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951.
Jinbo Fei Luru Dai Fuping Gao Jie Zhao Junbai Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(22):7332-7336
Great success has been achieved in recent years in the development of synthetic or assembled nanobiomaterials. Among these, biomolecule‐based nanoarchitectures with special optical property are of particular interest. Here, we demonstrate that vitamin B2 nanocrystals assembled as nanorods can be obtained with precise control. Excitingly, such one‐dimensional nanostructures not only exhibit intrinsic optical waveguiding properties but also the ability to sensitize oxygen to produce reactive oxygen species. With these properties, we applied the obtained vitamin B2 nanorods under remotely localized light illumination into single tumour cells in vitro for anticancer photodynamic therapy. Further, vitamin B2 nanorods were explored for in vivo photodynamic therapy by using a tumour model. With such bionanostructures, new features and functions of vitamin B2 and its derivatives have been developed. 相似文献
952.
Dandan Gao Rongji Liu Johannes Biskupek Ute Kaiser Yu‐Fei Song Carsten Streb 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(14):4692-4696
Electrocatalytic water splitting into H2 and O2 is a key technology for carbon‐neutral energy. Here, we report a modular materials design leading to noble metal‐free composite electrocatalysts, which combine high electrical conductivity, high OER and HER reactivity and high durability. The scalable bottom‐up fabrication allows the stable deposition of mixed metal oxide nanostructures with different functionalities on copper foam electrodes. The composite catalyst shows sustained OER and HER activity in 0.1 m aqueous KOH over prolonged periods (t>10 h) at low overpotentials (OER: ≈300 mV; HER: ≈100 mV) and high faradaic efficiencies (OER: ≈100 %, HER: ≈98 %). The new synthetic concept will enable the development of multifunctional, mixed metal oxide composites as high‐performance electrocatalysts for challenging energy conversion and storage reactions. 相似文献
953.
Kyuho Moon Fei Xu Mohammad R. Seyedsayamdost 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(18):6034-6038
The majority of natural product biosynthetic gene clusters in bacteria are silent under standard laboratory growth conditions, making it challenging to uncover any antibiotics that they may encode. Herein, bioactivity assays are combined with high‐throughput elicitor screening (HiTES) to access cryptic, bioactive metabolites. Application of this strategy in Saccharopolyspora cebuensis, with inhibition of Escherichia coli growth as a read‐out, led to the identification of a novel lanthipeptide, cebulantin. Extensive NMR spectroscopic analysis allowed the elucidation of the structure of cebulantin. Subsequent bioactivity assays revealed it to be an antibiotic selective for Gram‐negative bacteria, especially against Vibrio species. This approach, referred to as bioactivity‐HiTES, has the potential to uncover cryptic metabolites with desired biological activities that are hidden in microbial genomes. 相似文献
954.
Peng‐Fei Dai Xiao‐Shan Ning Hua Wang Xian‐Chao Cui Jie Liu Jian‐Ping Qu Yan‐Biao Kang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(16):5446-5449
Organic chemists now can construct carbon–carbon σ‐bonds selectively and sequentially, whereas methods for the selective cleavage of carbon–carbon σ‐bonds, especially for unreactive hydrocarbons, remain limited. Activation by ring strain, directing groups, or in the presence of a carbonyl or a cyano group is usually required. In this work, by using a sequential strategy site‐selective cleavage and borylation of C(aryl)?CH3 bonds has been developed under directing group free and transition metal free conditions. Methyl groups of various arenes are selectively cleaved and replaced by boryl groups. Mechanistic analysis suggests that it proceeds by a sequential intermolecular oxidation and coupling of a transient aryl radical, generated by radical decarboxylation, involving a pyridine‐stabilized persistent boryl radical. 相似文献
955.
Guang‐Yao Ran Xing‐Xing Yang Jing‐Fei Yue Wei Du Ying‐Chun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(27):9308-9312
An atom‐economic and highly efficient vinylogous umpolung strategy is developed for deconjugated carbonyl compounds, which generate electron‐deficient π‐allylpalladium complexes with Pd(OAc)2 under ligand‐free conditions. In cooperation with a chiral‐phosphonium‐based phase‐transfer catalyst, the asymmetric direct oxidative allylic alkylations of 3‐substituted oxindoles are furnished under O2 atmosphere. The γ‐ or even remote ?‐regioselective alkylation products, with substantial substituents, are delivered with excellent enantioselectivity, and can be further used to access diverse chiral spirocyclic architectures effectively. The Mukaiyama dienol silyl ether can be utilized similarly, indicating that the current active π‐allylpalladium species results from tautomerization of the PdII‐dienolate intermediate. 相似文献
956.
Titas Braukyla Rui Xia Maryte Daskeviciene Tadas Malinauskas Alytis Gruodis Vygintas Jankauskas Zhaofu Fei Cristina Momblona Cristina Roldn‐Carmona Paul J. Dyson Vytautas Getautis Mohammad Khaja Nazeeruddin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(33):11388-11394
The synthesis of three enamine hole‐transporting materials (HTMs) based on Tröger's base scaffold are reported. These compounds are obtained in a three‐step facile synthesis from commercially available materials without the need of expensive catalysts, inert conditions or time‐consuming purification steps. The best performing material, HTM3, demonstrated 18.62 % PCE in PSCs, rivaling spiro‐OMeTAD in efficiency, and showing markedly superior long‐term stability in non‐encapsulated devices. In dopant‐free PSCs, HTM3 outperformed spiro‐OMeTAD by a factror of 1.6. The high glass‐transition temperature (Tg=176 °C) of HTM3 also suggests promising perspectives in device applications. 相似文献
957.
Zhenghui Luo Fei Wu Teng Zhang Xuan Zeng Yiqun Xiao Tao Liu Cheng Zhong Xinhui Lu Linna Zhu Shihe Yang Chuluo Yang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(25):8608-8613
Electron transport materials (ETM) play an important role in the improvement of efficiency and stability for inverted perovskite solar cells (PSCs). This work reports an efficient ETM, named PDI‐C60, by the combination of perylene diimide (PDI) and fullerene. Compared to the traditional PCBM, this strategy endows PDI‐C60 with slightly shallower energy level and higher electron mobility. As a result, the device based on PDI‐C60 as electron transport layer (ETL) achieves high power conversion efficiency (PCE) of 18.6 %, which is significantly higher than those of the control devices of PCBM (16.6 %) and PDI (13.8 %). The high PCE of the PDI‐C60‐based device can be attributed to the more matching energy level with the perovskite, more efficient charge extraction, transport, and reduced recombination rate. To the best of our knowledge, the PCE of 18.6 % is the highest value in the PSCs using PDI derivatives as ETLs. Moreover, the device with PDI‐C60 as ETL exhibits better device stability due to the stronger hydrophobic properties of PDI‐C60. The strategy using the PDI/fullerene hybrid provides insights for future molecular design of the efficient ETM for the inverted PSCs. 相似文献
958.
Li‐Yuan Wu Yan‐Fei Mu Xiao‐Xuan Guo Wen Zhang Zhi‐Ming Zhang Min Zhang Tong‐Bu Lu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(28):9591-9595
Improving the stability of lead halide perovskite quantum dots (QDs) in a system containing water is the key for their practical application in artificial photosynthesis. Herein, we encapsulate low‐cost CH3NH3PbI3 (MAPbI3) perovskite QDs in the pores of earth‐abundant Fe‐porphyrin based metal organic framework (MOF) PCN‐221(Fex) by a sequential deposition route, to construct a series of composite photocatalysts of MAPbI3@PCN‐221(Fex) (x=0–1). Protected by the MOF the composite photocatalysts exhibit much improved stability in reaction systems containing water. The close contact of QDs to the Fe catalytic site in the MOF, allows the photogenerated electrons in the QDs to transfer rapidly the Fe catalytic sites to enhance the photocatalytic activity for CO2 reduction. Using water as an electron source, MAPbI3@PCN‐221(Fe0.2) exhibits a record‐high total yield of 1559 μmol g?1 for photocatalytic CO2 reduction to CO (34 %) and CH4 (66 %), 38 times higher than that of PCN‐221(Fe0.2) in the absence of perovskite QDs. 相似文献
959.
Wan‐Lei Yu Yong‐Chun Luo Lei Yan Dan Liu Zhu‐Yin Wang Peng‐Fei Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(32):11057-11061
A synergistic catalytic method combining photoredox catalysis, hydrogen‐atom transfer, and proton‐reduction catalysis for the dehydrogenative silylation of alkenes was developed. With this approach, a highly concise route to substituted allylsilanes has been achieved under very mild reaction conditions without using oxidants. This transformation features good to excellent yields, operational simplicity, and high atom economy. Based on control experiments, a possible reaction mechanism is proposed. 相似文献
960.
Fei Ye Florian Berger Hao Jia Joseph Ford Alan Wortman Jonas Brgel Christophe Genicot Tobias Ritter 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(41):14757-14761
Incorporation of the CF3 group into arenes has found increasing importance in drug discovery. Herein, we report the first photoredox‐catalyzed cross‐coupling of aryl thianthrenium salts with a copper‐based trifluoromethyl reagent, which enables a site‐selective late‐stage trifluoromethylation of arenes. The reaction proceeds with broad functional group tolerance, even for complex small molecules on gram scale. The method was further extended to produce pentafluoroethylated derivatives. 相似文献