sources simultaneously derived from several organelles, which gives superior therapeutic effect than that from a single organelle at the same photosensitizers concentration. This strategy is conceptually and operationally simple, providing an innovative approach and renewed awareness of improving therapeutic effect through three‐pronged PDT. 相似文献
130.
Wing Ying Chow Brendan P. Norman Norman B. Roberts Lakshminarayan R. Ranganath Christian Teutloff Robert Bittl Melinda J. Duer James A. Gallagher Hartmut Oschkinat 《Angewandte Chemie (International ed. in English)》2020,59(29):11937-11942
Alkaptonuria (AKU) is a rare disease characterized by high levels of homogentisic acid (HGA); patients suffer from tissue ochronosis: dark brown pigmentation, especially of joint cartilage, leading to severe early osteoarthropathy. No molecular mechanism links elevated HGA to ochronosis; the pigment's chemical identity is still not known, nor how it induces joint cartilage degradation. Here we give key insight on HGA‐derived pigment composition and collagen disruption in AKU cartilage. Synthetic pigment and pigmented human cartilage tissue both showed hydroquinone‐resembling NMR signals. EPR spectroscopy showed that the synthetic pigment contains radicals. Moreover, we observed intrastrand disruption of collagen triple helix in pigmented AKU human cartilage, and in cartilage from patients with osteoarthritis. We propose that collagen degradation can occur via transient glycyl radicals, the formation of which is enhanced in AKU due to the redox environment generated by pigmentation. 相似文献