共查询到20条相似文献,搜索用时 15 毫秒
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Dr. Devrani Mitra Dr. Hideaki Ogata Prof. Wolfgang Lubitz Brian C. Manor Prof. Thomas B. Rauchfuss Dr. Deborah Byrne Dr. Violaine Bonnefoy Prof. Francis E. Jenney Jr. Prof. Michael W. W. Adams Dr. Yoshitaka Yoda Dr. Ercan Alp Dr. Jiyong Zhao Prof. Stephen P. Cramer 《Angewandte Chemie (International ed. in English)》2013,52(2):724-728
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Dr. Andreas Schneider Dr. Christian Curado Thomas B. Lystbaek Prof. Sílvia Osuna Prof. Bernhard Hauer 《Angewandte Chemie (International ed. in English)》2023,62(22):e202305546
Terpene cyclases offer enormous synthetic potential, given their unique ability to forge complex hydrocarbon scaffolds from achiral precursors within a single cationic rearrangement cascade. Harnessing their synthetic power, however, has proved to be challenging owing to their generally low catalytic performance. In this study, we unveiled the catalytic potential of the squalene-hopene cyclase (SHC) by harnessing its structure and dynamics. First, we synergistically tailored the active site and entrance tunnel of the enzyme to generate a 397-fold improved (−)-ambroxide synthase. Our computational investigations explain how the introduced mutations work in concert to improve substrate acquisition, flow, and chaperoning. Kinetics, however, showed terpene-induced inactivation of the membrane-bound SHC to be the major turnover limitation in vivo. Merging this insight with the improved and stereoselective catalysis of the enzyme, we applied a feeding strategy to exceed 105 total turnovers. We believe that our results may bridge the gap for broader application of SHCs in synthetic chemistry. 相似文献
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Kazuki Inaba Yuna Naito Mina Tachibana Prof. Dr. Kazunobu Toshima Prof. Dr. Daisuke Takahashi 《Angewandte Chemie (International ed. in English)》2023,62(46):e202313773
Regio- and stereoselective formation of the 1,2-cis-furanosidic linkage has been in great demand for efficient synthesis of biologically active natural glycosides. In this study, we developed a regioselective and β-stereospecific d -/l -arabinofuranosylation promoted by a boronic acid catalyst under mild conditions. The glycosylations proceeded smoothly for a variety of diols, triols, and unprotected sugar acceptors to give the corresponding β-arabinofuranosides (β-Arbf) in high yields with complete β-stereoselectivity and high regioselectivity. The regioselectivity was completely reversed depending on the optical isomerism of the donor used and was predictable a priori using predictive models. Mechanistic studies based on DFT calculations revealed that the present glycosylation occurs through a highly dissociative concerted SNi mechanism. The usefulness of the glycosylation method was demonstrated by the chemical synthesis of trisaccharide structures of arabinogalactan fragments. 相似文献
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Cover Picture: Mo2B4O9—Connecting Borate and Metal-Cluster Chemistry (Angew. Chem. Int. Ed. 23/2017)
Martin K. Schmitt Dr. Oliver Janka Prof. Dr. Rainer Pöttgen Dr. Christopher Benndorf Dr. Marcos de Oliveira Jr. Prof. Dr. Hellmut Eckert Dr. Florian Pielnhofer Amadeus-Samuel Tragl Prof. Dr. Richard Weihrich Dr. Bastian Joachim Prof. Dr. Dirk Johrendt Prof. Dr. Hubert Huppertz 《Angewandte Chemie (International ed. in English)》2017,56(23):6345-6345
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