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1.
Long Yang Ralf Steinbock Alexej Scheremetjew Rositha Kuniyil Lars H. Finger Antonis M. Messinis Lutz Ackermann 《Angewandte Chemie (International ed. in English)》2020,59(27):11130-11135
A ruthenium‐catalyzed electrochemical dehydrogenative annulation reaction of imidazoles with alkynes has been established, enabling the preparation of various bridgehead N‐fused [5,6]‐bicyclic heteroarenes through regioselective electrochemical C?H/N?H annulation without chemical metal oxidants. Novel azaruthenabicyclo[3.2.0]heptadienes were fully characterized and identified as key intermediates. Mechanistic studies are suggestive of an oxidatively induced reductive elimination pathway within a ruthenium(II/III) regime. 相似文献
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Kuniyil Prabhakaran Birgit Schwenzer Steven P. DenBaars 《Applied Surface Science》2007,253(10):4773-4776
Nanoparticles of gallium nitride, synthesized by a low-temperature reaction between triethyl gallium and ammonia, were introduced onto silicon wafers containing a thin layer of chemically prepared silicon dioxide. At room temperature, the nanoparticles form unstructured agglomerates on the surface. However, upon annealing the samples beyond the decomposition temperature of the silicon dioxide layer, the gallium nitride particles self-organize to form triangular structures. The pattern formation is attributed to the domain separation associated with the (1 × 1)-(7 × 7) surface phase transformation followed by selective incorporation of the nanoparticles. 相似文献
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Mlanie M. Lorion Nikolaos Kaplaneris Jongwoo Son Rositha Kuniyil Lutz Ackermann 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(6):1698-1702
Bioorthogonal late‐stage diversification of structurally complex peptides has enormous potential for drug discovery and molecular imaging. In recent years, transition‐metal‐catalyzed C?H activation has emerged as an increasingly viable tool for peptide modification. Despite major accomplishments, these strategies largely rely on expensive palladium catalysts. We herein report an unprecedented cobalt(III)‐catalyzed peptide C?H activation, which enables the direct C?H functionalization of structurally complex peptides, and sets the stage for a multicatalytic C?H activation/alkene metathesis/hydrogenation strategy for the assembly of novel cyclic peptides. 相似文献
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Syed Farooq Adil Mohamed E. Assal Mohammed Rafi Shaik Mufsir Kuniyil Azhar Hashmi Mujeeb Khan Aslam Khan Muhammad Nawaz Tahir Abdulrahman Al-Warthan Mohammed Rafiq H. Siddiqui 《应用有机金属化学》2020,34(8):e5718
Graphene–metal nanocomposites have been found to remarkably enhance the catalytic performance of metal nanoparticle-based catalysts. In continuation of our previous report, in which highly reduced graphene oxide (HRG)-based nanocomposites were synthesized and evaluated, we present nanocomposites of graphene oxide (GRO) and ZnO nanoparticle-doped MnCO3 ([ZnO–MnCO3/(1%)GRO]) synthesized via a facile, straightforward co-precipitation technique. Interestingly, it was noticed that the incorporation of GRO in the catalytic system could noticeably improve the catalytic efficiency compared to a catalyst (ZnO–MnCO3) without GRO, for aerial oxidation of benzyl alcohol (BzOH) employing O2 as a nature-friendly oxidant under base-free conditions. The impacts of various reaction factors were thoroughly explored to optimize reaction conditions using oxidation of BzOH to benzaldehyde (BzH) as a model substrate. The catalysts were characterized using X-ray diffraction, thermogravimetric analysis, Fourier transform infrared spectroscopy, field-emission scanning electron microscopy, Energy dispersive X-ray spectroscopy (EDX), Brunauer-Emmett-Teller (BET), and Raman spectroscopy. The (1%)ZnO–MnCO3/(1%)GRO exhibited significant specific activity (67 mmol.g−1.hr−1) with full convversion of BzOH and >99% BzH selectivity within just 6 min. The catalytic efficiency of the (1%)ZnO–MnCO3/(1%)GRO nanocomposite was significantly better than the (1%)ZnO–MnCO3/(1%)HRG and (1%)ZnO–MnCO3 catalysts, presumably due to the existence of oxygen-possessing groups on the GRO surface and as well as a very high surface area that could have been instrumental in uniformly dispersing the active sites of the catalyst, i.e., ZnO–MnCO3. Under optimum circumstances, various kinds of alcohols were selectively transformed to respective carbonyls with full convertibility over the (1%)ZnO–MnCO3/(1%)GRO catalyst. Furthermore, the highly effective (1%)ZnO–MnCO3/(1%)GRO catalyst could be successfully reused and recycled over five consecutive runs with a marginal reduction in its performance and selectivity. 相似文献
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Dr. Matteo Virelli Wei Wang Dr. Rositha Kuniyil Jun Wu Prof. Dr. Giuseppe Zanoni Dr. Antonio Fernandez Jamie Scott Dr. Marc Vendrell Prof. Dr. Lutz Ackermann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(55):12712-12718
Arylated cyclobutanes were accessed by a versatile palladium-catalyzed secondary C(sp3)−H activation, exploiting chelation assistance by modular triazoles. The C−H arylation led to cyclobutane natural product derivatives in a highly regioselective fashion, setting the stage for the easy access to novel fluorogenic boron-dipyrrin (BODIPY)-labeled probes for live-cell imaging. 相似文献
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Dr. Qingqing Bu Dr. Rositha Kuniyil Zhigao Shen Dr. Elżbieta Gońka Prof. Dr. Lutz Ackermann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(69):16450-16454
C−H hydroxylation of aryl acetamides and alkyl phenylacetyl esters was accomplished via challenging distal weak O-coordination by versatile ruthenium(II/IV) catalysis. The ruthenium(II)-catalyzed C−H oxygenation of aryl acetamides proceeded through C−H activation, ruthenium(II/IV) oxidation and reductive elimination, thus providing step-economical access to valuable phenols. The p-cymene-ruthenium(II/IV) manifold was established by detailed experimental and DFT-computational studies. 相似文献
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Isaac Choi Valentin Müller Dr. Yanhui Wang Dr. Kai Xue Dr. Rositha Kuniyil Dr. Loren B. Andreas Dr. Volker Karius Dr. Johan G. Alauzun Prof. Dr. Lutz Ackermann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(66):15290-15297
We disclose the unprecedented hybrid-ruthenium catalysis for distal meta-C−H activation. The hybrid-ruthenium catalyst was recyclable, as was proven by various heterogeneity tests, and fully characterized with various microscopic and spectroscopic techniques, highlighting the physical and chemical stability. Thereby, the hybrid-ruthenium catalysis proved broadly applicable for meta-C−H alkylations of among others purine-based nucleosides and natural product conjugates. Additionally, its versatility was further reflected by meta-C−H activations through visible-light irradiation, as well as para-selective C−H activations. 相似文献
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Dr. Jicheng Wu Peijing Jia Dr. Rositha Kuniyil Dr. Peng Liu Prof. Dr. Weiping Tang 《Angewandte Chemie (International ed. in English)》2023,62(39):e202307144
Chemical synthesis of glycoconjugates is essential for studying the biological functions of carbohydrates. We herein report an efficient approach for the stereoselective synthesis of challenging α-linked glycoconjugates via a RhII/chiral phosphoric acid (CPA)-cocatalyzed dynamic kinetic anomeric O-alkylation of sugar-derived lactols via carbenoid insertion to the anomeric OH bond. Notably, we observed excellent anomeric selectivity, excellent diastereoselectivity, broad substrate scope, and high efficiency for this glycosylation reaction by exploring various parameters of the cocatalytic system. DFT calculations suggested that the anomeric selectivity was mainly determined by steric interactions between the C2-carbon of the carbohydrate and the phenyl group of the metal carbenoid, while π/π interactions with the C2−OBn substituent on the carbohydrate substrate play a significant role for diastereoselectivity at the newly generated stereogenic center. 相似文献