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131.
This paper treats the computational modeling of size dependence in microstructure models of metals. Different gradient crystal plasticity strategies are analyzed and compared. For the numerical implementation, a dual-mixed finite element formulation which is suitable for parallelization is suggested. The paper ends with a representative numerical example for polycrystals. 相似文献
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Martin Peng Esther Mittmann Lukas Wenger Prof. Dr. Jürgen Hubbuch Dr. Martin K. M. Engqvist Prof. Dr. Christof M. Niemeyer Dr. Kersten S. Rabe 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(70):15998-16001
Continuous flow systems for chemical synthesis are becoming a major focus in organic chemistry and there is a growing interest in the integration of biocatalysts due to their high regio- and stereoselectivity. Methods established for 3D bioprinting enable the fast and simple production of agarose-based modules for biocatalytic reactors if thermally stable enzymes are available. We report here on the characterization of four different cofactor-free phenacrylate decarboxylase enzymes suitable for the production of 4-vinylphenol and test their applicability for the encapsulation and direct 3D printing of disk-shaped agarose-based modules that can be used for compartmentalized flow microreactors. Using the most active and stable phenacrylate decarboxylase from Enterobacter spec. in a setup with four parallel reactors and a subsequent palladium(II) acetate-catalysed Heck reaction, 4-hydroxystilbene was synthesized from p-coumaric acid with a total yield of 14.7 % on a milligram scale. We believe that, due to the convenient direct immobilization of any thermostable enzyme and straightforward tuning of the reaction sequence by stacking of modules with different catalytic activities, this simple process will facilitate the establishment and use of cascade reactions and will therefore be of great advantage for many research approaches. 相似文献
135.
Magnus Pfaffenbach Ian Bakanas Nicholas R. O'Connor Jessica L. Herrick Richmond Sarpong 《Angewandte Chemie (International ed. in English)》2019,58(43):15304-15308
Divergent and enantiospecific total syntheses of the indolosesquiterpenoids xiamycins A, C, F, H and oridamycin A have been accomplished. The syntheses, which commence from (R)‐carvone, employ a key photoinduced benzannulation sequence to forge the carbazole moiety characteristic of these natural products. Late‐stage diversification from a common intermediate enabled the first syntheses of xiamycins C and F, and an unexpected one‐pot oxidative decarboxylation, which may prove general, led to xiamycin H. All synthetic intermediates and the natural products were tested for anti‐fungal activity. Xiamycin H emerged as an inhibitor of three agriculturally relevant fungal pathogens. 相似文献
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Dr. Pavlo Nikolaienko Marc Jentsch Dr. Ajit P. Kale Dr. Yunfei Cai Prof. Dr. Magnus Rueping 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(29):7177-7184
A hydrogen atom transfer-directed electrochemical intramolecular C−H amination has been developed in which the N-radical species are generated at the anode, and the base required for the reaction is generated at the cathode. A broad range of valuable pyrrolidines were prepared in good yields and with high chemoselectivity. The reaction was easily scaled up in both batch and continuous flow systems. 相似文献
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Marc Magre Bholanath Maity Alban Falconnet Luigi Cavallo Magnus Rueping 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(21):7099-7103
A magnesium‐catalyzed hydroboration of alkynes providing good yields and selectivities for a wide range of terminal and symmetrical and unsymmetrical internal alkynes has been developed. The compatibility with many functional groups makes this magnesium catalyzed procedure attractive for late stage functionalization. Experimental mechanistic investigations and DFT calculations reveal insights into the reaction mechanism of the magnesium catalyzed protocol. 相似文献